Angewandte Chemie International Edition最新文献_第5页

pH‐Driven Two‐Stage Conformational Switching Activates an Acid‐Responsive Chaperone pH驱动的两阶段构象转换激活酸响应伴侣蛋白

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2026-10-17 DOI: 10.1002/anie.7464206

Soojeong Ham, Yeon‐Ju Jung, Hyunhee Kim, Sun‐Shin Cha, Changhan Lee

{"title":"pH‐Driven Two‐Stage Conformational Switching Activates an Acid‐Responsive Chaperone","authors":"Soojeong Ham, Yeon‐Ju Jung, Hyunhee Kim, Sun‐Shin Cha, Changhan Lee","doi":"10.1002/anie.7464206","DOIUrl":"https://doi.org/10.1002/anie.7464206","url":null,"abstract":"Acidification rapidly denatures bacterial periplasmic proteins, yet this compartment lacks ATP‐dependent chaperones. We identify AchC as an acid‐responsive, ATP‐independent chaperone crucial for acid tolerance in Pseudomonas aeruginosa . As proton influx across the outer membrane leaves insufficient time for transcriptional or translational adaptation, AchC is activated post‐translationally. We reveal that AchC is activated by precisely tuned, conformational transitions driven by pH changes. At neutral pH, AchC is maintained as an inactive dimer. Upon acidification, it undergoes two structural transitions: C‐terminal conformational loosening under mildly acidic conditions (pH 4.0–5.5), followed by complete monomerization under severe acid stress (pH ≤ 3.0) to fully activate its substrate‐holding function. Once activated, AchC exhibits potent anti‐aggregation activity across a broad spectrum of substrates. Upon neutralization, AchC releases its substrates in refolding‐competent state in ATP‐independent manner. In vivo, the deletion of achC increases acid susceptibility, whereas its overexpression confers acid tolerance. Furthermore, this chaperone is important for biofilm formation, motility, and pathogenicity. Our findings demonstrate how this dynamic molecular remodeling directly couples environmental sensing to bacterial survival.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"155 1","pages":""},"PeriodicalIF":16.6,"publicationDate":"2026-10-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149208499","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

Radical Sulfinamidation of Alkenes Enabled by a PCET–HAT Relay PCET-HAT继电器实现烯烃自由基亚胺化

IF 17.6 1区化学

Angewandte Chemie International Edition Pub Date : 2026-10-17 Epub Date: 2026-09-01 DOI: 10.1002/anie.2451961

Fen-Ya Xiong, Jichao Huang, Xin-Yi Zhang, Yu-Jie Li, Zhihan Zhang, Wen-Jing Xiao, Liang-Qiu Lu

{"title":"Radical Sulfinamidation of Alkenes Enabled by a PCET–HAT Relay","authors":"Fen-Ya Xiong, Jichao Huang, Xin-Yi Zhang, Yu-Jie Li, Zhihan Zhang, Wen-Jing Xiao, Liang-Qiu Lu","doi":"10.1002/anie.2451961","DOIUrl":"10.1002/anie.2451961","url":null,"abstract":"<div>\u0000 \u0000 Sulfinamides and related sulfur(VI) motifs are widely represented in bioactive molecules; however, their direct installation onto alkenes has traditionally relied on Lewis acid- or transition metal-mediated two-electron pathways, with more recent advances dominated by photoinduced single-electron processes. Here, we report a metal- and light-free radical sulfinamidation of alkenes that proceeds through a radical chain mechanism enabled by a proton-coupled electron transfer–hydrogen atom transfer (PCET–HAT) relay, initiated by trace amounts of oxygen. This transformation operates under operationally simple conditions, enabling rapid access to structurally diverse sulfinamides with broad substrate scope and excellent functional group tolerance. The synthetic utility of this strategy is demonstrated by the late-stage functionalization of complex natural products and drug molecules. Mechanistic investigations combining experimental studies and density functional theory calculations reveal a PCET-initiated radical chain process in which a HAT event relays reactivity to generate sulfinyl radicals, accounting for the high efficiency and selectivity of the reaction. This work establishes a mechanistically distinct platform for alkene sulfinamidation and highlights the potential of radical chain processes enabled by PCET–HAT relays in synthetic chemistry.\u0000 </div>","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"65 43","pages":""},"PeriodicalIF":17.6,"publicationDate":"2026-10-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148860977","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

Thermodynamic Control of MnO2/Mn2+ Redox Chemistry in Aqueous Batteries 水电池中MnO2/Mn2+氧化还原化学的热力学控制

IF 17.6 1区化学

Angewandte Chemie International Edition Pub Date : 2026-10-17 Epub Date: 2026-08-23 DOI: 10.1002/anie.5077478

Xiaodie Lin, Xiaoliu Wang, Wensheng Wang, Jiajie Shen, Renren Sun, Chenjun Zhang, Ziqi Sun, Mengru Wang, Zongxian Yang, Jishi Wei, Feng Huo, Xiao Liang

{"title":"Thermodynamic Control of MnO2/Mn2+ Redox Chemistry in Aqueous Batteries","authors":"Xiaodie Lin, Xiaoliu Wang, Wensheng Wang, Jiajie Shen, Renren Sun, Chenjun Zhang, Ziqi Sun, Mengru Wang, Zongxian Yang, Jishi Wei, Feng Huo, Xiao Liang","doi":"10.1002/anie.5077478","DOIUrl":"10.1002/anie.5077478","url":null,"abstract":"<div>\u0000 \u0000 The MnO2/Mn2+ redox chemistry is attractive for energy-dense aqueous batteries, offering high theoretical capacity and favorable redox potential. However, the practical reversibility of this chemistry is severely limited by competing reaction pathways, including Mn3+ disproportionation, “dead Mn” accumulation, and parasitic reactions. Rather than focusing primarily on material-performance advances in the appealing Zn-MnO2 batteries, this review develops a thermodynamic framework for understanding MnO2/Mn2+ conversion chemistry. It emphasizes the fundamental thermodynamic principles governing MnO2/Mn2+ reaction–pathway selection, interfacial evolution, and failure mechanisms. Within this framework, controlling factors and representative strategies—including local proton and Mn2+ activities, interfacial water structure, and oxide formation/dissolution energetics—are systematically discussed through equilibrium-state, quasi-equilibrium-state, and concatenated thermodynamic regulation perspectives. Future research directions toward operando activity mapping, mediator selectivity design, and full-cell thermodynamic compatibility are also outlined. These insights aim to shift MnO2/Mn2+-based aqueous batteries from empirical optimization toward thermodynamic design rules for stable, efficient, and high-energy redox chemistry.\u0000 </div>","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"65 43","pages":""},"PeriodicalIF":17.6,"publicationDate":"2026-10-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148806113","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

Yuwei Gu

IF 17.6 1区化学

Angewandte Chemie International Edition Pub Date : 2026-10-17 Epub Date: 2026-09-10 DOI: 10.1002/anie.3221634

Yuwei Gu

引用次数: 0

Outside Front Cover: Flexible, Biocompatible Supercapacitors Weaved From Layered Phyllosilicates and Zwitterions via Ionicity (Angew. Chem. Int. Ed. 43/2026) 外封面：柔性的、生物相容性的超级电容器，由层状硅酸盐和两性离子通过离子性编织而成。化学。Int。艾德。43/2026)

IF 17.6 1区化学

Angewandte Chemie International Edition Pub Date : 2026-10-17 Epub Date: 2026-09-28 DOI: 10.1002/anie.2026-m2509042700

Md Roxy Islam, Pritha Sarkar, Tanmay Sarkar Akash, Amanda Gabriela Bernard, Siddhartha Das, Josh Marsh, Neil Cunningham, Gernot Rother, Kausik Mukhopadhyay

引用次数: 0

Transformative Masked Ortho-Quinone Chemistry: From Direct Guaiacol Activation to Lignin-Based Adhesives 转化掩膜邻醌化学：从愈创木酚直接活化到木质素基胶粘剂

IF 17.6 1区化学

Angewandte Chemie International Edition Pub Date : 2026-10-17 Epub Date: 2026-09-01 DOI: 10.1002/anie.5604332

Dominik P. Hoch, Keven Walter, Oliver Sipura, Jana Falkenhagen, Xinyang Peng, Leon Gerndt, Hamy Nguyen, Hans G. Börner

{"title":"Transformative Masked Ortho-Quinone Chemistry: From Direct Guaiacol Activation to Lignin-Based Adhesives","authors":"Dominik P. Hoch, Keven Walter, Oliver Sipura, Jana Falkenhagen, Xinyang Peng, Leon Gerndt, Hamy Nguyen, Hans G. Börner","doi":"10.1002/anie.5604332","DOIUrl":"10.1002/anie.5604332","url":null,"abstract":"Guaiacol moieties (1-hydroxy-2-methoxy-benzenes) are among the most abundant structural motifs in renewable biophenolic feedstocks, representing a potential industrial-scale stream from softwood lignin through biorefinery valorization. Here, the transformative chemistry of masked ortho-quinones (MoQs) is introduced, yielding reactive guaiacol derivatives to enable thiol-guaiacol connectivity (TGC) polymers. Phenyliodine(III)diacetate (PIDA) oxidizes guaiacols to chemically pure MoQs within minutes at room temperature, generating activated triguaiacol monomers that undergo thiol-MoQ Michael-type polyaddition with multithiols. This bulk polymerization leads to TGC-adhesives, reaching professional performance lap-shear strengths up to 16.9 ± 0.9 MPa. The robust strategy is extended to directly activate technical lignin, generating curable multi-MoQ prepolymers which bond aluminum with lap-shear strengths of 9.1 ± 0.7 MPa, positioning MoQs as a sustainable platform chemistry to bridge from lignin to high-performance materials.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"65 43","pages":""},"PeriodicalIF":17.6,"publicationDate":"2026-10-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/anie.5604332","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148860936","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Defect‐Anchored Pt–Ov–Ti Charge Bridges Enable Iodine‐Mediated Selective Photocatalytic Gold Recovery From Electronic Waste 缺陷锚定Pt-Ov-Ti电荷桥使碘介导的选择性光催化从电子废物中回收金

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2026-10-17 DOI: 10.1002/anie.7432783

Zhiyong Zhao, Shuai Yue, Jiachen Zhang, Mengxue Yang, Yuanyuan Lv, Yanxiao Li, Weitao Liu, Pengfei Wang, Sihui Zhan

{"title":"Defect‐Anchored Pt–Ov–Ti Charge Bridges Enable Iodine‐Mediated Selective Photocatalytic Gold Recovery From Electronic Waste","authors":"Zhiyong Zhao, Shuai Yue, Jiachen Zhang, Mengxue Yang, Yuanyuan Lv, Yanxiao Li, Weitao Liu, Pengfei Wang, Sihui Zhan","doi":"10.1002/anie.7432783","DOIUrl":"https://doi.org/10.1002/anie.7432783","url":null,"abstract":"Gold is indispensable to modern technologies, yet its supply remains heavily dependent on environmentally intensive primary mining. Rapidly accumulating electronic waste (e‐waste) represents a valuable urban mine, but Au recovery is still constrained by corrosive lixiviants, co‐dissolution of competing metals, and high reagent demand. Herein, defect‐anchored Pt–Ov–Ti charge bridges are proposed to couple photogenerated‐carrier dynamics with iodine redox cycling, achieving 98.25% Au dissolution within 2 h while limiting the co‐dissolution of competing metals to below 0.62%. Multiple lines of evidence indicate that Pt–Ov–Ti sites promote interfacial charge transfer and carrier utilization, enabling hole‐driven I − oxidation and O 2 ‐assisted iodine redox cycling. In situ characterization and theoretical calculations further reveal that Pt–Ov–Ti induces local interfacial redistribution, introduces Pt 5d‐derived frontier states, and enhances iodine species adsorption and charge transfer, enabling reversible interfacial electronic‐state evolution during iodide activation. This pathway enabled the dissolution of 196.04 mg of Au from 1 kg of discarded central processing units (CPUs) with Au accounting for 99.2% of the leached metals, while retaining >95% activity after 10 cycles and supporting catalyst recycling and iodine reuse. This work highlights defect‐associated interfacial charge‐transfer engineering as a promising strategy for directing photogenerated carriers toward selective ligand‐mediated leaching and sustainable precious‐metal recovery.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"37 1","pages":""},"PeriodicalIF":16.6,"publicationDate":"2026-10-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149198992","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

Bromide–Borate Coupling Enables Selective Electrochemical Oxidation of Glycerol to Dihydroxyacetone 溴化物-硼酸盐偶联使甘油选择性电化学氧化为二羟基丙酮

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2026-10-17 DOI: 10.1002/anie.3736248

Santosh Bimli, Pallav Sharma, Dongho Lee

引用次数: 0

CRISPR RNA Engineering Enables Single Nucleotide Polymorphism Discrimination in Nucleic Acid Detection CRISPR RNA工程使核酸检测中的单核苷酸多态性判别成为可能。

IF 17.6 1区化学

Angewandte Chemie International Edition Pub Date : 2026-10-17 Epub Date: 2026-08-14 DOI: 10.1002/anie.202600004

Tianrui Sun, Aijiao Yuan, Wenjing Xie, Guibin Jiang, Hanyong Peng

{"title":"CRISPR RNA Engineering Enables Single Nucleotide Polymorphism Discrimination in Nucleic Acid Detection","authors":"Tianrui Sun, Aijiao Yuan, Wenjing Xie, Guibin Jiang, Hanyong Peng","doi":"10.1002/anie.202600004","DOIUrl":"10.1002/anie.202600004","url":null,"abstract":"<div>\u0000 \u0000 Clustered Regularly Interspaced Short Palindromic Repeats (CRISPR)-based diagnostic systems have emerged as powerful platforms for sensitive nucleic acid detection, yet their clinical reliability is frequently constrained by off-target activation and insufficient discrimination of closely related sequences. This review synthesizes current advances aimed at enhancing the specificity of CRISPR diagnostics, with particular emphasis on the pivotal role of CRISPR RNA (crRNA) engineering. We detail how structural determinants of crRNA, including spacer length optimization, intentional mismatch design, secondary-structure modulation, chemical modification, strand-displacement gating, and synergistic design frameworks, govern CRISPR-mediated target recognition and define the energetic and kinetic thresholds for accurate cleavage. Key engineering strategies encompassing computational prediction and modeling, high-throughput screening, and hybrid guide architectures are systematically examined for their capacity to elevate single-nucleotide discrimination, stabilize reaction performance, and enable robust multiplexed detection for pathogen profiling and mutation identification. Despite rapid progress, outstanding challenges persist, including interference from complex clinical matrices, lack of unified evaluation standards, and scalability barriers that hinder clinical translation. Addressing these limitations through integrated crRNA design, system-level optimization, and standardized benchmarking will be essential for realizing the promise of CRISPR diagnostics. Ultimately, these advances are poised to support ultrasensitive, highly specific, and portable point-of-care testing, thereby accelerating precision medicine and strengthening infectious disease surveillance and management.\u0000 </div>","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"65 43","pages":""},"PeriodicalIF":17.6,"publicationDate":"2026-10-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148764274","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

Supramolecular Self-Assembly Enables Controlled Lithium Replenishment Toward High-Performance and Sustainable Regeneration of Spent LiFePO4 Batteries 超分子自组装技术可实现锂的受控补充，从而实现高性能和可持续的废磷酸铁锂电池再生。

IF 17.6 1区化学

Angewandte Chemie International Edition Pub Date : 2026-10-17 Epub Date: 2026-08-14 DOI: 10.1002/anie.4146793

Yixin Lin, Tiansheng Wang, Chaochao Gao, Jie Xu, Jiawen Chen, Zixi Lin, Guanghao Mao, Weihao Gao, Yixuan Tang, Jiaheng Zhang

{"title":"Supramolecular Self-Assembly Enables Controlled Lithium Replenishment Toward High-Performance and Sustainable Regeneration of Spent LiFePO4 Batteries","authors":"Yixin Lin, Tiansheng Wang, Chaochao Gao, Jie Xu, Jiawen Chen, Zixi Lin, Guanghao Mao, Weihao Gao, Yixuan Tang, Jiaheng Zhang","doi":"10.1002/anie.4146793","DOIUrl":"10.1002/anie.4146793","url":null,"abstract":"<div>\u0000 \u0000 With the rapid expansion of lithium–ion battery deployment, spent LiFePO4 (LFP) regeneration is vital for closing material loops. However, in conventional solid-state regeneration, limited solid–solid contact and the premature formation of a dense conductive carbon layer hinder the effective coordination of lithium replenishment, structural defect repair, and interfacial reconstruction, thereby limiting lithium utilization efficiency and structural restoration. This paper presents a self-assembled supramolecular (SAS) regeneration system spontaneously formed from trithiocyanuric acid (TMT) and lithium acetate (CH3COOLi). Through Li–S coordination and hydrogen-bonding interactions, the precursor self-assembles into an ordered supramolecular architecture that regulates the thermal evolution of the solid-state regeneration process. Unlike the independent thermal decomposition of mechanically mixed precursors in conventional solid-state regeneration, the ordered supramolecular architecture regulates the reaction sequence, enabling lithium to preferentially enter the LiFePO4 lattice before the formation of a dense conductive carbon layer, thereby achieving efficient lithium replenishment and structural restoration. Subsequently, an in situ generated N/S co-doped conductive carbon layer elevates interfacial conductivity of regenerated LFP. The regenerated cathode delivers 160.3 mAh g−1 (0.1 C) and 143.0 mAh g−1 (1 C), maintaining 88% capacity over 500 cycles at 1 C, while the pouch cell exhibits 81% capacity retention after 500 cycles at 0.5 C.\u0000 </div>","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"65 43","pages":""},"PeriodicalIF":17.6,"publicationDate":"2026-10-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148766484","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