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Mussel Foot Protein Membrane-Enclosed Crystalline Drug with Zero-Order Release Kinetics for Long-Acting Therapy

Angewandte Chemie 2025年

作者： Leihao Lu Jianchang Xu Xuehui Huang Leyi Hu Kangfan Ji Chuhuan Jiang Yanfang Wang Yue Qin Yang Zhang Juan Zhang Jiahao Hu Shenxi Qian Yingqi Huang Hongzhen Bai Xiangnan Zhang Prof. Fuyao Liu Prof. Zhen Gu Prof. Jinqiang Wang State Key Laboratory of Advanced Drug Delivery and Release Systems College of Pharmaceutical Sciences Zhejiang University Hangzhou 310058 China Jinhua Institute of Zhejiang University Jinhua 321299 China Department of Chemistry Hangzhou 310058 China Liangzhu Laboratory Hangzhou 311121 China Department of General Surgery Sir Run Run Shaw Hospital School of Medicine Zhejiang University Hangzhou 310016 China MOE Key Laboratory of Macromolecular Synthesis and Functionalization Department of Polymer Science and Engineering Zhejiang University Hangzhou 310027 China Institute of Fundamental and Transdisciplinary Research Zhejiang University Hangzhou 310009 China Department of Pharmacy Second Affiliated Hospital Zhejiang University School of Medicine Zhejiang University Hangzhou 310058 China

Injectable formulations with sustained and steady release capabilities are critically required to treat diseases requiring temporary or lifelong continuous therapy, especially for drugs with a short half-life. Additionally, achieving a sufficiently high drug loading in a single dose remains a persistent challenge. Herein, by mimicking the formation principles of mussel adhesive plaques, we have developed membrane-enclosed crystalline systems of insulin and progesterone as model macro- and small-molecular crystalline drugs. The system exhibits a substantial drug loading capacity (>90 %). It exhibits sustained and zero-order release kinetics, thereby facilitating the establishment of a subcutaneous reservoir containing a substantial drug load, enabling progressive and continuous release of the drug into the body. One single injection of membrane-enclosed insulin crystal can maintain normoglycemia in diabetic mice for up to 7 days. Meanwhile, membrane-coated progesterone crystals can sustain drug release in rats for over 7 days. The protein membrane can be cleared from the injection sites in 35 days. This system can serve as a versatile platform for the sustained release of various crystalline pharmaceuticals and the treatment of distinct diseases.

关键词： Drug delivery Biomimetics Zero order Sustained release Long-acting drug

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Wiring Covalent Organic Frameworks with Conducting Polymers

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Angewandte Chemie 2024年第45期136卷

作者： Yifan Gong Lejian Deng Xiaoyi Xu Dr. Ruoyang Liu Prof. Dr. Juan Li Prof. Dr. Ning Huang Prof. Dr. Donglin Jiang Integrative Sciences & Engineering NUS Graduate School National University of Singapore Singapore 119077 Singapore Department of Chemistry Faculty of Science National University of Singapore Singapore 117543 Singapore Joint School of National University of Singapore and Tianjin University International Campus of Tianjin University Binhai New City 350207 P. R. China. MOE Key Laboratory of Macromolecular Synthesis and Functionalization State Key Laboratory of Silicon Materials International Research Centre for X Polymers Department of Polymer Science and Engineering Zhejiang University Hangzhou 310027 China Institute of Crystalline Materials Shanxi University Taiyuan 030006 China

Covalent organic frameworks are a class of crystalline porous polymers formed by linking organic units into periodically aligned skeletons and pores. Here we report a strategy for wiring these frameworks with conducting polymers via wall engineering and polymerization. We anchored each edge site with one pyrrole unit, which is densely packed along the z direction yet protruded from pore walls. This assembly enables the polymerization of pyrrole units to form polypyrrole and creates a new polypyrrole chain conformation. The resultant framework constitutes six single file polypyrrole chains in each pore and develop spatially segregated yet built-in single molecular wires with exceptional stable polarons. Hall effect measurements revealed that the materials are p -type semiconductors, increase conductivity by eight orders of magnitude compared to the pristine frameworks, and achieve a carrier mobility as large as 13.2 cm 2 V −1 s −1 . Our results open an avenue to π electronic frameworks by interlayer molecular wiring with conducting polymers.

关键词： Covalent organic frameworks Single file molecular wire Polymerization π Electronic property Carrier mobility

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Mesenchymal Stem Cell-Derived Exosomes Laden Scaffold for Promoting Endometrium Regeneration and Fertility Restoration through Macrophage Immunomodulation

SSRN

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SSRN 2020年

作者： Xin, Liaobing Lin, Xiaona Wang, Xiufen Yu, Huaying Pan, Yibin Fei, Haiyi Ma, Lie Zhang, Songying Zhou, Feng Li, Chao Assisted Reproduction Unit Department of Obstetrics and Gynecology Sir Run Run Shaw Hospital School of Medicine Zhejiang University Hangzhou310016 China MOE Key Laboratory of Macromolecular Synthesis and Functionalization Department of Polymer Science and Engineering Zhejiang University Hangzhou310027 China Key Laboratory of Reproductive Dysfunction Management of Zhejiang Province No. 3 Qingchun East Road Jianggan District Hangzhou310016 China

Endometrial traumas caused by recurrent curettage, caesarean section and myomectomy always result in intrauterine adhesions (IUAs) and infertility. Umbilical cord-derived mesenchymal stem cell (MSC)-based therapies have shown some promise achievements in the treatment of IUAs for their easy collection, high proliferation and low immunogenicity. However, the potential tumorigenicity, low infusion and low retention of MSCs are still controversial and the clinical application of MSCs is limited. In contrast, MSC-derived exosomes exhibit a similar function to their source cells and are expected to overcome these limitations. Therefore, a novel and viable cell-free therapeutic strategy by MSC-derived exosomes was proposed in this study. Here, we designed a construct of exosomes and a collagen scaffold (CS/Exos) for endometrium regeneration, and investigated the regeneration mechanism through macrophage immunomodulation. The CS/Exos transplantation potently induced (i) endometrium regeneration, (ii) collagen remodeling, (iii) increased the expression of the estrogen receptor-alpha /progesterone receptor, and (iv) restored fertility. Mechanistically, CS/Exos facilitated CD163+ M2 macrophage polarization, reduced inflammation, and increased anti-inflammatory responses in vivo and in vitro. By RNA-seq, miRNAs enriched in exosomes were the main mediator for exosomes-induced macrophage polarization. Overall, we demonstrated that CS/Exos treatment facilitated endometrium regeneration and fertility restoration by immunomodulatory functions of miRNAs. Our research highlights the therapeutic prospects of CS/Exos for the management of IUAs. © 2020, The Authors. All rights reserved.

关键词： Cell culture

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Linker-Mediated Delocalized Excited States in Dimeric Acceptors Enable Efficient Exciton Dissociation with Negligible Energy-Level Offsets

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Angewandte Chemie 2024年第4期137卷

作者： Sheng-Yu Shi Chao Yang Xinjie Xu Zhi-Xi Liu Wanchun Duan Xing-Xing Chen Zhou Lu Hongping Zhou Zhi-Peng Yu Chang-Zhi Li Institutes of Physical Science and Information Technology School of Chemistry and Chemical Engineering Anhui University Hefei Anhui 230601 P. R. China School of Chemical and Environmental Engineering Anhui Polytechnic University Wuhu 241002 China Anhui Key Laboratory for Control and Applications of Optoelectronic Information Materials School of Physics and Electronic Information Anhui Normal University Wuhu 241002 China State Key Laboratory of Silicon Materials MOE Key Laboratory of Macromolecular Synthesis and Functionalization International Research Center for X Polymers Department of Polymer Science and Engineering Zhejiang University-Hangzhou Global Scientific and Technological Innovation Center Zhejiang University 310027 Hangzhou P. R. China Department of Materials Science and Engineering University of Science and Technology of China Hefei 230026 China

Efficient exciton dissociation at low energy offsets is key to overcoming voltage losses in organic solar cells. In this work, we developed two dimeric acceptors, i-YT and o-YT, by precisely controlling the position of an asymmetric electron-donating linker. It induced the foldamer conformation of i-YT with a para linkage (relative to the dicyano groups), while retaining the unfold conformation for o-YT. This subtle structural modification influenced the molecular assembly properties, enabled near-zero energy offset exciton dissociation and power conversion efficiencies exceeding 18 % for i-YT based organic solar cells. Detailed excitonic dynamics further revealed that the linker position critically influences three processes: the formation of delocalized singlet excited states, ultrafast charge transfer (~5 ps) in solid blends, and the suppression of exciton recombination. Additionally, devices based on i-YT demonstrated outstanding long-term stability, retaining 85 % of their initial efficiency after 1,400 hours of continuous illumination. These findings introduce a new class of dimeric acceptors that combine high efficiency with exceptional stability, offering a promising pathway toward low-energy-loss organic photovoltaics.

关键词： Organic Photovoltaics Dimeric Acceptor High Efficiency Stability Delocalized Excited State

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Frontispiece: Platelet-Drug Conjugates Engineered via One-step Fusion Approach for Metastatic and Postoperative Cancer Treatment

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Angewandte Chemie International Edition 2024年第37期63卷

作者： Zhengjie Zhao Yinxian Yang Tao Sheng Yuhang Bao Ruixi Yu Xinmin Yu Shuangxu Jia Qing Wu Chaojie Zhu Xinyuan Shen Wentao Zhang Ziyi Lu Kangfan Ji Xiaofeng Chen Xinyun Jiang Prof. Yuqi Zhang Prof. Zhen Gu Prof. Jicheng Yu State Key Laboratory of Advanced Drug Delivery and Release Systems Zhejiang Provincial Key Laboratory for Advanced Drug Delivery Systems College of Pharmaceutical Sciences Zhejiang University Hangzhou 310058 China Department of Hepatobiliary and Pancreatic Surgery the Second Affiliated Hospital School of Medicine Zhejiang University Hangzhou 310009 China Department of General Surgery Sir Run Run Shaw Hospital School of Medicine Zhejiang University Hangzhou 310016 China Liangzhu Laboratory Zhejiang University Hangzhou 311121 China Department of Burns and Wound Center Second Affiliated Hospital School of Medicine Zhejiang University Hangzhou 310009 China Jinhua Institute of Zhejiang University Jinhua 321299 China MOE Key Laboratory of Macromolecular Synthesis and Functionalization Department of Polymer Science and Engineering Zhejiang University Hangzhou 310027 China

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Platelet-Drug Conjugates Engineered via One-step Fusion Approach for Metastatic and Postoperative Cancer Treatment

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Angewandte Chemie 2024年第37期136卷

The exploration of cell-based drug delivery systems for cancer therapy has gained growing attention. Approaches to engineering therapeutic cells with multidrug loading in an effective, safe, and precise manner while preserving their inherent biological properties remain of great interest. Here, we report a strategy to simultaneously load multiple drugs in platelets in a one-step fusion process. We demonstrate doxorubicin (DOX)-encapsulated liposomes conjugated with interleukin-15 (IL-15) could fuse with platelets to achieve both cytoplasmic drug loading and surface cytokine modification with a loading efficiency of over 70 % within minutes. Due to their inherent targeting ability to metastatic cancers and postoperative bleeding sites, the engineered platelets demonstrated a synergistic therapeutic effect to suppress lung metastasis and postoperative recurrence in mouse B16F10 melanoma tumor models.

关键词： drug delivery platelet cancer immunotherapy liposome

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Frontispiz: Platelet-Drug Conjugates Engineered via One-step Fusion Approach for Metastatic and Postoperative Cancer Treatment

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Angewandte Chemie 2024年第37期136卷

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A novel asymmetric amphiphilic porous film of (PLA)-(PLA-b-PEG)-(PEG) with controlled gradual pore size

Results in Materials

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Results in Materials 2020年 6卷

作者： Huang, Ran Zhou, Boxin Nie, Zhuping Ding, Weiwei Jiang, Xilin Song, Yihu Department of Materials Technology and Engineering Research Institute of Zhejiang University-Taizhou Zhejiang Taizhou 318000 China State Key Laboratory of Microbial Metabolism and School of Life Sciences and Biotechnology Shanghai Jiao Tong University Shanghai 200240 China MOE Key Laboratory of Macromolecular Synthesis and Functionalization Department of Polymer Science and Engineering Zhejiang University Zhejiang Hangzhou 310027 China

A porous film of (PLA)-(PLA-b-PEG)-(PEG) is fabricated as a general biomedical device for potential applications. For the purpose of providing both mechanic strength and bio-friendly supporting, the film is designed to be asymmetric with a PLA-densed hydrophobic surface and a PEG-densed hydrophilic surface. Beyond the conventional technique to achieve amphiphilicity and porosity via simple blend of two typical biopolymers, a fine controlled processing is developed to achieve the gradual pore size along depth with the attendance of block polymer, which provides several advantages such as avoiding sharp phase separation, the gradual release of biofactors as a carrier, etc. © 2020 The Author(s)

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Synergistic Reversal of Inflammation-Mediated Degeneration in Intervertebral Discs: Phenylboric Acid-Grafted Hyaluronic Acid Hydrogel as an Anti-Oxidative Vehicle for Timp-3 Delivery and Promotion of Extracellular Matrix synthesis

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Acta Biomaterialia 2025年

作者： Yan Li Yuxiang Zhang Shuqin Wang Xiaojing Ma Chengxin Dai Yifan Wang Chenyi Ye Sunwen Pan Changyou Gao Weixu Li Department of Orthopedic Surgery the Second Affiliated Hospital Zhejiang University School of Medicine Hangzhou 310020 China Orthopedics Research Institute of Zhejiang University Hangzhou City Zhejiang Province China Department of Plastic Surgery Sir Run Run Shaw Hospital Zhejiang University School of Medicine Hangzhou China MOE Key Laboratory of Macromolecular Synthesis and Functionalization International Research Center for X Polymers Department of Polymer Science and Engineering Zhejiang University Hangzhou 310058 China Department of Pathology the Second Affiliated Hospital Zhejiang University School of Medicine Hangzhou China

Background : Intervertebral disc degeneration (IDD) is intricately linked to the aging process, wherein reactive oxygen species (ROS) and inflammatory responses markedly contribute to matrix degradation and hyperplasia. Injectable antioxidant hydrogels loaded with pharmacological agents hold immense promise for clinical translation in early intervention of IDD. Our previous study revealed that the tissue inhibitor of metalloproteinase-3 (TIMP3) is a pivotal regulator of matrix remodeling and inflammation. Results : We developed a biodegradable ROS-responsive hydrogel functionalized with phenylboronic acid (R-gel) as a controlled release carrier of TIMP3 (R-gel-TIMP3). R-gel-TIMP3 effectively scavenged ROS and provided sustained TIMP3 delivery, thereby attenuating inflammation-driven disc degeneration. In vitro, R-gel-TIMP3 exhibited negligible cytotoxicity, reduced ROS levels in the nucleus pulposus cells, and alleviated cellular senescence and apoptosis. In vivo, it decreased ROS accumulation, inflammatory M1 macrophages, matrix degradation, and neovascularization, significantly ameliorating IDD pathology. Conclusion : The synergistic action of ROS-responsive TIMP3 delivery markedly amplified the therapeutic efficacy against IDD, underscoring the therapeutic potential of R-gel-TIMP3 in IDD management. Statement of Significance 1 We synthesized an injectable bioactive ROS-responsive hydrogel as an anti-oxidative vehicle for TIMP3 protein delivery. 2 The hydrogel enabled sustained release of TIMP-3 in situ and acted as an efficient ROS scavenger to protect NPs against oxidative stress. 3 This treatment could effectively intervene in the progression of IDD from early stage, promote extracellular matrix synthesis, and ultimately reduce IDD in a rat model.

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Enabling Polymer Single Crystals to Be High-Performance Dielectric

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Angewandte Chemie 2023年第7期136卷

作者： Dr. Min Chen Prof. Wee-Liat Ong Prof. Boyu Peng Dr. Xuyun Guo Dr. Jie Ren Prof. Ye Zhu Prof. Hanying Li MOE Key Laboratory of Macromolecular Synthesis and Functionalization International Research Center for X Polymers Shanxi-Zheda Institute of Advanced Materials and Chemical Engineering Department of Polymer Science and Engineering Zhejiang University Hangzhou 310027 P. R. China ZJU-UIUC Institute College of Energy Engineering State Key Laboratory of Clean Energy Utilization Zhejiang University Hangzhou 310027 P. R. China Department of Applied Physics Research Institute for Smart Energy The Hong Kong Polytechnic University 0000 Hong Kong P. R. China

Semicrystalline polymer dielectrics (SPDs) are highly sought-after state-of-the-art dielectric materials. As the disorder in SPDs degrades their electrical properties, homogeneously ordered SPDs are desired. However, complex crystallization behaviors of polymers make such homogeneity elusive. Polymer lamellar single crystals (PLSCs), the most regularly-ordered form of SPDs possible under mild crystallizing conditions, are ideal platforms for understanding and developing high-performance dielectric materials. Here, a typical and widely used SPD, polyethylene (PE) is selected as the model material. We successfully obtained, large, uniform, and high-quality PE PLSCs and devised a non-destructive strategy to construct PE PLSC-based vertical capacitors. These nanometer-thick capacitors exhibit exceptional dielectric properties, with a high breakdown strength of 6.95 MV/cm and a low dielectric constant of 2.14±0.07, that outperform the properties of any existing neat PE. This work provides novel insights into exploring the performance possibility of ordered SPDs and reveals the PLSCs as potential high-performance dielectric materials.

关键词： Dielectrics Nano Capacitor Devices Polyethylene Polymer Single Crystals

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