Angewandte Chemie International Edition最新文献_第2页

A General Hydrotrifluoromethylation of Unactivated Olefins Enabled by Voltage-Gated Electrosynthesis. 利用电压门控电合成技术实现未活化烯烃的一般氢化三氟甲基化。

IF 16.1 1区化学

Angewandte Chemie International Edition Pub Date : 2025-01-21 Epub Date: 2024-11-11 DOI: 10.1002/anie.202415218

Eva M Alvarez, Jinxiao Li, Christian A Malapit

{"title":"A General Hydrotrifluoromethylation of Unactivated Olefins Enabled by Voltage-Gated Electrosynthesis.","authors":"Eva M Alvarez, Jinxiao Li, Christian A Malapit","doi":"10.1002/anie.202415218","DOIUrl":"10.1002/anie.202415218","url":null,"abstract":"Here we present the first successful hydrotrifluoromethylation of unactivated olefins under electrochemical conditions. Commercially available trifluoromethyl thianthrenium salt (TT+-CF3BF4 -, Ep/2=-0.85 V vs Fc/Fc+) undergoes electrochemical reduction to generate CF3 radicals which add to olefins with exclusive chemoselectivity. The resulting carbon centered radical undergoes a second cathodic reduction, instead of a classical HAT process, to generate a carbanion that can be terminated by protonation from solvent. The use of MgBr2 (+0.20 V onset oxidation potential) plays a key role as an enabling sacrificial reductant for the reaction to operate in an undivided cell. Guided by cyclic voltammetry (CV) studies, fine-tuning the solvent system, trifluoromethylating reagent's counteranion and careful selection of redox processes, this work led to the development of a voltage-gated electrosynthesis by pairing two redox processes with a narrow potential difference (ΔE≈1.00 V) allowing the reaction to proceed with two important advances: (a) high reactivity and selectivity towards hydrotrifluoromethylation over undesired dibromination, and (b) an unprecedented functional group tolerance, including aniline, phenols, unprotected alcohol, epoxide, trialkyl amine, and several redox sensitive heterocycles.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":" ","pages":"e202415218"},"PeriodicalIF":16.1,"publicationDate":"2025-01-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142370335","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

Upconversion/Downshifting Circularly Polarized Luminescence over 1200 nm in a Single Nanoparticle for Optical Anticounterfeiting and Information Encryption. 用于光学防伪和信息加密的单个纳米粒子中 1200 纳米以上的上转换/下转换圆偏振发光。

IF 16.1 1区化学

Angewandte Chemie International Edition Pub Date : 2025-01-21 Epub Date: 2024-11-07 DOI: 10.1002/anie.202417223

Bowen Yang, Xuefeng Yang, Yonghong Shi, Xue Jin, Tiesheng Li, Minghua Liu, Pengfei Duan

{"title":"Upconversion/Downshifting Circularly Polarized Luminescence over 1200 nm in a Single Nanoparticle for Optical Anticounterfeiting and Information Encryption.","authors":"Bowen Yang, Xuefeng Yang, Yonghong Shi, Xue Jin, Tiesheng Li, Minghua Liu, Pengfei Duan","doi":"10.1002/anie.202417223","DOIUrl":"10.1002/anie.202417223","url":null,"abstract":"Multimodal upconversion and downshifting circularly polarized luminescent materials hold significant potential for optical anticounterfeiting applications due to their exceptional chiroptical properties. However, constructing these materials within a single emitter remains challenging. In this study, a conceptual model of multimodal upconversion/downshifting circularly polarized luminescence (CPL) is realized within a single nanoparticle. A new type of nanoparticles with multilayer core-shell architecture is fabricated, capable of delivering upconversion/downshifting luminescence, when excited by a 980 nm laser. Utilizing a co-assembly strategy, multimodal upconversion/downshifting CPL emission, covering a broad emission range from ultraviolet (UV) to the second near-infrared (NIR-II) region, can be realized at the supramolecular level. These chiroptical properties closely follow the chirality of host matrix and are strongly dependent on the distribution mode of nanoparticles within the matrix films. The multimodal upconversion/downshifting CPL behavior enabled cutting-edge encryption applications including optical anticounterfeiting and information encryption. This work introduces a novel approach to designing multimodal upconversion/downshifting CPL materials and opens new avenues for the development of chiroptical functional materials.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":" ","pages":"e202417223"},"PeriodicalIF":16.1,"publicationDate":"2025-01-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142379635","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

Perylene-Embedded Helical Nanographenes with Emission up to 1010 nm: Synthesis, Structures, and Chiroptical Properties. 发射波长达 1010 纳米的包埋过烯螺旋纳米石墨：合成、结构和光电特性。

IF 16.1 1区化学

Angewandte Chemie International Edition Pub Date : 2025-01-21 Epub Date: 2024-11-06 DOI: 10.1002/anie.202416707

Gui-Fei Huo, Wei-Tao Xu, Jinlian Hu, Yi Han, Wei Fan, Wei Wang, Zhe Sun, Hai-Bo Yang, Jishan Wu

{"title":"Perylene-Embedded Helical Nanographenes with Emission up to 1010 nm: Synthesis, Structures, and Chiroptical Properties.","authors":"Gui-Fei Huo, Wei-Tao Xu, Jinlian Hu, Yi Han, Wei Fan, Wei Wang, Zhe Sun, Hai-Bo Yang, Jishan Wu","doi":"10.1002/anie.202416707","DOIUrl":"10.1002/anie.202416707","url":null,"abstract":"Near-infrared (NIR) circularly polarized absorbing or emitting materials offer distinct advantages over their visible-light counterparts and have attracted considerable interest across various fields. Materials exhibiting NIR chiroptical properties with high fluorescence quantum yields (ΦF) are particularly rare. In this study, we report the synthesis of a series of helical nanographenes (1, 2, 3, and 4), where perylene is fused with one to four hexa-peri-hexabenzocoronene (sub) units by a strategy involving Diels-Alder cycloaddition followed by a Scholl reaction. X-ray crystallographic analysis confirmed their structures, revealing helicene moieties integrated into a highly contorted framework. Benefiting from a similar distribution pattern of frontier molecular orbitals to perylene and extended π-conjugation, compounds 1-4 demonstrate respectable ΦF values of 31.9 %, 15.0 %, 13.7 %, and 6.5 %, respectively, with emission maxima reaching up to 1010 nm. Their enantiopure forms, isolated by preparative chiral HPLC, exhibit distinct circular dichroism signals and circularly polarized luminescence across a broad spectral range, extending from the ultraviolet to the NIR.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":" ","pages":"e202416707"},"PeriodicalIF":16.1,"publicationDate":"2025-01-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142370298","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

Photoclick and Release for Spatiotemporally Localized Theranostics of Single Cells via In Situ Generation of 1,3-Diaryl-1H-benzo[f]indazole-4,9-dione. 通过原位生成 1,3-二芳基-1H-苯并[f]吲唑-4,9-二酮实现单细胞时空定位治疗的光点击和释放。

IF 16.1 1区化学

Angewandte Chemie International Edition Pub Date : 2025-01-21 Epub Date: 2024-11-19 DOI: 10.1002/anie.202416111

Bao-Lin Li, Sitong Li, Cefei Zhang, Yuqiao Zhou, Xiaohu Zhao, Zhipeng Yu

{"title":"Photoclick and Release for Spatiotemporally Localized Theranostics of Single Cells via In Situ Generation of 1,3-Diaryl-1H-benzo[f]indazole-4,9-dione.","authors":"Bao-Lin Li, Sitong Li, Cefei Zhang, Yuqiao Zhou, Xiaohu Zhao, Zhipeng Yu","doi":"10.1002/anie.202416111","DOIUrl":"10.1002/anie.202416111","url":null,"abstract":"Bioorthogonal click-release chemistry is a cutting-edge tool for exploring and manipulating biomolecule functions in native biological systems. However, it is challenging to achieve the precise regulation or therapy of individual cells via click-release strategies driven by proximity and thermodynamics. Herein, we propose a novel photoclick-release approach based on a photo-induced cycloaddition between 4,4'-bis(N-arylsydnone) or C-bithienyl-diarylsydnone and 2-arylamino-naphthoquinone via irradiation with 405 or 485 nm light. It constructs 1,3-diaryl-1H-benzo[f]indazole-4,9-dione (BIZON) as a pharmacophore while releases an arylamine for fluorescence turn-on probing. Both photoclick reagents were tailored by connecting to the triphenyl phosphonium delivery motif for enrichment in the mitochondria of live cells. This enables an intracellular photoclick and release under the control of 405 or 485 nm light. We then discovered that the in situ photo-generated BIZON is capable of photosensitizing upon 485 or 520 nm light to produce singlet oxygen inside the mitochondria under aerobic conditions. Therefore, we realized wash-free fluorescence tracking and subsequent anti-cancer efficacy at single-cell resolution using global illumination, which provides a foundation for wavelength-gated single-cell theranostics.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":" ","pages":"e202416111"},"PeriodicalIF":16.1,"publicationDate":"2025-01-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142566710","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

Localized Water Restriction in Ternary Eutectic Electrolytes for Ultra-Low Temperature Hydrogen Batteries. 用于超低温氢电池的三元共晶电解质中的局部水限制。

IF 16.1 1区化学

Angewandte Chemie International Edition Pub Date : 2025-01-21 Epub Date: 2024-11-18 DOI: 10.1002/anie.202416800

Ziyue Li, Yuxiao Lin, Jiafeng Ruan, Mochou Liao, Fengmei Wang, Ruohan Jiang, Xuelian Qu, Qin Li, Jinyu Yang, Xinjie Li, Zihao Zhang, Yunsong Li, Dalin Sun, Fang Fang, Fei Wang

{"title":"Localized Water Restriction in Ternary Eutectic Electrolytes for Ultra-Low Temperature Hydrogen Batteries.","authors":"Ziyue Li, Yuxiao Lin, Jiafeng Ruan, Mochou Liao, Fengmei Wang, Ruohan Jiang, Xuelian Qu, Qin Li, Jinyu Yang, Xinjie Li, Zihao Zhang, Yunsong Li, Dalin Sun, Fang Fang, Fei Wang","doi":"10.1002/anie.202416800","DOIUrl":"10.1002/anie.202416800","url":null,"abstract":"Proton batteries are promising candidates for next-generation large-scale energy storage in extreme conditions due to the small ionic radius and efficient transport of protons. Hydrogen gas, with its low working potentials, fast kinetics, and stability, further enhances the performance of proton batteries but necessitates the development of novel electrolytes with low freezing points and reduced corrosion. This work introduces a localized water restriction strategy by incorporating a tertiary component with a high donor number, which forms strong bonds with water molecules. This approach restricts free water molecules and reduces the average hydrogen bond ratio and strength. As-prepared ternary eutectic electrolytes lowered the freezing point to -103 °C, significantly lower than the traditional binary electrolyte (9.5 m H3PO4, -93 °C). This electrolyte is highly compatible with the Cu0.79Co0.21[Fe(CN)6]0.64 ⋅ 4H2O (CoCuHCF) cathode, reducing material dissolution and current collector corrosion. The H2||CoCuHCF battery using this electrolyte demonstrated a high-power density of 23664.3 W kg-1, excellent performance at -80 °C, and stable cyclability over 1000 cycles (>30 days) at -50 °C. These findings provide a framework for proton electrolytes, highlighting the potential of hydrogen batteries in challenging environments.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":" ","pages":"e202416800"},"PeriodicalIF":16.1,"publicationDate":"2025-01-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142574871","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

Boron Enabled Directed [2+2]- and Dearomative [4+2]-Cycloadditions Initiated by Energy Transfer. 由能量转移引发的硼驱动的定向 [2+2]- 和二元[4+2]-环加成反应。

IF 16.1 1区化学

Angewandte Chemie International Edition Pub Date : 2025-01-21 Epub Date: 2024-11-07 DOI: 10.1002/anie.202416215

Souvik Adak, Partha Sarathi Hazra, Carter B Fox, M Kevin Brown

引用次数: 0

Converting Fe–N–C single-atom catalyst to a new FeNxSey cluster catalyst for proton-exchange membrane fuel cells

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2025-01-21 DOI: 10.1002/anie.202419501

Yang Zhao, Pengfei Yin, Yuanyuan Yang, Ruguang Wang, Cairong Gong, Jisi Li, Jiaxin Guo, Quanlu Wang, Tao Ling

{"title":"Converting Fe–N–C single-atom catalyst to a new FeNxSey cluster catalyst for proton-exchange membrane fuel cells","authors":"Yang Zhao, Pengfei Yin, Yuanyuan Yang, Ruguang Wang, Cairong Gong, Jisi Li, Jiaxin Guo, Quanlu Wang, Tao Ling","doi":"10.1002/anie.202419501","DOIUrl":"https://doi.org/10.1002/anie.202419501","url":null,"abstract":"Fe–N–C catalyst is the most promising alternative to platinum catalyst for proton-exchange membrane fuel cells (PEMFCs), however its high performance cannot be maintained for a long enough time in device. The construction of a new Fe coordination environment that is different from the square-planar Fe–N 4 configuration in Fe–N–C catalyst is expected to break current stability limits, which however remains unexplored. Here, we report the conversion of Fe–N–C to a new FeNxSey catalyst, where the Fe sites are three-dimensionally (3D) co-coordinated by N and Se atoms. The FeNxSey catalyst exhibits much better 4e– ORR activity and selectivity than the Fe–N–C catalyst. Specifically, the yields of H2O2 and ·OH radicals on FeNxSey are only one-quarter and one-third of that on Fe–N–C, respectively. Therefore, the FeNxSey catalyst exhibits outstanding stability, losing only 10 mV in E1/2 after 10,000 cycles, much smaller than that of the Fe–N–C catalyst (56 mV), representing the most stable Pt-free catalysts ever reported. Moreover, the 3D co-coordination structure inhibits the Fe demetallization in the presence of H2O2. As a result, the FeNxSey based PEMFC shows excellent durability, with the current density attenuation significantly lower than that of the Fe–N–C based device after accelerated durability testing.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"57 1","pages":""},"PeriodicalIF":16.6,"publicationDate":"2025-01-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142991358","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

Structural Snapshots, Trajectory and Thermodynamics of the Reversible μ-1,2-Peroxo/μ-1,1-Hydroperoxo Dicopper(II) Interconversion. 可逆 µ-1,2-过氧化物/µ-1,1-氢过氧化物二铜（II）相互转化的结构快照、轨迹和热力学。

IF 16.1 1区化学

Angewandte Chemie International Edition Pub Date : 2025-01-21 Epub Date: 2024-11-28 DOI: 10.1002/anie.202416022

Can-Jerome Spyra, David Hiller, Kim A Eisenlohr, Sebastian Dechert, Serhiy Demeshko, Disha Bhattacharya, Jana Lücken, Max C Holthausen, Franc Meyer

{"title":"Structural Snapshots, Trajectory and Thermodynamics of the Reversible μ-1,2-Peroxo/μ-1,1-Hydroperoxo Dicopper(II) Interconversion.","authors":"Can-Jerome Spyra, David Hiller, Kim A Eisenlohr, Sebastian Dechert, Serhiy Demeshko, Disha Bhattacharya, Jana Lücken, Max C Holthausen, Franc Meyer","doi":"10.1002/anie.202416022","DOIUrl":"10.1002/anie.202416022","url":null,"abstract":"Hydrogen bonds involving the oxygen atoms of intermediates that result from copper-mediated O2 activation play a key role for controlling the reactivity of Cux/O2 active sites in metalloenzymes and synthetic model complexes. However, structural insight into H-bonding in such transient species as well as thermodynamic information about proton transfer to or from the O2-derived ligands is scarce. Here we present a detailed study of the reversible interconversion of a μ1,2-peroxodicopper(II) complex ([1]+) and its μ1,1-hydroperoxo congener ([2]+) via (de)protonation, including the isolation and structural characterization of several H-bond donor (HBD) adducts of [1]+ and the determination of binding constants. For one of these adducts a temperature-dependent μ1,2-peroxo/μ1,1-hydroperoxo equilibrium associated with reversible H+-translocation is observed, its thermodynamics investigated experimentally and computationally, and effects of H-bonding on spectroscopic parameters of the CuII 2(μ1,2-O2) species are revealed. DFT calculations allowed to fully map and correlate the trajectories of H+-transfer and μ1,2-peroxo→μ1,1-peroxo rearrangement. These findings enhance our understanding of two key intermediates in bioinspired Cu2/O2 chemistry.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":" ","pages":"e202416022"},"PeriodicalIF":16.1,"publicationDate":"2025-01-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142370354","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 Pore Wall Chemistry Empowers Sonodynamic Activity of Two-Dimensional Covalent Organic Framework Heterojunctions for Pro-Oxidative Nanotherapy. 调节孔壁化学性质增强二维共价有机框架异质结的声动力活性，促进氧化性纳米疗法。

IF 16.1 1区化学

Angewandte Chemie International Edition Pub Date : 2025-01-21 Epub Date: 2024-11-09 DOI: 10.1002/anie.202416461

Ruohui Wu, Mengying Hua, Yanjia Lu, Liang Chen, Yu Chen, Zhongqian Hu

{"title":"Modulating Pore Wall Chemistry Empowers Sonodynamic Activity of Two-Dimensional Covalent Organic Framework Heterojunctions for Pro-Oxidative Nanotherapy.","authors":"Ruohui Wu, Mengying Hua, Yanjia Lu, Liang Chen, Yu Chen, Zhongqian Hu","doi":"10.1002/anie.202416461","DOIUrl":"10.1002/anie.202416461","url":null,"abstract":"Covalent organic frameworks (COFs) have garnered growing interest in the field of biomedicine; however, their application in sonodynamic therapy remains underexplored due to limited understanding of their intrinsic activity and structure-property relationships. Here, we present a pore wall chemistry modulation strategy for empowering sonodynamic activity to two-dimensional (2D) COF heterojunctions through in situ growth of COFs on bismuth oxycarbonate nanosheets (B NSs). Compared to the negligible sonodynamic effects observed in the pristine B NSs, the 2D heterojunction with vinyl-decorated COF pore walls demonstrates a 3.6-fold enhancement in sonocatalytic singlet oxygen generation. This performance also significantly outperforms that of isoreticular COFs functionalized with methoxy or non-substituted groups. Mechanistic studies reveal that the vinyl groups in the B@COF (BC) heterojunction facilitate the separation and transfer of charge carriers while also enhancing the adsorption of oxygen molecules. Furthermore, peroxymonosulfate (PMS) loading into the porous COFs boosts the therapeutic efficacy of antitumor nanotherapy via sonocatalytic dual oxidative species generation. These findings underscore the critical role of pore wall chemistry in modulating the sonocatalytic properties of COFs, and advance the development of COF-based sonosensitizers for pro-oxidative applications.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":" ","pages":"e202416461"},"PeriodicalIF":16.1,"publicationDate":"2025-01-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142386573","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 Ag/Cu₂O Interface for Efficient Neutral CO₂ Electroreduction to C₂H₄. 构建 Ag/Cu2O 界面，实现高效中性 CO2 电还原为 C2H4。

IF 16.1 1区化学

Angewandte Chemie International Edition Pub Date : 2025-01-21 Epub Date: 2024-11-14 DOI: 10.1002/anie.202417066

Zongnan Wei, Wenwen Wang, Tao Shao, Shuaibing Yang, Chang Liu, Duanhui Si, Rong Cao, Minna Cao

{"title":"Constructing Ag/Cu2O Interface for Efficient Neutral CO2 Electroreduction to C2H4.","authors":"Zongnan Wei, Wenwen Wang, Tao Shao, Shuaibing Yang, Chang Liu, Duanhui Si, Rong Cao, Minna Cao","doi":"10.1002/anie.202417066","DOIUrl":"10.1002/anie.202417066","url":null,"abstract":"Neutral CO2 electroreduction to multi-carbons (C2+) offers a promising pathway to reduce the CO2 and energy losses originating from the carbonate formation. However, the sluggish kinetics of C-C coupling brings a significant challenge of achieving high selectivity of a single product (such as ethylene), especially at industrial-relevant current densities (>300 mA cm-2). Here, we reported an optimized Ag-Cu2O interfacial catalyst that exhibited C2+ Faradaic efficiency (FE) of 73.6 % at 650 mA cm-2 in a flow cell. Remarkably, it obtained FEC2H4 of 66.0 % with a partial current density of 429.1 mA cm-2, making it stand out among the reported Cu-based electrocatalysts. In situ Raman spectra uncovered that the Ag/Cu2O interfaces enabled a high coverage of *CO around the partially reduced Cu+/Cu0 active sites. Furthermore, theoretical calculations demonstrated the enhanced CO formation and C-C coupling at the Ag/Cu2O interface. This work reported an unprecedented neutral CO2 electroreduction to C2H4 performance and provided an in-depth comprehension of the role of the bimetallic interface.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":" ","pages":"e202417066"},"PeriodicalIF":16.1,"publicationDate":"2025-01-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142520458","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