Chem Catalysis最新文献_第8页

Cooperative effects associated with high electrolyte concentrations in driving the conversion of CO2 to C2H4 on copper 高浓度电解质在推动铜上 CO2 向 C2H4 转化过程中的协同效应

IF 9.4

Chem Catalysis Pub Date : 2025-04-04 DOI: 10.1016/j.checat.2025.101338

Shaoyang Lin, Yuval Fishler, Soonho Kwon, Annette E. Böhme, Weixuan Nie, Matthias H. Richter, Moon Young Yang, Jesse E. Matthews, Zachery W.B. Iton, Brian C. Lee, Thomas F. Jaramillo, Harry A. Atwater, William A. Goddard, Wilson A. Smith, Kimberly A. See

{"title":"Cooperative effects associated with high electrolyte concentrations in driving the conversion of CO2 to C2H4 on copper","authors":"Shaoyang Lin, Yuval Fishler, Soonho Kwon, Annette E. Böhme, Weixuan Nie, Matthias H. Richter, Moon Young Yang, Jesse E. Matthews, Zachery W.B. Iton, Brian C. Lee, Thomas F. Jaramillo, Harry A. Atwater, William A. Goddard, Wilson A. Smith, Kimberly A. See","doi":"10.1016/j.checat.2025.101338","DOIUrl":"https://doi.org/10.1016/j.checat.2025.101338","url":null,"abstract":"Compared to a conventional electrolyte concentration of 1 M HCOOK, the use of a highly concentrated 7.1 M HCOOK electrolyte increases the Faradaic efficiency (FE) ratio of C2H4/CO from 2.2 ± 0.3 to 18.3 ± 4.8 at −1.08 V vs. reversible hydrogen electrode (RHE) on a Cu gas-diffusion electrode. Based on electrochemical analysis and ab initio molecular dynamics (AIMD) simulation, the identity and concentration of the cation and anion play more important roles in controlling the CO2R reaction pathway than the bulk CO2 solubility and the bulk pH of electrolytes. In situ attenuated reflectance surface enhanced infrared absorption spectroscopy (ATR-SEIRAS) suggests that, unlike 1 M HCOOK, the ∗CO-bridge-binding mode on Cu is dominant in 7.1 M HCOOK electrolyte, which potentially results in less CO release and higher yield of C2H4. This study demonstrates that although we can tailor the electrolyte composition to shift product selectivity, the factors that control the product selectivity are numerous and cannot be distilled down into one correlated property-reactivity relationship.","PeriodicalId":53121,"journal":{"name":"Chem Catalysis","volume":"1 1","pages":""},"PeriodicalIF":9.4,"publicationDate":"2025-04-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143776200","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Suppressing lattice oxygen oxidation in ruthenium oxide via equivalent substitution for sustainable oxygen evolution reaction in PEMWEs 通过等效取代持续析氧反应抑制氧化钌中的晶格氧氧化

IF 9.4

Chem Catalysis Pub Date : 2025-04-03 DOI: 10.1016/j.checat.2025.101335

Xiaojie Chen, Rongpeng Ma, Wenqi Jia, Xuejie Cao, Jinyang Zhang, Fangyi Cheng, Lifang Jiao

{"title":"Suppressing lattice oxygen oxidation in ruthenium oxide via equivalent substitution for sustainable oxygen evolution reaction in PEMWEs","authors":"Xiaojie Chen, Rongpeng Ma, Wenqi Jia, Xuejie Cao, Jinyang Zhang, Fangyi Cheng, Lifang Jiao","doi":"10.1016/j.checat.2025.101335","DOIUrl":"https://doi.org/10.1016/j.checat.2025.101335","url":null,"abstract":"Developing cost-effective Ru-based electrocatalysts for the acidic oxygen evolution reaction (OER) is crucial for proton-exchange membrane water electrolyzers (PEMWEs). However, the prominent lattice-oxygen-mediated mechanism (LOM) at high oxidative potential leads to crystal destruction and poor operational stability for RuO2. Here, we report that introducing equivalent Ti4+ into RuO2 can significantly suppress the oxidation of lattice oxygen. Spectroscopic and theoretical results demonstrate that Ti4+ incorporation not only decreases the LOM ratio by weakening Ru–O bond covalency but also suppresses the dynamic activation of lattice oxygen at high oxidative bias by inhibiting Ru–O bond contraction. Potential-resolved differential electrochemical mass spectrometry (DEMS) verified the decreased LOM ratio (from 53.45% to 5% at 1.8 V) after Ti4+ incorporation. The equivalent-Ti4+-substituted RuO2 not only exhibits an extended operation time of over 500 h at 100 mA cm−2 but also withstands fluctuating voltage input (1.5–1.8 V) for 120 h in PEMWEs.","PeriodicalId":53121,"journal":{"name":"Chem Catalysis","volume":"73 1","pages":""},"PeriodicalIF":9.4,"publicationDate":"2025-04-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143766700","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

SubTuner leverages physics-based modeling to complement AI in enzyme engineering toward non-native substrates SubTuner利用基于物理的建模来补充AI在酶工程对非天然底物

IF 9.4

Chem Catalysis Pub Date : 2025-03-28 DOI: 10.1016/j.checat.2025.101334

Qianzhen Shao, Asher C. Hollenbeak, Yaoyukun Jiang, Xinchun Ran, Brian O. Bachmann, Zhongyue J. Yang

{"title":"SubTuner leverages physics-based modeling to complement AI in enzyme engineering toward non-native substrates","authors":"Qianzhen Shao, Asher C. Hollenbeak, Yaoyukun Jiang, Xinchun Ran, Brian O. Bachmann, Zhongyue J. Yang","doi":"10.1016/j.checat.2025.101334","DOIUrl":"https://doi.org/10.1016/j.checat.2025.101334","url":null,"abstract":"We developed SubTuner, a physics-based computational tool that tackles the challenge of identifying enzyme mutants with enhanced activity for specified non-native substrates. To test the performance of SubTuner, we designed three tasks, all aiming to identify beneficial anion methyltransferase mutants for synthesis of non-native S-adenosyl-L-methionine analogs: first, in the conversion of ethyl iodide from a pool of 190 Arabidopsis thaliana Harmless to Ozone Layer 1 (AtHOL1) single-point mutants for an initial test of accuracy and speed; second, of ethyl, n-propyl, cyclopropylmethyl, and phenethyl iodides from a pool of 600 Aspergillus clavatus methyltransferase multi-point mutants for a test of generalizability; and, eventually, of bulkier substrates for AtHOL1 combined with experimental characterization for a test of a priori predictivity. All tests demonstrated SubTuner’s ability to accelerate enzyme engineering for non-native substrates, superior to existing bioinformatics and machine-learning-based tools. SubTuner, with its physical hypothesis, quantitative accuracy, and mechanism-informing ability, holds significant potential to aid enzyme engineering for substrate scope expansion.","PeriodicalId":53121,"journal":{"name":"Chem Catalysis","volume":"36 1","pages":""},"PeriodicalIF":9.4,"publicationDate":"2025-03-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143723935","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Enantioselective palladium-catalyzed α-arylation of primary alkylamines 钯催化伯烷基胺的α-芳基化反应

IF 9.4

Chem Catalysis Pub Date : 2025-03-28 DOI: 10.1016/j.checat.2025.101331

Zoutao Wang, Shuai Guo, Ziyang Shen, Ran Wei, Ruijie Jiang, Guodu Liu, Qinghai Zhou, Kang Du, Wenjun Tang

引用次数: 0

Recent progress in understanding mechanism of electrochemical oxygen evolution reaction via operando/in situ characterizations 利用operando/原位表征了解电化学析氧反应机理的最新进展

IF 9.4

Chem Catalysis Pub Date : 2025-03-28 DOI: 10.1016/j.checat.2025.101332

Rashid Mehmood, Fuxiang Zhang

{"title":"Recent progress in understanding mechanism of electrochemical oxygen evolution reaction via operando/in situ characterizations","authors":"Rashid Mehmood, Fuxiang Zhang","doi":"10.1016/j.checat.2025.101332","DOIUrl":"https://doi.org/10.1016/j.checat.2025.101332","url":null,"abstract":"Understanding the mechanism of the oxygen evolution reaction (OER) represents a bottleneck in designing efficient energy storage schemes based on water splitting. However, identifying the mechanism experimentally has proven a grand challenge. This could be due to the diverse nature of OER intermediates. Recent progress in operando/in situ characterizations has provided an unprecedented understanding of the OER mechanisms concerning active site identification, as well as other OER mechanisms. On this basis, we offer a comprehensive discussion on experimental evidence for identifying OER intermediates experimentally, aligning them with theoretical calculations in designing future green energy systems. Finally, some perspectives that are anticipated to be beneficial to addressing the current challenges in operando/in situ monitoring of active site identification and understanding of the underlying mechanisms of OER electrocatalysts are presented. This review aims to provide new insights into the rational design of OER catalytic materials and offers a complete understanding of OER mechanisms.","PeriodicalId":53121,"journal":{"name":"Chem Catalysis","volume":"64 1","pages":""},"PeriodicalIF":9.4,"publicationDate":"2025-03-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143723934","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Stretchable asymmetric dual-atom Cu(I) electrocatalyst for enhanced CO2 reduction to C2+ products 可拉伸的非对称双原子Cu(I)电催化剂，用于增强CO2还原为C2+产物

IF 9.4

Chem Catalysis Pub Date : 2025-03-24 DOI: 10.1016/j.checat.2025.101327

Ran Bu, Shuaiqiang Jia, YuHou Pei, Danyun Xu, Di Li, Qidong Ruan, Yuting Liu, Pengfei Mu, Enqing Gao, Yingying Lu, Bing Zhang

{"title":"Stretchable asymmetric dual-atom Cu(I) electrocatalyst for enhanced CO2 reduction to C2+ products","authors":"Ran Bu, Shuaiqiang Jia, YuHou Pei, Danyun Xu, Di Li, Qidong Ruan, Yuting Liu, Pengfei Mu, Enqing Gao, Yingying Lu, Bing Zhang","doi":"10.1016/j.checat.2025.101327","DOIUrl":"https://doi.org/10.1016/j.checat.2025.101327","url":null,"abstract":"Constructing precise catalytic sites and local microenvironments to achieve electrochemical CO2 conversion to valuable C2+ products remains a great challenge. Here, a porous crystalline covalent organic framework (COF) containing Br-bridged dual single-atom Cu(I) sites with an asymmetric coordination environment was rationally designed and confirmed by combining single-crystal X-ray diffraction and X-ray absorption fine structure analyses. The as-synthesized COF-based single-atom Cu catalyst exhibits exceptional performance in the electrochemical CO2 reduction reaction to C2+ products, which surpasses that of most previously reported single-atom catalysts with defined coordination structures. Operando Raman spectroscopy, theoretical calculations, and control experiments were employed to verify the mechanism behind the effectiveness of the catalyst. These investigations suggest that the flexible, asymmetrically coordinated dual-atom Cu(I) sites can lower the energy barrier for generating ∗CO and ∗COCHO intermediates, thereby promoting the formation of C–C bonds necessary for C2+ products.","PeriodicalId":53121,"journal":{"name":"Chem Catalysis","volume":"15 1","pages":""},"PeriodicalIF":9.4,"publicationDate":"2025-03-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143677973","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Strain relaxation enhances ammonia electrosynthesis from nitrate on Cu/CuAu core/shell nanocrystals with ordered intermetallic layers 应变弛豫增强了Cu/CuAu核/壳纳米晶体上有序金属间层的氨电合成

IF 9.4

Chem Catalysis Pub Date : 2025-03-24 DOI: 10.1016/j.checat.2025.101328

Qiang Gao, Bingqing Yao, Yuanqi Liu, Lei Shi, Zihao Yan, Libang Xu, Qian He, Huiyuan Zhu

{"title":"Strain relaxation enhances ammonia electrosynthesis from nitrate on Cu/CuAu core/shell nanocrystals with ordered intermetallic layers","authors":"Qiang Gao, Bingqing Yao, Yuanqi Liu, Lei Shi, Zihao Yan, Libang Xu, Qian He, Huiyuan Zhu","doi":"10.1016/j.checat.2025.101328","DOIUrl":"https://doi.org/10.1016/j.checat.2025.101328","url":null,"abstract":"Recycling ammonia (NH3) via the electrocatalytic nitrate reduction reaction (NO3RR) offers a sustainable, energy-efficient solution for closing the nitrogen cycle while simultaneously treating nitrate-rich wastewater. In this work, we synthesized core/shell Cu/CuAu nanocubes with precisely controlled ordered intermetallic layers using a facile seed-mediated method. The compressive surface strain of the nanocrystals was finely regulated by adjusting the layers of the CuAu shell. Specifically, the strain-relaxed Cu/CuAu catalysts exhibit high NO3RR performance for NH3 production, achieving a Faradic efficiency of 89.9% at −0.5 V vs. the reversible hydrogen electrode (RHE) and an exceedingly high yield rate of 11.3 mol h−1 g−1 at −0.6 V vs. RHE. Furthermore, Cu/CuAu catalysts show catalytic stability over 10 consecutive cycles and 12-h electrolysis. This atomic-level control of thickness allows precise tuning of the intrinsic strain to optimize catalytic reactivity, offering a promising strategy to enhance the performance of electrocatalytic ammonia synthesis.","PeriodicalId":53121,"journal":{"name":"Chem Catalysis","volume":"16 1","pages":""},"PeriodicalIF":9.4,"publicationDate":"2025-03-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143677974","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Cation-coupled electron transfer in the oxygen reduction reaction and beyond 氧还原反应中的阳离子偶联电子转移及其他

IF 9.4

Chem Catalysis Pub Date : 2025-03-20 DOI: 10.1016/j.checat.2025.101304

Yifei Xu, Bingjun Xu

引用次数: 0

Scaling solar hydrogen peroxide 太阳能过氧化氢垢

IF 9.4

Chem Catalysis Pub Date : 2025-03-20 DOI: 10.1016/j.checat.2025.101333

Emily H. Edwards

引用次数: 0

A Pt-Fe-Pt heterotrimer for selective hydrogenation of crotonaldehyde 用于巴豆醛选择性加氢的Pt-Fe-Pt异源三聚体