Angewandte Chemie International Edition最新文献_第2页

Stabilizing Lattice Oxygen to Enable Durable MnO2 Electrocatalyst for Simultaneous Acidic Hydrogen Production and Biomass Valorization

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2025-02-22 DOI: 10.1002/anie.202502847

Yingjie Song, Jialong Qian, Shengnan Li, Ziling Zhao, Hongwu Cheng, Kang Zou, Zishan Han, Zhenhua Li, Hao Li, Hua Zhou, Mingfei Shao

{"title":"Stabilizing Lattice Oxygen to Enable Durable MnO2 Electrocatalyst for Simultaneous Acidic Hydrogen Production and Biomass Valorization","authors":"Yingjie Song, Jialong Qian, Shengnan Li, Ziling Zhao, Hongwu Cheng, Kang Zou, Zishan Han, Zhenhua Li, Hao Li, Hua Zhou, Mingfei Shao","doi":"10.1002/anie.202502847","DOIUrl":"https://doi.org/10.1002/anie.202502847","url":null,"abstract":"Understanding and steering the stability of earth‐abundant electrocatalysts in acidic medium is essential for proton exchange membrane (PEM) water electrolyzer. Manganese oxide (MnO2) is one of the promising candidates for acidic oxygen evolution reaction (OER), but it still suffers from the overoxidation and the underlying mechanism remains elusive. Here, we observed that lattice oxygen was involved in the OER process on γ‐MnO2 via Mars‐van‐Krevelen mechanism. Combined with theoretical calculation, we revealed that the release of lattice oxygen lowers the energy barrier of Mn dissolution and compromises the electrode durability. Based on this finding, we propose a strategy to efficiently stabilize lattice oxygen and suppress Mn overoxidation by replacing OER with glucose oxidation to formic acid, which follows a Langmuir‐Hinshelwood mechanism. As a result, the durability of γ‐MnO2 was enhanced by 1100 times, enabling long stability up to 960 hours. Moreover, we demonstrated a production rate of 487.1 mmol h−1 for formic acid and 16.7 L h−1 for H2 at 40 A in a PEM electrolyzer, providing a sustainable and scalable route for converting water and biomass into valuable chemicals and fuels.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"65 1","pages":""},"PeriodicalIF":16.6,"publicationDate":"2025-02-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143470675","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

Sequence Similarity Network Guided Discovery of a Dehydrogenase for Asymmetric Carbonyl Dehydrogenation

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2025-02-22 DOI: 10.1002/anie.202501425

Yujing Hu, Jie Chen, Shaofang Qi, Hui Wang, Zhaoxuan Zhu, Yongzhen Peng, Wenjing Wang, Guixiang Huang, Zheng Fang, Yuxuan Ye, Zhiguo Wang, Kai Guo

{"title":"Sequence Similarity Network Guided Discovery of a Dehydrogenase for Asymmetric Carbonyl Dehydrogenation","authors":"Yujing Hu, Jie Chen, Shaofang Qi, Hui Wang, Zhaoxuan Zhu, Yongzhen Peng, Wenjing Wang, Guixiang Huang, Zheng Fang, Yuxuan Ye, Zhiguo Wang, Kai Guo","doi":"10.1002/anie.202501425","DOIUrl":"https://doi.org/10.1002/anie.202501425","url":null,"abstract":"Carbonyl dehydrogenation is one of the most valuable transformations in modern synthetic chemistry. Compared to traditional chemical synthesis methods, enzymatic dehydrogenation offers a greener and more selective alternative. However, except for a few rare natural dehydrogenases for desaturation, current enzymatic methods predominantly rely on enzyme’s promiscuity, which often suffer from lower efficiency and limited reaction controllability. Herein, we employed sequence similarity networks to mine natural dehydrogenases from a vast array of sequences with potential dehydrogenation activity. This approach led to the discovery of an uncharacterized FAD-dependent enzyme capable of efficiently performing the desymmetrizing desaturation of cyclohexanones, thereby generating diverse cyclohexenones bearing remote γ-quaternary stereocenters. The current method has enhanced the turnover frequency (TOF) by approximately 178-fold compared to the best existing biocatalytic strategies and displayed almost no overoxidation reactions. Through a combination of experimental assays and computational studies, we elucidated that this enzyme enhances its dehydrogenation capability via an unconventional proton relay system, absent in previously reported enzyme’s promiscuity systems. Additionally, this streamlined enzymatic process demonstrated scalability to gram-scale synthesis with maintained efficiency and selectivity, offering robust and sustainable alternatives for the synthesis of chiral cyclohexenones with high optical purity.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"14 1","pages":""},"PeriodicalIF":16.6,"publicationDate":"2025-02-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143471060","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

From Holodirected to Hemidirected Coordination Activated by Oxygenation Strategy: A Facile Route to Long Wave Infrared Birefringent Crystal

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2025-02-22 DOI: 10.1002/anie.202501481

Xin-Yang Li, Xiyue Cheng, Chun-Li Hu, Bing-Xuan Li, Zhengyang Zhou, Jian-Han Zhang, Shuiquan Deng, Jiang-Gao Mao, Fang Kong

{"title":"From Holodirected to Hemidirected Coordination Activated by Oxygenation Strategy: A Facile Route to Long Wave Infrared Birefringent Crystal","authors":"Xin-Yang Li, Xiyue Cheng, Chun-Li Hu, Bing-Xuan Li, Zhengyang Zhou, Jian-Han Zhang, Shuiquan Deng, Jiang-Gao Mao, Fang Kong","doi":"10.1002/anie.202501481","DOIUrl":"https://doi.org/10.1002/anie.202501481","url":null,"abstract":"Long wave infrared (LWIR) birefringent crystals are essential for infrared optical applications but such materials are rarely reported due to the requirements of large birefringence and wide infrared transmission range. This study proposes a facile route to create new LWIR birefringent crystal by oxygenation strategy in halides with cations containing lone pair electrons. Given the tendency of such cations to form holodirected geometry, a divalent oxygen was introduced to substitute the monovalent halogen to decrease the coordination number and activate the lone pair electrons. Our efforts in Rb+‐Sb3+‐Cl‐ system result three new structures, namely, Rb13Sb8Cl37, Rb3Sb2OCl7 and Rb2Sb2OCl6. The holodirected SbCl6 in Rb13Sb8Cl37 has been successfully translated to hemidirected SbOCl4 in Rb3Sb2OCl7 and Rb2Sb2OCl6, which are the first examples in alkali metal antimony(III) oxyhalides. The birefringence of Rb2Sb2OCl6 reached to 0.191@550 nm, which is 11.2 times that of Rb13Sb8Cl37 (0.017@550 nm). Large‐sized crystal of Rb2Sb2OCl6 have been successfully grown (6×6×2 mm3). It can exhibit good transmission performance in the range of 0.4‐13.5 μm, indicating its potential as a promising LWIR birefringent crystal. Our research not only opens up a new material system—alkali metal antimony(III) oxyhalides, but also provides a new strategy to create LWIR birefringent crystals.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"50 1","pages":""},"PeriodicalIF":16.6,"publicationDate":"2025-02-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143470713","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

Constructing Dense Morphology of Sn with High Reversibility under High Areal-capacity for Anode-Free Tin Batteries

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2025-02-22 DOI: 10.1002/anie.202425419

Fengyi Zhang, Xi Zhang, Yu Shu, Hongjie Xiao, Qiong Wang, Qiang Guo, Yonggang Wang, Jianhang Huang, Yongyao Xia

{"title":"Constructing Dense Morphology of Sn with High Reversibility under High Areal-capacity for Anode-Free Tin Batteries","authors":"Fengyi Zhang, Xi Zhang, Yu Shu, Hongjie Xiao, Qiong Wang, Qiang Guo, Yonggang Wang, Jianhang Huang, Yongyao Xia","doi":"10.1002/anie.202425419","DOIUrl":"https://doi.org/10.1002/anie.202425419","url":null,"abstract":"Sn electrode possesses high reversibility, redox kinetics and corrosion resistance, as well as non-toxic and environmental compatibility, which is competitive candidate for aqueous batteries. However, due to huge size of deposition particles and “dead Sn”, it is a great challenge to obtain high areal-capacity (> 5 mAh cm−2) and high coulombic efficiency (> 99%) simultaneously. Here, we demonstrate a highly reversible Sn redox electrochemistry with high areal-capacity enabled by thiourea additive. Systematical investigations reveal the participation of thiourea molecules in the electrical double layer, reducing exchange current density and suppressing rampant two-dimensional diffusion. As a result, flat and dense scale-like deposition Sn morphology is obtained, which enables high cycle stability with high areal-capacity of 10 mAh cm−2 for symmetrical cell with lean electrolyte (25 μL cm−2), and delivering a high average coulombic efficiency of 99.85% with practical high 5 mAh cm−2 area-capacity for asymmetrical cell. More importantly, anode-free Organic||Sn battery is developed, and 62% capacity retention can be obtained after 570 cycles.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"65 1","pages":""},"PeriodicalIF":16.6,"publicationDate":"2025-02-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143471056","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

Tandem Assembly and Etching Chemistry towards Mesoporous Conductive Metal-Organic Frameworks for Sodium Storage over 50,000 Cycles

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2025-02-21 DOI: 10.1002/anie.202500287

Jiahao Chen, Gaoyang Li, Fanxing Bu, Jiazhuang Tian, Lin Liu, Yifeng Wang, Jie Zhang, Xingjin Li, Xiang Li, Zhuo Yang, Dongliang Chao, Dongyuan Zhao

{"title":"Tandem Assembly and Etching Chemistry towards Mesoporous Conductive Metal-Organic Frameworks for Sodium Storage over 50,000 Cycles","authors":"Jiahao Chen, Gaoyang Li, Fanxing Bu, Jiazhuang Tian, Lin Liu, Yifeng Wang, Jie Zhang, Xingjin Li, Xiang Li, Zhuo Yang, Dongliang Chao, Dongyuan Zhao","doi":"10.1002/anie.202500287","DOIUrl":"https://doi.org/10.1002/anie.202500287","url":null,"abstract":"Despite two-dimensional (2D) conductive metal-organic frameworks (cMOFs) being attractive due to their intrinsic electrical conductivity and redox activity for energy applications, alleviating the constrained mass transfer within long-range micropore channels remains a significant challenge. Herein, we present a tandem assembly and etching chemistry, to incorporate perpendicularly aligned mesopores into the micropores of cMOF, via a bi-functional modulator. Synchrotron spectral and morphological analyses demonstrate that the elaborate ammonia modulator first coordinates with Zn2+ forming defects during the initial self-assembly of cMOF oligomers, which then initiates mesoporous cMOFs via in-situ etching. In-situ spectroscopy and theoretical simulations further reveal that such a unique perpendicular mesoporous structure shorts the micropore channels by two orders of magnitude and relaxes the inherent ion stacking within micropores, leading to five times faster Na+ transportation and a remarkable rate capability at 250 C and sodium storage lifespan over 50,000 cycles. Our protocol opens up a new avenue for introducing mesopores into microporous cMOFs for advanced energy applications and beyond.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"24 1","pages":""},"PeriodicalIF":16.6,"publicationDate":"2025-02-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143463073","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

Coordination Topology Design in Anion-Rich Solvated Electrolytes for High-Voltage Lithium Metal Batteries

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2025-02-21 DOI: 10.1002/anie.202423439

Ruowei Yi, Kui Xu, Wenlong Zhao, Zixu Ren, Qingyu Dong, Hui Shao, Yanbin Shen, Liwei Chen

{"title":"Coordination Topology Design in Anion-Rich Solvated Electrolytes for High-Voltage Lithium Metal Batteries","authors":"Ruowei Yi, Kui Xu, Wenlong Zhao, Zixu Ren, Qingyu Dong, Hui Shao, Yanbin Shen, Liwei Chen","doi":"10.1002/anie.202423439","DOIUrl":"https://doi.org/10.1002/anie.202423439","url":null,"abstract":"Electrolytes with anion-rich solvated structures are promising for high-voltage lithium metal batteries (LMBs) due to their good interfacial compatibility. Nevertheless, limited Li-ion transport of these electrolytes has hindered their high-rate application. Here we demonstrate that Li-ion transport in anion-rich solvated electrolytes could be facilitated by designing the coordination topology of anions in the solvation structure. Results show that, for a binary-anion electrolyte, equal-molar anions show the most expanded energy level distribution of solvation structures, thus reducing the Li-ion transport energy barrier, and resulting in a Li-ion conductivity even higher than that of the commercial carbonate electrolyte at a temperature range from -40 °C to 60 °C. More importantly, we identify a universal principle governing the Li-ion transport enhancement driven by anion configurations: only the combination of anions with multi-coordination sites shows facilitation in Li-ion transport, while the combination of centrosymmetric anions with the mono-coordination site harms it. The diversified anion-rich solvated structures also form stable interphases on the electrodes, enabling long-term cycling of 4.5 V LMBs at a high current density of 3.78 mA cm-2. Overall, our findings shine new light on developing practical electrolytes for energy-dense LMBs.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"29 1","pages":""},"PeriodicalIF":16.6,"publicationDate":"2025-02-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143463082","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

Promoting Li+-Solvents Desolvation by Engineering Nickel Single Atoms into Graphene Membrane toward Fast Sulfur Redox Kinetics

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2025-02-21 DOI: 10.1002/anie.202424390

Songjie He, Juan Yang, Zhibin Liu, Siyu Liu, Jiayi Yu, Jieshan Qiu

{"title":"Promoting Li+-Solvents Desolvation by Engineering Nickel Single Atoms into Graphene Membrane toward Fast Sulfur Redox Kinetics","authors":"Songjie He, Juan Yang, Zhibin Liu, Siyu Liu, Jiayi Yu, Jieshan Qiu","doi":"10.1002/anie.202424390","DOIUrl":"https://doi.org/10.1002/anie.202424390","url":null,"abstract":"Lithium-sulfur (Li-S) batteries featuring high energy density are expected to be next-generation energy storage devices, but are severely impeded by the suppressive Li+-solvents desolvation process at the electrode/electrolyte interface. Herein, a novel electrochemical in-situ doping coupled with self-assembly strategy is proposed to fabricate the graphene membrane anchored by Ni single atoms (Ni-SA-G), aimed at promoting the dissociation kinetics of Li+-solvents complex by combining electrocatalysis and nanochannel sieving effect. Theoretical simulation and in-situ Raman spectroscopy characterizations revealed that the Ni-O5 configuration within the Ni-SA-G membrane is capable of lowering the Li+-solvent dissociation energy barrier and promoting free Li+ migration, thereby delivering the fast sulfur redox kinetics. In addition, taking advantage of the Ni-SA-G membrane with a special transport channel, the large-sized solvent molecules and polysulfides were sieved and confined to a great degree. As a result, the Li-S batteries with the Ni-SA-G as cathode front-faces exhibit a high capacity of 1169 mAh g−1 with a good rate performance and outstanding long-term cycling stability, where a capacity decay of only 0.024% per cycle after 700 cycles can be achieved. Furthermore, the cell with a sulfur loading of 4.78 mg cm−2 delivers a high areal capacity of 4.0 mAh cm−2 at 0.2 C.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"3 1","pages":""},"PeriodicalIF":16.6,"publicationDate":"2025-02-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143471059","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

Planar Tetracoordinate Oxygen Atoms

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2025-02-21 DOI: 10.1002/anie.202500292

Gabriela Castillo-Toraya, Filiberto Ortíz-Chi, Jorge Barroso, Mesias Orozco-Ic, Luiz Leyva-Parra, Gabriel Merino

引用次数: 0

Dynamic Liquid Crystal Elastomers for Body Heat- and Sunlight-Driven Self-Sustaining Motion via Material-Structure Synergy

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2025-02-21 DOI: 10.1002/anie.202500527

Qing Liu, Zhi-Chao Jiang, Xue Jiang, Jing Zhao, Ying Zhang, Yue Liu, Jun-Bo Hou, Yao-Yu Xiao, Wei Pu, Yue Zhao

{"title":"Dynamic Liquid Crystal Elastomers for Body Heat- and Sunlight-Driven Self-Sustaining Motion via Material-Structure Synergy","authors":"Qing Liu, Zhi-Chao Jiang, Xue Jiang, Jing Zhao, Ying Zhang, Yue Liu, Jun-Bo Hou, Yao-Yu Xiao, Wei Pu, Yue Zhao","doi":"10.1002/anie.202500527","DOIUrl":"https://doi.org/10.1002/anie.202500527","url":null,"abstract":"Self-sustained actuators powered by natural, low-energy sources based on liquid crystal elastomers (LCEs) are attractive as they offer high safety, abundant energy availability, and practicality in applications. However, achieving stable self-sustaining motion with low-energy sources requires high actuation strain rates within a narrow temperature range near ambient conditions—a great challenge as LCEs with low nematic-to-isotropic transition temperatures (Tni) generally exhibit reduced actuation strain and strain rates. To address this, we synthesized a carbon nanotube-doped LCE with a low Tni and reversible Diels-Alder crosslinks, termed DALCE, and readily (re)fabricated it into specific structures (e.g., twisted-and-coiled or bimorph shapes). By leveraging material-structure synergy, we achieved both low Tni and high actuation strain rates, enabling self-rolling, self-breathing and autonomous twisting-untwisting movements powered by ambient/body temperature or natural sunlight. This low-energy, self-sustained actuator design opens new possibilities for LCE-based biomedical applications and naturally powered automatic devices.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"3 1","pages":""},"PeriodicalIF":16.6,"publicationDate":"2025-02-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143463076","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

Interfacial Asymmetrically Coordinated Zn-MOF for High-Efficiency Electrosynthetic Oxime.

IF 16.1 1区化学

Angewandte Chemie International Edition Pub Date : 2025-02-21 DOI: 10.1002/anie.202419550

Jiawei Kang, Peisen Liao, Runan Xiang, Wenpei Liao, Chenyu Yang, Shihan Wang, Qinghua Liu, Guangqin Li

{"title":"Interfacial Asymmetrically Coordinated Zn-MOF for High-Efficiency Electrosynthetic Oxime.","authors":"Jiawei Kang, Peisen Liao, Runan Xiang, Wenpei Liao, Chenyu Yang, Shihan Wang, Qinghua Liu, Guangqin Li","doi":"10.1002/anie.202419550","DOIUrl":"https://doi.org/10.1002/anie.202419550","url":null,"abstract":"Oximes are important intermediates for various chemicals synthesis such as pharmaceuticals, among which one vital precursor for producing neurological disease, antimicrobial and anticancer agents is piperidone oxime (PDO). Compared with conventional thermocatalytic method, it's more attractive to synthesize PDO via green electrocatalytic technology especially utilizing waste nitrogen oxides gas as nitrogen source. However, there are great challenges in catalyst design for high-efficiency electrosynthetic oxime due to the low electron transport rate and multiple competing reactions. Herein, we propose an interfacial coordination strategy based on metal-organic frameworks (MOF) electrocatalyst for the first time to promote oxime electrosynthesis, by building Zn-O bridges between graphite felt (GF) and zeolitic imidazolate framework (ZIF-7/CGF). Specially, ZIF-7/CGF delivers a Faraday efficiency (FE) of 75.9 % with yield up to 73.1 % for 1-methyl-4-piperidone oxime, which is far superior to the catalyst without Zn-O bridges (a FE of 10.7 % and yield of 10.3 %). In-depth mechanism study shows that the introducing Zn-O bridges can promote the electron transfer and induce Zn sites transforming into distorted tetrahedron (Zn-N3O) coordination mode, which benefits for intermediates adsorption and conversion. The developed strategy presents wide universalities towards various oximes electrosynthesis and adapts to other MOF materials (ZIF-8, ZIF-4). This work provides new insights for electrosynthetic organic chemicals and upgrading nitrogen cycle through rational design surficial coordinated electrocatalysts.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":" ","pages":"e202419550"},"PeriodicalIF":16.1,"publicationDate":"2025-02-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143466680","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