Angewandte Chemie International Edition最新文献_第3页

Heterointerface Anchored Ir with Localized Strong Orbital Coupling for Durable Proton Exchange Membrane Water Electrolysis. 具有局部强轨道耦合的异质界面锚定Ir用于持久质子交换膜水电解。

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2025-07-25 DOI: 10.1002/anie.202509985

Jing Ni,Zhaoping Shi,Jingsen Bai,Mingrui Yu,Xiaohui Liu,Kai Li,Tao Gan,Jiong Li,Jianbing Zhu,Minhua Shao,Meiling Xiao,Changpeng Liu,Wei Xing

{"title":"Heterointerface Anchored Ir with Localized Strong Orbital Coupling for Durable Proton Exchange Membrane Water Electrolysis.","authors":"Jing Ni,Zhaoping Shi,Jingsen Bai,Mingrui Yu,Xiaohui Liu,Kai Li,Tao Gan,Jiong Li,Jianbing Zhu,Minhua Shao,Meiling Xiao,Changpeng Liu,Wei Xing","doi":"10.1002/anie.202509985","DOIUrl":"https://doi.org/10.1002/anie.202509985","url":null,"abstract":"The imperative to minimize iridium usage in proton exchange membrane water electrolysis (PEMWE) process presents a pivotal challenge for hydrogen economy deployment, while inherent destabilization of iridium (Ir) active sites under corrosive operational conditions, originating from insufficient Ir bonding strength, remains a fundamental barrier. Here, we resolve this dilemma through heterointerface-engineered stabilization, where the strategically constructed Nb-TiO2 rutile/anatase heterophase homojunction stabilizes Ir sites with enhanced orbital overlap and intensified charge transfer. This atomic-scale anchoring mechanism, validated by operando characterization and theoretical calculations, strengthens Ir─Osupport bonding and optimizes *OOH adsorption energetics, thereby enabling concurrent activity-stability improvements. The resultant Ir@IrOx/m-Nb-TiO2 anode achieves exceptional PEMWE performance with ultralow loading (0.27 mgIr cm-2), requiring a low electrolysis voltage of 1.72 V to reach industrial current densities of 2 A cm-2, coupled with unprecedented durability with <1.7% voltage decay over 3000 h. This interface design philosophy establishes a general paradigm for developing active and stable supported electrocatalysts for PEMWE and beyond.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"124 1","pages":"e202509985"},"PeriodicalIF":16.6,"publicationDate":"2025-07-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144701396","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

Chemically Cross-Linked Polybenzimidazole Membranes with Ion-Conductive Sub-Nanometer Channels for Zinc-Iron Flow Batteries. 具有离子导电亚纳米通道的化学交联聚苯并咪唑膜用于锌铁液流电池。

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2025-07-25 DOI: 10.1002/anie.202511744

Yuqin Huang,Chenyi Liao,Qilei Song,Zhizhang Yuan,Xianfeng Li

{"title":"Chemically Cross-Linked Polybenzimidazole Membranes with Ion-Conductive Sub-Nanometer Channels for Zinc-Iron Flow Batteries.","authors":"Yuqin Huang,Chenyi Liao,Qilei Song,Zhizhang Yuan,Xianfeng Li","doi":"10.1002/anie.202511744","DOIUrl":"https://doi.org/10.1002/anie.202511744","url":null,"abstract":"Ion-selective membranes with sub-nanometer micropores are essential in various separation processes and energy-related devices. However, the absence of molecular-level insights into ion transport behavior in sub-nanochannels challenges the accurate construction of fit-for-purpose membranes. Herein, we design cross-linked polybenzimidazole membranes with varying angstrom-scale pores and functional group densities by in situ crosslinking reaction during dual-coagulation bath-induced phase separation process. The modulation of pore architecture and pore chemistry enables precise control of ion transport under confined channels. Molecular dynamics simulations and experimental results reveal that ion dehydration and ion-pore wall interactions are the two dominant mechanisms governing fast and selective ion transport within charged sub-nanometer channels. Based on \"dehydration-diffusion\" mechanism, membranes with low steric hindrance and weak ion-pore wall interactions facilitate low-energy-barrier ion transport. We demonstrate their applications in alkalescent zinc-iron flow batteries, achieving a high peak power density of 607.8 mW cm-2 and energy efficiency exceeding 80% at a current density of 200 mA cm-2. Our study advances the understanding of ion transport in membranes with sub-nanometer pores and provides guidelines for designing next-generation ion-selective membranes by regulating channel size and channel chemistry.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"37 1","pages":"e202511744"},"PeriodicalIF":16.6,"publicationDate":"2025-07-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144701023","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

Enhancing Oxygen Transport in Proton Exchange Membrane Fuel Cell Through Nanoconfined Triple Phase Interface Engineering. 纳米限制三相界面工程增强质子交换膜燃料电池中氧的输运。

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2025-07-25 DOI: 10.1002/anie.202507604

Juejin Teng,Min Wang,Quanbin Dai,Yilin Wang,Enyang Sun,Mingbo Wu,Zhongtao Li

{"title":"Enhancing Oxygen Transport in Proton Exchange Membrane Fuel Cell Through Nanoconfined Triple Phase Interface Engineering.","authors":"Juejin Teng,Min Wang,Quanbin Dai,Yilin Wang,Enyang Sun,Mingbo Wu,Zhongtao Li","doi":"10.1002/anie.202507604","DOIUrl":"https://doi.org/10.1002/anie.202507604","url":null,"abstract":"In proton exchange membrane fuel cells (PEMFCs), ionomer aggregation on Pt/C catalysts leads to increased oxygen transport resistance of conventional catalyst layers. This behavior significantly influences oxygen transport in the microenvironment at the triple-phase interface of Pt/C catalysts. To address this challenge, triazine-based covalent organic frameworks (COFs) were incorporated into the cathode catalyst layer, so that their well-defined pore structure and proton eligible triazine sites interact with terminal sulfonate groups of the Nafion ionomer. This interaction regulates the triple-phase microenvironment, enhances Pt utilization, and establishes directed oxygen-enriched transport channels. Under low-platinum loading conditions (-0.05 mgPt cm-2) in a H2─O2 PEMFC, the COF-modified system achieved a peak power density of 1.55 W cm-2, 1.3 times of conventional PEMFCs, with a 38% reduction in local oxygen transport resistance. This work presents a new design principle for high-performance low-platinum PEMFCs, as a new approach to further advance their commercialization.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"20 1","pages":"e202507604"},"PeriodicalIF":16.6,"publicationDate":"2025-07-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144701369","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

Synergistic Light-Ultrasound-Driven Hydrogen Production by Hydrogen Iodide Decomposition Over Dual-Molecular Ferroelectric Heterostructure. 双分子铁电异质结构上的碘化氢分解协同光超声驱动制氢。

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2025-07-25 DOI: 10.1002/anie.202510596

Zi Ning Zhou,Qing Dian Chong,Ya Wen Yang,Zong Wei Hu,Wei Ren,Sheng Sen Zhang,Qiong Ye

{"title":"Synergistic Light-Ultrasound-Driven Hydrogen Production by Hydrogen Iodide Decomposition Over Dual-Molecular Ferroelectric Heterostructure.","authors":"Zi Ning Zhou,Qing Dian Chong,Ya Wen Yang,Zong Wei Hu,Wei Ren,Sheng Sen Zhang,Qiong Ye","doi":"10.1002/anie.202510596","DOIUrl":"https://doi.org/10.1002/anie.202510596","url":null,"abstract":"Emerging catalytic systems for hydrogen production via solar and mechanical energy conversion often face critical challenges, including band mismatch, interfacial charge recombination, and insufficient charge migration driving forces. To address core issues of low carrier separation efficiency and poor multi-field coupling in molecular ferroelectrics, this study proposes a molecular engineering strategy of dual molecular ferroelectric heterojunctions. We report a facile one-pot solution synthesis of a molecular ferroelectric heterojunction composed of 4,4-difluoropiperidinium lead iodide and 4,4-difluorocyclohexylamine lead iodide ((4,4-DFPD)2PbI4/(4,4-DFCHA)2PbI4), tailored for hydrogen iodide (HI) decomposition under simultaneous light -ultrasonic activation. Under dual-field excitation, the heterojunction achieves a remarkable hydrogen evolution rate of 5.26 mmol g-1 h-1, outperforming its individual constituents ((4,4-DFPD)2PbI4 and (4,4-DFCHA)2PbI4) by factors of 4.5 and 2.4, respectively. Kelvin probe force microscopy (KPFM) confirms efficient charge separation at the heterointerface, facilitated by energy-level alignment and polarization coupling. Both experimental and theoretical investigations attribute the enhanced performance to suppressed charge recombination and the synergistic action of ferroelectric and piezoelectric fields, jointly promoting directional charge migration. This work not only introduces a viable molecular ferroelectric strategy for designing high-efficiency piezo-photocatalytic systems but underscores the critical role of interfacial charge dynamics in catalytic optimization, offering theoretical insights and practical guidelines for next-generation solar-driven catalysts.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"1 1","pages":"e202510596"},"PeriodicalIF":16.6,"publicationDate":"2025-07-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144701393","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

C60 Fullerene as the Active Site for CO2 Electroreduction. C60富勒烯作为CO2电还原活性位的研究

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2025-07-25 DOI: 10.1002/anie.202511924

Si-Wei Ying,Yuhang Wang,Peng Du,Qiang Wang,Changming Yue,Di Zhang,Zuo-Chang Chen,Jian-Wei Zheng,Su-Yuan Xie,Hao Li

{"title":"C60 Fullerene as the Active Site for CO2 Electroreduction.","authors":"Si-Wei Ying,Yuhang Wang,Peng Du,Qiang Wang,Changming Yue,Di Zhang,Zuo-Chang Chen,Jian-Wei Zheng,Su-Yuan Xie,Hao Li","doi":"10.1002/anie.202511924","DOIUrl":"https://doi.org/10.1002/anie.202511924","url":null,"abstract":"Fullerene (C60) was considered as a catalyst promoter in various electrochemical reactions, yet its catalytic role in enhancing catalytic performance beyond electron transfer remains a puzzle to chemists. Traditional simulations imply C60's inertness in CO2 reduction reaction (CO2RR) due to weak interaction with COOH* intermediates. Here, according to a pH-field coupled microkinetic model at reversible hydrogen electrode (RHE) scale, we demonstrate that C60 acts as molecular active sites to facilitate the CO2RR toward CO through a strong binding to COOH* in the electrochemical conditions. This binding is mainly due to the unique structure of C60 that induces large dipole moment changes to stabilize COOH* intermediates across different pH conditions. By detailed comparison of experimental CO2RR observations and quantitative pH-dependent modeling, this work provides new insights on C60-based catalysts, highlighting the large dipole moment change upon adsorption at curved surfaces should not be dismissed when analyzing the pH-dependent binding strength and electrocatalytic activity.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"55 1","pages":"e202511924"},"PeriodicalIF":16.6,"publicationDate":"2025-07-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144701397","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

Accessing N-Unprotected Unnatural α-Amino Acid Esters by Half-Sandwich Chiral-at-Ruthenium Aldehyde Catalysis: Scope and Mechanistic Study. 半夹心手性钌醛催化制备n -未保护的非天然α-氨基酸酯：范围和机理研究。

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2025-07-25 DOI: 10.1002/anie.202510811

Gang Chen,Gabriel N Morais,Hui Liang,Jing Zhao,Chuanyong Wang,Shuming Chen,Jiajia Ma

引用次数: 0

Interfacial Diffusion-Reaction Coupling Strategy for CO2 Reduction on Copper Surface in Acidic Medium. 酸性介质中铜表面CO2还原的界面扩散-反应耦合策略。

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2025-07-25 DOI: 10.1002/anie.202513306

Xinyu Chai,Pengfei Shi,Jinyu Zhao,Senhe Huang,Kaiyue Jiang,Chenbao Lu,Liqing He,Jie Chen,Tianfu Wang,Xiaodong Zhuang

{"title":"Interfacial Diffusion-Reaction Coupling Strategy for CO2 Reduction on Copper Surface in Acidic Medium.","authors":"Xinyu Chai,Pengfei Shi,Jinyu Zhao,Senhe Huang,Kaiyue Jiang,Chenbao Lu,Liqing He,Jie Chen,Tianfu Wang,Xiaodong Zhuang","doi":"10.1002/anie.202513306","DOIUrl":"https://doi.org/10.1002/anie.202513306","url":null,"abstract":"CO2 electroreduction reaction in acid medium to produce multicarbon (C2+) products has gained attention as an alternative to the traditional processes in neutral or alkaline solutions which often suffer from low single-pass conversion efficiency due to (bi)carbonate accumulation at the cathode. However, the CO2 conversion efficiency in acid remains unsatisfactory. Herein, a strong-polarized layer-covered Cu catalyst is developed as electrode for CO2 reduction reaction (CO2RR) in acid. Such a strong dipole moment layer is a sp3-hybridized nitrogen (sp3-N)-enriched azulene-based polymer, which acts as Lewis base to boost the CO2-diffusion kinetics in inner Helmholtz plane. Such unique electrode delivers nearly 84% C2 Faradaic efficiency at 200 mA cm-2, and demonstrates long-term stability over 40 h, which is the record for CO2RR in acidic media. In situ experiments manifest the moderate azulene-polarized sp3-N-enriched micro-environment can increase the local CO2/H2O ratio at electric double-layer to further stabilize the key intermediate atop-bound *CO. Theoretical calculations reveal that the strong-polarized layer decreases the reaction energy barrier for C-C coupling. This study not only uncovers the units with strong dipole moment on tuning sp3-N-enriched micro-environment, but also provides an interfacial diffusion-reaction coupling strategy to enhance the selectivity of CO2RR by decorating polycrystalline Cu with strong-polarized polymers.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"75 1","pages":"e202513306"},"PeriodicalIF":16.6,"publicationDate":"2025-07-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144701110","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

Rational Design Strategies in DNA-Encoded Libraries for Drug Discovery. 用于药物发现的dna编码文库的理性设计策略。

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2025-07-25 DOI: 10.1002/anie.202511839

Xudong Wang,Linjie Li,Xuanjing Shen,Xiaojie Lu

{"title":"Rational Design Strategies in DNA-Encoded Libraries for Drug Discovery.","authors":"Xudong Wang,Linjie Li,Xuanjing Shen,Xiaojie Lu","doi":"10.1002/anie.202511839","DOIUrl":"https://doi.org/10.1002/anie.202511839","url":null,"abstract":"DNA-encoded libraries (DELs) have emerged as a powerful and cost-effective platform for high-throughput screening, enabling the rapid identification of small-molecule ligands against a wide range of biological targets. However, traditional DEL approaches often rely on empirical and broad-based library construction, which can lead to low hit rates, off-target interactions, and limited chemical diversity around pharmaceutically relevant motifs. Recent technological advances have sought to address these limitations, shifting DELs from a largely blind screening tool to a more rational and precision-oriented strategy. In this review, we systematically examine the evolution of DEL methodologies, with a particular focus on innovations in library design that enhance hit quality and screening efficiency. Specifically, we highlight the emergence of fragment-based DEL strategies for exploring chemical space with minimal structures, the incorporation of covalent warheads to enable irreversible binding to specific residues, and the development of focused DELs tailored to particular protein families or binding motifs. Together, these advances mark a shift from blind, empirical screening toward a more strategic and hypothesis-driven application of DEL technology.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"699 1","pages":"e202511839"},"PeriodicalIF":16.6,"publicationDate":"2025-07-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144701112","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

Synthesis of Thiophenes from Pyridines Using Elemental Sulfur. 单质硫催化吡啶合成噻吩。

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2025-07-25 DOI: 10.1002/anie.202512321

Zi Liu,Michael F Greaney

引用次数: 0

Glycoconjugated Metallohelices Eliminate Cancer Stem-Like Cells via Modulating G-Quadruplex Surrounding Transcriptional Start Site of Sox2 Gene. 糖缀合金属螺旋通过调节Sox2基因转录起始位点周围的g -四重体消除癌症干细胞样细胞。

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2025-07-25 DOI: 10.1002/anie.202503488

Hongshuang Qin,Jie Yang,Tingting Cui,Hualong Song,Miles Postings,Peter Scott,Chunyu Wang,Chuanqi Zhao,Jinsong Ren,Xiaogang Qu

{"title":"Glycoconjugated Metallohelices Eliminate Cancer Stem-Like Cells via Modulating G-Quadruplex Surrounding Transcriptional Start Site of Sox2 Gene.","authors":"Hongshuang Qin,Jie Yang,Tingting Cui,Hualong Song,Miles Postings,Peter Scott,Chunyu Wang,Chuanqi Zhao,Jinsong Ren,Xiaogang Qu","doi":"10.1002/anie.202503488","DOIUrl":"https://doi.org/10.1002/anie.202503488","url":null,"abstract":"As an important pluripotency transcription factor, Sox2 plays key roles in the stemness maintenance of cancer stem-like cells (CSCs). Here, we found that a highly conserved G-rich region surrounding transcriptional start sites (TSSs) of Sox2 gene can form G-quadruplex (Sox2G4) both in vitro and in cells. More intriguingly, the glycoconjugated triplex metallohelice [Fe2LΔ-f 3]4+ (Δ-f) can enantioselectively stabilize Sox2G4. Sox2G4 stabilization induced by [Fe2LΔ-f 3]4+ (Δ-f) rather than Λ-f results in inhibition of Sox2 expression both in mRNA and protein levels in breast CSCs and decreases the cell viability and stemness of breast CSCs. These results indicate that [Fe2LΔ-f 3]4+ (Δ-f) has the enantioselectivity even in living cells. In vivo studies further demonstrate that Δ-f can reduce tumor initiation of breast CSCs. To our knowledge, this is the first report that targeting G-quadruplexes of pluripotency genes can regulate the fates of CSCs. Our work provides a new way to target CSC gene and eradicate cancer stem cells.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"19 1","pages":"e202503488"},"PeriodicalIF":16.6,"publicationDate":"2025-07-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144701118","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