ACS Catalysis 最新文献

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Deep-Learning-Driven Discovery and Engineering of Imine Reductase for the Efficient Synthesis of Chiral Opine Derivatives 深度学习驱动的亚胺还原酶的发现和工程,用于手性衍生物的高效合成
IF 12.9 1区 化学
ACS Catalysis Pub Date : 2026-10-16 DOI: 10.1021/acscatal.6c06352
Jia-Neng Xu,Min-Min Zhao,Cheng-Long Xu,Xiang Wang,Zhe Dou,Ya-Jun Wang
{"title":"Deep-Learning-Driven Discovery and Engineering of Imine Reductase for the Efficient Synthesis of Chiral Opine Derivatives","authors":"Jia-Neng Xu,Min-Min Zhao,Cheng-Long Xu,Xiang Wang,Zhe Dou,Ya-Jun Wang","doi":"10.1021/acscatal.6c06352","DOIUrl":"https://doi.org/10.1021/acscatal.6c06352","url":null,"abstract":"Abstract The narrow amine donor scope of imine reductases (IREDs) limits their application in the synthesis of opine compounds. Herein, we report a machine learning (ML)-guided protein engineering strategy to address this limitation. An IRED from an unclassified Ensifer, IRED5, was identified through deep-learning-based screening for its strict enantioselectivity toward methyl glycinate. Subsequent engineering using a few-shot learning for protein fitness prediction approach yielded the M178T/A208L/P241V/A36E/S67Q/Q187N (M6) variant with six mutations across the active site and protein surface. Kinetic analysis showed 156-fold toward methyl pyruvate and 72-fold improvements toward methyl glycinate in catalytic efficiency, respectively, over the wild-type (WT) enzyme. M6 accepted diverse keto esters and amino acid esters, enabling stereoselective formation of opine derivatives bearing two stereocenters. Structural and computational analyses revealed the molecular basis for activity enhancement. In preparative synthesis, M6 achieved complete conversion at a 3 M substrate loading, corresponding to a space time yield of 366 g·L–1·d–1. At a 4 M substrate loading, conversion remained high at 95.4% with a space time yield of 525 g·L–1·d–1, affording 10.5 g of enantiopure methyl N-(2-methoxy-2-oxoethyl)-d-alaninate (1a) in 75.0% isolated yield with > 99.9% ee. This work establishes an efficient biocatalytic route to opine compounds and demonstrates the utility of ML-guided enzyme engineering in expanding IRED synthetic capability.","PeriodicalId":9,"journal":{"name":"ACS Catalysis ","volume":"52 1","pages":""},"PeriodicalIF":12.9,"publicationDate":"2026-10-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149210185","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
Intelligent Agent-Driven Design of Dynamically Reconstructed Metal-Organic Frameworks toward Industrial-Scale Anion-Exchange-Membrane Water Electrolysis 面向工业规模阴离子交换膜电解的动态重构金属-有机框架的智能体驱动设计
IF 13.6 1区 化学
ACS Catalysis Pub Date : 2026-10-16 Epub Date: 2026-07-11 DOI: 10.1021/acscatal.6c03989
Liangliang Xu, Jiankang Wang, Canhui Zhang, Jinpei Huang, Jian Zhou, Zhichu Ren, Jiaxin Yao, Jinyang Li, Heqing Jiang, Minghua Huang, Zhengxiao Guo, Zhongfang Chen
{"title":"Intelligent Agent-Driven Design of Dynamically Reconstructed Metal-Organic Frameworks toward Industrial-Scale Anion-Exchange-Membrane Water Electrolysis","authors":"Liangliang Xu,&nbsp;Jiankang Wang,&nbsp;Canhui Zhang,&nbsp;Jinpei Huang,&nbsp;Jian Zhou,&nbsp;Zhichu Ren,&nbsp;Jiaxin Yao,&nbsp;Jinyang Li,&nbsp;Heqing Jiang,&nbsp;Minghua Huang,&nbsp;Zhengxiao Guo,&nbsp;Zhongfang Chen","doi":"10.1021/acscatal.6c03989","DOIUrl":"10.1021/acscatal.6c03989","url":null,"abstract":"<p>Metal-organic frameworks (MOFs) are omnipotent precatalysts, yet their catalytically operative structures are typically reconstructed in situ under working conditions. Such dynamic evolution obscures the true active phase and renders conventional descriptor engineering and AI screening based on pristine MOFs intrinsically unreliable. Here, we develop a reconstruction-involved intelligent agent-driven discovery framework to integrate literature knowledge extraction, operando-informed active-phase identification, closed-loop density functional theory, and machine learning to design MOF-derived catalysts for the oxygen evolution reaction (OER) from their actually reconstructed states, rather than their precursor structures. By integrating a multimodal in situ and operando diagnostic platform, we uncover a programmable phase evolution from the pristine MOF to metal hydroxides and subsequently to the catalytically active oxyhydroxide phases, thereby establishing the structural basis for reconstruction-governed catalyst discovery. Applied to NiM-MOF systems, the framework identifies oxygen-vacancy-rich NiM-OOH as the operative catalytic motif and distills a transferable, physically interpretable descriptor that links Ni electronic structure and dopant properties to OER overpotential across reconstructed compositions. Guided by this descriptor, the workflow pinpoints NiFe-OOH/Ov derived from NiFe-MOF as the optimal anode, achieving 1.0 A cm<sup>–2</sup> at 1.88 V in an anion-exchange-membrane water electrolyzer and sustaining stable operation for 1100 h at 1.0 A cm<sup>–2</sup> and 500 h at 2.0 A cm<sup>–2</sup>. Beyond identifying a high-performance NiFe system, this work provides a general blueprint for mechanistically grounded autonomous catalyst discovery in reconstruction-dominated electrocatalysis.</p>","PeriodicalId":9,"journal":{"name":"ACS Catalysis ","volume":"16 20","pages":"20063–20077"},"PeriodicalIF":13.6,"publicationDate":"2026-10-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148476532","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
Selectivity Maps for Electrochemical Ethylene Oxidation to Ethylene Oxide and Ethylene Glycol 电化学乙烯氧化成环氧乙烷和乙二醇的选择性图
IF 13.6 1区 化学
ACS Catalysis Pub Date : 2026-10-16 Epub Date: 2026-09-25 DOI: 10.1021/acscatal.6c05457
Pauline Schütt, Boaz Izelaar, Jakob Kibsgaard, Alexander Bagger
{"title":"Selectivity Maps for Electrochemical Ethylene Oxidation to Ethylene Oxide and Ethylene Glycol","authors":"Pauline Schütt,&nbsp;Boaz Izelaar,&nbsp;Jakob Kibsgaard,&nbsp;Alexander Bagger","doi":"10.1021/acscatal.6c05457","DOIUrl":"10.1021/acscatal.6c05457","url":null,"abstract":"<p>Electrochemical ethylene oxidation can produce ethylene oxide and ethylene glycol, but selectivity is limited by competition with the oxygen evolution reaction and overoxidation. At the same time, the mechanistic literature is fragmented across oxo-, peroxo-, and hydroxyl-mediated pathways, creating ambiguity and hindering systematic improvement. Using density functional theory (DFT) and scaling relations, we build a unified descriptor-based framework comparing the three pathways across fcc metals, metal(II) oxides, and rutile-structured oxides. The oxygen binding strength is found to control ethylene activation via oxo and peroxo species, while a carbon-based descriptor describes the hydroxyl pathway, and product binding defines an overoxidation limit. The resulting selectivity maps identify the catalyst properties required for each route, rationalize the high performance of individual catalysts such as oxidized Pd, and provide transferable guidelines for designing selective alkene oxidation catalysts.</p>","PeriodicalId":9,"journal":{"name":"ACS Catalysis ","volume":"16 20","pages":"20551–20561"},"PeriodicalIF":13.6,"publicationDate":"2026-10-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149049992","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
Oxidation-State-Modulated Cobalt Catalysts for Ambient Selective Hydrogenation of Bio-Derived Aldehydes: Toward Bio-Based Polyesters 氧化态调节的钴催化剂用于生物衍生醛的环境选择性加氢:制备生物基聚酯
IF 13.6 1区 化学
ACS Catalysis Pub Date : 2026-10-16 Epub Date: 2026-09-24 DOI: 10.1021/acscatal.6c04769
Ting Wang, Chencong Ruan, Cornelis Post, Wei Zhang, Tim G. W. Engels, Henk H. van de Bovenkamp, Yuqiang Yang, Dominic Gerlach, Vincent S. D. Voet, Rudy Folkersma, Katja Loos, Yutao Pei, Jun Yue, Petra Rudolf, Moniek Tromp, Hero J. Heeres, Xianhai Zeng, Peter J. Deuss
{"title":"Oxidation-State-Modulated Cobalt Catalysts for Ambient Selective Hydrogenation of Bio-Derived Aldehydes: Toward Bio-Based Polyesters","authors":"Ting Wang,&nbsp;Chencong Ruan,&nbsp;Cornelis Post,&nbsp;Wei Zhang,&nbsp;Tim G. W. Engels,&nbsp;Henk H. van de Bovenkamp,&nbsp;Yuqiang Yang,&nbsp;Dominic Gerlach,&nbsp;Vincent S. D. Voet,&nbsp;Rudy Folkersma,&nbsp;Katja Loos,&nbsp;Yutao Pei,&nbsp;Jun Yue,&nbsp;Petra Rudolf,&nbsp;Moniek Tromp,&nbsp;Hero J. Heeres,&nbsp;Xianhai Zeng,&nbsp;Peter J. Deuss","doi":"10.1021/acscatal.6c04769","DOIUrl":"10.1021/acscatal.6c04769","url":null,"abstract":"<p>Selective hydrogenation is a crucial process in the synthesis of chemical intermediates. Here, we report the efficient hydrogenation of 5-hydroxymethylfurfural (HMF) to 2,5-bishydroxymethylfuran (BHMF) over N-doped C-supported cobalt catalysts (CoNC) derived from ZIF-67 for the enzymatic synthesis of poly(2,5-furandimethylene adipate) (PFAd). By varying the oxidative pretreatment temperature, a series of CoNCX catalysts (where X denotes the oxidation temperature) were obtained, enabling effective tuning of catalytic activity. The optimized catalyst, CoNC200, achieved 93% HMF conversion and 99% BHMF selectivity, with a BHMF yield approximately 30% higher than that of the nonoxidized sample at 100 °C within 20 min. Notably, near-complete conversion and high selectivity can be achieved at room temperature within 8 h, while similar performance is obtained at 120 °C within 30 min, demonstrating high selectivity and efficiency across a wide temperature range. The low apparent activation energy (39.9 kJ mol<sup>–1</sup>) further confirms the high intrinsic activity of CoNC200. The enhanced low-temperature performance is attributed to the synergistic effect of CoOOH and Co<sub>3</sub>O<sub>4</sub> species with high-valence cobalt sites on the N-doped carbon support, as revealed by comprehensive characterization. Furthermore, the catalytic system is compatible with enzymatic polymerization, enabling direct conversion of crude BHMF mixtures containing residual HMF into polyesters using dimethyl adipate. The presence of HMF allows modulation of the polymer molecular weight without compromising the thermal properties. These findings underscore a robust and versatile strategy for integrating selective hydrogenation with mild enzymatic polycondensation toward bio-based polyesters.</p>","PeriodicalId":9,"journal":{"name":"ACS Catalysis ","volume":"16 20","pages":"20175–20188"},"PeriodicalIF":13.6,"publicationDate":"2026-10-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149049995","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
Electrophile-Dependent Chemo- and Regioselectivity in Cu/Pd-Catalyzed Allylboration of Enynes 铜/钯催化烯丙基硼化反应中亲电依赖的化学和区域选择性
IF 13.6 1区 化学
ACS Catalysis Pub Date : 2026-10-16 Epub Date: 2026-09-29 DOI: 10.1021/acscatal.6c05418
Asier Otero-Mougán, Mingming Huang, Israel Fernández, Martín Fañanás-Mastral
{"title":"Electrophile-Dependent Chemo- and Regioselectivity in Cu/Pd-Catalyzed Allylboration of Enynes","authors":"Asier Otero-Mougán,&nbsp;Mingming Huang,&nbsp;Israel Fernández,&nbsp;Martín Fañanás-Mastral","doi":"10.1021/acscatal.6c05418","DOIUrl":"10.1021/acscatal.6c05418","url":null,"abstract":"<p>Achieving chemo- and regiodivergence from common starting materials represents a central goal in organic synthesis to enable rapid access to structurally distinct molecular architectures. Herein, we report an electrophile-controlled, chemo- and regioselective allylboration of 1,3-enynes with allylic carbonates and bis(pinacolato)diboron. The nature of the carbonate electrophile dictates the reaction outcome, with allyl carbonates enabling the efficient synthesis of borylated 1,4-enallenes, whereas dienyl carbonates redirect the transformation toward propargylation, furnishing 1,3,7-dienynes with high regio- and stereoselectivity. DFT calculations reveal that this divergence originates from distinct reductive elimination pathways of a common η<sup>3</sup>-allyl-η<sup>1</sup>-allenyl Pd intermediate, which governs selectivity. Allyl-derived intermediates undergo 1,1′-type reductive elimination to afford tetrasubstituted allenes, whereas vinyl-substituted allyl-Pd species formed from dienyl carbonates engage in an intramolecular propargylic addition. This study provides mechanistic insights into allyl–allenyl palladium chemistry and establishes a regiodivergent strategy for accessing densely functionalized organoboronates from readily available starting materials.</p>","PeriodicalId":9,"journal":{"name":"ACS Catalysis ","volume":"16 20","pages":"20527–20540"},"PeriodicalIF":13.6,"publicationDate":"2026-10-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149090603","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/Copper-Catalyzed C(sp3)–H Bond Functionalization for Radical Cross-Coupling to Construct C(sp3)–C(sp3) Bonds 光氧化还原/铜催化C(sp3) -氢键功能化自由基交叉偶联构建C(sp3) -C (sp3)键
IF 13.6 1区 化学
ACS Catalysis Pub Date : 2026-10-16 Epub Date: 2026-10-06 DOI: 10.1021/acscatal.6c04942
Yi-Ming Li, Yi-Fei Kong, Ying-Chun Song, Jiang Cao, Qiu-Ping Liu, Yao Han, Daquan Chen, Yanmei Chen, Yuan-Yuan Sun, Jin-Heng Li, Yan-Ping Zhu
{"title":"Photoredox/Copper-Catalyzed C(sp3)–H Bond Functionalization for Radical Cross-Coupling to Construct C(sp3)–C(sp3) Bonds","authors":"Yi-Ming Li,&nbsp;Yi-Fei Kong,&nbsp;Ying-Chun Song,&nbsp;Jiang Cao,&nbsp;Qiu-Ping Liu,&nbsp;Yao Han,&nbsp;Daquan Chen,&nbsp;Yanmei Chen,&nbsp;Yuan-Yuan Sun,&nbsp;Jin-Heng Li,&nbsp;Yan-Ping Zhu","doi":"10.1021/acscatal.6c04942","DOIUrl":"10.1021/acscatal.6c04942","url":null,"abstract":"<p>The construction of C(sp<sup>3</sup>)–C(sp<sup>3</sup>) bonds is a pivotal transformation in medicinal chemistry, as it introduces three-dimensional complexity that is crucial for improving a compound's druggability and target selectivity. However, strategies for efficiently forming C(sp<sup>3</sup>)–C(sp<sup>3</sup>) bonds via C(sp<sup>3</sup>)–H alkylation have developed slowly, as the high bond dissociation energy of inert C(sp<sup>3</sup>)–H bonds renders their selective activation and functionalization challenging. Herein, we report a photoinduced copper-catalyzed C(sp<sup>3</sup>)–H bond functionalization strategy for constructing C(sp<sup>3</sup>)–C(sp<sup>3</sup>) bonds through the radical–radical cross-coupling of cyclopropanols with <em>N</em>-fluoroamides. This process precisely activates the C(sp<sup>3</sup>)–H bond of <em>N</em>-fluoroamide <em>via</em> an intramolecular 1,5-hydrogen atom transfer (1,5-HAT), followed by selective cross-coupling with the key radical generated from the ring-opening of a cyclopropanol. The copper center may play an important role in the cross-selective coupling of C(sp<sup>3</sup>)–C(sp<sup>3</sup>) bonds. The reaction exhibits good functional group tolerance, allowing the preparation of a variety of C(sp<sup>3</sup>) alkylation products encompassing 1°–1°, 1°–2°, and other C(sp<sup>3</sup>)–C(sp<sup>3</sup>) bond types. The practical utility of this method is further demonstrated through scale-up experiments, product transformations, and late-stage functionalization of complex natural products and drug molecules.</p>","PeriodicalId":9,"journal":{"name":"ACS Catalysis ","volume":"16 20","pages":"20297–20310"},"PeriodicalIF":13.6,"publicationDate":"2026-10-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149092489","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
Cp2TiCl2-Catalyzed Reductive Methylidenation of Alkyl Ketones with CH2Br2 cp2ticl2催化烷基酮与CH2Br2的还原甲基化反应
IF 13.6 1区 化学
ACS Catalysis Pub Date : 2026-10-16 Epub Date: 2026-09-25 DOI: 10.1021/acscatal.6c06010
Jieping Chen, Shannon S. Stahl
{"title":"Cp2TiCl2-Catalyzed Reductive Methylidenation of Alkyl Ketones with CH2Br2","authors":"Jieping Chen,&nbsp;Shannon S. Stahl","doi":"10.1021/acscatal.6c06010","DOIUrl":"10.1021/acscatal.6c06010","url":null,"abstract":"<p>Direct methylidenation of carbonyl compounds represents an appealing route to terminal alkenes. Existing methods for this transformation typically rely on stoichiometric phosphorus ylides (methylene Wittig) or organotitanium complexes (Tebbe or Petasis reagents). Here, we report a Cp<sub>2</sub>TiCl<sub>2</sub>-catalyzed method that uses CH<sub>2</sub>Br<sub>2</sub> as a readily available carbene precursor and Zn as the reductant for methylidenation of alkyl ketones. The reaction is proposed to proceed via the in situ generation of an alkyl–Zn species, which then generates a Ti–carbene intermediate. Alkali metal salts, such as KBF<sub>4</sub> and LiPF<sub>6</sub>, improve the reaction efficiency. Cyclic voltammetry studies implicate the alkali metal ions in promoting dissociation of chloride from Ti and enhancing reactivity with the alkyl–Zn reagent. The resulting protocol is operationally simple and offers a practical alternative to the use of stoichiometric methylidenation reagents.</p>","PeriodicalId":9,"journal":{"name":"ACS Catalysis ","volume":"16 20","pages":"19867–19873"},"PeriodicalIF":13.6,"publicationDate":"2026-10-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149050271","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
Elucidating the Synergistic Role of K-Co-Cu Ternary Interfaces in Selective CO2 Hydrogenation to Ethylene: A Combined DFT and Microkinetic Modeling Study 阐明K-Co-Cu三元界面在CO2选择性加氢制乙烯中的协同作用:DFT和微动力学模型的联合研究
IF 13.6 1区 化学
ACS Catalysis Pub Date : 2026-10-16 Epub Date: 2026-09-30 DOI: 10.1021/acscatal.6c05494
Shendong Guo, Ling Wang, Xiaowa Nie, Xinwen Guo
{"title":"Elucidating the Synergistic Role of K-Co-Cu Ternary Interfaces in Selective CO2 Hydrogenation to Ethylene: A Combined DFT and Microkinetic Modeling Study","authors":"Shendong Guo,&nbsp;Ling Wang,&nbsp;Xiaowa Nie,&nbsp;Xinwen Guo","doi":"10.1021/acscatal.6c05494","DOIUrl":"10.1021/acscatal.6c05494","url":null,"abstract":"<p>Direct CO<sub>2</sub> hydrogenation to value-added hydrocarbons provides a pivotal route for carbon resource recycling, yet achieving high selectivity toward specific products remains a significant challenge. In this study, we combined density functional theory calculations with microkinetic modeling (MKM) to systematically investigate the catalytic performance of a series of K<sub>2</sub>O-promoted Co<sub>2</sub>C surfaces, including K/C<span>o</span><sub>2</sub>C, K/Cu<sub>4</sub>-C<span>o</span><sub>2</sub>C, K/Cu-C<span>o</span><sub>2</sub>C(int), and K/C<span>o</span><sub>2</sub>C-Cu(inv) for CO<sub>2</sub> hydrogenation. The computational results reveal that both the Co/Cu atomic ratio and the interfacial structure decisively govern the catalytic performance. In particular, the K/Cu-C<span>o</span><sub>2</sub>C(int) surface, with a Co:Cu atomic ratio of 1:1 and the largest heterogeneous interface, exhibits moderate adsorption strengths for CO<sub>2</sub> and H<sub>2</sub>, effectively mitigating the active site poisoning that is prevalent on the pristine K/C<span>o</span><sub>2</sub>C surface. Potential energy surface analyses demonstrate that this tailored interfacial structure significantly reduces the barriers for both the reverse water-gas shift reaction and C–C coupling, while kinetically suppressing the competing CO-insertion and methanation pathways. Furthermore, MKM and degree of rate control analyses confirm that the K/Cu-C<span>o</span><sub>2</sub>C(int) interface model sustains balanced surface species coverage and delivers C<sub>2</sub>H<sub>4</sub> turnover frequency several orders of magnitude higher than that of the other catalyst configurations across 500–700 K. This work clarifies the atomic-scale modulation mechanism of K-Co-Cu ternary interfaces and provides guidance for the rational design of catalysts for selective CO<sub>2</sub>-to-olefins conversion.</p>","PeriodicalId":9,"journal":{"name":"ACS Catalysis ","volume":"16 20","pages":"20486–20499"},"PeriodicalIF":13.6,"publicationDate":"2026-10-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149090601","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
High-Density Iridium Single Atoms on Vanadium-Doped TiO2 for Electrochemical Water Oxidation Catalysis 钒掺杂TiO2上高密度铱单原子的电化学水氧化催化
IF 12.9 1区 化学
ACS Catalysis Pub Date : 2026-10-16 DOI: 10.1021/acscatal.6c04537
Chang Hyun Lee,Nodo Lee,Seungwoo Choi,Jun Ho Jang,Kyung Tae Kim,Ji Hoon Chung,Donghyeon Oh,Jung Sug Hong,Byung Soo Oh,Choul Kim,Young Hwan Min,Hui-Youn Shin,Myeong-Soo Chang,Zhipeng Wang,Sang Ho Oh,Hyacinthe Randriamahazaka,Ki Tae Nam
{"title":"High-Density Iridium Single Atoms on Vanadium-Doped TiO2 for Electrochemical Water Oxidation Catalysis","authors":"Chang Hyun Lee,Nodo Lee,Seungwoo Choi,Jun Ho Jang,Kyung Tae Kim,Ji Hoon Chung,Donghyeon Oh,Jung Sug Hong,Byung Soo Oh,Choul Kim,Young Hwan Min,Hui-Youn Shin,Myeong-Soo Chang,Zhipeng Wang,Sang Ho Oh,Hyacinthe Randriamahazaka,Ki Tae Nam","doi":"10.1021/acscatal.6c04537","DOIUrl":"https://doi.org/10.1021/acscatal.6c04537","url":null,"abstract":"Abstract Water oxidation in proton exchange membrane water electrolysis (PEMWE) uses IrO2 nanoparticles supported on corrosion-resistant TiO2. However, the low conductivity of TiO2 imposes electronic transport limitations that necessitate high Ir loadings for effective catalysis. Here, we present a catalyst design strategy that couples a heavily V-doped TiO2 support with high-density Ir single atoms, enabling water oxidation at minimal Ir loading. In this design, Ti-site-substituted V provides n-type doping, and selective V leaching creates cation vacancies that anchor Ir as isolated atoms. TEM with convolutional neural network (CNN)-based analysis shows Ir single-atom density increases with V content, accompanied by lower charge-transfer resistance and higher Ir-specific activity. The density functional theory indicates that cation-site Ir introduces a midgap state below V 3d levels and shifts neighboring V 3d orbitals toward the Fermi level. Ir1/V-TiO2 achieves 1480 A gIr–1 at 1.55 V vs RHE (1.3 wt % Ir) and demonstrates device-level PEMWE operation at an Ir loading as low as 0.027 mgIr cm–2.","PeriodicalId":9,"journal":{"name":"ACS Catalysis ","volume":"39 1","pages":""},"PeriodicalIF":12.9,"publicationDate":"2026-10-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149209936","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 Cu Valence Engineering in CuInS2 Enables Selective Photocatalytic CO2-to-C2H4 Conversion CuInS2中的不对称Cu价工程实现了选择性光催化co2到c2h4的转化
IF 13.6 1区 化学
ACS Catalysis Pub Date : 2026-10-16 Epub Date: 2026-09-24 DOI: 10.1021/acscatal.6c04590
Hang Zhao, Renjie Bi, Mingdong Ju, Xun Zhu, Rong Chen, Qiang Liao
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