Bimetallic clusterzymes-loaded dendritic mesoporous silica particle regulate arthritis microenvironment via ROS scavenging and YAP1 stabilization

Clusterzymes are synthetic enzymes exhibiting substantial catalytic activity and selectivity, which are uniquely driven by single-atom constructs. A dramatic increase in antioxidant capacity, 158 times more than natural trolox, is noted when single-atom copper is incorporated into gold-based cluster...

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Main Authors: Yang Jin, Chuan Hu, Jiechao Xia, Dingqi Xie, Lin Ye, Xinyi Ye, Li Jiang, Honghai Song, Yutao Zhu, Sicheng Jiang, Weiqing Li, Weiming Qi, Yannan Yang, Zhijun Hu
Format: Article
Language:English
Published: KeAi Communications Co., Ltd. 2024-12-01
Series:Bioactive Materials
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Online Access:http://www.sciencedirect.com/science/article/pii/S2452199X24003918
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author Yang Jin
Chuan Hu
Jiechao Xia
Dingqi Xie
Lin Ye
Xinyi Ye
Li Jiang
Honghai Song
Yutao Zhu
Sicheng Jiang
Weiqing Li
Weiming Qi
Yannan Yang
Zhijun Hu
author_facet Yang Jin
Chuan Hu
Jiechao Xia
Dingqi Xie
Lin Ye
Xinyi Ye
Li Jiang
Honghai Song
Yutao Zhu
Sicheng Jiang
Weiqing Li
Weiming Qi
Yannan Yang
Zhijun Hu
author_sort Yang Jin
collection DOAJ
description Clusterzymes are synthetic enzymes exhibiting substantial catalytic activity and selectivity, which are uniquely driven by single-atom constructs. A dramatic increase in antioxidant capacity, 158 times more than natural trolox, is noted when single-atom copper is incorporated into gold-based clusterzymes to form Au24Cu1. Considering the inflammatory and mildly acidic microenvironment characteristic of osteoarthritis (OA), pH-dependent dendritic mesoporous silica nanoparticles (DMSNs) coupled with PEG have been employed as a delivery system for the spatial-temporal release of clusterzymes within active articular regions, thereby enhancing the duration of effectiveness. Nonetheless, achieving high therapeutic efficacy remains a significant challenge. Herein, we describe the construction of a Clusterzymes-DMSNs-PEG complex (CDP) which remarkably diminishes reactive oxygen species (ROS) and stabilizes the chondroprotective protein YAP by inhibiting the Hippo pathway. In the rabbit ACLT (anterior cruciate ligament transection) model, the CDP complex demonstrated inhibition of matrix metalloproteinase activity, preservation of type II collagen and aggregation protein secretion, thus prolonging the clusterzymes' protective influence on joint cartilage structure. Our research underscores the efficacy of the CDP complex in ROS-scavenging, enabled by the release of clusterzymes in response to an inflammatory and slightly acidic environment, leading to the obstruction of the Hippo pathway and downstream NF-κB signaling pathway. This study illuminates the design, composition, and use of DMSNs and clusterzymes in biomedicine, thus charting a promising course for the development of novel therapeutic strategies in alleviating OA.
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spelling doaj-art-4d1ad7d4e19e4b4888c1d4aa08dae15a2025-08-20T02:18:46ZengKeAi Communications Co., Ltd.Bioactive Materials2452-199X2024-12-014261362710.1016/j.bioactmat.2024.09.004Bimetallic clusterzymes-loaded dendritic mesoporous silica particle regulate arthritis microenvironment via ROS scavenging and YAP1 stabilizationYang Jin0Chuan Hu1Jiechao Xia2Dingqi Xie3Lin Ye4Xinyi Ye5Li Jiang6Honghai Song7Yutao Zhu8Sicheng Jiang9Weiqing Li10Weiming Qi11Yannan Yang12Zhijun Hu13Department of Orthopaedic Surgery, Key Laboratory of Musculoskeletal System Degeneration and Regeneration Translational Research of Zhejiang Province, Sir Run Run Shaw Hospital, Medical College of Zhejiang University, Hangzhou, 310016, ChinaDepartment of Orthopaedic Surgery, Key Laboratory of Musculoskeletal System Degeneration and Regeneration Translational Research of Zhejiang Province, Sir Run Run Shaw Hospital, Medical College of Zhejiang University, Hangzhou, 310016, ChinaDepartment of Orthopaedic Surgery, Key Laboratory of Musculoskeletal System Degeneration and Regeneration Translational Research of Zhejiang Province, Sir Run Run Shaw Hospital, Medical College of Zhejiang University, Hangzhou, 310016, ChinaDepartment of Orthopaedic Surgery, Key Laboratory of Musculoskeletal System Degeneration and Regeneration Translational Research of Zhejiang Province, Sir Run Run Shaw Hospital, Medical College of Zhejiang University, Hangzhou, 310016, ChinaDepartment of Orthopaedic Surgery, Key Laboratory of Musculoskeletal System Degeneration and Regeneration Translational Research of Zhejiang Province, Sir Run Run Shaw Hospital, Medical College of Zhejiang University, Hangzhou, 310016, ChinaZhejiang University School of Medicine, Zhejiang University, Hangzhou, ChinaDepartment of Biochemistry and Molecular Biology, School of Basic Medical Sciences, Hangzhou Normal University, Hangzhou, ChinaDepartment of Orthopaedic Surgery, Key Laboratory of Musculoskeletal System Degeneration and Regeneration Translational Research of Zhejiang Province, Sir Run Run Shaw Hospital, Medical College of Zhejiang University, Hangzhou, 310016, ChinaDepartment of Orthopaedic Surgery, Key Laboratory of Musculoskeletal System Degeneration and Regeneration Translational Research of Zhejiang Province, Sir Run Run Shaw Hospital, Medical College of Zhejiang University, Hangzhou, 310016, ChinaDepartment of Orthopaedic Surgery, Key Laboratory of Musculoskeletal System Degeneration and Regeneration Translational Research of Zhejiang Province, Sir Run Run Shaw Hospital, Medical College of Zhejiang University, Hangzhou, 310016, ChinaZhejiang University School of Medicine, Zhejiang University, Hangzhou, ChinaZhejiang Center for Medical Device Evaluation, Zhejiang Medical Products Administration Hangzhou 310009, Zhejiang, China; Corresponding author. Zhejiang Center for Medical Device Evaluation, Zhejiang Medical Products Administration Hangzhou 310009, Zhejiang, China.Institute of Optoelectronics, Fudan University, Shanghai, 200433, China; South Australian ImmunoGENomics Cancer Institute, Faculty of Health and Medical Sciences, The University of Adelaide, Adelaide, South Australia, 5005, Australia; Corresponding author. South Australian ImmunoGENomics Cancer Institute, Faculty of Health and Medical Sciences, The University of Adelaide, Adelaide, South Australia, 5005, Australia.Department of Orthopaedic Surgery, Key Laboratory of Musculoskeletal System Degeneration and Regeneration Translational Research of Zhejiang Province, Sir Run Run Shaw Hospital, Medical College of Zhejiang University, Hangzhou, 310016, China; Corresponding author.Clusterzymes are synthetic enzymes exhibiting substantial catalytic activity and selectivity, which are uniquely driven by single-atom constructs. A dramatic increase in antioxidant capacity, 158 times more than natural trolox, is noted when single-atom copper is incorporated into gold-based clusterzymes to form Au24Cu1. Considering the inflammatory and mildly acidic microenvironment characteristic of osteoarthritis (OA), pH-dependent dendritic mesoporous silica nanoparticles (DMSNs) coupled with PEG have been employed as a delivery system for the spatial-temporal release of clusterzymes within active articular regions, thereby enhancing the duration of effectiveness. Nonetheless, achieving high therapeutic efficacy remains a significant challenge. Herein, we describe the construction of a Clusterzymes-DMSNs-PEG complex (CDP) which remarkably diminishes reactive oxygen species (ROS) and stabilizes the chondroprotective protein YAP by inhibiting the Hippo pathway. In the rabbit ACLT (anterior cruciate ligament transection) model, the CDP complex demonstrated inhibition of matrix metalloproteinase activity, preservation of type II collagen and aggregation protein secretion, thus prolonging the clusterzymes' protective influence on joint cartilage structure. Our research underscores the efficacy of the CDP complex in ROS-scavenging, enabled by the release of clusterzymes in response to an inflammatory and slightly acidic environment, leading to the obstruction of the Hippo pathway and downstream NF-κB signaling pathway. This study illuminates the design, composition, and use of DMSNs and clusterzymes in biomedicine, thus charting a promising course for the development of novel therapeutic strategies in alleviating OA.http://www.sciencedirect.com/science/article/pii/S2452199X24003918ClusterzymeSustained deliveryReactive oxygen speciesHippo pathwayRabbit anterior cruciate ligament transection model
spellingShingle Yang Jin
Chuan Hu
Jiechao Xia
Dingqi Xie
Lin Ye
Xinyi Ye
Li Jiang
Honghai Song
Yutao Zhu
Sicheng Jiang
Weiqing Li
Weiming Qi
Yannan Yang
Zhijun Hu
Bimetallic clusterzymes-loaded dendritic mesoporous silica particle regulate arthritis microenvironment via ROS scavenging and YAP1 stabilization
Bioactive Materials
Clusterzyme
Sustained delivery
Reactive oxygen species
Hippo pathway
Rabbit anterior cruciate ligament transection model
title Bimetallic clusterzymes-loaded dendritic mesoporous silica particle regulate arthritis microenvironment via ROS scavenging and YAP1 stabilization
title_full Bimetallic clusterzymes-loaded dendritic mesoporous silica particle regulate arthritis microenvironment via ROS scavenging and YAP1 stabilization
title_fullStr Bimetallic clusterzymes-loaded dendritic mesoporous silica particle regulate arthritis microenvironment via ROS scavenging and YAP1 stabilization
title_full_unstemmed Bimetallic clusterzymes-loaded dendritic mesoporous silica particle regulate arthritis microenvironment via ROS scavenging and YAP1 stabilization
title_short Bimetallic clusterzymes-loaded dendritic mesoporous silica particle regulate arthritis microenvironment via ROS scavenging and YAP1 stabilization
title_sort bimetallic clusterzymes loaded dendritic mesoporous silica particle regulate arthritis microenvironment via ros scavenging and yap1 stabilization
topic Clusterzyme
Sustained delivery
Reactive oxygen species
Hippo pathway
Rabbit anterior cruciate ligament transection model
url http://www.sciencedirect.com/science/article/pii/S2452199X24003918
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