Angewandte Chemie International Edition最新文献_第8页

Inside Back Cover: Separation of MnWOx and NaWSiOx Phases Boosts Oxidative Coupling of Methane 后盖内：MnWOx和NaWSiOx相的分离促进了甲烷的氧化偶联

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2025-06-26 DOI: 10.1002/anie.202513324

Yu Xie, Jiawei Cheng, Wangyang Wang, Yaoyao Han, Qiyuan Fan, Hui Li, Kang Cheng, Qinghong Zhang, Ye Wang

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A Bifunctional Organic Photocatalyst for Efficient Single-Electron and Energy Transfer Activation. 高效单电子和能量转移激活的双功能有机光催化剂。

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2025-06-26 DOI: 10.1002/anie.202509770

Sumitava Mallik,Hailong Wang,Nunzio Matera,Bi-Xiao Li,Stefano Stagni,Paolo Melchiorre

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MXene‐supported Ru–Ni: a Common Active Site for Hydrolysis, Hydrogen Oxidation, and Hydrogenation MXene负载的Ru-Ni：水解，氢氧化和氢化的常见活性位点

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2025-06-26 DOI: 10.1002/anie.202506869

Shuyan Guan, Yanyan Liu, Shuling Liu, Zechao Zhuang, Ruofan Shen, Huanhuan Zhang, Erjun Liang, Yanping Fan, Jianchun Jiang, Baozhong Liu, Yongfeng Wang, Dingsheng Wang, Baojun Li

{"title":"MXene‐supported Ru–Ni: a Common Active Site for Hydrolysis, Hydrogen Oxidation, and Hydrogenation","authors":"Shuyan Guan, Yanyan Liu, Shuling Liu, Zechao Zhuang, Ruofan Shen, Huanhuan Zhang, Erjun Liang, Yanping Fan, Jianchun Jiang, Baozhong Liu, Yongfeng Wang, Dingsheng Wang, Baojun Li","doi":"10.1002/anie.202506869","DOIUrl":"https://doi.org/10.1002/anie.202506869","url":null,"abstract":"Insights into the activation and conversion of hydrogen using a single‐mode catalyst is crucial for advancing fuels and fine chemical production. In this paper, the activation and conversion of H2 molecular in hydrogen production and application were investigated on RuM (M = Ni, Co, Cu, Fe)‐MXene catalysts. RuM (M = Ni, Co, Cu, Fe) bimetallic nanoclusters were uniformly distributed on Ti3C2 MXene. The optimal Ru2.5Ni2.5‐Ti3C2 exhibites the highest turnover frequency (TOF) value of 1833 min‐1 toward ammonia borane (AB, NH3BH3) hydrolysis. Meanwhile, the catalysts also showed good catalytic activity in hydrogen oxidation reaction (HOR) and phenylacetylene hydrogenation. The high activity is originl from the acceleration of the catalytic process by RuNi clusters‐Ti3C2 and the promotion of molecular transport by the special interface of RuNi cluster‐MXene. The RuNi clusters‐Ti3C2 with suiable d‐band provide a dependable platform for the regulated activation and conversion of H2 molecules and various reaction intermediates. The competitiveness of nano‐cluster‐MXene catalytic material is showcased for activation and conversion of hydrogen. This research of reaction‐inducing adaptation uncovered the pathway to explore multi‐functional catalysts in energy, chemistry and materials applications.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"67 1","pages":"e202506869"},"PeriodicalIF":16.6,"publicationDate":"2025-06-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144488794","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‐Adapting Lattice Respiration Enabled by Crystal Design and d‐p Orbital Hybridization towards Highly Stable Rechargeable Aluminum Batteries 通过晶体设计和d - p轨道杂交实现的自适应晶格呼吸作用，可实现高度稳定的可充电铝电池

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2025-06-26 DOI: 10.1002/anie.202510773

Huaizhi Wang, Yu Li, Bo Long, Shuqiang Li, Xueying Lu, Shijie Zhou, Feng Wu, Ying Bai, Chuan Wu

{"title":"Self‐Adapting Lattice Respiration Enabled by Crystal Design and d‐p Orbital Hybridization towards Highly Stable Rechargeable Aluminum Batteries","authors":"Huaizhi Wang, Yu Li, Bo Long, Shuqiang Li, Xueying Lu, Shijie Zhou, Feng Wu, Ying Bai, Chuan Wu","doi":"10.1002/anie.202510773","DOIUrl":"https://doi.org/10.1002/anie.202510773","url":null,"abstract":"Rechargeable aluminum batteries (RABs) are promising for large‐scale energy storage due to the appealing three‐electron transfer feature, low cost and high safety. However, the strong electrostatic interaction between Al3+ and host lattice induces severe lattice distortion and structural collapse, leading to poor cycle stability in RABs. Herein, we develop a new‐type FeWO4 cathode with a comprehensive consideration of the crystal structure and electronic structure. The three‐dimensional (3D) open framework and strong W–O covalent network of the FeWO4 greatly improve the storage of high charge density Al3+. Moreover, the d‐p orbital hybridization between the transition metal and oxygen facilitates electron delocalization, which effectively weakens the interaction with the trivalent cation (Al3+). Importantly, combining in situ characterizations and theoretical calculations, it is demonstrated that as‐prepared cathode exhibits a “self‐adapting lattice respiration” (SALR) effect. Specifically, the reversible W–O bond elongation/compression (Δd≈0.05 Å) during cycling reduces lattice strain and confines volume expansion to less than 3%. As results, the FeWO4 cathode delivers a high capacity of 192 mAh g–1 at 500 mA g–1 and long cycle life of over 2300 cycles with quiet low capacity decay of 0.01% per cycle in RABs.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"34 1","pages":"e202510773"},"PeriodicalIF":16.6,"publicationDate":"2025-06-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144488795","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

Vacancy-Induced Atomic Diffusion in a Molecular Metal Cluster Complex. 分子金属团簇配合物中空位诱导的原子扩散。

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2025-06-26 DOI: 10.1002/anie.202507444

Tetsuro Murahashi,Kosuke Iwata,Koshi Miyazawa,Kenta Kurashima,Hiroshige Yamaura,Bo Zhu,Yu Tian,Yuta Takahira,Koji Yamamoto,Tsubasa Omoda,Daisuke Hashizume,Shigeyoshi Sakaki

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A Dual-Atom La2 Catalyst for the Oxygen Reduction Reaction. 氧还原反应的双原子La2催化剂。

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2025-06-25 DOI: 10.1002/anie.202509063

Jingru Sun,Tianmi Tang,Siying Zhang,Siyu Chen,Yingying Duan,Xue Bai,Xiaoqin Xu,Xiaodi Niu,Zhenlu Wang,Jingqi Guan

{"title":"A Dual-Atom La2 Catalyst for the Oxygen Reduction Reaction.","authors":"Jingru Sun,Tianmi Tang,Siying Zhang,Siyu Chen,Yingying Duan,Xue Bai,Xiaoqin Xu,Xiaodi Niu,Zhenlu Wang,Jingqi Guan","doi":"10.1002/anie.202509063","DOIUrl":"https://doi.org/10.1002/anie.202509063","url":null,"abstract":"Rare earth lanthanum element has large atomic radius, multi-shell orbital electrons, and Fenton-like reaction inertia, on which a localized high-coordination structure can be easily formed for the favorable adsorption of reaction intermediates. However, for single-atom lanthanum sites, due to the loss of all the outmost s and d electrons, the practically vacuous outmost orbitals are stable but sleepy for the oxygen reduction reaction (ORR). Here, we synthesize a novel dual-atom La catalyst onto N-doped graphene (La2-NG) by a Joule ultrafast heating method, which shows a half-wave potential of 0.893 V for the ORR. The La2-NG-assembled zinc-air battery demonstrates a great open circuit voltage of 1.52 V and a maximal power density of 192 mW cm-2. Operando X-ray absorption spectra reveal the change of valence states of La and the dynamic structural evolution of La2-N6 moiety embedded onto the graphene during the ORR, through which the adsorption/desorption of oxygen reduction intermediates can be reasonably regulated. Theoretical calculations further demonstrate that the La2-N6 structure can decrease the reaction energy barrier and promote charge transfer.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"16 1","pages":"e202509063"},"PeriodicalIF":16.6,"publicationDate":"2025-06-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144478657","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

Regioreversed Carbosulfenylation of Fluoroalkenes via Nickel-Mediated Radical Sorting. 通过镍介导的自由基分选，区域逆转氟烯烃的碳亚砜化。

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2025-06-25 DOI: 10.1002/anie.202509664

Chuan Zhu,Qian Liu,Nannan Wang,Rui Ma,Kai Chen,Patrick J Walsh,Kai Guo,Chao Feng

{"title":"Regioreversed Carbosulfenylation of Fluoroalkenes via Nickel-Mediated Radical Sorting.","authors":"Chuan Zhu,Qian Liu,Nannan Wang,Rui Ma,Kai Chen,Patrick J Walsh,Kai Guo,Chao Feng","doi":"10.1002/anie.202509664","DOIUrl":"https://doi.org/10.1002/anie.202509664","url":null,"abstract":"Carbosulfenylation of olefins represents an important class of reactions for the synthesis of structurally diverse organosulfur compounds. Previous studies typically yield 1,2-regioselectivity. In the context of diversity-oriented synthesis, accessing the regioreversed products is desirable, significantly broadening the scope of these reactions. In this study, we report a nickel-catalyzed 2,1-carbosulfenylation of trifluoromethyl- and gem-difluoroalkenes, using free thiols and benzyl bromides as sulfur and carbon sources, respectively. The unusual regioselectivity observed is enabled by a 'radical sorting' mechanism. The Ni catalyst activates benzyl bromide to generate a benzylic radical that undergoes HAT with the thiol to form a sulfur-centered radical. The sulfur radical subsequently adds to the fluoroalkenes, resulting in an α-fluoroalkyl C-radical. This radical undergoes SH2 with a Ni-CH2Ar to form a C(sp3)-C(sp3) bond and quaternary center, ultimately producing valuable fluoroalkyl thioethers. Isotopic labeling experiments corroborate a hydrogen atom transfer (HAT) event within the working mechanism.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"10 1","pages":"e202509664"},"PeriodicalIF":16.6,"publicationDate":"2025-06-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144478659","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

Length Ratio‐Driven Configurational Modulation of Heteroleptic Pd6L6L'6 Cages 长度比驱动的异色pd6l6l6笼的构型调制

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2025-06-25 DOI: 10.1002/anie.202508367

Ziteng Guo, Hao Yu, Ningxu Han, Xinrui Zhang, Junjuan Shi, Ming Wang

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Copper-Tailored Molybdenum-Nickel Catalyst Boosts Hydrogen Oxidation and Suppresses Parasitic Oxygen Reduction for Durable Fuel Cells. 铜定制钼镍催化剂促进氢氧化并抑制耐用燃料电池的寄生氧还原。

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2025-06-25 DOI: 10.1002/anie.202508535

Min-Rui Gao,Lei Zhu,Xiao-Long Zhang,Yu Yang,Ye-Cheng Li,Ye-Hua Wang,Hui-Kun Yan,Fei-Yue Gao,Yu-Cai Zhang,Zhi-Zheng Wu,Shu-Ping Sun,Pu-Gan Lu,Wanjie Song,Xiaolin Ge,Tongwen Xu,Kai-Bin Tang

{"title":"Copper-Tailored Molybdenum-Nickel Catalyst Boosts Hydrogen Oxidation and Suppresses Parasitic Oxygen Reduction for Durable Fuel Cells.","authors":"Min-Rui Gao,Lei Zhu,Xiao-Long Zhang,Yu Yang,Ye-Cheng Li,Ye-Hua Wang,Hui-Kun Yan,Fei-Yue Gao,Yu-Cai Zhang,Zhi-Zheng Wu,Shu-Ping Sun,Pu-Gan Lu,Wanjie Song,Xiaolin Ge,Tongwen Xu,Kai-Bin Tang","doi":"10.1002/anie.202508535","DOIUrl":"https://doi.org/10.1002/anie.202508535","url":null,"abstract":"Numerous existing strategies struggle to mitigate reverse-current decay (RCD) during startup and shutdown in polymer electrolyte fuel cells to avoid cathode corrosion, but the added system complexity and cost are drawbacks. Here we report that modification of a molybdenum-nickel alloy through the doping of copper enables a non-noble electrocatalyst (MoNi3.6Cu0.4) that efficiently catalyzes hydrogen oxidation reaction (HOR) while catalytically inactive toward oxygen reduction reaction (ORR) in alkaline media, making it ideal for fuel-cell anode because the instantaneous interfacial potential jump originated from the parasitic ORR during device startup/shutdown can be surmounted. The catalyst, when assembled in the anode of an anion exchange membrane fuel cell, manifests substantially improved corrosion-resistant ability compared with that of state-of-the-art carbon-supported platinum (Pt/C) catalyst. The basis for the achieved performances reveals to be the copper dopants that increase the hydrogen bonding of interfacial water for enhanced HOR, yet weaken molecular oxygen adsorption while stabilizing hydroxyl adsorption for ORR suppression.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"45 1","pages":"e202508535"},"PeriodicalIF":16.6,"publicationDate":"2025-06-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144478689","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

Engineered C‐N Lyases for Stereoselective Synthesis of Tertiary Amines 三维选择性合成叔胺的工程C - N裂解酶

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2025-06-25 DOI: 10.1002/anie.202507311

Laura Bothof, Xiaofang Gong, Marrit E. Onclin, Peter Fodran, Gerrit J. Poelarends

{"title":"Engineered C‐N Lyases for Stereoselective Synthesis of Tertiary Amines","authors":"Laura Bothof, Xiaofang Gong, Marrit E. Onclin, Peter Fodran, Gerrit J. Poelarends","doi":"10.1002/anie.202507311","DOIUrl":"https://doi.org/10.1002/anie.202507311","url":null,"abstract":"Optically pure N‐functionalized α‐amino acids are valuable chiral building blocks for pharmaceuticals, nutraceuticals, and agrochemicals. Ethylenediamine‐N,N‐disuccinic acid lyase from Chelativorans sp. BNC1 catalyzes the addition of a wide range of aliphatic and aromatic primary amines to fumarate, producing the corresponding enantioenriched N‐substituted L‐aspartic acids. In this work, the enzyme was subjected to iterative cycles of site‐saturation mutagenesis and screened for increased activity for the addition of 2‐((methylamino)methyl)aniline to fumarate. The final variant displayed an activity of 3 orders of magnitude higher compared to the wild‐type enzyme. Unexpectedly, the enzyme catalyzed the hydroamination of fumarate with the aliphatic secondary amine of the starting substrate, rather than with the aromatic primary amine, leading to the formation of a tertiary amine. Exploring the substrate scope showed that the enzyme accepts various substituted N‐methyl‐1‐phenylmethanamines for the hydroamination of fumarate, yielding N,N‐disubstituted L‐aspartic acids in high optical purity (up to >99% ee). Furthermore, we showed that the enzyme accepts several ortho‐substituted anilines that were previously not accepted by the wild‐type enzyme, yielding the corresponding N‐arylated L‐aspartic acids in high enantiomeric excess (>99% ee). This serendipitous finding enables a new strategy for the biocatalytic synthesis of tertiary amines, unlocked within the C‐N lyase toolbox.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"101 1","pages":"e202507311"},"PeriodicalIF":16.6,"publicationDate":"2025-06-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144479123","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