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Recent Advances in Regulating Metal-Silica Interaction for Boosting Heterogeneous Catalytic Performance. 调节金属-二氧化硅相互作用提高非均相催化性能的研究进展。
IF 16.6 1区 化学
Angewandte Chemie International Edition Pub Date : 2025-10-01 DOI: 10.1002/anie.202512979
Zequan Ma,Zaihao Yuan,Jia Xue,Yilin Dong,Xu Tan,Fengyu Jin,Xiaoge Li,Yu Gu,Lin-Wei Chen,Kun Wang,Lei Wang
{"title":"Recent Advances in Regulating Metal-Silica Interaction for Boosting Heterogeneous Catalytic Performance.","authors":"Zequan Ma,Zaihao Yuan,Jia Xue,Yilin Dong,Xu Tan,Fengyu Jin,Xiaoge Li,Yu Gu,Lin-Wei Chen,Kun Wang,Lei Wang","doi":"10.1002/anie.202512979","DOIUrl":"https://doi.org/10.1002/anie.202512979","url":null,"abstract":"Heterogeneous catalysts are extensively utilized in the modern chemical industry, with catalytic processes primarily occurring on the surfaces of nanocrystals. Construction of an optimum surface/interface is of significant importance in regulating the catalytic performance. Strong metal-support interactions (SMSI) have been proven to be an efficient strategy to modulate the electronic and geometric properties of the supported nanocrystals by forming a thin amorphous coating layer and a new metal bond. The classical SMSI typically occurred on reducible metal oxides (TiO2, CeO2, Nb2O5, and Fe2O3) under a reduction environment. Nevertheless, the SMSI effect could be successfully engineered for the inert oxides (Al2O3, MgO, and SiO2) under much more severe conditions owing to the inertness of hard-to-reduce oxides compared with reducible oxides. Over the past few decades, it has been observed that the amorphous encapsulation layer could be induced under much higher temperatures, as well as the formation of a metal-Si bond, which significantly promotes various catalysis. In this review, we focus on the construction of metal-silica interaction and the dynamics of structure evolution of the metal crystals under certain reaction conditions, while highlighting their unique features in heterogeneous catalytic processes.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"71 1","pages":"e202512979"},"PeriodicalIF":16.6,"publicationDate":"2025-10-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145194752","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-Efficient Dual Formate Electrosynthesis via Coupled Formaldehyde Oxidation and CO2 Reduction at Ultra-Low Cell Voltage. 超低电池电压下甲醛氧化和CO2还原耦合的高能效双甲酸盐电合成
IF 16.6 1区 化学
Angewandte Chemie International Edition Pub Date : 2025-10-01 DOI: 10.1002/anie.202516232
Hyoseok Kim,Wonsik Jang,Jin Ho Lee,Hojeong Lee,Seunghyun Lee,Jongkyoung Kim,Dongrak Oh,Woo Yeong Noh,Miri Kim,Sun Gwan Cha,Jongchan Kim,Jae Sung Lee,Youngkook Kwon,Seungho Cho
{"title":"Energy-Efficient Dual Formate Electrosynthesis via Coupled Formaldehyde Oxidation and CO2 Reduction at Ultra-Low Cell Voltage.","authors":"Hyoseok Kim,Wonsik Jang,Jin Ho Lee,Hojeong Lee,Seunghyun Lee,Jongkyoung Kim,Dongrak Oh,Woo Yeong Noh,Miri Kim,Sun Gwan Cha,Jongchan Kim,Jae Sung Lee,Youngkook Kwon,Seungho Cho","doi":"10.1002/anie.202516232","DOIUrl":"https://doi.org/10.1002/anie.202516232","url":null,"abstract":"Electrochemical formate (HCOO-) production via CO2 reduction reaction (CO2RR) holds great promise for carbon-neutral energy systems; however, its practical implementation is significantly hindered by the high energy demand of anodic oxygen evolution reaction (OER). Replacing OER with a more energetically and economically favorable alternative anodic reaction is therefore essential. In this study, we developed a highly efficient Cu-Ag catalyst for anodic formaldehyde oxidation reaction (FOR). Systematic investigations employing in situ Raman spectroscopy and comprehensive electrochemical analyses revealed that Cu enables an earlier onset potential for FOR, and Ag enhances formaldehyde adsorption, leading to synergistically improved performance. The optimal Cu3Ag7 catalyst exhibited superior FOR performance, with an onset potential of -0.05 V versus the reversible hydrogen electrode (VRHE) and Faradaic efficiencies for HCOO- exceeding 90% from 0.1 to 0.5 VRHE. When coupled with CO2RR, the FOR||CO2RR system enabled dual-side HCOO- production, achieving a total HCOO- yield rate of 0.39 mmol h-1 cm-2 at an ultra-low cell voltage of 0.5 V, surpassing the performance of previously reported electrochemical HCOO- production systems. Furthermore, this study presents a versatile anodic strategy that integrates FOR with a range of cathodic reactions, offering an energy-efficient chemical synthesis approach for the advancement of sustainable electrochemical technologies.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"25 1","pages":"e202516232"},"PeriodicalIF":16.6,"publicationDate":"2025-10-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145194686","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
Facile One-Step Synthesis of 6 1 3 $6_1^3$ Link Cages by Coordination-Driven Self-Assembly. 协调驱动自组装快速一步合成6 1 3$ 6_1^3$连杆笼。
IF 16.6 1区 化学
Angewandte Chemie International Edition Pub Date : 2025-10-01 DOI: 10.1002/anie.202516490
Hui-Jun Feng,Shu-Ning Lan,Hui-Min Lu,Hui-Min Li,Pan-Pan Hua,Jun-Wen Wang
{"title":"Facile One-Step Synthesis of 6 1 3 $6_1^3$ Link Cages by Coordination-Driven Self-Assembly.","authors":"Hui-Jun Feng,Shu-Ning Lan,Hui-Min Lu,Hui-Min Li,Pan-Pan Hua,Jun-Wen Wang","doi":"10.1002/anie.202516490","DOIUrl":"https://doi.org/10.1002/anie.202516490","url":null,"abstract":"Among various [3]catenanes, 6 1 3 $6_1^3$ link cages have yet to be synthesized due to the difficulty of their synthesis. To address this challenge, a synthetic strategy based on the geometric characteristics of curved dipyridyl ligands and the precise regulation of the relative dimensions of the building blocks was developed. By relying on the rational design of the dimensions and conformation self-adaptation of the linkers, four 6 1 3 $6_1^3$ links and one Solomon link were synthesized by the assembly of curved dipyridyl ligands and half-sandwich rhodium/iridium(III) dinuclear fragments. Among the various structures mentioned, the metallo-cages with 6 1 3 $6_1^3$ topology were synthesized with high selectivity when the length of the long arms featuring a dipyridyl ligand minus the length of the binuclear building block was approximately 7 Å. Notably, this synthetic approach employing elongated dinuclear building blocks enabled the preparation of novel closed three-link chain cages with substantially expanded cavity dimensions compared with those of known analogues. Additionally, this construction strategy allows tuning of the cavity size of the resulting cages by modulating the dimensions of the building blocks.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"102 1","pages":"e202516490"},"PeriodicalIF":16.6,"publicationDate":"2025-10-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145194925","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
Bis(azuleno)pentalenes with Six Consecutive Odd-Membered Rings. 具有六个连续奇数元环的双(azuleno)戊烯。
IF 16.6 1区 化学
Angewandte Chemie International Edition Pub Date : 2025-10-01 DOI: 10.1002/anie.202513158
Qing Jiang,Tianzuo Wang,Yi Han,Haipeng Wei,Yunfeng Deng,Yanhou Geng,Chunyan Chi
{"title":"Bis(azuleno)pentalenes with Six Consecutive Odd-Membered Rings.","authors":"Qing Jiang,Tianzuo Wang,Yi Han,Haipeng Wei,Yunfeng Deng,Yanhou Geng,Chunyan Chi","doi":"10.1002/anie.202513158","DOIUrl":"https://doi.org/10.1002/anie.202513158","url":null,"abstract":"Non-alternant, non-benzenoid polycyclic hydrocarbons (PHs) exhibit unique optical and electronic properties distinct from their well-studied benzenoid π-conjugated counterparts. However, the synthesis of such π-systems, particularly those composed exclusively of odd-membered carbocycles, remains a significant challenge. Herein, we report the first synthesis of three diazuleno[a,e]pentalene derivatives (AP-1, AP-2, and AP-3), featuring fused five- and seven-membered rings, via a palladium-catalyzed homoannulation of o-alkynylazulenyliodide. These compounds possess a 24 π-electron system with six consecutively fused odd-membered rings in a 7-5-5-5-5-7 topology. Comprehensive characterization by X-ray crystallography, NMR spectroscopy, and theoretical calculations (ACID, NICS) reveals an electronic structure comprising two aromatic azulene units fused to a central antiaromatic pentalene core. The resulting molecules display a small HOMO-LUMO gap and amphoteric redox behavior, arising from the interplay between the aromatic and antiaromatic subunits. Notably, AP-1 and AP-2 can undergo reversible protonation and deprotonation processes upon exposure to acid and base. Furthermore, solution-processed organic field-effect transistors based on AP-2 show p-type semiconducting behavior with a maximum hole mobility of 0.72 cm2 V-1 s-1, demonstrating the potential of non-alternant, non-benzenoid PHs for applications in organic electronics.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"99 1","pages":"e202513158"},"PeriodicalIF":16.6,"publicationDate":"2025-10-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145194750","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
Intergrowth of Prismatic and Octahedral Layers to Inhibit Fe Migration in Oxide Cathodes for Sodium-Ion Batteries. 棱镜层和八面体层共同生长抑制铁在钠离子电池氧化物阴极中的迁移。
IF 16.6 1区 化学
Angewandte Chemie International Edition Pub Date : 2025-10-01 DOI: 10.1002/anie.202509816
Tong Zhang,Zihao Song,Yuesen Li,Yaohui Huang,Jingyu Su,Weibo Hua,Fujun Li
{"title":"Intergrowth of Prismatic and Octahedral Layers to Inhibit Fe Migration in Oxide Cathodes for Sodium-Ion Batteries.","authors":"Tong Zhang,Zihao Song,Yuesen Li,Yaohui Huang,Jingyu Su,Weibo Hua,Fujun Li","doi":"10.1002/anie.202509816","DOIUrl":"https://doi.org/10.1002/anie.202509816","url":null,"abstract":"Fe-based layered oxides have emerged as promising sustainable cathode materials for sodium-ion batteries (SIBs) due to their earth abundance. However, the oxidation of Fe3+ to Fe4+ is typically accompanied by its migration to Na layers for capacity and voltage decay. Herein, we demonstrated that Fe migration can be suppressed by modulating the prismatic (P) and octahedral (O) intergrowth at deeply charged states in O3-Na0.8Fe0.4Ni0.1Mn0.4M0.15O2 (M = Ca, Mg). The strong bonding of O2-─Ca2+─O2- in Na layers prevents the gliding of transition-metal (TM) layers and mitigates the P- to O-type stacking transition at ≥ 3.7 V, which alleviates formation of vacant tetrahedra in O-type stacking structure to restrict Fe migration. At the same time, Mg incorporation in TM layers promotes an upward shift of Fe 3d states toward the Fermi level and facilitates the sluggish redox of Fe3+/Fe4+. These enable its high specific capacity of 136 mAh g-1 and outstanding cycling stability with capacity retention of 72% after 1000 cycles. This work paves the pathway for design of sustainable cathode materials for SIBs and beyond.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"102 1","pages":"e202509816"},"PeriodicalIF":16.6,"publicationDate":"2025-10-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145194749","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
Asymmetric Acetylene Activation Enables Enhanced Electrochemical Ethylene Formation Kinetics. 不对称乙炔活化增强了电化学乙烯形成动力学。
IF 16.6 1区 化学
Angewandte Chemie International Edition Pub Date : 2025-10-01 DOI: 10.1002/anie.202516885
Yanran Han,Chuanqi Cheng,Fanpeng Chen,Bin Zhang,Bo-Hang Zhao
{"title":"Asymmetric Acetylene Activation Enables Enhanced Electrochemical Ethylene Formation Kinetics.","authors":"Yanran Han,Chuanqi Cheng,Fanpeng Chen,Bin Zhang,Bo-Hang Zhao","doi":"10.1002/anie.202516885","DOIUrl":"https://doi.org/10.1002/anie.202516885","url":null,"abstract":"Copper (Cu)-based catalysts with weak ethylene (C2H4) adsorption exhibit a robust ability to suppress the overhydrogenation of electrocatalytic acetylene (C2H2) hydrogenation (EAH), providing a green alternative for C2H4 production. However, the unsatisfactory C2H4 formation kinetics due to the sluggishness of C2H2 reactants still limit its practical application potential. Herein, borate-decorated oxide-derived copper nanoparticles (OD Cu-B NPs) are designed to promote C2H2 activation and adsorption. As a result, the as-prepared catalysts deliver a partial current density of 720 mA cm-2 with a turnover frequency of 48.33 s-1, greatly outperforming the bare OD Cu counterpart. The symmetric electron distribution of C2H2 is revealed to be broken over the Cu-borate interface, making it easier to activate and adsorb, which accounts for the lowered hydrogenation barrier and enhanced selectivity, consequently promoting C2H4 formation kinetics through the EAH process.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"39 1","pages":"e202516885"},"PeriodicalIF":16.6,"publicationDate":"2025-10-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145194690","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
Photoredox/Nickel-Cocatalyzed Asymmetric C-O and C-S Couplings for Atroposelective Synthesis of N-Heterobiaryls. 光氧化还原/镍共催化的不对称C-O和C-S偶联在氨选择性合成n -杂双芳基中的应用。
IF 16.6 1区 化学
Angewandte Chemie International Edition Pub Date : 2025-09-30 DOI: 10.1002/anie.202516584
Tian-Zhen Li,Cheng-Cheng Tian,Wei Chen,Zi-Yun Zou,Jia-Liang Yang,Fang-Xi Liu,Xinyao Li,Hong-Hao Zhang,Feng Shi
{"title":"Photoredox/Nickel-Cocatalyzed Asymmetric C-O and C-S Couplings for Atroposelective Synthesis of N-Heterobiaryls.","authors":"Tian-Zhen Li,Cheng-Cheng Tian,Wei Chen,Zi-Yun Zou,Jia-Liang Yang,Fang-Xi Liu,Xinyao Li,Hong-Hao Zhang,Feng Shi","doi":"10.1002/anie.202516584","DOIUrl":"https://doi.org/10.1002/anie.202516584","url":null,"abstract":"Photoredox/nickel-cocatalyzed cross-couplings have emerged as powerful methods for constructing carbon-heteroatom bonds under mild conditions. Despite their rapid development, catalytic asymmetric C(sp2)-heteroatom couplings remain largely underexplored and challenging. Herein, we established photoredox/nickel-cocatalyzed asymmetric C-O and C-S couplings of racemic heterobiaryl triflates with diverse oxygen and sulfur nucleophiles. This straightforward protocol enables highly enantioselective C(sp2)-O and C(sp2)-S bond formation under mild reaction conditions, providing diverse axially chiral N-heterobiaryls (>100 examples) with excellent atroposelectivity and functional group tolerance. These axially chiral N-heterobiaryls can be further transformed into valuable chiral compounds, including commonly used chiral ligands and organocatalysts, while the resultant C-S coupling products can serve directly as chiral ligands in asymmetric catalysis. This study represents the first highly enantioselective photoredox/Ni-cocatalyzed asymmetric C(sp2)-heteroatom bond coupling and introduces a new strategy for atroposelective synthesis of N-heterobiaryl atropisomers with wide applicability. Mechanistic investigations reveal that both C-O and C-S couplings proceed via an energy-transfer pathway: the C-O coupling follows a kinetic resolution mechanism, while the C-S coupling proceeds via dynamic kinetic asymmetric transformation, thus providing valuable insights into this class of C(sp2)-heteroatom couplings and advancing this field.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"104 1","pages":"e202516584"},"PeriodicalIF":16.6,"publicationDate":"2025-09-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145189304","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
Proton Conduction, Dielectric Relaxation, Photoluminescence, and Photochromism Governed by Humidity and Alcohol Vapors in a Uranyl-Cobalt Framework with Labile Coordination Sites. 具有不稳定配位的铀酰-钴骨架中湿度和酒精蒸气控制的质子传导、介电弛豫、光致发光和光致变色。
IF 16.6 1区 化学
Angewandte Chemie International Edition Pub Date : 2025-09-30 DOI: 10.1002/anie.202517109
Jakub J Zakrzewski,Aleksander Hoffman,Junhao Wang,Marzena Pander,Dariusz Matoga,Hiroko Tokoro,Shin-Ichi Ohkoshi,Szymon Chorazy
{"title":"Proton Conduction, Dielectric Relaxation, Photoluminescence, and Photochromism Governed by Humidity and Alcohol Vapors in a Uranyl-Cobalt Framework with Labile Coordination Sites.","authors":"Jakub J Zakrzewski,Aleksander Hoffman,Junhao Wang,Marzena Pander,Dariusz Matoga,Hiroko Tokoro,Shin-Ichi Ohkoshi,Szymon Chorazy","doi":"10.1002/anie.202517109","DOIUrl":"https://doi.org/10.1002/anie.202517109","url":null,"abstract":"Stimuli-responsive coordination polymers serve as an efficient platform for the generation of functional systems, showing tunable magnetic, electrical, optical, and mechanical features, as well as their rich combinations. We report a truly multifunctional material based on a coordination framework employing photoluminescent uranyl(VI) cations bonded through cyanido bridges to cobalt(III) centers and between themselves by hydroxido and 1,4-diazabicyclo[2.2.2]octane-N,N'-dioxide linkers. This material reveals proton conduction, dielectric relaxation, and visible light emission, all switchable by relative humidity (RH). Moreover, the reported system shows affinity to organic solvents, which efficiently quench the emission. The sorption with a RH-reversible shape-memory effect was found for methanol and acetonitrile vapors, while the unusual RH-activated sorption appears for ethanol. More importantly, the adsorption of simple alcohols activates visible-light photochromism, leading to an optical memory effect present after their desorption. The observed adsorption of solvents and the related modification of the optical properties are possible not only due to the flexibility of the framework but also owing to extraordinarily labile coordination sites of uranium(VI) centers involving aqua and bridging hydroxido ligands, which can be selectively exchanged by specific solvent molecules.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"4 1","pages":"e202517109"},"PeriodicalIF":16.6,"publicationDate":"2025-09-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145189351","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 C2 Selectivity in Electrocatalytic CO2 Reduction Via Synergy of Plasmonic Hot Electrons and Photothermal Effect. 等离子体热电子与光热效应协同作用增强电催化CO2还原中C2选择性。
IF 16.6 1区 化学
Angewandte Chemie International Edition Pub Date : 2025-09-30 DOI: 10.1002/anie.202515432
Linlin Chen,Cenfeng Fu,Canyu Hu,Yu Bai,Yawen Jiang,Yuan Zhong,Xinyu Wang,Chuansheng Hu,Ran Long,Yingpu Bi,Yujie Xiong
{"title":"Enhancing C2 Selectivity in Electrocatalytic CO2 Reduction Via Synergy of Plasmonic Hot Electrons and Photothermal Effect.","authors":"Linlin Chen,Cenfeng Fu,Canyu Hu,Yu Bai,Yawen Jiang,Yuan Zhong,Xinyu Wang,Chuansheng Hu,Ran Long,Yingpu Bi,Yujie Xiong","doi":"10.1002/anie.202515432","DOIUrl":"https://doi.org/10.1002/anie.202515432","url":null,"abstract":"Surface plasmon-enhanced electrocatalytic CO2 reduction offers an attractive dimension beyond conventional electrocatalytic methods by optimizing photon utilization to simplify electrocatalytic reactor designs and enhance reaction activity/selectivity. However, the synergistic regulation mechanism of the complex multiple plasmonic effects on the CO2 reduction reaction, particularly under electrochemical bias, remains to be thoroughly investigated. This study, based on copper plasmonic electrodes, reveals the key role of localized surface plasmon resonance (LSPR) in enhancing CO2 conversion and facilitating the transition of the key intermediate *CO from bridge to atop adsorption configuration. Through a combination of experiments and density functional theory calculations, we show that the synergy of plasmonic hot electrons and photothermal effect effectively reduces the C─C coupling energy barrier. Systematic measurements clarify the correlation between the plasmonic excitation of the electrode and the enhanced selectivity of C2 products. Under optimized conditions, synergetic plasmonic effects significantly promote the CO2 conversion and enhance the Faradaic efficiency (FE) of C2 products, with a maximum increase from 57% to 87%. This work not only provides a new perspective for understanding the complex synergistic mechanisms of plasmonic effects, but also opens a new avenue for achieving selective electrocatalytic CO2 conversion.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"6 1","pages":"e202515432"},"PeriodicalIF":16.6,"publicationDate":"2025-09-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145189303","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
Alkynyl‐Germanium Architectures Through Electrochemical Low‐Valent Iron‐Catalyzed Conjunctive Coupling 通过电化学低价铁催化的共轭偶联研究炔基锗结构
IF 16.6 1区 化学
Angewandte Chemie International Edition Pub Date : 2025-09-30 DOI: 10.1002/anie.202516109
Haifeng Chen, Magnus Rueping
{"title":"Alkynyl‐Germanium Architectures Through Electrochemical Low‐Valent Iron‐Catalyzed Conjunctive Coupling","authors":"Haifeng Chen, Magnus Rueping","doi":"10.1002/anie.202516109","DOIUrl":"https://doi.org/10.1002/anie.202516109","url":null,"abstract":"Catalytic cross‐coupling by transition metals has transformed carbon–germanium (C─Ge) bond formation in organic synthesis. The formation of unsaturated C(sp)─Ge bonds, however, remains a largely uncharted frontier. We herein report the construction of congested alkynyl–germane architectures via iron‐catalyzed coupling of alkynyl chlorides with chlorogermanes, affording a broad spectrum of germane products. The methodology also enables late‐stage functionalization of natural products and drug‐derived molecules bearing C(sp)─Ge bonds, thereby demonstrating its synthetic utility. The scalability of the reaction and the facile derivatization of the products further underscore the robustness and versatility of this protocol. Mechanistic investigations reveal that LnFe⁰ species serve as the initiating catalyst and provide insights into the pathway of this new iron‐catalyzed electrophile cross‐coupling.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"1 1","pages":""},"PeriodicalIF":16.6,"publicationDate":"2025-09-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145188637","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
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