Advancements in Inhalation Technologies for Pulmonary Delivery of Protein Therapeutics

✅ 全文

用于蛋白质治疗药物肺部递送的吸入技术进展

作者 Mayumi Ikeda-Imafuku; Hiroko Fukuda; Tatsuya Fukuta; Kazunori Kadota 期刊 Chemical and Pharmaceutical Bulletin 发表日期 2025 ISSN 0009-2363 DOI 10.1248/cpb.c25-00532 类型 原创研究 (Original Research)

📄 英文摘要 English Abstract

EN

Inhalation delivery of protein therapeutics has emerged as a promising non-invasive alternative to traditional injectable formulations that offers potential for both localized and systemic treatment of pulmonary diseases. This review comprehensively summarizes the current advances in inhalable protein formulations, with emphasis on design strategies, formulation technologies, barriers to effective delivery, and disease-specific applications. Key aspects include the role of particle size, surface charge, and protein engineering in optimizing lung deposition and cellular uptake, as well as techniques such as spray freeze drying and PEGylation to enhance protein stability. The review also explores novel therapeutic approaches that target cystic fibrosis, asthma, idiopathic pulmonary fibrosis, chronic obstructive pulmonary disease, lung infections, and cancer, including the use of antibodies, nanobodies, exosomes, and albumin-based carriers. Clinical translation remains limited, but ongoing innovation in delivery systems and molecular design is thought to hold significant promise for expanding the therapeutic landscape of inhaled protein drugs.

📄 中文摘要 Chinese Abstract

中文
吸入给药蛋白疗法已成为传统注射制剂的一种有前景的无创替代方法,为肺部疾病的局部和全身治疗提供了潜力。本综述全面总结了可吸入蛋白制剂的最新进展,重点阐述了设计策略、制剂技术、有效递送的障碍以及疾病特异性应用。关键方面包括粒径、表面电荷和蛋白工程在优化肺部沉积和细胞摄取中的作用,以及喷雾冷冻干燥和PEG化等技术在提高蛋白稳定性方面的应用。

📋 英文结构化总结 English Structured Summary

全文整理

EN

Background:

Inhalation delivery of protein therapeutics has emerged as a promising non-invasive alternative to traditional injectable formulations that offers potential for both localized and systemic treatment of pulmonary diseases. This review comprehensively summarizes the current advances in inhalable protein formulations, with emphasis on design strategies, formulation technologies, barriers to effective delivery, and disease-specific applications. Key aspects include the role of particle size, surface charge, and protein engineering in optimizing lung deposition and cellular uptake, as well as techniques such as spray freeze drying and PEGylation to enhance protein stability.

Methods:

N/A - Review article

Results:

The review highlights that protein-based inhalation formulations include therapeutic antibodies, cytokines, enzymes, and other bioactive proteins, as well as protein-based drug carriers. Modifications to aerodynamic particle size, surface charge, and hydrophobicity greatly influence adhesion to alveolar epithelial cells and endocytosis efficiency. Barriers to pulmonary delivery include metabolic enzymes (e.g., neutrophil elastase, MMP-2, MMP-9) and protein aggregation induced by physical stresses such as spray drying or nebulization. Alternative technologies like lyophilization and freeze spray drying, along with excipients such as trehalose, mannitol, and amino acids, are used to avoid thermal denaturation and stabilize proteins.

Data Summary:

Among FDA-approved protein therapeutics across all routes of administration, monoclonal antibodies represent the largest proportion, accounting for approximately half of the total. Typical spray-drying processes involve drying temperatures ranging between 60 and 100 °C, which can cause irreversible heat-induced denaturation of proteins. The inclusion of albumin as an excipient has been reported to reduce particle aggregation, enhance spherical morphology and uniformity, and improve respirable deposition.

Conclusions:

Clinical translation remains limited, but ongoing innovation in delivery systems and molecular design is thought to hold significant promise for expanding the therapeutic landscape of inhaled protein drugs. The review also discusses the challenges and future of the clinical translation of protein-based nanoparticles.

Practical Significance:

The review explores novel therapeutic approaches that target cystic fibrosis, asthma, idiopathic pulmonary fibrosis, chronic obstructive pulmonary disease, lung infections, and cancer, including the use of antibodies, nanobodies, exosomes, and albumin-based carriers. Pulmonary delivery aimed at achieving systemic effects has been primarily investigated in the context of treatment for diabetes, particularly with insulin and other related peptides (e.g., Afrezza®).

📋 中文结构化总结 Chinese Structured Summary

中文

背景:

吸入给药蛋白疗法已成为传统注射制剂的一种有前景的无创替代方法,为肺部疾病的局部和全身治疗提供了潜力。本综述全面总结了可吸入蛋白制剂的最新进展,重点阐述了设计策略、制剂技术、有效递送的障碍以及疾病特异性应用。关键方面包括粒径、表面电荷和蛋白工程在优化肺部沉积和细胞摄取中的作用,以及喷雾冷冻干燥和PEG化等技术在提高蛋白稳定性方面的应用。

方法:

不适用——综述类文章

结果:

本综述强调,基于蛋白的吸入制剂包括治疗性抗体、细胞因子、酶及其他生物活性蛋白,以及基于蛋白的药物载体。空气动力学粒径、表面电荷和疏水性的修饰显著影响与肺泡上皮细胞的黏附及胞吞效率。肺部递送的障碍包括代谢酶(如中性粒细胞弹性蛋白酶、MMP-2、MMP-9)以及由喷雾干燥或雾化等物理应力引起的蛋白聚集。替代技术如冷冻干燥和喷雾冷冻干燥,以及海藻糖、甘露醇和氨基酸等辅料,被用于避免热变性并稳定蛋白。

数据概要:

在所有给药途径的FDA批准蛋白治疗药物中,单克隆抗体占比最大,约占总数的二分之一。典型的喷雾干燥工艺涉及60至100°C的干燥温度,可能导致蛋白的不可逆热诱导变性。据报道,添加白蛋白作为辅料可减少颗粒聚集,增强球形形态和均匀性,并改善可吸入沉积率。

结论:

临床转化仍然有限,但递送系统和分子设计的持续创新被认为在拓展吸入蛋白药物的治疗前景方面具有重要潜力。本综述还讨论了基于蛋白的纳米颗粒临床转化面临的挑战与未来展望。

实践意义:

本综述探讨了针对囊性纤维化、哮喘、特发性肺纤维化、慢性阻塞性肺疾病、肺部感染和癌症的新型治疗方法,包括抗体、纳米抗体、外泌体和白蛋白基载体的应用。旨在实现全身效应的肺部递送主要在糖尿病治疗领域进行了研究,尤其是胰岛素及其他相关肽类药物(如Afrezza®)。

📖 英文全文 English Full Text

EN

Chem. Pharm. Bull. 74, 28–36 (2026) Vol. 74, No. 1 https://doi.org/10.1248/cpb.c25-00532 Current Topics

Introduction to Various Inhaled Formulation Technologies Supporting Diverse Therapeutic Modalities Review

Advancements in Inhalation Technologies for Pulmonary Delivery of Protein Therapeutics Mayumi Ikeda-Imafuku,* Hiroko Fukuda, Tatsuya Fukuta, and Kazunori Kadota* Department of Physical Pharmaceutics, School of Pharmaceutical Sciences, Wakayama Medical University, 25–1 Shichibancho, Wakayama 640–8156, Japan. * Correspondence: imayu@wakayama-med.ac.jp; kazunori-kadota@wakayama-med.ac.jp Received July 31, 2025 Inhalation delivery of protein therapeutics has emerged as a promising non-invasive alternative to traditional injectable formulations that offers potential for both localized and systemic treatment of pulmonary diseases. This review comprehensively summarizes the current advances in inhalable protein formulations, with emphasis on design strategies, formulation technologies, barriers to effective delivery, and diseasespecific applications. Key aspects include the role of particle size, surface charge, and protein engineering in optimizing lung deposition and cellular uptake, as well as techniques such as spray freeze drying and PEGylation to enhance protein stability. The review also explores novel therapeutic approaches that target cystic fibrosis, asthma, idiopathic pulmonary fibrosis, chronic obstructive pulmonary disease, lung infections, and cancer, including the use of antibodies, nanobodies, exosomes, and albumin-based carriers. Clinical translation remains limited, but ongoing innovation in delivery systems and molecular design is thought to hold significant promise for expanding the therapeutic landscape of inhaled protein drugs. Key words

der inhaler (DPI) delivery, including the use of PEGylation. Finally, we discuss the challenges and future of the clinical translation of protein-based nanoparticles.

The development of therapeutic agents utilizing proteins as active pharmaceutical ingredients has accelerated in recent years, driven by advances in biopharmaceuticals.1,2) Intravenous administration has traditionally been the primary route for protein-based formulations. However, as an efficient, non-invasive alternative, inhalation of proteins has gained increasing attention.3) The lungs provide an ideal site for drug absorption due to their large surface area, extensive vascularization, and the ability to bypass first-pass metabolism.4) Nonetheless, pulmonary administration of proteins presents several challenges, including enzymatic degradation, particle deposition, and potential immune responses. In practice, many protein-based inhalation therapies under development are designed to exert their effects locally within the lungs. Pulmonary delivery aimed at achieving systemic effects has been primarily investigated in the context of treatment for diabetes, particularly with insulin and other related peptides (e.g., Afrezza®).5) In this review, we summarize the latest research trends in protein inhalation formulations, focusing on design principles, formulation technologies, immunological safety, and diseasespecific applications. We also highlight recent advances in drying techniques and nanoparticle engineering for dry pow- 2.

Protein-based inhalation formulations include therapeutic antibodies, cytokines, enzymes, and other bioactive proteins, as well as protein-based drug carriers. Among U.S. Food and Drug Administration (FDA)-approved protein therapeutics across all routes of administration, monoclonal antibodies represent the largest proportion, accounting for approximately half of the total.6) Other approved protein drugs include coagulation factors, enzymes, fusion proteins, hormones, vehicles, and growth factors. When used as drug delivery carriers, proteins are valued for their high biocompatibility and biodegradability. Serum albumin as an endogenous component in human serum has been extensively studied as a drug carrier due to its high drug-binding capacity, favorable permeability, and low immunogenicity.7,8) Serum albumin has also been well studied in nanoformulations, which are used to improve uptake and drug loading.9–11) Other proteins from natural products, such as silk fibroin and gelatin, have also attracted attention as formulation materials capable of modulating particle rigidity and disintegration properties.12–14)

© 2026 The Author(s). This is an open access article distributed under the terms of Creative Commons Attribution-NonCommercial 4.0 License (https://creativecommons.org/licenses/by-nc/4.0/). Published by The Pharmaceutical Society of Japan. 28

Chem. Pharm. Bull. Vol. 74, No. 1 (2026) been comprehensively reviewed elsewhere.20) Unlike intravenously injectable formulations, there are currently no clear regulatory standards regarding protein aggregates in inhalable products. The establishment of new guidelines for both formulation design and analytical evaluation is therefore urgently required. 3.3. Interfacial Stress during Inhalation Interfacial stress in inhalation formulations refers to the physicochemical impact of drugs or nanoparticles on the pulmonary air–liquid interface, particularly the surfactant film lining the alveoli. To assess the ‘interfacial stress’ exerted by inhaled aerosols on lung surfactant function, Bäckman et al. developed a modified constrained drop surfactometer (CDS), which enabled quantification of drug or particle effects via surface tension.26) Micronized albumin was demonstrated to impair surfactant function, with minimum surface tension exceeding 10 mN/m, thereby compromising interfacial stability. In contrast, inhaled corticosteroids and lactose did not exhibit such effects. The surface activity of protein-based formulations is suggested by these findings to interfere with pulmonary surfactant function, which highlights the importance of CDS-based evaluation in toxicity assessment. Surface charge is also a critical parameter influencing interfacial stress. Positively charged nanoparticles reportedly electrostatically interact with pulmonary surfactant, forming microscale particle–vesicle complexes.27) Such aggregationinduced structural alterations are thought to impair the biophysical function of the surfactant layer. 3.4. Control of Particle Distribution In inhalation formulations, a particle size range of 1–5 µm is considered to be optimal for pulmonary deposition, and a narrow particle size distribution, reflected by a low geometric standard deviation, contributes to consistent inhalation performance.24) Particles that are too large tend to deposit in the oropharyngeal region, while those that are too small are likely to be exhaled before reaching the lungs. Precise control of the aerodynamic particle size is therefore critical. To investigate the impact of initial particle size, paclitaxel was encapsulated in albumin microparticles of 0.5, 1.0, and 3.0 µm, and formulated into dry powders with a consistent aerodynamic diameter (approx. 5 µm).28) Their intrapulmonary distribution and antitumor activity were assessed in a murine lung cancer model. The formulations prepared from particles with initial sizes of 1.0–3.0 µm demonstrated sustained drug release and prolonged pulmonary retention, which resulted in good therapeutic outcomes. These findings underscore the significance of the initial particle size as a critical factor in the therapeutic efficacy of inhalable formulations and they highlight the need to carefully consider this parameter during formulation design and quality control.

Modifications to aerodynamic particle size, surface charge, and hydrophobicity are well known to greatly influence adhesion to alveolar epithelial cells and the efficiency of endocytosis, primarily by affecting the interaction with and penetration through the mucus layer.15) These design parameters also affect the site of particle deposition (e.g., bronchi vs. alveoli) and the risk of clearance by alveolar macrophages. Additionally, proteins have been used as excipients in some formulations. For example, the inclusion of albumin as an excipient has been reported to reduce particle aggregation, to enhance spherical morphology and uniformity, and to improve respirable deposition.16)

3.1. Enzymes The lungs contain a variety of metabolic enzymes, including CYPs and esterases, which can significantly affect the local efficacy, systemic exposure, and safety of administered drugs.17) Neutrophil elastase, a serine protease stored in the primary granules of neutrophils, plays a critical role in host defense against bacterial infections.18) Neutrophil elastase transcriptionally and post-translationally activates mucin genes, thereby inducing excessive production and secretion of airway mucus. Its secretion is elevated in pulmonary diseases such as cystic fibrosis, chronic obstructive pulmonary disease (COPD), and in acute lung injury.18,19) Matrix metalloproteinases (MMPs), particularly MMP-2 and MMP-9, are upregulated in acute respiratory distress syndrome and act as key mediators of tissue damage and inflammatory amplification.19) These proteolytic enzymes may impair the therapeutic efficacy of protein-based inhalation formulations. The expression of these enzymes can vary depending on the pathological condition, so it is crucial to perform disease-specific evaluations during formulation development. 3.2. Aggregation Protein aggregation is a major difficulty in the development of inhalable protein formulations. Physical stresses associated with spray drying or nebulization (i.e., shear forces, thermal exposure, air-liquid interfacial stress, and rapid dehydration) can induce structural denaturation and aggregation, potentially leading to local immune responses or toxicity in the lungs.20) Depending on the size and type of aggregates, clearance by alveolar macrophages may be hindered, so there are concerns about the induction of chronic inflammation. In the preparation of DPIs, thermal denaturation is a concern when drying is performed using an oven.21) Typical spray-drying processes involve drying temperatures ranging between 60 and 100 °C, which can cause irreversible heatinduced denaturation of proteins.22–24) To avoid such thermal degradation, there are some promising alternative technologies, such as lyophilization and freeze spray drying.21,25) Other stabilization strategies include the addition of excipients such as trehalose, mannitol, and amino acids (e.g., glycine) to preserve hydrogen bonding and suppress structural denaturation.24) Such additives are particularly effective due to their ability to replace water molecules through hydrogen bonding (the water replacement hypothesis) and to form a glassy matrix upon drying, thereby restricting molecular mobility and stabilizing protein structure. Alternatively, hydrophobic polymers and surfactants may be employed to prevent denaturation at the air–liquid interface. The risks and mechanisms of protein aggregation in inhalation formulations have

4.1. Drying Methods for Protein Drugs in DPI Formulations Several drying techniques have been explored for the development of protein-based dry powder inhalers, including lyophilization, spray drying, spray freeze drying (SFD), and supercritical fluid (SCF) drying (Fig. 1). Among them, SFD has been suggested to have considerable promise for particle engineering and inhalation applications because it has the advantage of preventing protein aggregation. In addition, emerging methods, such as supercritical drying, are gaining atten29

Difference in the Drying Process for DPI Formulation tion as potential alternatives.29) The choice of drying method should be optimized based on the physicochemical properties of the protein, the selected excipients, and the intended therapeutic application. In spray drying, atomized liquid droplets are dried by exposure to hot air, often yielding uniform, spherical particles with good aerodynamic properties.30,31) In protein formulation, parameters such as the protein concentration during atomization greatly influence the resulting particle morphology and aerosolization efficiency, as shown in studies that used serum albumin.32) SFD, in contrast, subjects the formulation to much lower thermal stress than conventional spray drying, and it tends to produce porous particles that are favorable for inhalation.33,34) Compared with conventional freeze drying, SFD has also been shown to reduce oxidation in lipid-based systems, which suggests additional potential advantages in preventing protein oxidation.35) As an example of SFD for inhalable protein formulation, Ito et al. successfully formulated a decoy protein as a DPI using SFD (while preserving antibody activity) by incorporating trehalose and leucine as stabilizing excipients.36) In comparison of SFD and spray drying using deoxyribonuclease, Maa et al. found that spray drying produced small, dense particles of approximately 3 µm, while SFD produced particles of approximately 8–10 µm, which were porous. SFD was therefore superior to spray drying in terms of aerosolization, and the aerodynamic particle size of the particles produced by SFD was smaller.37) SCFs, such as carbon dioxide, exist under conditions above their critical temperature and pressure, and they exhibit properties of both gases and liquids.38) In supercritical drying, a transition from liquid to SCF and then to the vapor phase is used to precipitate and dry the protein by exploiting the antisolvent effect of SCFs.29) This technique allows precise control over particle formation and it has gained attention as a viable drying method for protein inhalation formulations. The drying method was shown in studies on whey protein aerogels to significantly influence the structural, adsorptive, and mechanical properties.39) Compared with freeze drying, supercritical drying produced denser aerogels with higher oil retention capacity. Lyophilization remains the most widely used drying technique for injectable protein formulations. Although it typically results in solid cakes that are less amenable to particle design,

it can be suitable in certain nanoparticle-based formulations, such as lysozyme.40) Nebulizers mechanically generate aerosols from liquid formulations, making them suitable for patients with limited inspiratory capacity. In contrast, DPIs offer advantages in portability and storage stability, but their efficacy depends on the patient’s ability to generate sufficient inspiratory flow. With recent advancements in powder formulation technologies, DPIs have gained attention for delivering proteins and nanoparticle-based drugs, which has led to a decline in the use of nebulizers for formulation development. Nonetheless, nebulizers remain widely used in basic research due to their simplicity and the ease of administration.41)

5. Inhalable Protein-Based Therapies for Lung Local Diseases

5.1. Cystic Fibrosis Cystic fibrosis is a genetic disorder caused by mutations in the cystic fibrosis transmembrane conductance regulator protein, leading to the accumulation of viscous mucus in the lungs and resulting in chronic infection and inflammation.42) Effective management requires strategies to enhance mucus clearance, control infection, and restore cystic fibrosis transmembrane conductance regulator function. Alpha-1 antitrypsin (AAT) is a serine protease inhibitor that protects tissues from esterases derived from neutrophils and other inflammatory cells. AAT deficiency is associated with the development of pulmonary emphysema. Griese et al. investigated the pulmonary administration of AAT in patients with cystic fibrosis. No significant improvement was seen in lung function, but there were reductions in elastase activity, pro-inflammatory cytokines, and enhancements in bactericidal capacity.43) Two inhalation modes were tested via a SMART CARD-connected device (AKITA1 inhalation device with a Pari LC Plus, or a Pari LC Star nebulizer), and there were no differences in outcomes. Although subsequent clinical development of AAT for cystic fibrosis has slowed, its inhalational pre-treatment has shown promising anti-inflammatory and cytoprotective effects in models of acute lung injury induced by toxic gases such as phosgene, which suggests potential applications in other pulmonary diseases.44) Recombinant human deoxyribonuclease I (rhDNase, Pulmozyme®) is approved in many countries as an inhaled therapeutic for cystic fibrosis. Its efficacy in reducing mucus viscosity and improving lung function has been shown in clinical stud30

ies. Frederiksen et al. reported that 12 months of rhDNase inhalation significantly improved forced expiratory volume in 1 s (FEV1) and that it reduced the incidence of respiratory infections, including those caused by Staphylococcus aureus, potentially contributing to the slowing of disease progression.45) A biosimilar drug, Tigeras®, has also been developed, and has been shown to be both effective and safe.46) Lactoferrin is an approx. 83 kDa glycoprotein with antimicrobial, anti-inflammatory, and immunomodulatory activities, and it has attracted attention as a candidate for inhaled therapy in patients with cystic fibrosis.47) Marshall et al. developed spray-dried powder formulations containing lactoferrin or apolactoferrin combined with aminoglycoside antibiotics (tobramycin or gentamicin), and tested them in cystic fibrosis lung infection models.48) These formulations demonstrated multiple beneficial effects, including inhibition of biofilm formation, disruption of existing biofilms, and enhanced antibiotic penetration. The resulting particles measured between 1.5–1.9 µm, with 90% being under 5 µm, which indicates good aerosolization and suitability for inhalation. This combination is thought to represent a promising protein-based DPI candidate for the treatment of chronic infections in patients with cystic fibrosis. ALX-009, an inhalable formulation combining lactoferrin and hypothiocyanite, exhibited potent bactericidal activity against Pseudomonas aeruginosa and Burkholderia cepacia complex in sputum samples of patients with cystic fibrosis.49) ALX-009 has shown superior antibacterial activity to tobramycin, with enhanced effects observed upon twice-daily administration. ALX-009 is suggested by these results to be a promising therapeutic option for multidrug-resistant infections in cystic fibrosis. Additionally, lactoferrin has been demonstrated to have protective effects in models of acute respiratory distress syndrome and oxygen toxicity, so there is potential utility in severe respiratory diseases beyond CF.50) 5.2. Idiopathic Pulmonary Fibrosis Inhaled interferongamma (IFN-γ) is a cytokine with both antifibrotic properties and macrophage-activating functions, and it has attracted interest as a potential therapeutic agent for idiopathic pulmonary fibrosis. Nebulized administration of IFN-γ reportedly suppressed the transforming growth factor-beta (TGF-β) signaling pathway and inhibited fibrosis progression in the lungs.51,52) In a safety study involving patients with idiopathic pulmonary fibrosis over an 80-week period, bronchoalveolar lavage fluid IFN-γ concentrations were shown to have increased by 60-fold. This was accompanied by a reversal of the declining trends in diffusing capacity of the lungs for carbon monoxide and total lung capacity. Systemic exposure was minimal, and no adverse events were observed. Subcutaneous administration had previously shown no clinical benefit, and there was no detection of IFN-γ in bronchoalveolar lavage fluid, so these findings highlight the significance of direct pulmonary delivery via inhalation. PRS-220 is an inhaled Anticalin® protein that targets CCN2 (formerly known as connective tissue growth factor, or CTGF). In preclinical idiopathic pulmonary fibrosis models, PRS-220 demonstrated greater antifibrotic efficacy than systemically administered antibodies.53) Due to its selective pulmonary distribution and low systemic exposure, PRS-220 also exhibited a favorable safety profile. Notably, in ex vivo and human lung tissue slice models, PRS-220 showed stronger antifibrotic activity than other therapeutic agents such as nint-

edanib and pamrevlumab. These results underscore the potential of PRS-220 as a promising inhaled protein-based therapy for idiopathic pulmonary fibrosis, offering both efficient lung delivery and a potent therapeutic effect. 5.3. Asthma The therapeutic potential of inhaled interferon-λ2/3 (IFN-λ2/3) in an allergen-induced asthma model was investigated by Won et al.54) Administration of IFN-λ2/3 after asthma onset led to a marked reduction in airway inflammation and hyperresponsiveness. Inhalation of IFN-λ significantly suppressed pro-inflammatory cytokines associated with T-helper 2 (Th2) and Th17 responses (including interleukin (IL)-4, IL-5, IL-13, and IL-17A) and also promoted an anti-inflammatory response characterized by an increase in IL-10-producing CD4+ T cells. IFN-λ may therefore serve as a promising inhaled protein-based therapeutic candidate for asthma management. Nanobodies, which are small antibody fragments (approx. 15 kDa) composed of the variable region of antibodies, offer advantages for inhalation therapy due to their high pulmonary distribution and intrinsic stability.55) LQ036, a nanobody that targets the α1 chain of the IL-4 receptor (IL-4Rα1), significantly suppressed airway inflammation, goblet cell hyperplasia, and immunoglobulin E (IgE) production in a humanized asthma model.56) Inhaled administration of LQ036 resulted in high local concentration and prolonged retention within the lungs. Compared with full-length antibodies, fragmented antibodies such as nanobodies exhibit reduced aggregation tendencies, making them attractive candidates for inhaled delivery systems. Depemokimab (GSK3511294) is a long-acting monoclonal antibody with high affinity for IL-5, and it has been shown to significantly reduce exacerbations in patients with severe eosinophilic asthma when administered subcutaneously once every six months (Phase III, NCT04719832).57) Although Depemokimab itself has not been developed for inhalation, studies have demonstrated that inhaled anti–IL-5 monoclonal antibodies can significantly attenuate airway inflammation and hyperresponsiveness in allergen-induced asthma mouse models.58) Inhalation may therefore offer therapeutic efficacy comparable to that of intravenous administration. IL-33 is a key cytokine involved in mucosal inflammatory diseases, including asthma. A human-derived, inhalable single-domain antibody (UdAb A12) that selectively inhibits IL-33 signaling was developed by Huange et al. In an allergic airway inflammation model, UdAb A12 exhibited strong anti-inflammatory effects. Compared with the control immunoglobulin G (IgG) antibody itepekimab, UdAb A12 demonstrated superior pulmonary distribution and local efficacy, which indicates its potential as a novel platform for inhaled antibody therapeutics.59) 5.4. COPD DAS181 is an inhalable fusion protein composed of a human epithelial growth factor and a bacterial sialidase. It was designed to inhibit viral entry into host cells. Inhaled administration of DAS181 in a COPD mouse model (cigarette smoke exposure combined with influenza infection) effectively suppressed pneumonia progression, reduced viral load, inhibited pro-inflammatory cytokines (IL-6, IL-1β, and tumor necrosis factor (TNF)), and preserved lung function, as indicated by maintained pulmonary compliance.60) Furthermore, DAS181 modulated the expression of immunoregulatory Siglecs in lung macrophages and promoted memory T cell re31

sponses, which suggests enhanced protection against reinfection. Compared with oseltamivir, DAS181 exhibited superior efficacy in suppressing pneumonia. These findings highlight its dual function as an inhalable protein therapeutic that combines antiviral activity with immune modulation, offering a novel strategy for respiratory viral infections in COPD. In addition, inhaled IFN-γ, which was previously discussed in the context of asthma, and inhaled AAT, which has been described in CF treatment, have also gained attention for their potential application in COPD management.51,61) 5.5. Infections Inhaled antibody therapies for coronavirus disease 2019 (COVID-19) have been developed to achieve direct viral suppression at the pulmonary site of infection. Inhaled delivery of the neutralizing antibody 1212C2 has been shown to significantly reduce the severe acute respiratory syndrome coronavirus 2 (SARS-CoV-2) viral load in the lungs of hamsters and to improve histopathological scores.62) Other promising candidates include the nanobody PiN-21 (a multivalent single-domain antibody) and inhaled Regdanvimab (IN-006), both of which exhibited high pulmonary concentrations and potent antiviral efficacy.63) The achievement of high lung concentrations in inhaled antibody therapies results from a combination of factors, including molecular size optimization, tailored inhalation device design, and limited systemic absorption. PiN-21, due to its small nanobody structure, demonstrated enhanced diffusion and deep lung penetration. IN-006, on the other hand, achieved over 100-fold higher pulmonary concentrations compared to intravenous administration, which has been attributed to its muco-trapping capability via binding to mucin.62–64) 5.6. Lung Cancer Inhaled administration of cetuximab has been shown in lung cancer models to have antitumor efficacy.65) Pharmacokinetic studies using neonatal Fc receptor (FcRn)-knockout mice and non-human primate models suggest that the FcRn plays a greater role in local pulmonary retention than in systemic absorption from the lungs. Pulmonary delivery of monoclonal antibodies may therefore enable high local concentrations in the lungs while minimizing systemic exposure, which makes inhaled mAb therapy a promising approach for chronic respiratory diseases, particularly in outpatient or home-care settings. An inhalable liposomal formulation (CTX-OB-LPs) in which osimertinib, an epidermal growth factor (EGFR) tyrosine kinase inhibitor (EGFR-TKI), is encapsulated within cetuximab-conjugated liposomes, was developed by Daram et al.66) This formulation exhibited strong antitumor activity in a non-small cell lung cancer (NSCLC) model, as evidenced by enhanced cytotoxicity, suppression of colony formation, and reduced cell migration. In this context, cetuximab was utilized to confer tumor-targeting ability upon pulmonary delivery. Future studies are warranted to assess how cetuximab modification influences in vivo biodistribution and pharmacokinetics. Bevacizumab is an anti-vascular endothelial growth factor (VEGF) monoclonal antibody that is widely used in the treatment of NSCLC. However, systemic intravenous administration requires high doses and is associated with significant systemic toxicity. An inhalable dry powder formulation of bevacizumab using spray drying technology was developed by Shepard et al.67) In a rat NSCLC model, it demonstrated equivalent tumor suppression to intravenous administration at only one-tenth of the dose. The inhaled formulation retained

VEGF-inhibitory activity and it showed good physicochemical stability. Inhaled anti-VEGF antibody therapies may therefore represent a novel strategy for lung cancer treatment by reducing adverse effects and improving patient compliance. Given the growing number of antibody-based therapies in oncology (including molecular targeted agents and immune checkpoint inhibitors), there is thought to be considerable potential for expanding inhaled formulations of therapeutic antibodies in the future. 5.7. Other Lung Inflammation Diseases Granulocytemacrophage colony-stimulating factor (GM-CSF) is a cytokine secreted by various cell types, including macrophages, T cells, and endothelial cells. It plays a crucial role in immune regulation and alveolar macrophage function. GM-CSF has been applied in the treatment of autoimmune pulmonary alveolar proteinosis (aPAP), a rare disease characterized by the accumulation of surfactant proteins and lipids in the alveoli, leading to progressive respiratory insufficiency.68) A dry powder inhalation formulation of GM-CSF was approved in 2024 in Japan and is marketed under the brand name Sargmalin®. Favorable responses have been reported in patients, which demonstrates the therapeutic potential of inhaled GM-CSF in managing this otherwise difficult-to-treat condition.69)

6. Albumin and Other Proteins as a Drug Delivery Carrier

6.1. Albumin as a Carrier of Anti-cancer Agents Serum albumin is the most abundant protein in serum and has high biocompatibility and biodegradability. In addition, it is actively uptaken by cancer cells via a surface protein, secreted protein acidic and rich in cysteine. Albumin is also a ligand of glycoprotein 60 (gp60) that is overexpressed in cancer vascular endothelial cells, and gp60 supports the distribution of albumin in tumors by transcytosis. Serum albumin is therefore commonly used as a drug carrier for cancer treatment. Paclitaxel-loaded albumin microparticle dry powders with different sizes (0.5, 1, 3 µm) were developed by Chaurasiya et al. for lung cancer.28) Compared with the Taxol solution, the microparticles showed a higher antitumor effect in lung cancer orthotopic model mice. While 66% of paclitaxel accumulated in the liver in the Taxol solution group, more than 78% of paclitaxel was distributed in tumors in the microparticleadministrated group. Compared to the particle with a size of 0.5 µm, the particle with 1 and 3 µm accumulated tumor better, probably due the long retention time in the lungs. Other groups use albumin nanoparticles as a carrier for inhalation.10,70–72) Nanoparticle formation is expected to increase the penetration and cellular uptake, and to take advantage of controlled release.73) Albumin particles were sometimes converted into powder using spray-dryer with heat,28,70) SFD,74) or lyophilized,75) whereas sometimes they administrated as a solution.10,71,72) The negative surface charge of albumin is considered to be advantageous in inhalation formulations because it reduces electrostatic interactions with mucin, thereby enhancing mucus penetration. A novel formulation (PEG-pHSA@PMB) was developed by Li et al., in which polymyxin B was electrostatically loaded onto chemically modified, PEGylated human serum albumin with enhanced negative charge.76) This system was designed to exploit the acidic environment of infection 32

Mucus Targeting Strategies for Inhalable Particles is the predominant route, but rapid clearance by the liver and spleen limits systemic bioavailability. Inhalation has emerged as an alternative strategy to achieve localized delivery to the lungs, with reduced systemic exposure. Intratracheal administration of exosomes derived from canine stem cells (cST-Exo) demonstrated anti-inflammatory effects in an lipopolysaccharide-induced acute lung injury (ALI) mouse model, including the induction of M2 macrophages and regulatory T cells, suppression of pro-inflammatory cytokines (TNF-α, TGF-β), and upregulation of antiinflammatory cytokine IL-10.80) Compared with intravenous injection, airway-localized delivery exhibited greater therapeutic efficacy, supporting the potential of inhaled exosome-based therapies for pulmonary diseases. Inhalation of exosomes derived from lung spheroid cells reportedly improved cardiac function, inhibited fibrosis, and promoted cardiomyocyte proliferation in both mouse and pig models of myocardial infarction.81) Noninvasive inhaled administration could therefore represent a novel delivery route for cardiac regenerative therapies. In the context of infectious disease prevention, Wang et al. developed an inhalable hybrid nanovaccine (NVRBDMLipo) that was composed of SARS-CoV-2 receptor-binding domain (RBD)-expressing cell-derived nanovesicles fused with lung surfactant-mimicking liposomes (MLipo).82) Intratracheal administration of MLipo induced robust mucosal and systemic immune responses, which included high titers of RBD-specific secretory IgA (sIgA) and IgG, activation of both CD4+ and CD8+ T cells, and broad-spectrum neutralization against viral variants. The vaccine also activated pulmonary macrophages via the TLR4/NF-κB pathway and demonstrated a favorable safety profile, positioning it as a promising nextgeneration inhalable vaccine candidate. 6.4. PEGylation PEGylation, which is the covalent attachment of PEG chains, has been widely employed to enhance the stability and pharmacokinetics of protein therapeutics.83) The PEG moiety protects the protein from renal clearance and enzymatic degradation, while also reducing immunogenicity. For example, PEGylated interferons and granulocyte colonystimulating factor have enabled reduced dosing frequencies (ranging from once weekly to once monthly) thereby improv-

sites, where a pH-triggered surface charge shift facilitates drug release. The combination of mild negative charge and polyethylene glycol (PEG)-mediated hydrophilicity improved mucus permeability, while pH-responsiveness enabled sitespecific drug release. Such charge modulation strategies are thought to represent a key design principle in the development of inhalable particulate drug delivery systems. 6.2. Mucoadhesion/Mucodegradating Proteins To achieve site-specific therapy for lung cancer, Jeong et al. developed an inhalable nanomedicine termed thMAP@Cur nanoparticles, which was based on a mucoadhesive peptide derived from adhesion proteins.41) This formulation involved thiol modification of a dopamine-containing mucin-binding protein. The resulting redox-responsive nanoparticles (thMAP NPs) were loaded with curcumin, a compound with known antitumor activity, forming thMAP@Cur NPs. These particles exhibited redox-triggered drug release specifically within the reductive environment of cancer cells. When administered via nebulization, thMAP@Cur NPs demonstrated prolonged pulmonary retention and high tumor localization in a lung metastasis model. This study exemplifies a mucoadhesion-based strategy for enhancing site-specific drug delivery (Fig. 2). In contrast, other approaches aim to disrupt the mucus barrier rather than to interact with it. Sousa et al. incorporated mucolytic enzymes derived from pineapple, specifically papain and bromelain, into poly(acrylic acid) nanoparticles to degrade mucus and to enhance penetration.77) Local enzymatic degradation of the mucus structure significantly increased permeability. Notably, bromelain exhibited superior deep tissue penetration compared to papain in an ex vivo porcine intestinal mucus model. Such strategies to enhance penetration into the deep lung may be particularly advantageous for pulmonary administration aimed at achieving systemic circulation. 6.3. Extracellular Vesicles Exosomes are naturally derived membrane-bound vesicles (30–150 nm in diameter) that encapsulate proteins, nucleic acids, and lipids, and they play a critical role in intercellular communication. Due to their low immunogenicity, biocompatibility, and intrinsic targeting capability, exosomes have garnered attention as promising nanocarriers for drug delivery.78,79) Intravenous administration 33

ing patient adherence and treatment outcomes.84,85) However, challenges remain, such as that the PEGylation may mask the active site of the protein, potentially diminishing bioactivity, and the induction of anti-PEG antibodies has been reported.86) Maintaining a balance between preserving biological activity and selecting the most appropriate modification sites is therefore essential in formulation design. Although still in the experimental stage, several studies have explored PEGylation as a strategy to enhance the pharmacological performance of inhaled protein therapeutics. Dornase alfa (recombinant human DNase I, rhDNase) is a mucolytic enzyme that is widely used in CF treatment via inhalation, but its short pulmonary residence time remains a limitation. N-terminal PEGylation of rhDNase with 20–40 kDa PEG chains was shown in a mouse model to prolong lung retention time to over 15 d.87) This improvement is because PEGylation attenuated rapid clearance by alveolar macrophages, which enabled sustained therapeutic concentrations in the pulmonary environment. In addition, the PEGylated rhDNase retained enzymatic activity while reducing systemic absorption and hepatic accumulation, thereby improving both local efficacy and safety. These findings support the utility of PEGylation in optimizing inhaled protein therapeutics for clinical application. Inhalable protein formulations using PEG-based polymers have also been investigated. An inhalable dry powder formulation composed of a protein complexed with vitamin B12-modified PEG–poly(glutamic acid), targeting the vitamin B12 internalization receptor (CD320), was developed by Nieto-Orellana et al., and it achieved efficient delivery to the lungs.88) PEG–poly(glutamic acid) can form electrostatic interactions with proteins, allowing for the formulation of non-covalent complexes without requiring covalent linkage between the drug and PEG. The significance of PEGylation in inhalation formulations has been extensively reviewed by Guichard et al.89) PEGylation enhances the pulmonary retention and the stability of inhaled proteins through multiple mechanisms, including molecular size optimization, reduced interaction with mucus, protection against enzymatic degradation, and evasion of macrophage-mediated clearance. However, PEG chains can hinder systemic absorption, so careful design is required when systemic therapeutic effects are desired.

📖 中文全文 Chinese Full Text

中文

化学与药学通报 74, 28–36 (2026) 第74卷第1期 https://doi.org/10.1248/cpb.c25-00532 当前专题

**吸入制剂技术综述:支持多种治疗模式**

**综述:蛋白质治疗药物肺部递送吸入技术的进展**

Mayumi Ikeda-Imafuku,* Hiroko Fukuda, Tatsuya Fukuta, and Kazunori Kadota* 和歌山医科大学药学院物理药剂学系,日本和歌山市七番町25–1,邮编640–8156 *通讯作者:imayu@wakayama-med.ac.jp;kazunori-kadota@wakayama-med.ac.jp 收稿日期:2025年7月31日

蛋白质治疗药物的吸入递送作为一种有前景的非侵入性替代传统注射制剂的方法,为肺部疾病的局部和全身治疗提供了潜力。本综述全面总结了可吸入蛋白质制剂的最新进展,重点涵盖设计策略、制剂技术、有效递送的障碍以及疾病特异性应用。关键方面包括粒径、表面电荷和蛋白质工程在优化肺沉积和细胞摄取中的作用,以及喷雾冷冻干燥和PEG化等提高蛋白质稳定性的技术。本综述还探讨了针对囊性纤维化、哮喘、特发性肺纤维化、慢性阻塞性肺疾病、肺部感染和癌症的新型治疗方法,包括抗体、纳米抗体、外泌体和基于白蛋白的载体的应用。尽管临床转化仍然有限,但递送系统和分子设计的持续创新被认为在拓展吸入蛋白质药物的治疗前景方面具有重要潜力。

**关键词** 干粉吸入器(DPI)递送,包括PEG化的应用。最后,我们讨论了蛋白质基纳米颗粒临床转化的挑战与未来。

近年来,以蛋白质为原料药的药物开发在生物制药进步的推动下加速发展。静脉给药传统上是蛋白质制剂的主要给药途径。然而,作为一种高效、非侵入性的替代方式,蛋白质吸入疗法日益受到关注。肺部因其巨大的表面积、丰富的血管分布以及可避免首过效应的特点,成为理想的药物吸收部位。然而,蛋白质的肺部给药仍面临诸多挑战,包括酶降解、颗粒沉积以及潜在的免疫反应。实际上,许多正在开发的蛋白质吸入疗法旨在发挥肺部局部作用。以全身效应为目标的肺部递送主要在糖尿病治疗背景下进行研究,尤其是胰岛素及其他相关肽类药物(如Afrezza®)。

在本综述中,我们总结了蛋白质吸入制剂的最新研究趋势,重点关注设计原理、制剂技术、免疫安全性和疾病特异性应用。我们还强调了干燥技术和纳米颗粒工程在干粉吸入器(DPI)制剂中的最新进展。

蛋白质吸入制剂包括治疗性抗体、细胞因子、酶及其他生物活性蛋白质,以及基于蛋白质的药物载体。在美国食品药品监督管理局(FDA)批准的所有给药途径的蛋白质治疗药物中,单克隆抗体占比最大,约占总数的半数。其他已批准的蛋白质药物包括凝血因子、酶、融合蛋白、激素、载体和生长因子。作为药物递送载体时,蛋白质因其高生物相容性和可生物降解性而受到重视。血清白蛋白作为人血清中的内源性成分,因其高药物结合能力、良好的渗透性和低免疫原性,已被广泛研究作为药物载体。血清白蛋白在纳米制剂中的应用也得到深入研究,用于提高摄取率和载药量。其他天然来源的蛋白质,如丝素蛋白和明胶,因其可调节颗粒刚性和崩解特性而作为制剂材料受到关注。

© 2026 作者。本文采用知识共享署名-非商业性使用4.0国际许可协议(https://creativecommons.org/licenses/by-nc/4.0/)发布。由日本药学会出版。 28

化学与药学通报 第74卷第1期(2026)已在其他地方进行了全面综述。与静脉注射制剂不同,目前尚无明确关于吸入产品中蛋白质聚集体的监管标准。因此,亟需建立制剂设计与分析评估的新指南。

**3.3 吸入过程中的界面应力** 吸入制剂中的界面应力是指药物或纳米颗粒对肺部气-液界面(特别是肺泡内衬的表面活性剂膜)产生的物理化学影响。为评估吸入气溶胶对肺表面活性剂功能的“界面应力”,Bäckman等人开发了一种改进型约束滴表面活性计(CDS),可通过表面张力量化药物或颗粒的影响。研究表明,微粉化白蛋白会损害表面活性剂功能,其最低表面张力超过10 mN/m,从而破坏界面稳定性。相比之下,吸入性皮质类固醇和乳糖未表现出这些效应。这些发现表明,基于蛋白质的制剂的表面活性可能干扰肺表面活性剂功能,突显了基于CDS的评估在毒性评价中的重要性。

表面电荷也是影响界面应力的关键参数。据报道,带正电的纳米颗粒会与肺表面活性剂发生静电相互作用,形成微米级颗粒-囊泡复合物。这种聚集诱导的结构改变被认为会损害表面活性剂层的生物物理功能。

**3.4 颗粒分布的控制** 在吸入制剂中,1–5 µm的粒径范围被认为是肺部沉积的最佳范围,而窄的粒径分布(表现为低几何标准偏差)有助于实现一致的吸入性能。过大的颗粒倾向于沉积在口咽部,而过小的颗粒则可能在到达肺部前被呼出。因此,精确控制空气动力学粒径至关重要。

为研究初始粒径的影响,研究人员将紫杉醇包封于0.5、1.0和3.0 µm的白蛋白微粒中,并将其制成具有相同空气动力学直径(约5 µm)的干粉。在小鼠肺癌模型中评估了其肺内分布和抗肿瘤活性。由1.0–3.0 µm初始颗粒制备的制剂表现出持续的药物释放和延长的肺部滞留,从而获得良好的治疗效果。这些发现强调了初始粒径作为吸入制剂治疗疗效关键因素的重要性,并突显了在制剂设计和质量控制中需仔细考虑该参数的必要性。

空气动力学粒径、表面电荷和疏水性的改变已知会显著影响肺泡上皮细胞的粘附和内吞效率,主要通过影响与粘液层的相互作用及穿透能力。这些设计参数还影响颗粒沉积部位(如支气管与肺泡)以及被肺泡巨噬细胞清除的风险。此外,某些制剂中蛋白质被用作赋形剂。例如,添加白蛋白作为赋形剂可减少颗粒聚集,增强球形形态和均匀性,并改善可吸入沉积。

**3.1 酶** 肺部含有多种代谢酶,包括细胞色素P450(CYPs)和酯酶,这些酶可显著影响药物的局部疗效、全身暴露和安全性。中性粒细胞弹性蛋白酶是一种储存在中性粒细胞初级颗粒中的丝氨酸蛋白酶,在宿主防御细菌感染中起关键作用。中性粒细胞弹性蛋白酶在转录和翻译后水平激活粘蛋白基因,从而诱导气道粘液的过度产生和分泌。其在囊性纤维化、慢性阻塞性肺疾病(COPD)和急性肺损伤等肺部疾病中的分泌升高。基质金属蛋白酶(MMPs),特别是MMP-2和MMP-9,在急性呼吸窘迫综合征中上调,是组织损伤和炎症放大的关键介质。这些蛋白水解酶可能损害基于蛋白质的吸入制剂的治疗疗效。这些酶的表达可能因病理状况而异,因此在制剂开发过程中进行疾病特异性评估至关重要。

**3.2 聚集** 蛋白质聚集是开发可吸入蛋白质制剂的主要难题。喷雾干燥或雾化相关的物理应力(即剪切力、热暴露、气-液界面应力和快速脱水)可诱导结构变性和聚集,可能导致肺部局部免疫反应或毒性。根据聚集体的尺寸和类型,肺泡巨噬细胞的清除可能受阻,因此存在引发慢性炎症的担忧。

在DPI制备中,若使用烘箱干燥,热变性是一个问题。典型的喷雾干燥过程涉及60至100°C的干燥温度,可能导致蛋白质不可逆的热诱导变性。为避免此类热降解,有前景的替代技术包括冷冻干燥和喷雾冷冻干燥。其他稳定策略包括添加赋形剂,如海藻糖、甘露醇和氨基酸(如甘氨酸),以维持氢键并抑制结构变性。这些添加剂特别有效,因其能够通过氢键替代水分子(水替代假说),并在干燥时形成玻璃态基质,从而限制分子流动性并稳定蛋白质结构。或者,可使用疏水性聚合物和表面活性剂防止气-液界面处的变性。吸入制剂中蛋白质聚集的风险和机制已在此前综述。

**4. DPI制剂中蛋白质药物的干燥方法** 已探索多种干燥技术用于开发基于蛋白质的干粉吸入器,包括冷冻干燥、喷雾干燥、喷雾冷冻干燥(SFD)和超临界流体(SCF)干燥(图1)。其中,SFD被认为在颗粒工程和吸入应用中具有显著优势,因其可防止蛋白质聚集。此外,超临界干燥等新兴方法正作为潜在替代方案受到关注。干燥方法的选择应根据蛋白质的理化性质、所选赋形剂和治疗应用进行优化。

在喷雾干燥中,雾化液滴通过热空气干燥,通常产生具有良好空气动力学特性的均匀球形颗粒。在蛋白质制剂中,雾化过程中的蛋白质浓度等参数显著影响所得颗粒形态和气雾化效率,如使用血清白蛋白的研究所示。

相比之下,SFD对制剂施加的热应力远低于传统喷雾干燥,且倾向于产生有利于吸入的多孔颗粒。与传统冷冻干燥相比,SFD还被证明可减少脂质系统中的氧化,提示其在防止蛋白质氧化方面具有额外潜在优势。作为SFD用于可吸入蛋白质制剂的实例,Ito等人通过使用海藻糖和亮氨酸作为稳定赋形剂,成功将诱饵蛋白制成DPI(同时保留抗体活性)。

在比较SFD和喷雾干燥脱氧核糖核酸酶时,Maa等人发现喷雾干燥产生约3 µm的小而致密颗粒,而SFD产生约8–10 µm的多孔颗粒。因此,SFD在气雾化方面优于喷雾干燥,且SFD产生的颗粒空气动力学粒径更小。

超临界流体(如二氧化碳)在高于其临界温度和压力的条件下存在,兼具气体和液体的性质。在超临界干燥中,利用从液体到超临界流体再到蒸汽相的转变,通过超临界流体的抗溶剂效应沉淀和干燥蛋白质。该技术可精确控制颗粒形成,并作为蛋白质吸入制剂的可行干燥方法受到关注。研究表明,干燥方法显著影响乳清蛋白气凝胶的结构、吸附和机械性能。与冷冻干燥相比,超临界干燥产生密度更高、保油能力更强的气凝胶。

冷冻干燥仍是注射用蛋白质制剂中最广泛使用的干燥技术。尽管其通常产生不利于颗粒设计的固体蛋糕状物,但在某些纳米颗粒制剂(如溶菌酶)中可能适用。

雾化器从液体制剂中机械产生气溶胶,适用于吸气能力有限的患者。相比之下,DPI在便携性和储存稳定性方面具有优势,但其疗效取决于患者产生足够吸气流量的能力。随着粉末制剂技术的最新进展,DPI在递送蛋白质和纳米颗粒药物方面受到关注,导致雾化器在制剂开发中的使用减少。尽管如此,雾化器因其简单性和给药便利性,在基础研究中仍广泛使用。

**5. 肺部局部疾病的吸入蛋白质疗法**

**5.1 囊性纤维化** 囊性纤维化是由囊性纤维化跨膜传导调节蛋白突变引起的遗传性疾病,导致肺部粘液积聚,引发慢性感染和炎症。有效管理需要增强粘液清除、控制感染和恢复囊性纤维化跨膜传导调节蛋白功能的策略。

α-1抗胰蛋白酶(AAT)是一种丝氨酸蛋白酶抑制剂,可保护组织免受中性粒细胞和其他炎症细胞来源的酯酶损害。AAT缺乏与肺气肿的发生相关。Griese等人研究了囊性纤维化患者肺部给予AAT的效果。虽未见肺功能显著改善,但弹性蛋白酶活性降低,促炎细胞因子减少,杀菌能力增强。通过SMART CARD连接设备(AKITA1吸入器配Pari LC Plus或Pari LC Star雾化器)测试了两种吸入模式,结果无差异。尽管AAT用于囊性纤维化的后续临床开发放缓,但其在光气等有毒气体诱导的急性肺损伤模型中显示出有前景的抗炎和细胞保护作用,提示在其他肺部疾病中的潜在应用。

重组人脱氧核糖核酸酶I(rhDNase,Pulmozyme®)在许多国家被批准为囊性纤维化的吸入治疗药物。临床研究已证明其降低粘液粘度和改善肺功能的疗效。Frederiksen等人报告,12个月的rhDNase吸入显著改善了1秒用力呼气容积(FEV1),并减少了包括金黄色葡萄球菌在内的呼吸道感染发生率,可能有助于减缓疾病进展。生物类似药Tigeras®也已开发,并证明安全有效。

乳铁蛋白是一种约83 kDa的糖蛋白,具有抗菌、抗炎和免疫调节活性,作为囊性纤维化患者吸入治疗的候选药物受到关注。Marshall等人开发了含有乳铁蛋白或脱铁乳铁蛋白与氨基糖苷类抗生素(妥布霉素或庆大霉素)组合的喷雾干燥粉末制剂,并在囊性纤维化肺部感染模型中进行了测试。这些制剂表现出多种有益作用,包括抑制生物膜形成、破坏现有生物膜和增强抗生素渗透。所得颗粒尺寸为1.5–1.9 µm,90%小于5 µm,表明具有良好的气雾化和吸入适用性。该组合被认为代表了治疗囊性纤维化患者慢性感染的有前景的蛋白质基DPI候选药物。

ALX-009是一种结合乳铁蛋白和次硫氰酸盐的可吸入制剂,在囊性纤维化患者痰液样本中对铜绿假单胞菌和伯克霍尔德菌复合体表现出强效杀菌活性。ALX-009显示出优于妥布霉素的抗菌活性,每日两次给药后效果增强。这些结果表明,ALX-009是治疗囊性纤维化多重耐药感染的有前景的治疗选择。此外,乳铁蛋白在急性呼吸窘迫综合征和氧中毒模型中显示出保护作用,提示其在囊性纤维化以外的严重呼吸系统疾病中的潜在用途。

**5.2 特发性肺纤维化** 吸入性干扰素-γ(IFN-γ)是一种具有抗纤维化和巨噬细胞激活功能的细胞因子,作为特发性肺纤维化的潜在治疗药物受到关注。据报道,雾化给予IFN-γ可抑制转化生长因子-β(TGF-β)信号通路并抑制肺部纤维化进展。在一项涉及特发性肺纤维化患者为期80周的安全性研究中,支气管肺泡灌洗液中的IFN-γ浓度增加了60倍。伴随一氧化碳弥散量和总肺容量下降趋势的逆转。全身暴露极少,未观察到不良事件。皮下给药先前未显示临床益处,且未在支气管肺泡灌洗液中检测到IFN-γ,因此这些发现突显了通过吸入直接肺部递送的重要性。

PRS-220是一种靶向CCN2(旧称结缔组织生长因子,CTGF)的吸入性Anticalin®蛋白。在临床前特发性肺纤维化模型中,PRS-220显示出优于全身给药抗体的抗纤维化疗效。由于其选择性肺部分布和低全身暴露,PRS-220还表现出良好的安全性。值得注意的是,在离体和人肺组织切片模型中,PRS-220显示出比尼达尼布和帕姆雷卢单抗等其他治疗药物更强的抗纤维化活性。这些结果突显了PRS-220作为特发性肺纤维化有前景的吸入蛋白质疗法的潜力,兼具高效肺部递送和强效治疗作用。

**5.3 哮喘** Won等人研究了吸入性干扰素-λ2/3(IFN-λ2/3)在过敏原诱导哮喘模型中的治疗潜力。哮喘发作后给予IFN-λ2/3导致气道炎症和反应性显著降低。IFN-λ吸入显著抑制了与T辅助2(Th2)和Th17反应相关的促炎细胞因子(包括白细胞介素(IL)-4、IL-5、IL-13和IL-17A),并促进了以产生IL-10的CD4+ T细胞增加为特征的抗炎反应。因此,IFN-λ可能成为哮喘管理的有前景的吸入蛋白质治疗候选药物。

纳米抗体是小的抗体片段(约15 kDa),由抗体的可变区组成,因其高肺部分布和固有稳定性而在吸入疗法中具有优势。LQ036是一种靶向IL-4受体α1链(IL-4Rα1)的纳米抗体,在人体化哮喘模型中显著抑制了气道炎症、杯状细胞增生和免疫球蛋白E(IgE)产生。吸入给予LQ036导致肺部高浓度和延长滞留。与全长抗体相比,纳米抗体等片段抗体表现出降低的聚集倾向,使其成为吸入递送系统的有前景候选药物。

Depemokimab(GSK3511294)是一种高亲和力抗IL-5的长效单克隆抗体,皮下给药每六个月一次在重度嗜酸性粒细胞性哮喘患者中显著减少了急性发作(III期,NCT04719832)。尽管Depemokimab本身未开发用于吸入,但研究表明,吸入性抗IL-5单克隆抗体可在过敏原诱导的哮喘小鼠模型中显著减轻气道炎症和反应性。因此,吸入可能提供与静脉给药相当的治疗疗效。

IL-33是参与粘膜炎症疾病(包括哮喘)的关键细胞因子。Huange等人开发了一种人源化可吸入单域抗体(UdAb A12),选择性抑制IL-33信号传导。在过敏性气道炎症模型中,UdAb A12表现出强效抗炎作用。与对照免疫球蛋白G(IgG)抗体itepekimab相比,UdAb A12显示出更优的肺部分布和局部疗效,表明其作为吸入抗体治疗新平台的潜力。

**5.4 慢性阻塞性肺疾病(COPD)** DAS181是一种由人上皮生长因子和细菌唾液酸酶组成的可吸入融合蛋白,旨在抑制病毒进入宿主细胞。在COPD小鼠模型(香烟烟雾暴露联合流感感染)中吸入给予DAS181有效抑制了肺炎进展,降低了病毒载量,抑制了促炎细胞因子(IL-6、IL-1β和肿瘤坏死因子(TNF)),并保持了肺功能(表现为肺顺应性维持)。此外,DAS181调节了肺巨噬细胞中免疫调节性Siglecs的表达,并促进了记忆T细胞反应,提示增强了对再感染的保护。与奥司他韦相比,DAS181在抑制肺炎方面表现出更优疗效。这些发现突显了其作为可吸入蛋白质治疗药物的双重功能,结合抗病毒活性和免疫调节,为COPD呼吸道病毒感染提供了新策略。

此外,先前在哮喘背景下讨论的吸入性IFN-γ和已在囊性纤维化治疗中描述的吸入性AAT,也因其在COPD管理中的潜在应用受到关注。

**5.5 感染** 针对2019冠状病毒病(COVID-19)的吸入抗体疗法旨在感染肺部部位直接抑制病毒。吸入给予中和抗体1212C2显著降低了仓鼠肺部的严重急性呼吸综合征冠状病毒2(SARS-CoV-2)病毒载量,并改善了组织病理学评分。其他有前景的候选药物包括纳米抗体PiN-21(一种多价单域抗体)和吸入性Regdanvimab(IN-006),两者均表现出高肺部浓度和强效抗病毒疗效。

吸入抗体疗法实现高肺浓度是多种因素共同作用的结果,包括分子大小优化、定制化吸入装置设计和有限的全身吸收。PiN-21因其小的纳米抗体结构而表现出增强的扩散和深肺渗透能力。IN-006则通过结合粘蛋白的粘液捕获能力,实现了比静脉给药高100倍以上的肺部浓度。

**5.6 肺癌** 在肺癌模型中,吸入给予西妥昔单抗显示出抗肿瘤疗效。使用新生儿Fc受体(FcRn)敲除小鼠和非人灵长类动物模型的药代动力学研究表明,FcRn在局部肺部滞留中的作用大于从肺部全身吸收的作用。因此,单克隆抗体的肺部递送可在实现肺部高局部浓度的同时最小化全身暴露,使吸入性mAb疗法成为慢性呼吸系统疾病(特别是在门诊或家庭护理环境中)的有前景方法。

Daram等人开发了一种可吸入脂质体制剂(CTX-OB-LPs),其中奥希替尼(一种表皮生长因子受体(EGFR)酪氨酸激酶抑制剂(EGFR-TKI))被包封于西妥昔单抗偶联的脂质体中。该制剂在非小细胞肺癌(NSCLC)模型中表现出强效抗肿瘤活性,表现为增强的细胞毒性、抑制集落形成和减少细胞迁移。在此背景下,西妥昔单抗被用于赋予肺部递送的肿瘤靶向能力。未来研究需评估西妥昔单抗修饰如何影响体内生物分布和药代动力学。

贝伐珠单抗是一种抗血管内皮生长因子(VEGF)单克隆抗体,广泛用于NSCLC治疗。然而,全身静脉给药需要高剂量并伴随显著全身毒性。Shepard等人使用喷雾干燥技术开发了贝伐珠单抗的可吸入干粉制剂。在大鼠NSCLC模型中,仅以十分之一剂量即表现出与静脉给药相当的肿瘤抑制效果。吸入制剂保留了VEGF抑制活性,并显示出良好的理化稳定性。因此,吸入性抗VEGF抗体疗法可能通过减少不良反应和提高患者依从性,成为肺癌治疗的新策略。

鉴于肿瘤学中基于抗体疗法(包括分子靶向药物和免疫检查点抑制剂)的日益增多,未来治疗性抗体吸入制剂的拓展被认为具有巨大潜力。

**5.7 其他肺部炎症性疾病** 粒细胞-巨噬细胞集落刺激因子(GM-CSF)是一种由多种细胞类型(包括巨噬细胞、T细胞和内皮细胞)分泌的细胞因子,在免疫调节和肺泡巨噬细胞功能中起关键作用。GM-CSF已用于治疗自身免疫性肺泡蛋白沉积症(aPAP),这是一种以肺泡内表面活性蛋白和脂质积聚为特征的罕见疾病,导致进行性呼吸功能不全。

GM-CSF干粉吸入制剂于2024年在日本获批,商品名为Sargmalin®。患者中报告了良好应答,证明了吸入性GM-CSF在治疗这一难治性疾病中的治疗潜力。

**6. 白蛋白及其他蛋白质作为药物递送载体**

**6.1 白蛋白作为抗癌药物载体** 血清白蛋白是血清中最丰富的蛋白质,具有高生物相容性和可生物降解性。此外,它通过表面蛋白“富含半胱氨酸的分泌性酸性蛋白”被癌细胞主动摄取。白蛋白也是糖蛋白60(gp60)的配体,gp60在癌血管内皮细胞中过表达,并通过胞吞作用支持白蛋白在肿瘤中的分布。因此,血清白蛋白常被用作癌症治疗的药物载体。

Chaurasiya等人开发了不同尺寸(0.5、1、3 µm)的载紫杉醇白蛋白微粒干粉用于肺癌。与Taxol溶液相比,微粒在肺癌原位模型小鼠中显示出更高的抗肿瘤效果。在Taxol溶液组中,66%的紫杉醇积聚在肝脏,而在微粒给药组中,超过78%的紫杉醇分布于肿瘤。与0.5 µm颗粒相比,1和3 µm颗粒的肿瘤积聚更好,可能是由于肺部滞留时间长。

其他研究组使用白蛋白纳米颗粒作为吸入载体。纳米颗粒形成有望提高穿透性和细胞摄取,并利用控释优势。白蛋白颗粒有时使用加热喷雾干燥器、SFD或冷冻干燥转化为粉末,有时则以溶液形式给药。

白蛋白的负表面电荷被认为在吸入制剂中具有优势,因其减少与粘蛋白的静电相互作用,从而增强粘液渗透。Li等人开发了一种新型制剂(PEG-pHSA@PMB),其中多粘菌素B被静电加载到化学修饰的PEG化人血清白蛋白上,增强负电荷。该系统旨在利用感染部位的酸性环境。

**6.4 PEG化** PEG化即PEG链的共价连接,已被广泛用于提高蛋白质治疗药物的稳定性和药代动力学。PEG部分保护蛋白质免受肾脏清除和酶降解,同时降低免疫原性。例如,PEG化干扰素和粒细胞集落刺激因子实现了给药频率的降低(从每周一次到每月一次),从而改善了患者依从性。

# 翻译

位点,其中pH触发的表面电荷转换促进了药物释放。微弱的负电荷与聚乙二醇(PEG)介导的亲水性相结合,提高了黏液渗透性,而pH响应性则实现了位点特异性药物释放。此类电荷调控策略被认为代表了可吸入微粒药物递送系统开发中的关键设计原则。

## 6.2. 黏液黏附/黏液降解蛋白

为实现肺癌的位点特异性治疗,Jeong等人开发了一种名为thMAP@Cur纳米颗粒的可吸入纳米药物,该药物基于源自黏附蛋白的黏液黏附肽。该制剂涉及对一种含多巴胺的黏结合蛋白进行巯基修饰。所得的氧化还原响应性纳米颗粒(thMAP NPs)负载了姜黄素——一种具有已知抗肿瘤活性的化合物——形成thMAP@Cur NPs。这些颗粒在癌细胞的还原性环境中表现出氧化还原触发的特异性药物释放。通过雾化给药后,thMAP@Cur NPs在肺转移模型中表现出延长的肺部滞留时间和较高的肿瘤靶向性。该研究例证了一种基于黏液黏附的策略,用于增强位点特异性药物递送(图2)。

相比之下,其他方法旨在破坏黏液屏障而非与其相互作用。Sousa等人将源自菠萝的黏液溶解酶——具体为木瓜蛋白酶和菠萝蛋白酶——掺入聚丙烯酸(poly(acrylic acid))纳米颗粒中,以降解黏液并增强渗透。黏液结构的局部酶降解显著增加了渗透性。值得注意的是,在离体猪肠道黏液模型中,菠萝蛋白酶相较于木瓜蛋白酶表现出更优的深层组织穿透能力。此类增强深层肺部渗透的策略,对于旨在实现全身循环的肺部给药可能尤为有利。

## 6.3. 细胞外囊泡

外泌体是天然来源的膜结合囊泡(直径30–150 nm),其内包裹蛋白质、核酸和脂质,在细胞间通讯中发挥关键作用。由于其低免疫原性、生物相容性和内在靶向能力,外泌体作为药物递送的有前景的纳米载体已受到广泛关注。静脉给药……

提高患者依从性和治疗效果。然而,挑战依然存在,例如PEG化可能遮蔽蛋白质的活性位点,从而潜在降低生物活性,且已有抗PEG抗体诱导的报道。因此,在制剂设计中,在保持生物活性与选择最合适的修饰位点之间维持平衡至关重要。

尽管仍处于实验阶段,已有若干研究探索了PEG化作为增强吸入性蛋白质治疗药物药理性能的策略。

阿法链道酶(重组人DNase I,rhDNase)是一种黏液溶解酶,广泛用于囊性纤维化(CF)的吸入治疗,但其肺部滞留时间较短仍是一个局限性。在动物模型中,用20–40 kDa PEG链对rhDNase进行N端PEG化,可将肺部滞留时间延长至超过15天。这一改善是因为PEG化减弱了肺泡巨噬细胞的快速清除,从而在肺部环境中维持了持续的治疗浓度。此外,PEG化的rhDNase在保留酶活性的同时,减少了全身吸收和肝脏蓄积,从而提高了局部疗效和安全性。这些发现支持了PEG化在优化吸入性蛋白质治疗药物用于临床应用方面的实用性。

基于PEG聚合物的可吸入蛋白质制剂也已被研究。Nieto-Orellana等人开发了一种可吸入干粉制剂,其由蛋白质与维生素B12修饰的PEG-聚(谷氨酸)复合而成,靶向维生素B12内化受体(CD320),实现了向肺部的高效递送。PEG-聚(谷氨酸)可与蛋白质形成静电相互作用,从而允许形成非共价复合物,而无需药物与PEG之间的共价连接。

Guichard等人已广泛综述了PEG化在吸入制剂中的意义。PEG化通过多种机制增强吸入蛋白质的肺部滞留和稳定性,包括分子尺寸优化、减少与黏液的相互作用、防止酶降解以及逃避巨噬细胞介导的清除。然而,PEG链可能阻碍全身吸收,因此在期望全身治疗效果时需要审慎设计。