Enhanced In Vitro Antiviral Activity of Ivermectin-Loaded Nanostructured Lipid Carriers against Porcine Epidemic Diarrhea Virus via Improved Intracellular Delivery

✅ 全文

伊维菌素负载纳米结构脂质载体通过改善细胞内递送增强对猪流行性腹泻病毒的体外抗病毒活性

作者 Xiaolin Xu; Shasha Gao; Qindan Zuo; Jiahao Gong; Xinhao Song; Yongshi Liu; Jing Xiao; Xiaofeng Zhai; Haifeng Sun; Mingzhi Zhang; Xiuge Gao; Dawei Guo 期刊 Pharmaceutics 发表日期 2024 卷/期/页码 Vol. 16(5) ISSN 1999-4923 DOI 10.3390/pharmaceutics16050601 类型 原创研究 (Original Research)

📄 英文摘要 English Abstract

EN

Porcine epidemic diarrhea virus (PEDV) is an acute enteric coronavirus, inducing watery diarrhea and high mortality in piglets, leading to huge economic losses in global pig industry. Ivermectin (IVM), an FDA-approved antiparasitic agent, is characterized by high efficacy and wide applicability. However, the poor bioavailability limits its application. Since the virus is parasitized inside the host cells, increasing the intracellular drug uptake can improve antiviral efficacy. Hence, we aimed to develop nanostructured lipid carriers (NLCs) to enhance the antiviral efficacy of IVM. The findings first revealed the capacity of IVM to inhibit the infectivity of PEDV by reducing viral replication with a certain direct inactivation effect. The as-prepared IVM-NLCs possessed hydrodynamic diameter of 153.5 nm with a zeta potential of −31.5 mV and high encapsulation efficiency (95.72%) and drug loading (11.17%). IVM interacted with lipids and was enveloped in lipid carriers with an amorphous state. Furthermore, its encapsulation in NLCs could enhance drug internalization. Meanwhile, IVM-NLCs inhibited PEDV proliferation by up to three orders of magnitude in terms of viral RNA copies, impeding the accumulation of reactive oxygen species and mitigating the mitochondrial dysfunction caused by PEDV infection. Moreover, IVM-NLCs markedly decreased the apoptosis rate of PEDV-induced Vero cells. Hence, IVM-NLCs showed superior inhibitory effect against PEDV compared to free IVM. Together, these results implied that NLCs is an efficient delivery system for IVM to improve its antiviral efficacy against PEDV via enhanced intracellular uptake.

📄 中文摘要 Chinese Abstract

中文
猪流行性腹泻病毒(PEDV)是一种急性肠道冠状病毒,可引发仔猪水样腹泻和高死亡率,给全球养猪业造成巨大经济损失。现有PEDV疫苗包括灭活疫苗和弱毒疫苗,但由于新突变株的不断出现,该病在养猪业中仍频繁发生。面对新发或再发疾病的风险,亟需开发新型抗病毒化合物。药物重定位已成为治疗新兴疾病的一个有吸引力的选择,因为针对特定病原体开发新的有效药物既耗时又昂贵。伊维菌素(IVM)是一种经FDA批准的广谱、高效、低毒的抗寄生虫药物。研究表明,它对病毒具有潜在的治疗效果。然而,IVM在水中的溶解度低(仅6–9微克/毫升),生物利用度差,限制了其临床应用。纳米结构脂质载体(NLCs)是新一代脂质纳米颗粒,由固体脂质和液体脂质混合物组成,可提高所包封生物活性化合物的溶解度、稳定性和生物利用度。

📋 英文结构化总结 English Structured Summary

全文整理

EN

Background:

Porcine epidemic diarrhea virus (PEDV) is an acute enteric coronavirus, inducing watery diarrhea and high mortality in piglets, leading to huge economic losses in the global pig industry. Available PEDV vaccines include inactivated and attenuated vaccines, but these diseases are still frequent in the pig breeding industry, partly due to the emergence of new mutant strains. With the risk of emerging or re-emerging diseases, there is an urgent need to develop new antiviral compounds. Drug repurposing has become an attractive option for treating emerging diseases, as developing new effective drugs against a particular pathogen is time-consuming and expensive. Ivermectin (IVM) is an FDA-approved, broad-spectrum, high-efficiency, low-toxicity antiparasitic drug. Studies have shown that it has potential therapeutic effects against viruses. However, the low solubility of IVM in water (only 6–9 micrograms per milliliter) and the poor bioavailability limit its clinical applications. Nanostructured lipid carriers (NLCs) are a new generation of lipid nanoparticles consisting of a mixture of solid and liquid lipids, enhancing the solubility, stability, and bioavailability of encapsulated bioactive compounds.

Methods:

Ivermectin (IVM, 91%) was purchased from the China Institute of Veterinary Drug Control. African green monkey epithelial cells (Vero) and PEDV strain CV777 were maintained in the laboratory. IVM-NLCs were prepared using the high-shear-ultrasound and high-pressure homogenization methods. A certain amount of oleic acid (OA), palmitic acid (PA), Tween 20, and IVM was mixed as the oil phase and heated up to 70 °C until complete melting. In parallel, poloxamer 188 was dissolved in water as the aqueous phase and heated at the same temperature.

Results:

The findings first revealed the capacity of IVM to inhibit the infectivity of PEDV by reducing viral replication with a certain direct inactivation effect. The as-prepared IVM-NLCs possessed a hydrodynamic diameter of 153.5 nm with a zeta potential of −31.5 mV and high encapsulation efficiency (95.72%) and drug loading (11.17%). IVM interacted with lipids and was enveloped in lipid carriers with an amorphous state. Furthermore, its encapsulation in NLCs could enhance drug internalization. IVM-NLCs inhibited PEDV proliferation by up to three orders of magnitude in terms of viral RNA copies, impeding the accumulation of reactive oxygen species and mitigating the mitochondrial dysfunction caused by PEDV infection. Moreover, IVM-NLCs markedly decreased the apoptosis rate of PEDV-induced Vero cells. Hence, IVM-NLCs showed superior inhibitory effect against PEDV compared to free IVM.

Data Summary:

The IVM-NLCs had a hydrodynamic diameter of 153.5 nm, a zeta potential of −31.5 mV, encapsulation efficiency of 95.72%, and drug loading of 11.17%. IVM-NLCs inhibited PEDV proliferation by up to three orders of magnitude in terms of viral RNA copies.

Conclusions:

IVM-NLCs showed superior inhibitory effect against PEDV compared to free IVM. These results implied that NLCs is an efficient delivery system for IVM to improve its antiviral efficacy against PEDV via enhanced intracellular uptake.

Practical Significance:

This study aimed to verify the potential of IVM-NLC as an alternative promising therapeutic drug for PEDV, addressing the poor bioavailability of IVM and enhancing its antiviral activity, thereby potentially reducing the huge economic losses in the global pig industry caused by PEDV outbreaks.

📋 中文结构化总结 Chinese Structured Summary

中文

背景:

猪流行性腹泻病毒(PEDV)是一种急性肠道冠状病毒,可引发仔猪水样腹泻和高死亡率,给全球养猪业造成巨大经济损失。现有PEDV疫苗包括灭活疫苗和弱毒疫苗,但由于新突变株的不断出现,该病在养猪业中仍频繁发生。面对新发或再发疾病的风险,亟需开发新型抗病毒化合物。药物重定位已成为治疗新兴疾病的一个有吸引力的选择,因为针对特定病原体开发新的有效药物既耗时又昂贵。伊维菌素(IVM)是一种经FDA批准的广谱、高效、低毒的抗寄生虫药物。研究表明,它对病毒具有潜在的治疗效果。然而,IVM在水中的溶解度低(仅6–9微克/毫升),生物利用度差,限制了其临床应用。纳米结构脂质载体(NLCs)是新一代脂质纳米颗粒,由固体脂质和液体脂质混合物组成,可提高所包封生物活性化合物的溶解度、稳定性和生物利用度。

方法:

伊维菌素(IVM,纯度91%)购自中国兽医药品监察所。非洲绿猴上皮细胞(Vero细胞)和PEDV CV777毒株由本实验室保存。采用高剪切超声和高压均质法制备IVM-NLCs。将一定量的油酸(OA)、棕榈酸(PA)、吐温20和IVM混合作为油相,加热至70°C直至完全熔融。同时,将泊洛沙姆188溶解于水中作为水相,加热至相同温度。

结果:

研究结果首次揭示了IVM通过降低病毒复制并具有一定的直接灭活作用来抑制PEDV感染性的能力。所制备的IVM-NLCs的水动力学直径为153.5 nm,zeta电位为−31.5 mV,包封率高(95.72%),载药量为11.17%。IVM与脂质相互作用,以无定形状态被包裹在脂质载体中。此外,将其包封于NLCs中可增强药物的内化。IVM-NLCs在病毒RNA拷贝数方面抑制PEDV增殖达三个数量级,阻碍了活性氧的积累,并缓解了PEDV感染引起的线粒体功能障碍。此外,IVM-NLCs显著降低了PEDV诱导的Vero细胞的凋亡率。因此,与游离IVM相比,IVM-NLCs对PEDV表现出更优的抑制效果。

数据摘要:

IVM-NLCs的水动力学直径为153.5 nm,zeta电位为−31.5 mV,包封率为95.72%,载药量为11.17%。IVM-NLCs在病毒RNA拷贝数方面抑制PEDV增殖达三个数量级。

结论:

与游离IVM相比,IVM-NLCs对PEDV表现出更优的抑制效果。这些结果表明,NLCs是一种高效的IVM递送系统,可通过增强细胞内摄取来提高其对PEDV的抗病毒效力。

实际意义:

本研究旨在验证IVM-NLC作为PEDV替代治疗药物的潜力,解决IVM生物利用度差的问题并增强其抗病毒活性,从而有望减少PEDV暴发给全球养猪业造成的巨大经济损失。

📖 英文全文 English Full Text

EN

pharmaceutics Article

Enhanced In Vitro Antiviral Activity of Ivermectin-Loaded Nanostructured Lipid Carriers against Porcine Epidemic Diarrhea Virus via Improved Intracellular Delivery Xiaolin Xu 1 , Shasha Gao 1 , Qindan Zuo 1 , Jiahao Gong 1 , Xinhao Song 1 , Yongshi Liu 1 , Jing Xiao 1 , Xiaofeng Zhai 1,2 , Haifeng Sun 1 , Mingzhi Zhang 3 , Xiuge Gao 1 and Dawei Guo 1, * 1

2 3 *

Citation: Xu, X.; Gao, S.; Zuo, Q.; Gong, J.; Song, X.; Liu, Y.; Xiao, J.; Zhai, X.; Sun, H.; Zhang, M.; et al. Enhanced In Vitro Antiviral Activity of Ivermectin-Loaded Nanostructured Lipid Carriers against Porcine Epidemic Diarrhea Virus via Improved Intracellular Delivery. Pharmaceutics 2024, 16, 601. https://doi.org/10.3390/ pharmaceutics16050601

Engineering Center of Innovative Veterinary Drugs, Center for Veterinary Drug Research and Evaluation, MOE Joint International Research Laboratory of Animal Health and Food Safety, College of Veterinary Medicine, Nanjing Agricultural University, 1 Weigang, Nanjing 210095, China Academy for Advanced Interdisciplinary Studies, Nanjing Agricultural University, Nanjing 210095, China Jiangsu Key Laboratory of Pesticide Science, College of Sciences, Nanjing Agricultural University, 1 Weigang, Nanjing 210095, China Correspondence: gdawei0123@njau.edu.cn; Tel.: +86-25-8439-6215; Fax: +86-25-8439-8669

Abstract: Porcine epidemic diarrhea virus (PEDV) is an acute enteric coronavirus, inducing watery diarrhea and high mortality in piglets, leading to huge economic losses in global pig industry. Ivermectin (IVM), an FDA-approved antiparasitic agent, is characterized by high efficacy and wide applicability. However, the poor bioavailability limits its application. Since the virus is parasitized inside the host cells, increasing the intracellular drug uptake can improve antiviral efficacy. Hence, we aimed to develop nanostructured lipid carriers (NLCs) to enhance the antiviral efficacy of IVM. The findings first revealed the capacity of IVM to inhibit the infectivity of PEDV by reducing viral replication with a certain direct inactivation effect. The as-prepared IVM-NLCs possessed hydrodynamic diameter of 153.5 nm with a zeta potential of −31.5 mV and high encapsulation efficiency (95.72%) and drug loading (11.17%). IVM interacted with lipids and was enveloped in lipid carriers with an amorphous state. Furthermore, its encapsulation in NLCs could enhance drug internalization. Meanwhile, IVM-NLCs inhibited PEDV proliferation by up to three orders of magnitude in terms of viral RNA copies, impeding the accumulation of reactive oxygen species and mitigating the mitochondrial dysfunction caused by PEDV infection. Moreover, IVM-NLCs markedly decreased the apoptosis rate of PEDV-induced Vero cells. Hence, IVM-NLCs showed superior inhibitory effect against PEDV compared to free IVM. Together, these results implied that NLCs is an efficient delivery system for IVM to improve its antiviral efficacy against PEDV via enhanced intracellular uptake. Keywords: ivermectin; antivirus; nanostructured lipid carriers; porcine epidemic diarrhea virus; intracellular delivery

Academic Editor: Sofia Lima Received: 28 March 2024 Revised: 18 April 2024 Accepted: 25 April 2024 Published: 29 April 2024

Copyright: © 2024 by the authors. Licensee MDPI, Basel, Switzerland. This article is an open access article distributed under the terms and conditions of the Creative Commons Attribution (CC BY) license (https:// creativecommons.org/licenses/by/ 4.0/).

1. Introduction Swine diarrhea is one of the main infectious diseases affecting the pig industry, among which viral diarrhea has the highest incidence and causes the most serious damage [1]. Coronaviruses are important pathogens causing diarrhea in piglets and mainly include porcine epidemic diarrhea virus (PEDV), porcine infectious gastroenteritis virus (TGEV), porcine delta coronavirus (PDCoV), and porcine acute diarrhea syndrome coronavirus (SADS-CoV). Currently, PEDV and TGEV are the most widely distributed viral pathogens of porcine diarrhea [2]. PEDV is a member of the genus α-coronavirus, a single-stranded, positive-stranded RNA virus with a capsid, which can cause acute diarrhea, vomiting, and dehydration in piglets, with a lethality rate of up to 90%, inducing significant economic losses to the pig industry worldwide [3–5]. Available PEDV vaccines include inactivated and attenuated vaccines, but these diseases are still frequent in the pig breeding industry, Pharmaceutics 2024, 16, 601. https://doi.org/10.3390/pharmaceutics16050601

partly due to the emergence of new mutant strains [6]. With the risk of emerging or re-emerging diseases, there is an urgent need to develop new antiviral compounds [4,7,8]. Recently, drug repurposing has become an attractive option for treating emerging diseases, as developing new effective drugs against a particular pathogen is time-consuming and expensive [9]. In contrast, approved substances are easily available, and their potential side effects are well characterized [10]. Drug repurposing is a strategy for converting an FDA-approved or investigational drug from its original use to a new use [11]. The greatest benefit of repurposed drugs is the omission of critical and time-consuming drug development phases, which significantly reduces the time required to produce effective antiviral drugs [12]. Ivermectin (IVM) is an FDA-approved, broad-spectrum, high-efficiency, low-toxicity antiparasitic drug [13,14]. It is a kind of hexadecameric ring macrolide drug, and its biological activity is broad [15]. Studies have shown that it has potential therapeutic effects against viruses [16]. In vitro investigations have demonstrated that IVM could effectively restrict infection caused by a variety of RNA and DNA viruses, including HIV-1, dengue virus (DENV), related flaviviruses, influenza A, and Venezuelan equine encephalitis virus (VEEV) [17–21]. Recent studies have indicated that it is a potent inhibitor of SARS-CoV2 [22]. However, the low solubility of IVM in water, only 6-9 micrograms per milliliter, and the poor bioavailability limit its clinical applications [23,24]. Nanostructured lipid carriers are a new generation of lipid nanoparticles consisting of a mixture of solid and liquid lipids [25]. It is a cutting-edge nano-delivery system that enhances the solubility, stability, and bioavailability of the encapsulated bioactive compounds by protecting them from adverse environmental conditions and regulates their release by enabling them to exert their active effects at the right time and site [26–28]. In this study, we determined that IVM could inhibit the infectivity of PEDV, and then, formulated nanostructured lipid carriers could be used strategically to tackle the low solubility and the poor bioavailability of IVM. The results showed that NLCs could enhance the antiviral activity of IVM by improving intracellular delivery. This study aimed to verify the potential of IVM-NLC as an alternative promising therapeutic drug for PEDV. 2. Materials and Methods 2.1. Chemical, Cells, and Viruses Ivermectin (IVM, 91%) was purchased from the China Institute of Veterinary Drug Control (Beijing, China). African green monkey epithelial cells (Vero) and PEDV strain CV777 (GenBank Accession No. KT323979) were maintained in the laboratory. 2.2. Preparation of IVM-NLCs The high-shear-ultrasound and high-pressure homogenization methods were used to prepare IVM-NLCs [29,30]. Briefly, a certain amount of oleic acid (OA) (Aladdin, Shanghai, China), palmitic acid (PA, Aladdin, Shanghai, China), Tween 20 (Aladdin, Shanghai, China), and IVM was mixed as the oil phase and heated up to 70 ◦ C until complete melting. In parallel, poloxamer 188 (Yunhong Chemical Preparations and Accessories Technology Corporation, Shanghai, China) was dissolved in water as the aqueous phase and heated at the same temperature. Then, the aqueous phase was poured into the oil phase under magnetic stirring at 700 rpm. Subsequently, the mixture was homogenized at 11,000 rpm for 5 min with a High Shear Dispersion Emulsifying Machine (FM200, IKA, Staufen, Germany), and then treated by probe sonication at 300 W for 20 min with an Ultrasonic Cell Disruptor (JY96-II, Scientz, Ningbo, China). The obtained oil-in-water (O/W) emulsion was rapidly transferred into cold water under high-shear conditions for 1 min and cooled to form the NLCs. The hot O/W system was cycled four times in a high-pressure homogenizer (AH-BASIC, ATS, Suzhou, China) at 700 bar to obtain IVM-NLCs in bulk.

2.3. Characterization of IVM-NLCs 2.3.1. Hydrodynamic Diameter (HD), Polydispersity Index (PDI), and Zeta Potential (ZP) Prior to measurement, all the samples were diluted appropriately with deionized water. The HD, PDI, and ZP of IVM-NLCs were characterized using dynamic light scattering (DLS) with the Zetasizer (Malvern Instruments Ltd., Malvern, Worcestershire, UK). 2.3.2. Transmission Electron Microscopy (TEM) The morphology of the IVM-NLCs was observed by TEM (Tecnai 12, Philips, Amsterdam, The Netherlands). Briefly, the diluted IVM-NLCs were dropped onto 300-mesh copper grids. After drying, the samples were negatively stained for 2 min using a 2% (w/v) phosphotungstic acid solution. The dried samples were then subjected to TEM analysis. 2.3.3. X-ray Diffraction (XRD) and Fourier Transform Infrared Spectroscopy (FT-IR) PA, IVM, physical mixtures of PA and IVM, lyophilized NLCs, and IVM-NLC powder were studied using XRD (D8 Advance, Bruker AXS, Karlsruhe, Germany) to analyze the changes in the crystal structure of IVM during NLC formation. In addition, the above samples were placed in a crucible and compacted onto slides. Subsequently, XRD with Cu/Kα radiation source were scanned at 4◦ /min in the range of 5◦ ~50◦ under the conditions of 40 kV/40 mA. After that, PA, IVM, physical mixture of IVM and PA, lyophilized NLCs, and IVM-NLC powder IRs were recorded using an FT-IR spectrometer (IS5&N380, Nicolet, Waltham, MA, USA). Prior to FT-IR spectroscopy, the samples were mixed with potassium bromide (KBr) in a ratio of 1:150 (w/w) and pressed into thin slices using a high-pressure hydraulic press. The prepared flake samples were then placed on an FT-IR spectrometer and scanned under a wave number range from 4000 cm−1 to 500 cm−1 . 2.3.4. Entrapment Efficiency (EE) and Drug Loading (DL) The EE and DL of IVM-NLCs were determined by ultrafiltration centrifugation combined with high-performance liquid chromatography (HPLC). The diluted IVM-NLCs were added to methanol, vortexed, and sonicated to break the emulsion. The supernatant was centrifuged, and the weight of IVM (Wtotal ) in the emulsion was determined by HPLC. In addition, the dilution of IVM-NLCs was placed in ultra-filtration centrifuge tube (MWCO: 100 kDa, Millipore, Bilrika, MA, USA) at high speed, and the weight of free IVM (Wfree ) in the emulsion was determined by HPLC. The DL and EE of IVM-NLCs were calculated using the following formulas: EE (%) = (Wtotal − Wfree )/Wtotal DL (%) = (Wtotal − Wfree )/WNLCs where Wtotal is the total content of applied IVM in NLCs, Wfree is the amount of free IVM in the supernatant phase, and WNLCs is the content of the lipid used in the preparation of the IVM-NLCs. 2.4. Cell Culture Vero cells were grown in Dulbecco’s Modified Eagle’s Medium (DMEM, Gibco, Waltham, MA, USA) with 1% penicillin–streptomycin (HyClone, Logan, UT, USA) and 5% Fetal Bovine Serum (FBS) (Gibco, CA, USA). Cells were placed in a humidified cell culture incubator with 5% CO2 at 37 ◦ C. 2.5. Cell Viability Evaluation The cytotoxicity of IVM and IVM-NLCs was tested in Vero cells using the Cell Counting kit-8 (CCK-8, KeyGen Biotech Co., Ltd., Nanjing, China) method. Vero cells were seeded in a 96-well plate overnight at a density of 10,000 cells per well in 100 µL fresh medium. After plating, cells were treated with IVM and IVM-NLCs for 24 h and 48 h. Subsequently, CCK-8 (10 µL/well) was added to each well and incubated at 37 ◦ C for 1 h, and the OD

values at 450 nm were measured. Cell viability was calculated using the following formula: cell viability (%) = (ODtreated − ODblank )/(ODuntreated − ODblank ) × 100%. 2.6. In Vitro Cellular Uptake Qualitative and quantitative assessment of in vitro cellular uptake of coumarin-6 (C6) in Vero cells using fluorescence microscopy (Thermo Fisher, Waltham, MA, USA) and flow cytometry (BD Biosciences, New York, NY, USA), respectively. Briefly, Vero cells were seeded into a 6-well culture plate at the density of 2 × 105 cells per well and incubated overnight. The cells were then treated with free C6 or C6-NLCs, and cells without any treatment were used as a control. After 4 h, cells were washed with cold PBS, fixed in 4% paraformaldehyde for 10–15 min, labeled with DAPI, and visualized by fluorescence microscopy. In addition, to further investigate the cellular uptake process of C6 and C6NLCs, after the termination of uptake, treated cells were separated with 0.25% trypsin, centrifuged at 1000 rpm for 5 min, and suspended in PBS, and fluorescent signals in cells were analyzed by flow cytometry. 2.7. TCID50 Assay To determine the 50% tissue culture infectious dose (TCID50 ), PEDV samples were diluted 10-fold with maintenance solution and used to inoculate Vero cells. Briefly, Vero cells were seeded in a 96-well plate overnight. Then, the medium was discarded, washed twice with maintenance solution, and 100 µL diluted virus solution per well and maintenance solution was added to the negative control wells. The cell culture plates were placed in an incubator at 37 ◦ C and incubated for 1 h. After that, the old maintenance solution was discarded, and 100 µL of maintenance solution was added to the incubator for continued cultivation and monitoring of CPE. TCID50 /mL was calculated according to the method of Reed–Muench. 2.8. Antiviral Assay Cells were infected with PEDV at multiplicity of infection (MOI) of 0.05. One hour later, the inoculum was removed, and the cells were washed with serum-free DMEM. Subsequently, cells were incubated separately with DMEM, NLCs, IVM, and IVM-NLCs. The antiviral effect of NLCs, IVM, and IVM-NLCs on PEDV infection was then evaluated by quantitative real-time polymerase chain reaction (RT-qPCR), Western blot, and indirect immunofluorescence assay (IFA). There exists a possible target for inhibition at each stage of viral infection [31,32]. To determine at which stage IVM blocked infection, IVM as well as PEDV were added to cells with different treatments: Inactivation assay: The mixture of IVM with PEDV was placed at 37 ◦ C for 3 h. Vero cells were infected with the pretreated PEDV for 1 h. After incubation, the supernatant was discarded and replaced with a maintenance solution without any drugs to continue the culture. Total RNA was extracted and quantified by RT-qPCR. Attachment assay: Vero cells were pre-cooled at 4 ◦ C, followed by incubation with 5 µM IVM for 1 h, and then infection with PEDV for 1 h at 4 ◦ C. After discarding the supernatant, the cells were washed twice with pre-cooled serum-free DMEM. Total RNA was extracted and quantified by RT-qPCR. Adsorption assay: After pre-cooling at 4 ◦ C, Vero cells were infected with PEDV at ◦ 4 C for 1 h. After discarding the supernatant and washing with pre-cooled serum-free DMEM, the cells were treated with 5 µM IVM in DMEM containing 2% FBS for 1 h at 37 ◦ C. Total RNA was extracted and quantified by RT-qPCR. Replication assay: Vero cells were infected with PEDV for 1 h at 37 ◦ C. To remove non-adsorbed virus particles, the cells were washed with pre-cooled serum-free DMEM, incubated with DMEM for 4 h, and then treated with 5 µM IVM for 12 h. Total RNA was extracted and quantified by RT-qPCR.

Release assay: Vero cells were infected with PEDV for 10 h at 37 ◦ C. The supernatant was discarded, and after washing with serum-free DMEM, the cells were incubated separately with IVM in DMEM containing 2% FBS. Total RNA was extracted and quantified by RT-qPCR. 2.9. One-Step Growth Curve Vero cells at 80–90% confluence were infected with 0.05 MOI of PEDV. Subsequently, the control DMEM, NLCs, IVM, and IVM-NLCs were added and subjected to further incubation at 37 ◦ C. The TCID50 was recorded at 1, 4, 8, 12, 24, 36, 48, 60, and 72 hpi according to the Reed–Muench method. PEDV titers were calculated, and viral growth curves were plotted by determining TCID50 at different time points. 2.10. RT-qPCR RT-qPCR was based on SYBR Green method. The PEDV total RNA was extracted from the cells in a 6-well plate using RNAiso Plus (Takara, Tokyo, Japan) according to the manufacturer’s protocol. The concentration and purity of total RNA were assessed by Nanodrop (Thermo Fisher Scientific, Waltham, MA, USA). The total RNA was reverse transcribed into cDNA using cDNA synthesis kit (Vazyme, Nanjing, China) and stored at −20 ◦ C. The target genes were evaluated in triplicate using SYBR qPCR Master Mix (Vazyme, Nanjing, China). Absolute fluorescence was quantitatively referenced as described in [33]. 2.11. Western Blot Analysis Vero cells were cultured to approximately 80–90% confluence in 6-well plates, and infected with 0.05 MOI of PEDV. After 1 h of infection, the cell monolayers were incubated with control DMEM, NLCs, IVM, and IVM-NLCs (5 µM) for 24 h, and then treated with lysis buffer (100 µL/well) to extract total protein, followed by the quantification of protein concentration using bicinchoninic acid (BCA) protein assay kit according to the manufacturer’s instructions (Solarbio, Beijing, China). Sodium dodecyl sulfate (SDS) loading buffer was added to the collected cell extracts and boiled for 10 min. Equivalent amounts of proteins were loaded and electrophoresed on 12% sodium dodecyl sulfate polyacrylamide gel electrophoresis (SDS-PAGE), and then transferred to nitrocellulose filter (NC) membranes followed by blocking with 5% skim milk for 2 h. Subsequently, the expression of the PEDV N protein was determined. The expression of GAPDH was investigated to represent the same amounts of protein sample loading. 2.12. IFA The inhibitory effect of NLCs, IVM, and IVM-NLCs against PEDV in Vero cells was further evaluated by immunofluorescence. Vero cells in 24-well plates were infected with PEDV at 0.05 MOI. After 1 h of incubation, free viruses were removed by extensive rinsing. Then, the cells were incubated with control DMEM (containing 2% FBS) or NLCs, IVM, and IVM-NLCs, respectively. Twenty-four hours later, cells were fixed with 4% formaldehyde for 15 min. After permeabilization with 0.1% Triton X-100, the cells were incubated with the mouse monoclonal antibody against the PEDV N protein (1:200 dilution) at 4 ◦ C overnight and washed three times with phosphate-buffered solution with Tween 20 (PBST) for 10 min each. Then, the cells were incubated with FITC-conjugated goat anti-mouse antibody (1:200 dilution) for 1 h, and counterstained with DAPI at room temperature for 10 min. After washing three times, the photographs were obtained by fluorescence microscopy. 2.13. Determination of Reactive Oxygen Species (ROS) Generation ROS level was assessed using a 2′ ,7′ -dichlorofluorescein diacetate (DCFH-DA)-based ROS assay kit (Nanjing Kaiji Biotechnology Co., Ltd., Nanjing, China). Briefly, wellgrown Vero cells were inoculated in 12-well plates, and an inoculum of 0.05 MOI of PEDV (500 µL/well) was added to Vero cells grown to 80–90% fusion. After 1 h of infection, the cell monolayer was rinsed and then covered with NLCs, IVM, and IVM-NLCs, respectively.

After that, the cells were incubated with DCFH-DA for 20 min at 37 ◦ C in the dark. The fluorescence changes in cells in each group were observed under a fluorescence microscope (Ex = 488 nm, Em = 507 nm) (Thermo Fisher, MA, USA). 2.14. Mitochondrial Membrane Potential (MMP) Analysis JC-1 assay kit (KeyGen Biotech Co., Ltd., Nanjing, China) was used to detect MMP changes. Well-grown Vero cells were inoculated in 12-well plates, and an inoculum of 0.05 MOI of PEDV (500 µL/well) was added to Vero cells grown to 80–90% fusion. After 1 h of infection, the cell monolayer was rinsed and then covered with NLCs, IVM, and IVM-NLCs. Subsequently, the cells were washed with PBS. JC-1 (10 µg/mL) was added to each sample and incubated at 37 ◦ C in the dark for 15 min. The fluorescence changes in cells in each group were observed under a fluorescence microscope (green fluorescence, Ex = 488 nm, Em = 507 nm; red fluorescence, Ex = 525 nm, Em = 590 nm) (Thermo Fisher, MA, USA). 2.15. Apoptosis Assay Apoptosis rate of PEDV-infected Vero cells was assessed with Annexin V-FITC/PI double staining kit (KeyGen Biotech Co., Ltd., Nanjing, China) according to the manufacturer’s instructions. The cells were seeded into 6-well plates and then stained with Annexin V-FITC and PI in dark. Cells were analyzed by flow cytometry (Ex = 488 nm, Em = 525 nm). Cell-Quest software (Becton Dickinson, San Jose, CA, USA) was employed to analyze the data. 2.16. Statistical Analysis All data are presented as mean ± standard deviation (SD), and experiments were conducted in triplicate. GraphPad Prism 8.0 software was used for statistical analysis. Differences between the two groups were assessed using t-test (mean ± SD). When comparing several groups, one-way analysis of variance (ANOVA) was employed. Statistics were applied to differences with * p < 0.05 and ** p < 0.01. 3. Results and Discussion 3.1. IVM Inhibited the Infectivity of PEDV Numerous studies have recently reported the antiviral properties of IVM, which could impede viruses by hindering nuclear input that was reliant on specific IMPα/β1dependent viral proteins [2]. This study investigated the antiviral activity of IVM against PEDV in vitro. Prior to assessing its inhibitory potency, cytotoxicity assays were conducted on Vero cells. The results indicated that cell viability remained above 80% at concentrations ranging from 0 to 10 µM (Figure 1A). After excluding cytotoxicity, the inhibitory effect of IVM on PEDV-infected Vero cells was evaluated. Specifically, Vero cells were infected with 0.05 MOI of PEDV and subsequently treated with varying concentrations of IVM. Furthermore, a discernible difference was observed among the virus control group after 2.5 or 5 µM IVM treatment, and cell viability could reach more than 80% after 10 µM IVM treatment, as illustrated in Figure 1B. We calculated the concentration for 50% of maximal effect (EC50 ) value, which reflected the concentration of IVM required to abolish infectious virus particle production by 50%. The EC50 value for IVM following infection with PEDV in Vero cells was 4.63 µM (Figure 1C). Furthermore, the administration of IVM at concentrations of 1.25, 2.5, 5, and 10 µM resulted in a reduction of PEDV RNA N copies at 12 h post-infection from 6.1 to 5.8, 5.5, 4.8, and 3.8 lg copies, respectively, in comparison to the untreated cohort (Figure 1D). Notably, the PEDV nucleocapsid (N) protein, an RNA-binding protein crucial for the virus life cycle, could serve as a precise and early diagnostic target for PEDV infection [34,35]. The inhibitory effect of IVM on PEDV proliferation was verified by detecting the expression level of PEDV N protein. Specifically, the infected cells were incubated with different concentrations of IVM. As shown in Figure 1E, at 24 hpi, a strong fluorescent signal was observed within the PEDVinfected Vero cells treated with DMSO by indirect immunofluorescence. However, we

to the untreated cohort (Figure 1D). Notably, the PEDV nucleocapsid (N) protein, an RNA-binding protein crucial for the virus life cycle, could serve as a precise and early diagnostic target for PEDV infection [34,35]. The inhibitory effect of IVM on PEDV proliferation was verified by detecting the expression level of PEDV N protein. Specifically, the 7 of 15 infected cells were incubated with different concentrations of IVM. As shown in Figure 1E, at 24 hpi, a strong fluorescent signal was observed within the PEDV-infected Vero cells treated with DMSO by indirect immunofluorescence. However, we observed a significant observed a significant and concentration-dependent infected and concentration-dependent difference between difference untreatedbetween infecteduntreated cells and IVMcells and IVM-treated infected cells, which was in accordance with the growth curves of treated infected cells, which was in accordance with the growth curves of the virus. the virus.

Figure 1. 1. IVM inhibited the infectivity of PEDV. (A) Cytotoxicity of Vero Vero cells treated treated with with different different Figure concentrations of IVM at the appointed time via CCK-8 assay. Medium containing 0.05% DMSO concentrations of IVM at the appointed time via CCK-8 assay. Medium containing 0.05% DMSO 50 of IVM (v/v) served as control. (B) Antiviral activity of IVM was measured by CCK-8 assay. (C) EC (v/v) served as control. (B) Antiviral activity of IVM was measured by CCK-8 assay. (C) EC50 of was calculated with GraphPad Prism 8.0. (D) PEDV N RNA copies of Vero cells infected with PEDV IVM was calculated with GraphPad Prism 8.0. (D) PEDV N RNA copies of Vero cells infected with after different treatments of IVM by RT-qPCR. (E) Indirect immunofluorescence assay of PEDVPEDV after different treatments of IVM by RT-qPCR. (E) Indirect immunofluorescence assay of PEDVinfected Vero cells after treatment with different concentrations of IVM or without treatment. Blue, infected Vero cells after treatment with different concentrations IVM orµm. without Blue, DAPI; green, FITC-conjugated goat anti-mouse antibody. Scaleofbar = 50 Errortreatment. bars represent DAPI; green, deviation FITC-conjugated goat anti-mouse antibody. Scale barvalue = 50 was µm.calculated Error barsby represent the standard from three repeated experiments. The mean the onethe from three repeated mean wascompared calculatedwith by the waystandard analysis deviation of variance (ANOVA) (mean ± experiments. SD, n = 3). * pThe < 0.05, ** value p < 0.01, the one-way analysis of variance (ANOVA) (mean ± SD, n = 3). * p < 0.05, ** p < 0.01, compared with the PEDV group. PEDV group.

3.2. Effect of IVM in Diverse Stages of PEDV Life Cycle 3.2. Effect of IVM in Diverse Stages of PEDV Life Cycle The present study investigated the underlying mechanism of the antiviral properties Thebypresent study investigated mechanism of the its antiviral properties of IVM analyzing their impact on the the underlying proliferation of PEDV during replication cycle. of IVM by analyzing their impact on the proliferation of PEDV during its replication cycle. The schematic diagram is shown in Figure 2A. The direct inactivation potential of IVM on The schematic diagram is shown in Figure 2A. The direct inactivation potential of IVM PEDV was initially evaluated, and the results demonstrated a 10-fold reduction in the on PEDV was initially evaluated, and the results demonstrated a 10-fold reduction in number of PEDV via RT-qPCR depicted in Figure 2B. In the adsorption process of PEDV, the number of PEDV via RT-qPCR depicted in Figure 2B. In the adsorption process of there was no significant difference between the experimental group and the control group PEDV, there was no significant difference between the experimental group and the control group in terms of their suppression effect on PEDV adsorption (Figure 2C). In the invasion process of PEDV, the results revealed that IVM treatment decreased the infectious virus titer by about 10-fold relative to the control group (Figure 2D), implying IVM had slight influence on PEDV invasion. In addition, as shown in Figure 2E, IVM reduced the number of PEDV N RNA copies by nearly 102 -fold, implying that IVM may suppress PEDV mainly via inhibiting PEDV replication. In addition, the effect of IVM on the release of PEDV progeny is shown in Figure 2F. There was no noticeable difference in the virus titers of PEDV compared to the control group, suggesting that IVM had no inhibitory effect on the release of PEDV progeny. To sum up, IVM exerted its suppressive effect on PEDV primarily by inhibiting virus invasion and replication with a certain direct inactivation effect in vitro.

via inhibiting PEDV replication. In addition, the effect of IVM on the release of PEDV progeny is shown in Figure 2F. There was no noticeable difference in the virus titers of PEDV compared to the control group, suggesting that IVM had no inhibitory effect on the release of PEDV progeny. To sum up, IVM exerted its suppressive effect on PEDV primarily by inhibiting virus invasion and replication with a certain direct inactivation effect in 8 of 15 vitro.

Figure2.2.IVM IVMtreatment treatmentatat multiple stages of inhibition of PEDV proliferation. (A) Schematic diaFigure multiple stages of inhibition of PEDV proliferation. (A) Schematic diagram gram of the effect of IVM on the replication cycle of PEDV. (B) Effect of IVM on direct inactivation of the effect of IVM on the replication cycle of PEDV. (B) Effect of IVM on direct inactivation of PEDV. of PEDV. Effect of IVM on the (C) adsorption, (D) invasion, (E) replication, and (F) release processes Effect of IVM on the (C) adsorption, (D) invasion, (E) replication, and (F) release processes of infected of infected cells. The mean value was calculated by the t-test (mean ± SD, n = 3). * p < 0.05, ** p < 0.01, cells. The mean value was calculated by the t-test (mean ± SD, n = 3). * p < 0.05, ** p < 0.01, compared compared with the PEDV group. with the PEDV group.

3.3. Characterization Characterization of of IVM-Loaded IVM-Loaded Nanostructured Nanostructured Lipid Lipid Carriers Carriers 3.3. Theprepared preparedIVM-NLCs IVM-NLCsthrough throughthe the high-pressure homogenization technique exThe high-pressure homogenization technique exhibhibited characteristics a homogeneous, opaque, milky white liquid fluited characteristics of a of homogeneous, opaque, and and milky white liquid withwith highhigh fluidity. idity. The hydrodynamic diameter (HD) zeta potential (ZP)IVM-NLCs, of the IVM-NLCs, as ilThe hydrodynamic diameter (HD) and zetaand potential (ZP) of the as illustrated lustrated in Figure 3A,B, demonstrated a narrow normal distribution. The as-prepared in Figure 3A,B, demonstrated a narrow normal distribution. The as-prepared IVM-NLCs IVM-NLCsanpossessed an HD of 153.5 ± 0.80anm with a polydispersity index (PDI)±of0.007, 0.153 possessed HD of 153.5 ± 0.80 nm with polydispersity index (PDI) of 0.153 ± 0.007, indicating a high particle size distribution homogeneity indicating a high degree ofdegree particleofsize distribution homogeneity (Table S1). (Table ZP wasS1). alsoZP a was so a critical factor to stability of colloidal dispersion. In general, stable critical factor to evaluate theevaluate stabilitythe of colloidal dispersion. In general, stable dispersion dispersion of a nanoparticle system was when achieved the absolute of ZP exceeded of a nanoparticle system was achieved thewhen absolute value of value ZP exceeded 30 mV due to electrical repulsion [36]. The of ZP IVM-NLCs was − 31.5−31.5 ± 0.569 mV,mV, indicat30 mV due to electrical repulsion [36].ZP The of IVM-NLCs was ± 0.569 indiing favorable stability. The morphology of IVM-NLCs was examined using transmission electron microscopy (TEM), revealing spherical or ellipsoidal particles with uniform size distribution and no observed agglomeration (Figure 3C). The mean distribution size of IVM-NLCs was determined to be 39.54 ± 9.17 nm (Figure 3D). Notably, the particle size of IVM-NLCs was significantly smaller than the HD. The reason for this disparity is that dynamic light scattering (DLS) provides an indirect measurement of particle size by detecting the fluctuation in scattered light intensity due to Brownian motion in a hydrated state, whereas TEM requires the sample to be in a dry state during testing [37,38]. DL and EE were important parameters for evaluating the preparation of NLCs. Increasing EE could enhance drug efficacy and reduce adverse drug reactions. Increasing DL could lead to a more stable formulation, while reducing the use of excipients and thus their potential toxicity. The EE and DL of the prepared IVM-NLCs measured by HPLC were 95.72 ± 0.30% and 11.17 ± 0.75%, respectively (Table S1). The prepared IVM-NLCs was based on the

tecting the fluctuation in scattered light intensity due to Brownian motion in a hydrated state, whereas TEM requires the sample to be in a dry state during testing [37,38]. DL and EE were important parameters for evaluating the preparation of NLCs. Increasing EE could enhance drug efficacy and reduce adverse drug reactions. Increasing DL could lead to a more stable formulation, while reducing the use of excipients and thus their potential 9 of 15 toxicity. The EE and DL of the prepared IVM-NLCs measured by HPLC were 95.72 ± 0.30% and 11.17 ± 0.75%, respectively (Table S1). The prepared IVM-NLCs was based on laboratory preparation ofof IVM-SLNs IVM-NLCshad had the laboratory preparation IVM-SLNs[30]. [30].Compared Compared with with IVM-SLNs, IVM-NLCs smallerHD HDand andmore moreuniform uniformdistribution, distribution,which whichimproved improvedEE EEand andDL. DL. smaller

Figure of of thethe optimized IVM-NLCs. (A) (A) Hydrodynamic diameter (HD)(HD) and and (B) Figure3.3.Characterization Characterization optimized IVM-NLCs. Hydrodynamic diameter zeta potential (ZP) of the IVM-NLCs were determined by DLS. (C) The morphology of the IVM(B) zeta potential (ZP) of the IVM-NLCs were determined by DLS. (C) The morphology of the IVMNLCs NLCswas wasobserved observedby byTEM, TEM,and and(D) (D)the thesize sizedistribution distributionwas wasobtained obtainedvia viaanalysis analysisofofthe theparticles particles from several TEM images. Scale bar = 100 nm. (E) X-ray diffraction (XRD) spectra and (F) Fourier from several TEM images. Scale bar = 100 nm. (E) X-ray diffraction (XRD) spectra and (F) Fourier transform infrared (FT-IR) spectra for IVM-NLCs, NLCs, physical mixture, IVM, and PA were transform infrared (FT-IR) spectra for IVM-NLCs, NLCs, physical mixture, IVM, and PA were shown. shown.

The conversion of drugs from a crystalline to an amorphous state had been found to The conversion of drugs from a crystalline to an amorphous state had been found to enhance drug loading and improve the stability of nanodrug delivery systems [39]. The enhance drug loading and improve the stability of nanodrug delivery systems [39]. The X-ray diffraction pattern was used for crystallographic analysis [40]. As shown in Figure 3E, X-ray diffraction pattern was usedbefor crystallographic Asthe shown in Figure apparent diffraction peaks could observed near 10◦ , analysis 15◦ , and [40]. 20◦ in pattern of IVM, 3E, apparent diffraction peaks could be observed near 10°, 15°, and 20° in the pattern of indicating hat IVM was a crystalline structure. The diffraction peaks observed in the IVM, indicating that IVM was a crystalline structure. The diffraction peaks observed in XRD patterns of IVM were still observed in the physical mixture of PA and IVM. The the XRD patterns of were still observedsignificantly in the physical of PA IVM. The sharp diffraction of IVM IVM-NLCs disappears nearmixture 10◦ , while theand characteristic sharp diffraction of IVM-NLCs disappears significantly near 10°, while the characteristic ◦ ◦ diffraction peaks persist near 15 and 20 but unlike IVM, which suggest that the IVM has diffraction persist near 15° and 20° but unlike forces, IVM, which suggest that theofIVM has reacted in peaks the NLCs, weakening its intermolecular and the crystallinity the IVM reacted in the NLCs, weakening its intermolecular forces, and the crystallinity of the IVM has also weakened. In addition, the diffraction peaks observed in NLCs were consistent has also weakened. In addition, diffraction peaksinobserved were consistent with IVM-NLCs, indicating thatthe IVM was dispersed NLCs inin anNLCs amorphous form. The FT-IR spectra of PA, IVM, physical mixture of IVM and PA, freeze-dried IVM-NLC powder, and NLC powder are displayed in Figure 3F. The characteristic absorption peak of C=C at 1680 cm−1 in IVM-NLCs disappeared and the characteristic peak of C-O-C stretching vibration of IVM group at 1050–1200 cm−1 was significantly reduced; the sharp peak at 3650 cm−1 for IVM is a stretching vibration of the alcohol hydroxyl group, which also occurs in IVM-PA mixtures and IVM-NLCs; IVM had the O-H stretching vibration peak of hydroxyl group at 3468 cm−1 , and so did the physical mixture of IVM and PA; while the O-H stretching vibration peak of IVM-NLCs was blue-shifted, suggesting that the binding between drug and carrier occurred, marking the successful preparation of nanostructured lipid carriers; the waveforms of IVM and IVM-NLCs were basically similar, indicating that the lipid carriers did not change the skeletal structure of IVM, and IVM was wrapped in the lipid carriers in non-crystalline form. The XRD and FT-IR results were in agreement, Pharmaceutics 2024, 16, 601

occurs in IVM-PA mixtures and IVM-NLCs; IVM had the O-H stretching vibration peak of hydroxyl group at 3468 cm−1, and so did the physical mixture of IVM and PA; while the O-H stretching vibration peak of IVM-NLCs was blue-shifted, suggesting that the binding between drug and carrier occurred, marking the successful preparation of nanostructured lipid carriers; the waveforms of IVM and IVM-NLCs were basically similar, indicating 10 of 15 that the lipid carriers did not change the skeletal structure of IVM, and IVM was wrapped in the lipid carriers in non-crystalline form. The XRD and FT-IR results were in agreement, and IVM was transformed from crystals to amorphous in IVM-NLCs, encapsulated into and IVM was transformed from crystals to amorphous in IVM-NLCs, encapsulated into the nanostructured lipid matrix in an amorphous state. the nanostructured lipid matrix in an amorphous state. 3.4. NLCs NLCs Improved Improved Cellular Cellular Uptake Uptake of of IVM IVM 3.4. Sincethe thevirus virusisisparasitized parasitizedwithin within host cells, increasing intracellular drug upSince thethe host cells, increasing intracellular drug uptake takeimprove can improve antiviral efficacy [41,42]. In order to evaluate in vitro biocompatibilcan antiviral efficacy [41,42]. In order to evaluate the inthe vitro biocompatibility of ity of IVM-NLCs and IVM, cytotoxicity assays were conducted by incubating Vero cells IVM-NLCs and IVM, cytotoxicity assays were conducted by incubating Vero cells with with varying concentrations of IVM or IVM-NLCs and respectively.The Theresults results varying concentrations of IVM or IVM-NLCs for for 24 24 and 4848 h,h,respectively. for Vero cells are presented in Figure S1. The relative survival of cells after exposure to for Vero cells are presented in Figure S1. The relative survival of cells after exposure to IVM-NLCs (0–10 µM) for 24 and 48 h was greater than 80%, indicating that IVM-NLCs IVM-NLCs (0–10 µM) for 24 and 48 h was greater than 80%, indicating that IVM-NLCs have good good biocompatibility. biocompatibility. The The experimental experimental findings findings demonstrated demonstrated aa significant significant enenhave hancement in in the the biocompatibility biocompatibility of of IVM-NLCs IVM-NLCs in in comparison comparison to to IVM. IVM. Additionally, Additionally,the the hancement cytotoxicityofofIVM-NLCs IVM-NLCsononVero Vero cells exhibited a dosetime-dependent relationcytotoxicity cells exhibited a doseandand time-dependent relationship. ship.fluorescence The fluorescence microscopy results depicted in Figure 4A indicated that C6-NLCs The microscopy results depicted in Figure 4A indicated that C6-NLCs disdisplayed more pronounced fluorescence signals than free C6. Moreover, the fluorescence played more pronounced fluorescence signals than free C6. Moreover, the fluorescence intensity exhibited exhibited by by C6-NLCs C6-NLCs was was significantly significantly higher higher than than that that of of free free C6, C6, as as depicted depicted intensity in Figure Figure4B. 4B. Furthermore, Furthermore, the the mean mean fluorescence fluorescence intensity intensity of of C6-NLCs C6-NLCs in in Vero Verocells cellswas was in 3.7-fold greater greater than than that that of of free free C6, C6, as as determined determined through through flow flow cytometry cytometry analysis analysis in in 3.7-fold Figure Figure 4C. 4C. These These findings findings collectively collectively suggested suggested that that NLCs NLCs hold hold potential potential as as aa delivery delivery carrier carrierfor foraugmenting augmentingthe thecellular cellularuptake uptakeof ofIVM. IVM.

Figure 4. Effect of NLCs on the cellular uptake of coumarin-6 (C6) in Vero cells. (A) Representative fluorescence microscope images of various preparations uptake in Vero cells. (B) Cell uptake was determined by flow cytometry of C6 in Vero cells after treatment with free C6 and C6-NLCs and (C) mean intracellular fluorescence intensity. Scale bar = 50 µm. The mean value was calculated by the t-test (mean ± SD, n = 3). ** p < 0.01, for C6-NLCs vs. free C6.

3.5. NLCs Enhanced the Antiviral Activity of IVM against PEDV The present study initially assessed the cell viability of Vero cells infected with PEDV using IVM-NLCs through the CCK-8 assay (Figure S1). The inhibitory effect of IVM-NLCs on PEDV-infected Vero cells is shown in Figure S2. The EC50 value for IVM-NLCs following infection with PEDV in Vero cells was 3.57 µM (Figure 5A). The EC50 value for IVM-NLCs was lower than IVM and confirmed that IVM-NLCs exhibited higher antiviral activity than IVM. The results illustrated in Figure 5B indicated that NLCs improved the viability of Vero cells at 48 h post-treatment in comparison to free IVM. To assess the impact of NLCs, IVM, and IVM-NLCs on PEDV replication, the one-step growth curve was generated through

using IVM-NLCs through the CCK-8 assay (Figure S1). The inhibitory effect of IVM-NLCs on PEDV-infected Vero cells is shown in Figure S2. The EC50 value for IVM-NLCs following infection with PEDV in Vero cells was 3.57 µM (Figure 5A). The EC50 value for IVMNLCs was lower than IVM and confirmed that IVM-NLCs exhibited higher antiviral activity than IVM. The results illustrated in Figure 5B indicated that NLCs improved 11 ofthe 15 viability of Vero cells at 48 h post-treatment in comparison to free IVM. To assess the impact of NLCs, IVM, and IVM-NLCs on PEDV replication, the one-step growth curve was generated the through the PEDV titerwith following treatment withIn5Figure µM of5C, each measuring PEDVmeasuring titer following treatment 5 µM of each agent. at agent. In Figure 5C,toatproliferate, 12 hpi, PEDV to proliferate, with a period 12 hpi, PEDV began withbegan a period of rapid proliferation fromof24rapid hpi toprolifer48 hpi 6.5 TCID50/0.1 mL at 60 hpi. After 60 ationa from hpititer to 48ofhpi and a peak viral titer of 10 and peak 24 viral 106.5 TCID mL at 60 hpi. After 60 h, PEDV proliferation 50 /0.1 h, PEDV proliferation decreased due to cell collapse. Compared to the negative control decreased due to cell collapse. Compared to the negative control group, significant viral group, significant viral titerininhibition was observed in cells treatedthe with IVM-NLCs. titer inhibition was observed cells treated with IVM-NLCs. Therefore, changes in the titer of PEDV that IVM-NLCs indeedverified possessed antiviral activity against Therefore, theverified changes in the titer of PEDV thatsuperior IVM-NLCs indeed possessed suviral replication. perior antiviral activity against viral replication.

Figure 5. 5. Anti-PEDV (A)(A) ECEC 50 of IVM-NLCs waswas calculated with Figure Anti-PEDV activity activityof ofIVM-NLCs IVM-NLCson onVero Verocells. cells. calculated 50 of IVM-NLCs GraphPad Prism 8.0. (B) Antiviral activity of NLCs, IVM, and IVM-NLCs (5.0 µM) measured by with GraphPad Prism 8.0. (B) Antiviral activity of NLCs, IVM, and IVM-NLCs (5.0 µM) measured by CCK-8 assay. (C) One-step growth curve of virus after treatment or without treatment with NLCs, CCK-8 assay. (C) One-step growth curve of virus after treatment or without treatment with NLCs, IVM, and IVM-NLCs. (D) PEDV N RNA copies of Vero cells infected with PEDV after the treatment IVM, and IVM-NLCs. (D) PEDV N RNA copies of Vero cells infected with PEDV after the treatment with NLCs, IVM, and IVM-NLCs by RT-qPCR. (E) Western blot analysis of the expression level of with NLCs, IVM, and IVM-NLCs by RT-qPCR. (E) Western blot analysis of the expression level of PEDV N protein under the treatment of NLCs, IVM, and IVM-NLCs. (F) Indirect immunofluoresPEDV protein under thecells. treatment NLCs, IVM, FITC-conjugated and IVM-NLCs. (F) Indirect immunofluorescence cence N assay of infected Blue, of DAPI; green, goat anti-mouse antibody. (G) assay of infected Blue, DAPI;(ROS) green,level FITC-conjugated goatpost anti-mouse (G)(H) Cellular Cellular reactivecells. oxygen species in infected cells differentantibody. treatments. Mitoreactive oxygen species (ROS) level in infected cells post different treatments. Mitochondrial chondrial membrane potential (MMP) infected cells post different treatments.(H) Scale bar = 50 µm. membrane in infected cells post treatments. Scale barThe = 50mean µm. Error Error bars potential represent(MMP) the standard deviation fromdifferent three repeated experiments. valuebars was calculatedthe bystandard the one-way analysis variance (ANOVA) (mean ±The SD,mean n = 3).value * p

Additionally, RT-qPCR analysis revealed that IVM-NLCs exhibited a greater reduction in PEDV N RNA copies, as expected in Figure 5D. To validate the inhibitory impact of IVM-NLCs on the proliferation of PEDV, we assessed the expression level of PEDV N protein. Specifically, the Western blot assay demonstrated a significant reduction in the expression level of PEDV N protein upon treatment with IVM-NLCs (Figure 5E). Although the downregulation of PEDV N protein expression was observed in both IVM and IVM-NLCs treatment groups, a more pronounced effect was observed in the IVM-NLCtreated group. Additionally, we incubated infected cells with NLCs, IVM, and IVM-NLCs. At 24 hpi, a strong fluorescent signal was observed in PEDV-infected Vero cells by IFA. However, a marked difference was observed in the number of infected cells in the IVMNLCs treated group versus the untreated PEDV-infected group, as indicated by green fluorescence (Figure 5F). These findings collectively indicated that NLCs may enhance the antiviral activity of IVM against PEDV.

Reactive oxygen species (ROS) were toxic byproducts of cellular metabolism, primarily generated by mitochondria in mammalian cells, and were involved in regulating multiple physiological functions of cells [43]. We investigated the effect of IVM-NLCs on ROS production during PEDV infection. Our findings, as depicted in Figure 5G, revealed a substantial increase in DCF fluorescence intensity in infected Vero cells. Conversely, cells treated with IVM-NLCs exhibited a significant reduction in ROS generation compared to those treated with IVM alone. The results indicated that ROS was involved in the antiviral effect of IVM-NLCs. ROS caused mitochondrial membrane damage, resulting in MMP disorder [44]. In normal cells, JC-1 emitted red fluorescence. In contrast, in PEDV-infected Vero cells, JC-1 exhibited green fluorescence, which indicated that PEDV had disrupted the mitochondrial membrane potential of Vero cells, resulting in its decline. Following treatment with IVM-NLCs, the mitochondrial membrane potential was notably restored (Figure 5H). In summary, compared with IVM, IVM-NLCs could improve the inhibition of MMP damage and impede intracellular ROS accumulation in infected Vero cells. 3.6. Effect of IVM-NLCs on the Apoptosis Rate in PEDV-Infected Vero Cells To investigate the mechanism of PEDV inhibition by ivermectin, an AnnexinV-FITC/PI kit was used to detect the apoptosis of the cells by flow cytometry. The results showed that PEDV could induce apoptosis rate of 20.9 ± 1.89% (Figure 6A), and the apoptosis rates of IVM- and IVM-NLC-treated PEDV-infected groups were significantly reduced to 16.4 ± 1.17 and 13.9 ± 1.59 (Figure 6B), which indicated that they play an important Pharmaceutics 2024, 16, x FOR PEER biological REVIEW function in PEDV-induced apoptosis. These findings suggested that IVM-NLCs 13 of 16 reduced ROS accumulation in PEDV-infected Vero cells by improving the inhibition of MMP damage, thereby reducing apoptosis in infected cells.

Figure of of PEDV-infected VeroVero cellscells afterafter treatment with IVM-NLCs. (A) Apoptosis assay Figure6.6.Apoptosis Apoptosis PEDV-infected treatment with IVM-NLCs. (A) Apoptosis was performed in PEDV-infected Vero cells treated NLCs, (5 µM), IVM-NLCs (5 µM). assay was performed in PEDV-infected Vero cells with treated withIVM NLCs, IVM and (5 µM), and IVM-NLCs (5 The µM).graph (B) The graph represents the percentage of apoptosis in Vero cells after treatment. Thevalue mean (B) represents the percentage of apoptosis in Vero cells after treatment. The mean value was calculated by the one-way of variance (ANOVA) (mean ** p < 0.01. was calculated by the one-way analysisanalysis of variance (ANOVA) (mean ± SD, n±=SD, 3). n**=p3). < 0.01.

4.4.Conclusions Conclusions Herein, Herein,the theinhibitory inhibitoryeffect effectofofIVM IVMon onPEDV PEDVininvitro vitrowas wasfirst firstdemonstrated. demonstrated.IVM IVM could inhibit PEDV by the direct inactivation of viral particles and the could inhibit PEDV by the direct inactivation of viral particles and theinhibition inhibitionofofthe the replication replicationphase. phase.Subsequently, Subsequently,IVM-NLCs IVM-NLCswere weresuccessfully successfullydeveloped developedwith withexcellent excellent physicochemical andand improved solubility, it could a promising nanocarphysicochemicalproperties properties improved solubility, it serve couldasserve as a promising rier for IVM with an increased enhanced efficacy. According nanocarrier for IVM with an solubility increasedand solubility andpharmacological enhanced pharmacological efficacy. toAccording biological to tests, IVM-NLCs exhibited stronger antiviral activity against than free biological tests, IVM-NLCs exhibited stronger antiviral PEDV activity against

PEDV than free IVM and reduced PEDV-induced mitochondrial dysfunction, which prevented ROS generation and improved viability of infected Vero cell. Moreover, IVMNLCs also reduced PEDV-induced cell apoptosis rate. In view of the in vitro results, it would be necessary to carry out in vivo tests as soon as possible, to explore its potential in the clinical treatment of PEDV. Consequently, IVM-NLCs were demonstrated to be a

Pharmaceutics 2024, 16, 601 13 of 15

IVM and reduced PEDV-induced mitochondrial dysfunction, which prevented ROS generation and improved viability of infected Vero cell. Moreover, IVM-NLCs also reduced PEDV-induced cell apoptosis rate. In view of the in vitro results, it would be necessary to carry out in vivo tests as soon as possible, to explore its potential in the clinical treatment of PEDV. Consequently, IVM-NLCs were demonstrated to be a potential drug against PEDV, which might provide a basis for the development of novel drugs to antagonize PEDV.

📖 中文全文 Chinese Full Text

中文

# 药剂学

## 文章

**通过改善细胞内递送增强载伊维菌素纳米结构脂质载体对猪流行性腹泻病毒的体外抗病毒活性**

Xiaolin Xu¹, Shasha Gao¹, Qindan Zuo¹, Jiahao Gong¹, Xinhao Song¹, Yongshi Liu¹, Jing Xiao¹, Xiaofeng Zhai¹,², Haifeng Sun¹, Mingzhi Zhang³, Xiuge Gao¹, Dawei Guo¹,*

¹ 南京农业大学兽医学院,农业部动物健康与食品安全联合国际研究实验室,兽药研究与评价中心,创新兽药工程中心,南京 210095,中国 ² 南京农业大学前沿交叉学科研究院,南京 210095,中国 ³ 南京农业大学理学院,江苏省农药科学重点实验室,南京 210095,中国

* 通讯作者:gdawei0123@njau.edu.cn;电话:+86-25-8439-6215;传真:+86-25-8439-8669

**摘要:** 猪流行性腹泻病毒(PEDV)是一种急性肠道冠状病毒,可引起仔猪水样腹泻和高死亡率,给全球养猪业造成巨大经济损失。伊维菌素(IVM)是一种经FDA批准的抗寄生虫药物,具有高效性和广谱适用性。然而,其较差的生物利用度限制了应用。由于病毒寄生于宿主细胞内,提高细胞内药物摄取可改善抗病毒疗效。因此,我们旨在开发纳米结构脂质载体(NLCs)以增强IVM的抗病毒疗效。研究结果首次揭示了IVM通过降低病毒复制并具有一定的直接灭活作用来抑制PEDV感染性的能力。所制备的IVM-NLCs具有153.5 nm的流体动力学直径、-31.5 mV的zeta电位、高包封率(95.72%)和载药量(11.17%)。IVM与脂质相互作用并以无定形状态被包裹在脂质载体中。此外,其在NLCs中的包封可增强药物内化。同时,IVM-NLCs在病毒RNA拷贝数方面抑制PEDV增殖达三个数量级,阻碍了活性氧的积累并减轻了PEDV感染引起的线粒体功能障碍。此外,IVM-NLCs显著降低了PEDV诱导的Vero细胞凋亡率。因此,与游离IVM相比,IVM-NLCs对PEDV表现出更优的抑制作用。综上所述,这些结果表明NLCs是一种高效的IVM递送系统,可通过增强细胞内摄取来提高其对PEDV的抗病毒疗效。

**关键词:** 伊维菌素;抗病毒;纳米结构脂质载体;猪流行性腹泻病毒;细胞内递送

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## 1. 引言

猪腹泻是影响养猪业的主要传染病之一,其中病毒性腹泻发病率最高、危害最严重[1]。冠状病毒是引起仔猪腹泻的重要病原体,主要包括猪流行性腹泻病毒(PEDV)、猪传染性胃肠炎病毒(TGEV)、猪德尔塔冠状病毒(PDCoV)和猪急性腹泻综合征冠状病毒(SADS-CoV)。目前,PEDV和TGEV是分布最广泛的猪腹泻病毒病原体[2]。PEDV是α冠状病毒属的成员,为有包膜的单股正链RNA病毒,可引起仔猪急性腹泻、呕吐和脱水,致死率高达90%,给全球养猪业造成重大经济损失[3-5]。现有的PEDV疫苗包括灭活疫苗和减毒疫苗,但这些疾病在养猪业中仍频繁发生,部分原因是新突变株的出现[6]. 在新发或再发疾病风险下,迫切需要开发新的抗病毒化合物[4,7,8]。

近年来,药物重定位已成为治疗新兴疾病的一种有吸引力的选择,因为针对特定病原体开发新的有效药物既耗时又昂贵[9]. 相比之下,已批准的药物易于获得,其潜在副作用也已得到充分表征[10]。药物重定位是将FDA批准或研究中的药物从其原始用途转换为新用途的策略[11]。重定位药物的最大优势是省略了关键且耗时的药物开发阶段,从而显著缩短了生产有效抗病毒药物所需的时间[12]。

伊维菌素(IVM)是一种经FDA批准的广谱、高效、低毒的抗寄生虫药物[13,14]。它是一种十六元环大环内酯类药物,生物活性广泛[15]。研究表明,它具有抗病毒的治疗潜力[16]。体外研究表明,IVM可有效限制多种RNA和DNA病毒的感染,包括HIV-1、登革病毒(DENV)、相关黄病毒、甲型流感和委内瑞拉马脑炎病毒(VEEV)[17-21]。近期研究表明,它是SARS-CoV-2的强效抑制剂[22]。然而,IVM在水中的溶解度低,仅为6-9微克/毫升,且生物利用度差,限制了其临床应用[23,24]。

纳米结构脂质载体是由固体脂质和液体脂质混合物组成的新一代脂质纳米粒[25]. 它是一种前沿的纳米递送系统,通过保护包封的生物活性化合物免受不利环境条件的影响并调节其释放,使其在正确的时间和部位发挥活性作用,从而增强其溶解度、稳定性和生物利用度[26-28]。

在本研究中,我们确定了IVM可抑制PEDV的感染性,然后配制纳米结构脂质载体可策略性地解决IVM溶解度低和生物利用度差的问题。结果表明,NLCs可通过改善细胞内递送来增强IVM的抗病毒活性。本研究旨在验证IVM-NLC作为PEDV替代治疗药物的潜力。

## 2. 材料与方法

### 2.1. 试剂、细胞和病毒 伊维菌素(IVM,91%)购自中国兽医药品监察所(北京,中国)。非洲绿猴上皮细胞(Vero)和PEDV毒株CV777(GenBank登录号:KT323979)由实验室保存。

### 2.2. IVM-NLCs的制备 采用高剪切超声和高压均质法制备IVM-NLCs[29,30]。简而言之,将一定量的油酸(OA)(阿拉丁,上海,中国)、棕榈酸(PA,阿拉丁,上海,中国)、吐温20(阿拉丁,上海,中国)和IVM混合作为油相,加热至70°C直至完全熔融。同时,将泊洛沙姆188(运宏化学制剂与辅料技术有限公司,上海,中国)溶于水作为水相,并在相同温度下加热。然后,在700 rpm磁力搅拌下将水相倒入油相中。随后,使用高剪切分散乳化机(FM200,IKA,Staufen,德国)在11,000 rpm下均质5分钟,然后使用超声波细胞破碎仪(JY96-II,Scientz,宁波,中国)在300 W下探针超声处理20分钟。将所得的油包水(O/W)乳液在高速剪切条件下快速转移至冷水中1分钟,冷却形成NLCs。将热的O/W体系在高压均质机(AH-BASIC,ATS,苏州,中国)中在700 bar下循环四次,得到IVM-NLCs。

### 2.3. IVM-NLCs的表征

#### 2.3.1. 流体动力学直径(HD)、多分散指数(PDI)和Zeta电位(ZP) 测量前,所有样品均用去离子水适当稀释。使用Zetasizer(Malvern Instruments Ltd.,Malvern,Worcestershire,UK)通过动态光散射(DLS)表征IVM-NLCs的HD、PDI和ZP。

#### 2.3.2. 透射电子显微镜(TEM) 通过TEM(Tecnai 12,Philips,Amsterdam,荷兰)观察IVM-NLCs的形态。简而言之,将稀释的IVM-NLCs滴在300目铜网上。干燥后,样品用2%(w/v)磷钨酸溶液负染2分钟。然后对干燥的样品进行TEM分析。

#### 2.3.3. X射线衍射(XRD)和傅里叶变换红外光谱(FT-IR) 使用XRD(D8 Advance,Bruker AXS,Karlsruhe,德国)研究PA、IVM、PA和IVM的物理混合物、冻干NLCs和IVM-NLC粉末,以分析IVM在NLC形成过程中晶体结构的变化。此外,将上述样品放入坩埚中并压紧在载玻片上。随后,使用Cu/Kα辐射源的XRD在40 kV/40 mA条件下以4°/min的速度在5°~50°范围内扫描。之后,使用FT-IR光谱仪(IS5&N380,Nicolet,Waltham,MA,USA)记录PA、IVM、IVM和PA的物理混合物、冻干NLCs和IVM-NLC粉末的红外光谱。在FT-IR光谱分析之前,将样品与溴化钾(KBr)以1:150(w/w)的比例混合,并使用高压液压机压成薄片。然后将制备的薄片样品置于FT-IR光谱仪上,在4000 cm⁻¹至500 cm⁻¹的波数范围内扫描。

#### 2.3.4. 包封率(EE)和载药量(DL) 通过超滤离心结合高效液相色谱(HPLC)测定IVM-NLCs的EE和DL。将稀释的IVM-NLCs加入甲醇中,涡旋并超声以破乳。离心上清液,通过HPLC测定乳液中IVM的重量(Wtotal)。此外,将IVM-NLCs的稀释液置于超滤离心管(MWCO:100 kDa,Millipore,Bilrika,MA,USA)中高速离心,通过HPLC测定乳液中游离IVM的重量(Wfree)。IVM-NLCs的DL和EE使用以下公式计算:

EE (%) = (Wtotal − Wfree) / Wtotal × 100%

DL (%) = (Wtotal − Wfree) / WNLCs × 100%

其中Wtotal是NLCs中应用的IVM总含量,Wfree是上清液中游离IVM的量,WNLCs是制备IVM-NLCs中使用的脂质含量。

### 2.4. 细胞培养 Vero细胞在杜尔贝科改良伊格尔培养基(DMEM,Gibco,Waltham,MA,USA)中培养,含1%青霉素-链霉素(HyClone,Logan,UT,USA)和5%胎牛血清(FBS)(Gibco,CA,USA)。细胞置于含5% CO₂的37°C加湿细胞培养箱中。

### 2.5. 细胞活力评估 使用Cell Counting Kit-8(CCK-8,KeyGen Biotech Co.,Ltd.,南京,中国)方法在Vero细胞中测试IVM和IVM-NLCs的细胞毒性。将Vero细胞以每孔10,000个细胞的密度接种于96孔板中,在100 µL新鲜培养基中过夜。接种后,用IVM和IVM-NLCs处理细胞24 h和48 h。随后,每孔加入CCK-8(10 µL/孔),在37°C下孵育1 h,并测量450 nm处的OD值。细胞活力使用以下公式计算:

细胞活力 (%) = (OD处理组 − OD空白组) / (OD未处理组 − OD空白组) × 100%

### 2.6. 体外细胞摄取 分别使用荧光显微镜(Thermo Fisher,Waltham,MA,USA)和流式细胞术(BD Biosciences,New York,NY,USA)对Vero细胞中香豆素-6(C6)的体外细胞摄取进行定性和定量评估。简而言之,将Vero细胞以每孔2×10⁵个细胞的密度接种于6孔培养板中并过夜孵育。然后用游离C6或C6-NLCs处理细胞,未做任何处理的细胞作为对照。4 h后,用冷PBS洗涤细胞,用4%多聚甲醛固定10-15分钟,用DAPI标记,并通过荧光显微镜观察。此外,为进一步研究C6和C6-NLCs的细胞摄取过程,在摄取终止后,用0.25%胰蛋白酶分离处理过的细胞,以1000 rpm离心5分钟,悬浮于PBS中,并通过流式细胞术分析细胞中的荧光信号。

### 2.7. TCID₅₀测定 为确定50%组织培养感染剂量(TCID₅₀),将PEDV样品用维持液10倍稀释并接种Vero细胞。简而言之,将Vero细胞接种于96孔板中过夜。然后弃去培养基,用维持液洗涤两次,每孔加入100 µL稀释的病毒液,阴性对照孔加入维持液。将细胞培养板置于37°C培养箱中孵育1 h。之后,弃去旧的维持液,加入100 µL维持液继续培养并观察细胞病变效应(CPE)。根据Reed-Muench方法计算TCID₅₀/mL。

### 2.8. 抗病毒测定 以0.05的感染复数(MOI)用PEDV感染细胞。1 h后,去除接种物,用无血清DMEM洗涤细胞。随后,将细胞分别与DMEM、NLCs、IVM和IVM-NLCs一起孵育。然后通过定量实时聚合酶链反应(RT-qPCR)、蛋白质印迹和间接免疫荧光测定(IFA)评估NLCs、IVM和IVM-NLCs对PEDV感染的抗病毒效果。

病毒感染每个阶段都可能存在抑制靶点[31,32]。为确定IVM在哪个阶段阻断感染,将IVM和PEDV以不同处理方式加入细胞:

**灭活测定:** 将IVM与PEDV的混合物在37°C下放置3 h。用预处理的PEDV感染Vero细胞1 h。孵育后,弃去培养基,更换为不含任何药物的维持液继续培养。提取总RNA并通过RT-qPCR定量。

**吸附测定:** 将Vero细胞在4°C下预冷,然后用5 µM IVM孵育1 h,再在4°C下用PEDV感染1 h。弃去上清液后,用预冷的无血清DMEM洗涤细胞两次。提取总RNA并通过RT-qPCR定量。

**侵入测定:** 在4°C下预冷后,将Vero细胞在4°C下用PEDV感染1 h。弃去上清液并用预冷的无血清DMEM洗涤后,将细胞在37°C下用含2% FBS的DMEM中的5 µM IVM处理1 h。提取总RNA并通过RT-qPCR定量。

**复制测定:** 将Vero细胞在37°C下用PEDV感染1 h。为去除未吸附的病毒颗粒,用预冷的无血清DMEM洗涤细胞,与DMEM一起孵育4 h,然后用5 µM IVM处理12 h。提取总RNA并通过RT-qPCR定量。

**释放测定:** 将Vero细胞在37°C下用PEDV感染10 h。弃去上清液,用无血清DMEM洗涤后,将细胞分别与含2% FBS的DMEM中的IVM一起孵育。提取总RNA并通过RT-qPCR定量。

### 2.9. 一步生长曲线 将80-90%汇合的Vero细胞用0.05 MOI的PEDV感染。随后,加入对照DMEM、NLCs、IVM和IVM-NLCs,在37°C下继续孵育。根据Reed-Muench方法在1、4、8、12、24、36、48、60和72 hpi记录TCID₅₀。计算PEDV滴度,并通过测定不同时间点的TCID₅₀绘制病毒生长曲线。

### 2.10. RT-qPCR RT-qPCR基于SYBR Green法。使用RNAiso Plus(Takara,东京,日本)按照制造商的方案从6孔板中的细胞中提取PEDV总RNA。通过Nanodrop(Thermo Fisher Scientific,Waltham,MA,USA)评估总RNA的浓度和纯度。使用cDNA合成试剂盒(Vazyme,南京,中国)将总RNA逆转录为cDNA并储存在-20°C。使用SYBR qPCR Master Mix(Vazyme,南京,中国)一式三份评估靶基因。绝对荧光定量参照文献[33]所述。

### 2.11. 蛋白质印迹分析 将Vero细胞在6孔板中培养至约80-90%汇合,并用0.05 MOI的PEDV感染。感染1 h后,将细胞单层与对照DMEM、NLCs、IVM和IVM-NLCs(5 µM)一起孵育24 h,然后用裂解缓冲液(100 µL/孔)处理以提取总蛋白,随后按照制造商的说明使用二辛可宁酸(BCA)蛋白测定试剂盒(Solarbio,北京,中国)定量蛋白浓度。将十二烷基硫酸钠(SDS)上样缓冲液加入收集的细胞提取物中并煮沸10分钟。将等量蛋白上样并在12%十二烷基硫酸钠聚丙烯酰胺凝胶电泳(SDS-PAGE)上电泳,然后转移到硝酸纤维素(NC)滤膜上,用5%脱脂牛奶封闭2 h。随后,检测PEDV N蛋白的表达。检测GAPDH的表达以代表相同的蛋白样品上样量。

### 2.12. IFA 通过免疫荧光进一步评估NLCs、IVM和IVM-NLCs对Vero细胞中PEDV的抑制作用。将24孔板中的Vero细胞用0.05 MOI的PEDV感染。孵育1 h后,通过充分洗涤去除游离病毒。然后,将细胞分别与对照DMEM(含2% FBS)或NLCs、IVM和IVM-NLCs一起孵育。24 h后,用4%甲醛固定细胞15分钟。用0.1% Triton X-100透化后,将细胞在4°C下与针对PEDV N蛋白的小鼠单克隆抗体(1:200稀释)一起孵育过夜,然后用含吐温20的磷酸盐缓冲液(PBST)洗涤三次,每次10分钟。然后,将细胞与FITC偶联的山羊抗小鼠抗体(1:200稀释)一起孵育1 h,并在室温下用DAPI复染10分钟。洗涤三次后,通过荧光显微镜获取照片。

### 2.13. 活性氧(ROS)生成测定 使用基于2',7'-二氯荧光素二乙酸酯(DCFH-DA)的ROS测定试剂盒(南京凯基生物技术有限公司,南京,中国)评估ROS水平。简而言之,将生长良好的Vero细胞接种于12孔板中,并将0.05 MOI的PEDV接种物(500 µL/孔)加入生长至80-90%融合的Vero细胞中。感染1 h后,洗涤细胞单层,然后分别用NLCs、IVM和IVM-NLCs覆盖。之后,将细胞在37°C避光条件下与DCFH-DA孵育20 min。在荧光显微镜下观察各组细胞的荧光变化(Ex = 488 nm,Em = 507 nm)(Thermo Fisher,MA,USA)。

### 2.14. 线粒体膜电位(MMP)分析 使用JC-1测定试剂盒(KeyGen Biotech Co.,Ltd.,南京,中国)检测MMP变化。将生长良好的Vero细胞接种于12孔板中,并将0.05 MOI的PEDV接种物(500 µL/孔)加入生长至80-90%融合的Vero细胞中。感染1 h后,洗涤细胞单层,然后用NLCs、IVM和IVM-NLCs覆盖。随后,用PBS洗涤细胞。将JC-1(10 µg/mL)加入各样品中,在37°C避光条件下孵育15 min。在荧光显微镜下观察各组细胞的荧光变化(绿色荧光,Ex = 488 nm,Em = 507 nm;红色荧光,Ex = 525 nm,Em = 590 nm)(Thermo Fisher,MA,USA)。

### 2.15. 凋亡测定 使用Annexin V-FITC/PI双染试剂盒(KeyGen Biotech Co.,Ltd.,南京,中国)按照制造商的说明评估PEDV感染的Vero细胞的凋亡率。将细胞接种于6孔板中,然后在避光条件下用Annexin V-FITC和PI染色。通过流式细胞术分析细胞(Ex = 488 nm,Em = 525 nm)。使用Cell-Quest软件(Becton Dickinson,San Jose,CA,USA)分析数据。

### 2.16. 统计分析 所有数据以平均值±标准差(SD)表示,实验一式三份进行。使用GraphPad Prism 8.0软件进行统计分析。两组之间的差异使用t检验评估(平均值±SD)。比较多组时,采用单因素方差分析(ANOVA)。统计学差异以* p < 0.05和** p < 0.01表示。

## 3. 结果与讨论

### 3.1. IVM抑制PEDV的感染性 近期大量研究报道了IVM的抗病毒特性,其可通过阻碍依赖于特定IMPα/β1的病毒蛋白的核输入来抑制病毒[2]。本研究在体外研究了IVM对PEDV的抗病毒活性。在评估其抑制效力之前,对Vero细胞进行了细胞毒性测定。结果表明,在0至10 µM浓度范围内,细胞活力保持在80%以上(图1A)。排除细胞毒性后,评估了IVM对PEDV感染的Vero细胞的抑制作用。具体而言,用0.05 MOI的PEDV感染Vero细胞,然后用不同浓度的IVM处理。此外,在2.5或5 µM IVM处理后,病毒对照组之间观察到明显差异,10 µM IVM处理后细胞活力可达80%以上,如图1B所示。我们计算了半数最大效应浓度(EC₅₀)值,该值反映了消除50%感染性病毒颗粒产生所需的IVM浓度。IVM在Vero细胞中感染PEDV后的EC₅₀值为4.63 µM(图1C)。此外,以1.25、2.5、5和10 µM浓度的IVM处理后,在感染后12 h,PEDV RNA N拷贝数分别从6.1降至5.8、5.5、4.8和3.8 lg拷贝,与未处理组相比(图1D)。

值得注意的是,PEDV核衣壳(N)蛋白是一种对病毒生命周期至关重要的RNA结合蛋白,可作为PEDV感染的精确早期诊断靶点[34,35]。通过检测PEDV N蛋白的表达水平验证了IVM对PEDV增殖的抑制作用。具体而言,将感染的细胞与不同浓度的IVM一起孵育。如图1E所示,在24 hpi时,通过间接免疫荧光在DMSO处理的PEDV感染的Vero细胞中观察到强荧光信号。然而,我们观察到未处理的感染细胞与IVM处理的感染细胞之间存在显著的浓度依赖性差异,这与病毒的生长曲线一致。

**图1. IVM抑制PEDV的感染性。** (A) 通过CCK-8测定在不同时间用不同浓度IVM处理的Vero细胞的细胞毒性。含0.05% DMSO(v/v)的培养基作为对照。(B) 通过CCK-8测定IVM的抗病毒活性。(C) IVM的EC₅₀使用GraphPad Prism 8.0计算。(D) 通过RT-qPCR检测经不同IVM处理后PEDV感染的Vero细胞的PEDV N RNA拷贝数。(E) 用不同浓度IVM处理或未处理的PEDV感染的Vero细胞的间接免疫荧光测定。蓝色,DAPI;绿色,FITC偶联的山羊抗小鼠抗体。比例尺= 50 µm。误差线表示三次重复实验的标准差。平均值通过单因素方差分析(ANOVA)计算(平均值±SD,n = 3)。* p < 0.05,** p < 0.01,与PEDV组相比。

### 3.2. IVM在PEDV生命周期不同阶段的作用 本研究通过分析IVM对PEDV复制周期增殖的影响,研究了其抗病毒特性的潜在机制。示意图如图2A所示。首先评估了IVM对PEDV的直接灭活潜力,结果显示通过RT-qPCR检测到的PEDV数量减少了10倍,如图2B所示。在PEDV的吸附过程中,实验组和对照组在抑制PEDV吸附方面无显著差异(图2C)。在PEDV的侵入过程中,结果显示IVM处理使感染性病毒滴度相对于对照组降低了约10倍(图2D),表明IVM对PEDV侵入有轻微影响。此外,如图2E所示,IVM将PEDV N RNA拷贝数降低了近10²倍,表明IVM可能主要通过抑制PEDV复制来抑制PEDV。此外,IVM对PEDV子代释放的影响如图2F所示。与对照组相比,PEDV的病毒滴度无明显差异,表明IVM对PEDV子代的释放无抑制作用。总之,IVM主要通过抑制病毒侵入和复制对PEDV发挥抑制作用,并在体外具有一定的直接灭活作用。

**图2. IVM在PEDV增殖抑制多个阶段的处理。** (A) IVM对PEDV复制周期影响的示意图。(B) IVM对PEDV直接灭活的影响。IVM对感染细胞的(C)吸附、(D)侵入、(E)复制和(F)释放过程的影响。平均值通过t检验计算(平均值±SD,n = 3)。* p < 0.05,** p < 0.01,与PEDV组相比。

### 3.3. 载伊维菌素纳米结构脂质载体的表征 通过高压均质技术制备的IVM-NLCs呈现均匀、不透明、乳白色液体特征,具有高流动性。IVM-NLCs的流体动力学直径(HD)和zeta电位(ZP)如图3A、B所示,呈窄正态分布。所制备的IVM-NLCs的HD为153.5 ± 0.80 nm,多分散指数(PDI)为0.153 ± 0.007,表明粒径分布均匀性高(表S1)。ZP也是评估胶体分散体系稳定性的关键因素。通常,当ZP的绝对值超过30 mV时,由于电排斥作用,纳米粒子体系可实现稳定分散[36]。IVM-NLCs的ZP为-31.5 ± 0.569 mV,表明具有良好的稳定性。使用透射电子显微镜(TEM)检查IVM-NLCs的形态,显示为球形或椭球形颗粒,粒径分布均匀,未见团聚现象(图3C)。IVM-NLCs的平均分布粒径为39.54 ± 9.17 nm(图3D)。值得注意的是,IVM-NLCs的粒径明显小于HD。造成这种差异的原因是动态光散射(DLS)通过检测水合状态下布朗运动引起的散射光强度波动来间接测量粒径,而TEM要求样品在测试时处于干燥状态[37,38]。

DL和EE是评估NLCs制备的重要参数。提高EE可增强药效并减少不良反应。提高DL可导致更稳定的制剂,同时减少赋形剂的使用及其潜在毒性。通过HPLC测定制备的IVM-NLCs的EE和DL分别为95.72 ± 0.30%和11.17 ± 0.75%(表S1)。所制备的IVM-NLCs基于实验室制备的IVM-SLNs[30]。与IVM-SLNs相比,IVM-NLCs具有更小的HD和更均匀的分布,从而提高了EE和DL。

**图3. 优化IVM-NLCs的表征。** (A) 流体动力学直径(HD)和(B) IVM-NLCs的zeta电位(ZP)通过DLS测定。(C) IVM-NLCs的形态通过TEM观察,(D) 粒径分布通过分析多个TEM图像中的颗粒获得。比例尺= 100 nm。(E) X射线衍射(XRD)图谱和(F) IVM-NLCs、NLCs、物理混合物、IVM和PA的傅里叶变换红外(FT-IR)光谱。

将药物从晶态转化为无定形态已被发现能够提高药物载量并改善纳米药物递送系统的稳定性[39]。X射线衍射图谱被用于晶体学分析[40]。如图3E所示,在伊维菌素(IVM)的衍射图谱中,可在10°、15°和20°附近观察到明显的衍射峰,表明IVM具有晶体结构。在PA与IVM的物理混合物XRD图谱中仍可观察到IVM的衍射峰。IVM-NLCs在10°附近的尖锐衍射峰显著消失,而15°和20°附近的特征衍射峰虽仍存在,但与IVM有所不同,这表明IVM在NLCs中发生了反应,削弱了其分子间作用力,IVM的结晶度也随之降低。此外,NLCs中观察到的衍射峰与IVM-NLCs一致,表明IVM以无定形形式分散在NLCs中。PA、IVM、IVM与PA的物理混合物、冻干粉IVM-NLC以及NLC粉末的FT-IR光谱如图3F所示。IVM-NLCs中1680 cm⁻¹处的C=C特征吸收峰消失,IVM基团在1050–1200 cm⁻¹处的C-O-C伸缩振动特征峰显著减弱;IVM在3650 cm⁻¹处的尖锐峰为醇羟基的伸缩振动峰,该峰在IVM-PA混合物和IVM-NLCs中同样出现;IVM在3468 cm⁻¹处具有羟基的O-H伸缩振动峰,IVM与PA的物理混合物亦然;而IVM-NLCs的O-H伸缩振动峰发生蓝移,表明药物与载体之间发生了结合,标志着纳米结构脂质载体的成功制备;IVM与IVM-NLCs的波形基本相似,表明脂质载体未改变IVM的骨架结构,IVM以非晶态形式包裹在脂质载体中。XRD与FT-IR结果一致,表明IVM在IVM-NLCs中由晶体转变为无定形态,并以无定形状态包封于纳米结构脂质基质中。

3.4. NLCs增强IVM的细胞摄取

由于病毒寄生于宿主细胞内,提高细胞内药物摄取可增强抗病毒疗效[41,42]。为评估IVM-NLCs与IVM的体外生物相容性,将Vero细胞与不同浓度的IVM或IVM-NLCs分别孵育24和48小时,进行细胞毒性检测。Vero细胞的结果如图S1所示。IVM-NLCs(0–10 µM)处理24和48小时后,细胞相对存活率均大于80%,表明IVM-NLCs具有良好的生物相容性。实验结果表明,与IVM相比,IVM-NLCs的生物相容性显著提高。此外,IVM-NLCs对Vero细胞的毒性呈现剂量和时间依赖性关系。如图4A所示的荧光显微镜结果显示,C6-NLCs比游离C6呈现更明显的荧光信号。此外,如图4B所示,C6-NLCs的荧光强度显著高于游离C6。如图4C所示,通过流式细胞术分析,C6-NLCs在Vero细胞中的平均荧光强度是游离C6的3.7倍。这些结果共同表明,NLCs作为递送载体具有增强IVM细胞摄取的潜力。

图4. NLCs对Vero细胞中香豆素-6(C6)细胞摄取的影响。(A)不同制剂在Vero细胞中摄取的代表性荧光显微镜图像。(B)通过流式细胞术检测Vero细胞经游离C6和C6-NLCs处理后C6的细胞摄取情况。(C)平均细胞内荧光强度。比例尺=50 µm。均值通过t检验计算(均值±SD,n=3)。** p < 0.01,C6-NLCs与游离C6比较。

3.5. NLCs增强IVM对PEDV的抗病毒活性

本研究首先通过CCK-8检测评估了IVM-NLCs对PEDV感染的Vero细胞活力的影响(图S1)。IVM-NLCs对PEDV感染的Vero细胞的抑制作用如图S2所示。IVM-NLCs在PEDV感染的Vero细胞中的EC50值为3.57 µM(图5A)。IVM-NLCs的EC50值低于IVM,证实IVM-NLCs比IVM具有更高的抗病毒活性。图5B所示结果表明,与游离IVM相比,NLCs在处理后48小时提高了Vero细胞的活力。为评估NLCs、IVM和IVM-NLCs对PEDV复制的影响,通过测定经每种制剂5 µM处理后的PEDV病毒滴度,绘制了一步生长曲线。如图5C所示,在12 hpi时,PEDV开始增殖,从24 hpi到48 hpi进入快速增殖期,在60 hpi达到峰值病毒滴数10⁶·⁵ TCID₅₀/0.1 mL。60小时后,由于细胞病变,PEDV增殖下降。与阴性对照组相比,经IVM-NLCs处理的细胞中观察到显著的病毒滴度抑制。因此,PEDV滴度的变化证实了IVM-NLCs确实具有优于IVM的抗病毒活性,可抑制病毒复制。

图5. IVM-NLCs对Vero细胞的抗PEDV活性。(A)IVM-NLCs的EC50通过GraphPad Prism 8.0计算。(B)通过CCK-8检测NLCs、IVM和IVM-NLCs(5.0 µM)的抗病毒活性。(C)经NLCs、IVM和IVM-NLCs处理或未处理的一步病毒生长曲线。(D)通过RT-qPCR检测经NLCs、IVM和IVM-NLCs处理后PEDV感染的Vero细胞中PEDV N RNA拷贝数。(E)Western blot分析NLCs、IVM和IVM-NLCs处理下PEDV N蛋白的表达水平。(F)感染细胞的间接免疫荧光检测。蓝色,DAPI;绿色,FITC标记的羊抗鼠抗体。(G)不同处理后感染细胞中活性氧(ROS)水平。(H)不同处理后感染细胞的线粒体膜电位(MMP)。比例尺=50 µm。误差线代表三次重复实验的标准差。均值通过单因素方差分析(ANOVA)计算(均值±SD,n=3)。* p < 0.05,** p < 0.01。

此外,RT-qPCR分析显示,如图5D所示,IVM-NLCs对PEDV N RNA拷贝数的降低作用更为显著。为验证IVM-NLCs对PEDV增殖的抑制作用,我们评估了PEDV N蛋白的表达水平。具体而言,Western blot检测表明,经IVM-NLCs处理后,PEDV N蛋白的表达水平显著降低(图5E)。尽管在IVM和IVM-NLCs处理组中均观察到PEDV N蛋白表达的下调,但在IVM-NLCs处理组中效果更为明显。此外,我们将感染细胞与NLCs、IVM和IVM-NLCs共同孵育。在24 hpi时,通过IFA在PEDV感染的Vero细胞中观察到强烈的荧光信号。然而,如图5F绿色荧光所示,IVM-NLCs处理组与未处理的PEDV感染组在感染细胞数量上存在显著差异。这些结果共同表明,NLCs可能增强IVM对PEDV的抗病毒活性。

活性氧(ROS)是细胞代谢的有毒副产物,主要由哺乳动物细胞线粒体产生,参与调节细胞的多种生理功能[43]。我们研究了IVM-NLCs对PEDV感染期间ROS产生的影响。如图5G所示,我们的结果显示,感染的Vero细胞中DCF荧光强度显著增加。相反,与单独使用IVM处理的细胞相比,经IVM-NLCs处理的细胞ROS生成显著减少。结果表明,ROS参与了IVM-NLCs的抗病毒作用。ROS会导致线粒体膜损伤,引起MMP紊乱[44]。在正常细胞中,JC-1发出红色荧光。而在PEDV感染的Vero细胞中,JC-1呈现绿色荧光,表明PEDV破坏了Vero细胞的线粒体膜电位,导致其下降。经IVM-NLCs处理后,线粒体膜电位得到显著恢复(图5H)。总之,与IVM相比,IVM-NLCs能够改善对MMP损伤的抑制,并阻碍感染Vero细胞中ROS的积累。

3.6. IVM-NLCs对PEDV感染Vero细胞凋亡率的影响

为探究伊维菌素抑制PEDV的机制,使用AnnexinV-FITC/PI试剂盒通过流式细胞术检测细胞凋亡。结果显示,PEDV可诱导20.9 ± 1.89%的凋亡率(图6A),而IVM和IVM-NLCs处理的PEDV感染组凋亡率分别显著降低至16.4 ± 1.17和13.9 ± 1.59(图6B),表明它们在PEDV诱导的凋亡中发挥重要的生物学功能。这些发现表明,IVM-NLCs通过改善对MMP损伤的抑制,减少PEDV感染Vero细胞中ROS的积累,从而降低感染细胞的凋亡率。

图6. IVM-NLCs处理后PEDV感染Vero细胞的凋亡。(A)PEDV感染的Vero细胞经NLCs、IVM(5 µM)和IVM-NLCs(5 µM)处理后的凋亡检测。(B)柱状图表示处理后Vero细胞的凋亡百分比。均值通过单因素方差分析(ANOVA)计算(均值±SD,n=3)。** p < 0.01。

4. 结论

本研究首次证实了IVM在体外对PEDV的抑制作用。IVM可通过直接灭活病毒颗粒和抑制复制阶段来抑制PEDV。随后,成功开发了具有优良理化性质和增溶效果的IVM-NLCs,其可作为有前景的纳米载体,提高IVM的溶解度和药理疗效。根据生物学测试,IVM-NLCs比游离IVM表现出更强的抗PEDV活性,并减轻了PEDV诱导的线粒体功能障碍,从而阻止ROS生成并提高感染Vero细胞的活力。此外,IVM-NLCs还降低了PEDV诱导的细胞凋亡率。鉴于体外结果,有必要尽快开展体内实验,以探索其在PEDV临床治疗中的潜力。因此,IVM-NLCs被证实是一种潜在的抗PEDV药物,可能为开发拮抗PEDV的新型药物提供基础。