Journal of the American Chemical Society最新文献_第3页

Quantum Interference in a Molecular Analog of the Crystalline Silicon Unit Cell 晶体硅单晶胞分子模拟中的量子干涉

IF 15 1区化学

Journal of the American Chemical Society Pub Date : 2025-05-01 DOI: 10.1021/jacs.5c04272

Matthew O. Hight, Ashley E. Pimentel, Timothy C. Siu, Joshua Y. Wong, Jennifer Nguyen, Veronica Carta, Timothy A. Su

{"title":"Quantum Interference in a Molecular Analog of the Crystalline Silicon Unit Cell","authors":"Matthew O. Hight, Ashley E. Pimentel, Timothy C. Siu, Joshua Y. Wong, Jennifer Nguyen, Veronica Carta, Timothy A. Su","doi":"10.1021/jacs.5c04272","DOIUrl":"https://doi.org/10.1021/jacs.5c04272","url":null,"abstract":"This manuscript describes the emergence of destructive σ-quantum interference (σ-DQI) in sila-adamantane, a molecule whose cluster core is isostructural with the crystalline silicon unit cell. To reveal these σ-DQI effects, we take a bridge-cutting approach where we conceptually pare sila-adamantane down to its bicyclic Si[3.3.1] and linear oligosilane forms. Scanning tunneling microscopy break-junction (STM-BJ) measurements reveal that conductance in single-molecule junctions of the tricyclic sila-adamantane is 2.7-times lower than their bicyclic Si[3.3.1] analog. The only structural difference between their cluster cores is a remote dimethylsilylene bridge that is present in sila-adamantane yet absent in Si[3.3.1]. Density functional theory calculations reveal that this dimethylsilylene enforces C3 symmetry at the sila-diamondoid bridgeheads, allowing each electrode to couple into the three cluster bridge dimensions equally. Though each bridge alignment is sterically equivalent, they have profound electronic differences: when electrodes align with the long branches of sila-adamantane, strong σ-DQI interactions occur between frontier molecular orbitals that suppress electronic transmission across the molecular junction. We exploit these alignment-dependent σ-DQI effects to create new forms of stereoelectronic conductance switches, where a reversible mechanical stimulus controls which pathway through the diamondoid framework the electrodes align through. This represents the first example of dynamic modulation of σ-DQI and enables us to achieve switching ratios (average on/off ∼5.6) higher than previously reported σ-stereoelectronic switches. These studies reveal how the innate dimensionality and symmetry of crystalline silicon influence charge transport at its most fundamental level, and how these principles can be harnessed to control quantum interference in single-molecule electronics.","PeriodicalId":49,"journal":{"name":"Journal of the American Chemical Society","volume":"44 1","pages":""},"PeriodicalIF":15.0,"publicationDate":"2025-05-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143898118","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Monomeric Two-coordinate Beryllium Imido and Boryloxide Complexes Featuring Be–N and Be–O Triple Bonds 具有Be-N和Be-O三键的双配位铍亚胺和硼氧化物配合物

IF 15 1区化学

Journal of the American Chemical Society Pub Date : 2025-05-01 DOI: 10.1021/jacs.5c04320

Christoph Helling, David J. D. Wilson, Cameron Jones

{"title":"Monomeric Two-coordinate Beryllium Imido and Boryloxide Complexes Featuring Be–N and Be–O Triple Bonds","authors":"Christoph Helling, David J. D. Wilson, Cameron Jones","doi":"10.1021/jacs.5c04320","DOIUrl":"https://doi.org/10.1021/jacs.5c04320","url":null,"abstract":"The 2p elements possess a unique propensity to participate in multiple bonding. Realization of multiple bonding involving the 2s elements, however, is challenging and remains exceedingly rare. In this contribution, we present the syntheses, detailed characterization, and molecular structures of heteroleptic beryllium imido and boryloxide complexes of the type [(HCNDip)2YXBeAr(OEt2)n]m (Y,X = C,N or B,O; n = 0, 1; m = 1, 2; Dip = 2,6-iPr2C6H3) by salt metathesis and arene elimination approaches. Systematic adjustment of the steric demand of the aryl substituent resulted in the isolation of monomeric, two-coordinate beryllium imido and boryloxide complexes, (HCNDip)2CNBeTip (9, Tip = 2,4,6-iPr3C6H2) and (HCNDip)2BOBeArDip (12, ArDip = 2,6-Dip2C6H3), containing virtually linear C–N–Be–C and B–O–Be–C arrangements and extremely short Be–N (1.434(2) Å, 1.437(3) Å) and Be–O (1.4035(14) Å) bonds, respectively. These were shown by in-depth computational electronic structure and bonding analyses to possess unprecedented triple bond character. The Be–O bond in 12 constitutes the first s-block metal–oxygen multiple bond.","PeriodicalId":49,"journal":{"name":"Journal of the American Chemical Society","volume":"5 1","pages":""},"PeriodicalIF":15.0,"publicationDate":"2025-05-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143898119","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Atomically Dispersed High-Valent d0-Metal Breaks the Activity–Stability Trade-Off in Proton Exchange Membrane Water Electrolysis 原子分散的高价金属打破了质子交换膜电解中活性-稳定性的权衡

IF 15 1区化学

Journal of the American Chemical Society Pub Date : 2025-05-01 DOI: 10.1021/jacs.5c00936

Jaehyuk Shim, Kangjae Lee, Yunjae Yu, Hyeon Seok Lee, Heejong Shin, Kug-Seung Lee, Megalamane S. Bootharaju, Sanghwi Han, Gyu Seong Yi, Hyojoo Ko, Sihwa Lee, Jaeyune Ryu, Minho Kim, Byoung-Hoon Lee, Taeghwan Hyeon, Yung-Eun Sung

{"title":"Atomically Dispersed High-Valent d0-Metal Breaks the Activity–Stability Trade-Off in Proton Exchange Membrane Water Electrolysis","authors":"Jaehyuk Shim, Kangjae Lee, Yunjae Yu, Hyeon Seok Lee, Heejong Shin, Kug-Seung Lee, Megalamane S. Bootharaju, Sanghwi Han, Gyu Seong Yi, Hyojoo Ko, Sihwa Lee, Jaeyune Ryu, Minho Kim, Byoung-Hoon Lee, Taeghwan Hyeon, Yung-Eun Sung","doi":"10.1021/jacs.5c00936","DOIUrl":"https://doi.org/10.1021/jacs.5c00936","url":null,"abstract":"Green hydrogen production via proton exchange membrane water electrolysis (PEMWE) faces economic feasibility challenges, primarily due to its reliance on noble metal catalysts. While cost-effective Ru-based catalysts show promise as alternatives to expensive Ir-based catalysts for an anodic oxygen evolution reaction, their long-term performance is compromised by overoxidation at high current densities. In addressing this challenge, we present a cooperative dual-site strategy for atomic-scale incorporation of high-valent d0-metal cations into RuO2. This synthesis results in uniformly distributed Ru–O–d0metal bonds, effectively reconciling the activity and stability trade-off. Leveraging these effects, our optimized Ta1/RuO2 catalyst demonstrates exceptional performance, with a low overpotential of 164 ± 2 mV and stable operation for 1000 h at 100 mA cm–2. In practical PEMWE systems, Ta1/RuO2 achieves 1.58 V at 2 A cm–2, surpassing the 2026 Department of Energy target, and maintains remarkable stability over 650 h at 500 mA cm–2. This breakthrough offers a highly active and durable PEMWE system suitable for industrial-scale applications.","PeriodicalId":49,"journal":{"name":"Journal of the American Chemical Society","volume":"48 1","pages":""},"PeriodicalIF":15.0,"publicationDate":"2025-05-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143898113","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Anchoring Side Chains to Carbonate Groups for Reviving Stable Polycarbonate-Based Solid-State Lithium Metal Batteries 锚定碳酸盐基团侧链以恢复稳定的聚碳酸酯基固态锂金属电池

IF 15 1区化学

Journal of the American Chemical Society Pub Date : 2025-05-01 DOI: 10.1021/jacs.5c00760

Hantao Xu, Wei Deng, Jingyuan Yu, Lei Shi, Wenwei Zhang, Juncai Long, Chaobin He, Lin Xu

{"title":"Anchoring Side Chains to Carbonate Groups for Reviving Stable Polycarbonate-Based Solid-State Lithium Metal Batteries","authors":"Hantao Xu, Wei Deng, Jingyuan Yu, Lei Shi, Wenwei Zhang, Juncai Long, Chaobin He, Lin Xu","doi":"10.1021/jacs.5c00760","DOIUrl":"https://doi.org/10.1021/jacs.5c00760","url":null,"abstract":"Polycarbonate-based electrolytes are ideal electrolytes for solid-state lithium metal batteries (LMBs) due to their wider electrochemical windows and considerable ionic conductivities compared with conventional solid polymer electrolytes. However, polycarbonates encounter severe interfacial side reactions with lithium metal, leading to the interfacial degradation of polymers. Herein, a spontaneously formed restricted conformation is designed via the in situ anchoring of side chains to suppress the interfacial degradation of polycarbonate-based electrolytes. The restricted conformation enables the side chains to shield and protect the degradable ester bonds of cyclic carbonates, suppressing contact and interfacial degradation between polycarbonates and lithium metal anodes. As a proof of concept, the protected polycarbonate-based electrolyte demonstrates a stable cycling capability of the Li/Li cell beyond 1000 h at a current density of 0.5 mA cm–2, and the assembled LiNi0.8Co0.1Mn0.1O2/Li pouch cell also achieves similar improvement in cycling performance. This work indicates that the strategy of constructing restricted conformations via anchoring side chains is a feasible avenue for fabricating highly stable polycarbonate-based solid-state LMBs.","PeriodicalId":49,"journal":{"name":"Journal of the American Chemical Society","volume":"88 1","pages":""},"PeriodicalIF":15.0,"publicationDate":"2025-05-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143893561","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Direct Observation of C–F Bond Formation from Isolable Palladium(IV) Systems via an Outer-Sphere Pathway 通过外球途径直接观察可分离钯（IV）体系的C-F键形成

IF 15 1区化学

Journal of the American Chemical Society Pub Date : 2025-05-01 DOI: 10.1021/jacs.5c01147

Haobin Li, Rui Feng, Guo Wang, Yimeng Wang, Wenxi Liu, Shuai Guo

引用次数: 0

Enzyme- and DNAzyme-Driven Transient Assembly of DNA-Based Phase-Separated Coacervate Microdroplets 酶和dnazyme驱动的基于dna相分离凝聚微滴的瞬时组装

IF 15 1区化学

Journal of the American Chemical Society Pub Date : 2025-04-30 DOI: 10.1021/jacs.5c00637

Yunlong Qin, Yang Sung Sohn, Rachel Nechushtai, Fan Xia, Fujian Huang, Itamar Willner

{"title":"Enzyme- and DNAzyme-Driven Transient Assembly of DNA-Based Phase-Separated Coacervate Microdroplets","authors":"Yunlong Qin, Yang Sung Sohn, Rachel Nechushtai, Fan Xia, Fujian Huang, Itamar Willner","doi":"10.1021/jacs.5c00637","DOIUrl":"https://doi.org/10.1021/jacs.5c00637","url":null,"abstract":"An assembly of dissipative, transient, DNA-based microdroplet (MD) coacervates in the presence of auxiliary enzymes (endonucleases and nickases) or MD-embedded DNAzyme is introduced. Two pairs of different Y-shaped DNA core frameworks modified with toehold tethers are cross-linked by complementary toehold-functionalized duplexes, engineered to be cleaved by EcoRI or HindIII endonucleases, or cross-linked by palindromic strands that include pre-engineered Nt.BbvCI or Nb.BtsI nicking sites, demonstrating transient evolution/depletion of phase-separated MD coacervates. By mixing the pairs of endonuclease- or nickase-responsive MDs, programmed or gated transient formation/depletion of MD frameworks is presented. In addition, by cross-linking a pre-engineered Y-shaped core framework with a sequence-designed fuel strand, phase separation of MD coacervates with embedded Mg2+-DNAzyme units is introduced. The DNAzyme-catalyzed cleavage of a ribonucleobase-modified hairpin substrate, generating the waste product of the metabolite fragments, leads to the metabolite-driven separation of the cross-linked coacervates, resulting in the temporal evolution and depletion of the DNAzyme-functionalized MDs. By employing a light-responsive caged hairpin structure, the light-modulated fueled evolution and depletion of the DNAzyme-active MDs are presented. The enzyme- or DNAzyme-catalyzed transient evolution/depletion of the MD coacervates provides protocell frameworks mimicking dynamic transient processes of native cells. The possible application of MDs as functional carriers for the temporal, dose-controlled release of loads is addressed.","PeriodicalId":49,"journal":{"name":"Journal of the American Chemical Society","volume":"44 1","pages":""},"PeriodicalIF":15.0,"publicationDate":"2025-04-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143893672","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Trilocked Photodynamic Senolytic Inducer Potentiating Immunogenic Senescent Cell Removal for Liver Fibrosis Resolution 三锁光动力衰老诱导剂增强免疫原性衰老细胞清除肝纤维化解决方案

IF 15 1区化学

Journal of the American Chemical Society Pub Date : 2025-04-30 DOI: 10.1021/jacs.5c03498

Pei Lu, Huihui Zhou, Xiaoxiao Xu, Ying Long, Jian-Hui Jiang, Fenglin Wang

{"title":"Trilocked Photodynamic Senolytic Inducer Potentiating Immunogenic Senescent Cell Removal for Liver Fibrosis Resolution","authors":"Pei Lu, Huihui Zhou, Xiaoxiao Xu, Ying Long, Jian-Hui Jiang, Fenglin Wang","doi":"10.1021/jacs.5c03498","DOIUrl":"https://doi.org/10.1021/jacs.5c03498","url":null,"abstract":"Liver fibrosis is a major global health problem without effective therapies, and targeted elimination of senescent cells is beneficial for hepatic function and organism survival. We report a new trilocked photodynamic senolytic inducer (PDSI) strategy for liver fibrosis resolution using a type-I photodynamic agent for immunogenic clearance of senescent cells. We demonstrate that this trilocked PDSI not only facilitates efficient production of superoxide anions (O2•–) in lysosomes of senescent cells for photodynamic therapy, but also permits NIR fluorescence and photoacoustic (NIRF/PA) imaging of senescent cells. Mechanistic investigation reveals that the trilocked PDSI elicited senescent cell clearance predominantly via the immunogenic necroptosis pathway. Moreover, this PDSI with a liver-targeting moiety enables high-contrast NIRF/PA imaging and effective liver fibrosis resolution in vivo. This liver-targeting PDSI exhibits remarkable immunogenic ablation of senescent cells, with enhancing dendritic cell maturation and cytotoxic T cell recruitment in liver fibrosis. Our study highlights the potential of trilocked type I PDSI for boosting immunity for senescent cell clearance and liver fibrosis treatment.","PeriodicalId":49,"journal":{"name":"Journal of the American Chemical Society","volume":"114 1","pages":""},"PeriodicalIF":15.0,"publicationDate":"2025-04-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143894028","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Semiconducting Polyaromatic Covalent Organic Frameworks Constructed through Self-Aldol Condensation 通过自醛醇缩合构建的半导体多芳共价有机骨架

IF 15 1区化学

Journal of the American Chemical Society Pub Date : 2025-04-30 DOI: 10.1021/jacs.5c04944

Xiaoyi Xu, Yaoqian Feng, Hongzheng Chen, Ning Huang

{"title":"Semiconducting Polyaromatic Covalent Organic Frameworks Constructed through Self-Aldol Condensation","authors":"Xiaoyi Xu, Yaoqian Feng, Hongzheng Chen, Ning Huang","doi":"10.1021/jacs.5c04944","DOIUrl":"https://doi.org/10.1021/jacs.5c04944","url":null,"abstract":"The construction of semiconducting covalent organic frameworks (COFs) via single-component self-polymerization is of broad interest in reticular chemistry. Herein, two semiconducting polyaromatic COFs with all-fused-ring conjugation structures were synthesized through the self-aldol condensation of indanone-based building blocks. The resulting COFs exhibit n-type semiconducting properties and exceptional stability under harsh acidic and alkaline conditions. The electrical conductivity and charge carrier mobility of the polyaromatic COFs reached up to 5.5 × 10–3 S cm–1 and 0.62 cm2 V–1 s–1, which ranked as the highest values among n-type semiconducting COFs. The high crystallinity, intrinsic porosity, excellent conductivity, and abundant five-membered rings as active sites render these COFs as effective metal-free electrocatalysts toward oxygen reduction reaction (ORR). Notably, one of these COFs shows a half-wave potential of up to 0.77 V under alkaline conditions, which constitutes one of the highest values among the reported metal-free ORR electrocatalysts. In addition, owing to the strong robustness of the polyaromatic COFs, they also exhibit long-term catalytic durability. This study not only expands the diversity of semiconducting COFs but also establishes new paradigms for the development of high-performance metal-free electrocatalysts toward the ORR process.","PeriodicalId":49,"journal":{"name":"Journal of the American Chemical Society","volume":"36 1","pages":""},"PeriodicalIF":15.0,"publicationDate":"2025-04-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143893678","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Rhodium-Catalyzed [5 + 1 + 2] Reaction of Yne-Vinylcyclopropenes and CO: The Application of Vinylcyclopropenes for Higher-Order Cycloaddition 铑催化乙烯基环丙烯与CO的[5 + 1 + 2]反应：乙烯基环丙烯在高阶环加成中的应用

IF 15 1区化学

Journal of the American Chemical Society Pub Date : 2025-04-30 DOI: 10.1021/jacs.5c02041

Zhiqiang Huang, Zhi-Xiang Yu

{"title":"Rhodium-Catalyzed [5 + 1 + 2] Reaction of Yne-Vinylcyclopropenes and CO: The Application of Vinylcyclopropenes for Higher-Order Cycloaddition","authors":"Zhiqiang Huang, Zhi-Xiang Yu","doi":"10.1021/jacs.5c02041","DOIUrl":"https://doi.org/10.1021/jacs.5c02041","url":null,"abstract":"Transition metal-catalyzed higher-order cycloadditions involving vinylcyclopropenes (VCPEs) have not been realized to synthesize challenging medium-sized rings, partially due to their poor stability and many competing side reactions. We report here a Rh-catalyzed [5 + 1 + 2] reaction of yne-VCPEs and CO for the synthesis of eight-membered carbocycles with trienone moiety, which so far can be accessed by only limited reactions. The key to this higher-order cycloaddition is that once C–C cleavage of VCPE (C5 synthon) to form a six-membered metallacycle is initiated, CO (C1 synthon) insertion happens before alkyne (C2 synthon) insertion, attributing to the special reactivity of the sp2 carbon in the vinylcyclopropene. Quantum chemical calculations have been applied to support this reaction pathway. The present [5 + 1 + 2] reaction has a broad scope, and the C2 synthon can also be extended to alkenes and allene. Of the same importance, the present reaction can be catalyzed by either [Rh(CO)2Cl]2 or a cheaper complex, RhCl3·nH2O.","PeriodicalId":49,"journal":{"name":"Journal of the American Chemical Society","volume":"20 1","pages":""},"PeriodicalIF":15.0,"publicationDate":"2025-04-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143890208","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Self-Adaptive Release of Stem Cell-Derived Exosomes from a Multifunctional Hydrogel for Accelerating MRSA-Infected Diabetic Wound Repair 多功能水凝胶中干细胞衍生外泌体的自适应释放加速mrsa感染的糖尿病伤口修复

IF 15 1区化学

Journal of the American Chemical Society Pub Date : 2025-04-30 DOI: 10.1021/jacs.5c02184

Xiang Wang, Jiantong Dong, Jingjing Kang, Xujing Chen, Xiaoqin Hong, Jiaming Chen, Wei Du, Hong Cai, Dingbin Liu

{"title":"Self-Adaptive Release of Stem Cell-Derived Exosomes from a Multifunctional Hydrogel for Accelerating MRSA-Infected Diabetic Wound Repair","authors":"Xiang Wang, Jiantong Dong, Jingjing Kang, Xujing Chen, Xiaoqin Hong, Jiaming Chen, Wei Du, Hong Cai, Dingbin Liu","doi":"10.1021/jacs.5c02184","DOIUrl":"https://doi.org/10.1021/jacs.5c02184","url":null,"abstract":"Chronic diabetic wounds are prone to severe skin necrosis and bacterial infections, with elevated reactive oxygen species (ROS) and persistent inflammation further hindering the healing process. Developing smart dressings with multifunctional therapeutic capabilities to simultaneously combat infections, reduce oxidative stress, alleviate inflammation, and promote tissue regeneration remains a significant challenge. Here, we introduce a self-adaptive yet multifunctional hydrogel (Exo-Gel) designed to accelerate methicillin-resistant Staphylococcus aureus (MRSA)-infected diabetic wound repair. Exo-Gel utilizes choline phosphate (CP) groups to both anchor stem cell-derived exosomes (Exo) via electrostatic interactions and disrupt bacterial membranes, providing inherent bacteriostatic effects. Additionally, ROS-responsive thioketal (TK) linkers enable the self-adaptive release of exosomes based on local ROS levels while also scavenging excess ROS. This synergistic system facilitates wound healing by modulating oxidative stress, reducing inflammation, promoting M2 macrophage polarization, and enhancing cell proliferation, myofibroblast migration, angiogenesis, and collagen deposition to accelerate tissue regeneration. In diabetic Sprague–Dawley rats with MRSA-infected full-thickness wounds, Exo-Gel achieved remarkable bacteriostatic activity and accelerated wound healing. Exo-Gel offers a cost-effective, multifunctional, and self-adaptive therapeutic strategy for managing chronic diabetic wounds, requiring no external components or operations, making it highly practical and translatable for clinical applications.","PeriodicalId":49,"journal":{"name":"Journal of the American Chemical Society","volume":"52 1","pages":""},"PeriodicalIF":15.0,"publicationDate":"2025-04-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143890215","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0