Angewandte Chemie International Edition最新文献_第7页

A FRET Autophagy Imaging Platform by Macrocyclic Amphiphile 大环双亲化合物的 FRET 自噬成像平台

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2024-12-13 DOI: 10.1002/anie.202420793

Ze-Tao Jiang, Jie Chen, Fang-Yuan Chen, Yuan-Qiu Cheng, Shun-Yu Yao, Rong Ma, Wen-Bo Li, Hongzhong Chen, Dong-Sheng Guo

{"title":"A FRET Autophagy Imaging Platform by Macrocyclic Amphiphile","authors":"Ze-Tao Jiang, Jie Chen, Fang-Yuan Chen, Yuan-Qiu Cheng, Shun-Yu Yao, Rong Ma, Wen-Bo Li, Hongzhong Chen, Dong-Sheng Guo","doi":"10.1002/anie.202420793","DOIUrl":"https://doi.org/10.1002/anie.202420793","url":null,"abstract":"Autophagy is a ubiquitous process of organelle interaction in eukaryotic cells, in which various organelles or proteins are recycled and operated through the autophagy pathway to ensure nutrient and energy homeostasis. Although numerous fluorescent probes have been developed to image autophagy, these environment‐responsive probes suffer from inherent deficiencies such as inaccuracy and limited versatility. Here, we present a modular macrocyclic amphiphile Förster Resonance Energy Transfer (FRET) platform (SC6A12C/NCM, SN), constructed through the amphiphilic assembly of sulfonatocalix[6]arene (SC6A12C) with N‐cetylmorpholine (NCM) for lysosome targeting. The hydrophobic fluorophore BPEA (FRET donor) was entrapped within the inner hydrophobic phase and showed strong fluorescence emission. Attributed to the broad‐spectrum encapsulation of SC6A12C, three commercially available organelle probes (Mito‐Tracker Red, ER Tracker Red, and RhoNox‐1) were selected as SC6A12C guests (FRET acceptors). During autophagy process, the formation of intracellular host‐guest complexes leads to strong FRET signal, allowing us to visualize the fusion of mitochondria, endoplasmic reticulum, and Golgi apparatus with lysosomes, respectively. This study provides a versatile and accessible platform for imaging organelle autophagy.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"22 1","pages":""},"PeriodicalIF":16.6,"publicationDate":"2024-12-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142815790","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

Rapidly Generated, Ultra‐Stable, and Switchable Photoinduced Radicals: A Solid‐State Photochromic Paradigm for Reusable Paper Light‐Writing 快速生成、超稳定、可切换的光诱导自由基：可重复使用的纸质光书写的固态光致变色范例

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2024-12-13 DOI: 10.1002/anie.202422856

Xiaoyan Xu, Ihor Sahalianov, Hao Sun, Zhongyu Li, Shengliang Wu, Boru Jiang, Hans Ågren, Glib V. Baryshnikov, Man Zhang, Liangliang Zhu

{"title":"Rapidly Generated, Ultra‐Stable, and Switchable Photoinduced Radicals: A Solid‐State Photochromic Paradigm for Reusable Paper Light‐Writing","authors":"Xiaoyan Xu, Ihor Sahalianov, Hao Sun, Zhongyu Li, Shengliang Wu, Boru Jiang, Hans Ågren, Glib V. Baryshnikov, Man Zhang, Liangliang Zhu","doi":"10.1002/anie.202422856","DOIUrl":"https://doi.org/10.1002/anie.202422856","url":null,"abstract":"Although photochromic molecules have attracted widespread interest in various fields, solid‐state photochromism remains a formidable challenge, owing to the substantial conformational constraints that hinder traditional molecular photoisomerization processes. Benefiting from the significant color change upon radical generation, chemical systems enabling a photoinduced radical (PIR) behavior through photoinduced electron transfer (PET) could be ideal candidates for solid‐state photochromism within minimized need of conformational freedom. However, the transient nature of radicals causes a dilemma in this scheme. Herein, we present a general crystal engineering strategy for rapidly generated (7‐s irradiation to saturation) and ultra‐stable (lasting 12 weeks) PIRs in the solid state, based on the anti‐parallel alignment of para‐hydroxyphenyl groups of persulfurated arenes to form a strong non‐covalent network for efficient PET and radical stabilization. Using this strategy, a PIR platform was constructed, with a superior photochromic behavior remaining in different solid forms (even in the fully‐ground sample) due to their transcendent crystallization ability. On this basis, our compounds can be further processed into reusable papers for light‐writing, accompanied by water fumigation for modulating the reversible process. This work provides new insights into addressing solid‐state photochromism and can inspire a wide range of optical material design from the switchable radical perspective.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"93 1","pages":""},"PeriodicalIF":16.6,"publicationDate":"2024-12-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142815795","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

Operando Evolution of a Hybrid Metallic Alloy Interphase for Reversible Aqueous Zinc Batteries

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2024-12-13 DOI: 10.1002/anie.202416047

Mingqiang Liu, Kai Yang, Qiming Xie, Nantao Hu, Mingzheng Zhang, Ruwei Chen, Wei Zhang, Jichao Zhang, Feng Shao, Hongzhen He, Roby Soni, Xiaoxia Guo, Jinlong Yang, Guanjie He, Feng Pan, Lu Yao, Thomas S Miller

{"title":"Operando Evolution of a Hybrid Metallic Alloy Interphase for Reversible Aqueous Zinc Batteries","authors":"Mingqiang Liu, Kai Yang, Qiming Xie, Nantao Hu, Mingzheng Zhang, Ruwei Chen, Wei Zhang, Jichao Zhang, Feng Shao, Hongzhen He, Roby Soni, Xiaoxia Guo, Jinlong Yang, Guanjie He, Feng Pan, Lu Yao, Thomas S Miller","doi":"10.1002/anie.202416047","DOIUrl":"https://doi.org/10.1002/anie.202416047","url":null,"abstract":"Aqueous Zn-ion batteries (AZIBs) are widely acknowledged as viable future energy storage solutions, particularly for low-cost stationary applications. However, the interfacial instability of zinc anodes represents a major challenge to the commercial potential of Zn-ion systems, promoting an array of side reactions including spontaneous corrosion, hydrogen evolution, and dendrite growth that destabilize cell performance, lower Coulombic efficiency (CE) and ultimately lead to early cell failure. While other commercially relevant battery systems benefit from a spontaneously forming solid electrolyte interphase (SEI), no such layer forms in AZIBs. Herein, we have designed and engineered an operando evolved metallic alloy interphase for AZIBs. This interfacial layer is initially deposited in the form of a thin film of Ag and In, but develops in situ to become an intimate mix of an AgxZny alloy and metallic indium. Importantly, this dual-heterometallic layer acts to synergistically regulate the migration of zinc ions through the alloy interphase and enables the dense, planar deposition Zn, simultaneously overcoming all major drivers of Zn anode degradation. Symmetric and full cells containing this modified metallic zinc anode exhibit stable electrochemical performance, offering high-capacity retention. Hence, this scalable approach represents a viable route towards the commercial utilization of this energy storage system.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"22 1","pages":""},"PeriodicalIF":16.6,"publicationDate":"2024-12-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142816440","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

Highly Oriented and Ordered Co‐Assembly Monolayers for Inverted Perovskite Solar Cells

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2024-12-13 DOI: 10.1002/anie.202418883

Yilin Chang, Le Liu, Lu Qi, Jiajia Du, Qinglin Du, Zhibin Yu, Zhiwei Ma, Tonggang Jiu, Yuliang Li

引用次数: 0

Synthesis of Arenesulfenyl Fluorides and Fluorosulfenylation of Alkenes, Alkynes, and α-Diazocarbonyl Compounds

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2024-12-13 DOI: 10.1002/anie.202422120

Nathan Faialaga, Dana Gephart, Breno Silva, Richard Y. Liu

{"title":"Synthesis of Arenesulfenyl Fluorides and Fluorosulfenylation of Alkenes, Alkynes, and α-Diazocarbonyl Compounds","authors":"Nathan Faialaga, Dana Gephart, Breno Silva, Richard Y. Liu","doi":"10.1002/anie.202422120","DOIUrl":"https://doi.org/10.1002/anie.202422120","url":null,"abstract":"Sulfenyl fluorides are organic compounds of sulfur in formal oxidation state +2 with the formula R–S–F. Although the chloride, bromide, and iodide analogues have been extensively described in the literature, arenesulfenyl fluorides remain essentially unstudied. These structures have been implicated as putative intermediates in established processes to access polyfluorinated sulfur species; however, definitive and direct evidence of their existence has not been obtained, nor has a systematic understanding of their reactivity. Here, we report the synthesis, isolation, and spectroscopic characterization of several arenesulfenyl fluorides, including structural analysis of 2,4-dinitrobenzenesulfenyl fluoride and 4-cyano-2-nitrobenzenesulfenyl fluoride by single-crystal X-ray diffraction. The functional group undergoes direct, efficient, and highly regioselective anti-addition to alkenes and alkynes, as well as insertion by carbenes. The resulting α- or β-fluoro thioether adducts can be readily transformed into useful fluorinated motifs, for example by modification of the sulfur groups (to sulfonamides or sulfonyl fluorides), by sulfur elimination (to generate formal C–H fluorination products), or by Julia–Kocienski olefination (to form vinyl fluorides). Thus, we establish that sulfenyl fluorides are unexpectedly accessible and stable compounds, which serve as versatile reagents for the production of fluorinated organic compounds.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"14 1","pages":""},"PeriodicalIF":16.6,"publicationDate":"2024-12-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142820980","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

Energy Transfer (EnT) Catalysis of non-Symmetrical Borylated Dienes: Origin of Reaction Selectivity in Competing EnT Processes

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2024-12-13 DOI: 10.1002/anie.202418651

Hao Fang, Alejandro García Eguizábal, Yu Jen Hsueh, Constantin G Daniliuc, Ignacio Funes Ardoiz, John Molloy

{"title":"Energy Transfer (EnT) Catalysis of non-Symmetrical Borylated Dienes: Origin of Reaction Selectivity in Competing EnT Processes","authors":"Hao Fang, Alejandro García Eguizábal, Yu Jen Hsueh, Constantin G Daniliuc, Ignacio Funes Ardoiz, John Molloy","doi":"10.1002/anie.202418651","DOIUrl":"https://doi.org/10.1002/anie.202418651","url":null,"abstract":"Energy transfer catalysis (EnT) has had a profound impact on contemporary organic synthesis enabling the construction of higher in energy, complex molecules, via efficient access to the triplet excited state. Despite this, intermolecular reactivity, and the unique possibility to access several reaction pathways via a central triplet diradical has rendered control over reaction outcomes, an intractable challenge. Extended chromophores such as non-symmetrical dienes have the potential to undergo [2+2] cycloaddition, [4+2] cycloaddition or geometric isomerisation, which, in combination with other mechanistic considerations (site- and regioselectivity), results in chemical reactions that are challenging to regulate. Herein, we utilise boron as a tool to probe reactivity of non-symmetrical dienes under EnT catalysis, paying particular attention to the impact of boron hybridisation effects on the target reactivity. Through this, a highly site- and regioselective [2+2] cycloaddition was realised with the employed boron motif effecting reaction efficiency. Subtle modifications to the core scaffold enabled a [4+2] cycloaddition, while a counterintuitive regiodivergence was observed in geometric isomerisation versus [2+2] cycloaddition. The observed reactivity was validated via a mechanistic investigation, determining the origin of regiodivergence and reaction selectivity in competing EnT processes.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"73 1","pages":""},"PeriodicalIF":16.6,"publicationDate":"2024-12-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142816438","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

Anomalous Role of Carbon in Pd-Catalyzed Selective Hydrogenation

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2024-12-13 DOI: 10.1002/anie.202421351

Peng Zhai, Divakar R. Aireddy, Mark B. Berko, Ahmad Arshadi, Michael J. Zachman, David A. Cullen, Ye Xu, Kunlun Ding

{"title":"Anomalous Role of Carbon in Pd-Catalyzed Selective Hydrogenation","authors":"Peng Zhai, Divakar R. Aireddy, Mark B. Berko, Ahmad Arshadi, Michael J. Zachman, David A. Cullen, Ye Xu, Kunlun Ding","doi":"10.1002/anie.202421351","DOIUrl":"https://doi.org/10.1002/anie.202421351","url":null,"abstract":"Carbonaceous species, including subsurface carbidic carbon and surface carbon, play crucial roles in heterogeneous catalysis. Many reports suggested the importance of subsurface carbon in the selective hydrogenation of alkynes over Pd-based catalysts. However, the role of surface carbon has been largely overlooked. We demonstrate that subsurface carbon in Pd is not responsible for the selectivity in acetylene hydrogenation. In contrast, the structure of surface carbonaceous species plays a decisive role in hydrogenation selectivity. Electron microscopy and spectroscopy evidence, along with theoretical modelling, reveal that partial graphitization of surface carbonaceous species results in unique spatial confinement of surface reaction intermediates, thus altering the reaction energy landscape in favour of ethylene desorption as opposed to over-hydrogenation. This mechanism for selectivity control is analogous to enzyme catalysis, where the active centers selectively attract reactants and release products. Similar mechanism might be present in CO/CO2 hydrogenation and alkane dehydrogenation reactions.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"10 1","pages":""},"PeriodicalIF":16.6,"publicationDate":"2024-12-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142816446","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

Interface Engineering of MOF Nanosheets for Accelerated Redox Kinetics in Lithium‐Sulfur Batteries

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2024-12-13 DOI: 10.1002/anie.202421726

Zhibin Cheng, Yiyang Chen, Jie Lian, Xingli Chen, Shengchang Xiang, Banglin Chen, Zhangjing Zhang

{"title":"Interface Engineering of MOF Nanosheets for Accelerated Redox Kinetics in Lithium‐Sulfur Batteries","authors":"Zhibin Cheng, Yiyang Chen, Jie Lian, Xingli Chen, Shengchang Xiang, Banglin Chen, Zhangjing Zhang","doi":"10.1002/anie.202421726","DOIUrl":"https://doi.org/10.1002/anie.202421726","url":null,"abstract":"Modifying the separator is considered as an effective strategy for achieving High performance lithium‐sulfur (Li‐S) batteries. However, most modification layers are excessively thick, with catalytic active sites primarily located within the material's interior. This configuration severely impacts Li+ transport and the efficient catalytic conversion of polysulfides. Therefore, there is an urgent need to develop a multifunctional separator that integrates ultrathin design, catalytic activity, and ion sieving capabilities. Herein, we successfully linked TCPP(Ni) as a secondary ligand with Zr‐BTB nanosheets to create an ultra‐thin separator modification layer (Zr‐TCPP(Ni)) with efficient ion sieving and catalytic properties. The resultant multifunctional separators provide robust ion sieving capabilities that promote rapid Li+ transport and intercept polysulfides shuttling. Therefore, The Zr‐TCPP(Ni)@PP cell maintains 79.45% of its initial capacity after 400 cycles at a high rate of 3 C, while achieving an impressive areal capacity of 4.55 mA h cm‐2 even with high sulfur content of 80 wt% at 0.5 C. This work provides valuable insights for rational design of MOF interface engineering in high energy density Li‐S batteries.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"4 1","pages":""},"PeriodicalIF":16.6,"publicationDate":"2024-12-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142815789","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

A Scalable Pore-Space-Partitioned Metal-Organic Framework Powered by Polycatenation Strategy for Efficient Acetylene Purification

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2024-12-13 DOI: 10.1002/anie.202421992

Zhen-Hua Guo, Xue-Qian Wu, Ya-Pan Wu, Dong-Sheng Li, Guoping Yang, Yao-Yu Wang

{"title":"A Scalable Pore-Space-Partitioned Metal-Organic Framework Powered by Polycatenation Strategy for Efficient Acetylene Purification","authors":"Zhen-Hua Guo, Xue-Qian Wu, Ya-Pan Wu, Dong-Sheng Li, Guoping Yang, Yao-Yu Wang","doi":"10.1002/anie.202421992","DOIUrl":"https://doi.org/10.1002/anie.202421992","url":null,"abstract":"Efficient separation of acetylene (C2H2) from carbon dioxide (CO2) and ethylene (C2H4) is a significant challenge in the petrochemical industry due to their similar physicochemical properties. Pore space partition (PSP) has shown promise in enhancing gas adsorption capacity and selectivity by reducing pore size and increasing the density of guest binding sites. Herein, we firstly employ the 2D→3D polycatenation strategy to construct a PSP metal-organic framework (MOF) Ni-dcpp-bpy, incorporating functional N/O sites to enhance C2H2 purification. The polycatenated framework with optimized pore size and regularity, exhibiting significant improvements over traditional PSP MOFs by resolving the critical contradiction of balancing C2H2 uptake (98.5 cm3 g-1 at 298 K, 100 kPa) and selectivity of C2H2/CO2 (3.4), C2H2/C2H4 (5.9), and C2H2/CH4 (96.4) in a MOF. Breakthrough experiments confirm high-purity C2H4 (> 99.9%) and high C2H2 productivity from binary and ternary mixtures. Notably, Ni-dcpp-bpy exhibits excellent water stability, scalability, and regenerability after 20 cycles for separating C2H2/CO2. Theoretical calculations verify that the strong binding of C2H2 is mainly attributed to the C−H···O/N interactions between host Ni-dcpp-bpy and guest C2H2 molecules. The polycatenation strategy not only improved industrial C2H2 purification efficiency but also enriched the design diversity of customized MOFs for other gas separation applications.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"30 1","pages":""},"PeriodicalIF":16.6,"publicationDate":"2024-12-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142816445","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

Modulating the Coverage of Adsorbed Hydrogen via Hydrogen Spillover Enables Selective Electrocatalytic Hydrogenation of Phenol to Cyclohexanone

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2024-12-13 DOI: 10.1002/anie.202419178

Yuanbo Liu, Kaiyue Ji, Xi Wang, Qiujin Shi, An-Zhen Li, Zhuoqun Yin, Yu-Quan Zhu, Haohong Duan

{"title":"Modulating the Coverage of Adsorbed Hydrogen via Hydrogen Spillover Enables Selective Electrocatalytic Hydrogenation of Phenol to Cyclohexanone","authors":"Yuanbo Liu, Kaiyue Ji, Xi Wang, Qiujin Shi, An-Zhen Li, Zhuoqun Yin, Yu-Quan Zhu, Haohong Duan","doi":"10.1002/anie.202419178","DOIUrl":"https://doi.org/10.1002/anie.202419178","url":null,"abstract":"Selective electrocatalytic hydrogenation (ECH) of phenol is a sustainable route to produce cyclohexanone, an industrially important feedstock for polymer synthesis. However, attaining high selectivity and faradaic efficiency (FE) of cyclohexanone remain challenging, owning to over-hydrogenation of phenol to cyclohexanol and competition of hydrogen evolution reaction (HER). Herein, by employing hydrogen spillover effect, we modulate adsorbed hydrogen species (Hads) coverage on Pt surface via migration to TiO2 in an anatase TiO2-supported Pt catalyst. In ECH of phenol, a high selectivity (94%) and good FE (63%) of cyclohexanone are obtained, showing more advantageous performance compared with previous reports. Cyclic voltammetry (CV) tests and electrochemical Raman spectroscopy reveal that Hads migrated from Pt to TiO2. We propose that TiO2-induced hydrogen spillover contributes to low Hads coverage over Pt, which effectively hinders over-hydrogenation of cyclohexanone and HER. We establish a scaling relationship between the intensity of hydrogen spillover and cyclohexanone selectivity by varying the types of anatase TiO2, and show the universality of the strategy over other reducible metal oxides as the support (rutile TiO2, CeO2 and WO3). This work showcases an effective strategy for tuning hydrogenation selectivity in electro-catalysis, by taking advantage of thermo-catalytically well-documented hydrogen spillover effect.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"51 1","pages":""},"PeriodicalIF":16.6,"publicationDate":"2024-12-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142820977","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