Chem Catalysis最新文献

Repurposing type I aldolase for stereospecific radical coupling with light 将Ⅰ型醛缩酶重新用于光立体特异性自由基偶联

IF 9.4

Chem Catalysis Pub Date : 2024-11-21 DOI: 10.1016/j.checat.2024.101191

Jinhai Yu, Yingdi Hao, Xiaoqiang Huang

引用次数: 0

Efficient nitrate-to-ammonia conversion for circular nitrogen economy 将硝酸盐高效转化为氨气，实现循环氮经济

IF 9.4

Chem Catalysis Pub Date : 2024-11-21 DOI: 10.1016/j.checat.2024.101193

Gabriel F. Costa, Raphael Nagao

引用次数: 0

Enhanced electrochemical reduction of CO2 to CO by ZnO nanorods enriched with oxygen vacancies 富含氧空位的氧化锌纳米棒增强了将 CO2 还原成 CO 的电化学过程

IF 9.4

Chem Catalysis Pub Date : 2024-11-21 DOI: 10.1016/j.checat.2024.101192

Zhongnan Ling, Yaoyu Yin, Xinchen Kang, Xianliang Li, Ran Duan, Shuming Zhou, Huanyan Liu, Guang Mo, Zhongjun Chen, Xuehui Wu, Rongjuan Feng, Zhonghua Wu, Buxing Han, Xueqing Xing

{"title":"Enhanced electrochemical reduction of CO2 to CO by ZnO nanorods enriched with oxygen vacancies","authors":"Zhongnan Ling, Yaoyu Yin, Xinchen Kang, Xianliang Li, Ran Duan, Shuming Zhou, Huanyan Liu, Guang Mo, Zhongjun Chen, Xuehui Wu, Rongjuan Feng, Zhonghua Wu, Buxing Han, Xueqing Xing","doi":"10.1016/j.checat.2024.101192","DOIUrl":"https://doi.org/10.1016/j.checat.2024.101192","url":null,"abstract":"The efficiency of converting CO2 to other valuable chemicals via the electrochemical reduction pathway depends on the electrocatalyst. In this work, an approach to prepare the ZnO catalysts used for the CO2 electrocatalytic reduction was proposed, aiming at regulating the oxygen vacancy concentration in ZnO nanorods by changing the heat treatment temperature. The results show that the faradaic efficiency of CO2 reduction to CO is significantly improved. An unprecedented faradaic efficiency of 98.3% and a current density of 786.56 mA cm−2 were achieved using the ZnO catalyst heat treated at 500°C. It is revealed that the oxygen vacancy concentration, combined with density functional theory, can improve the performance of the ZnO electrocatalytic reduction of carbon dioxide (CO2RR) by accelerating the activation of CO2 molecules and reducing the energy barrier of CO formation. This work is helpful for the development of robust and efficient ZnO catalysts and their application in the CO2RR.","PeriodicalId":53121,"journal":{"name":"Chem Catalysis","volume":"13 1","pages":""},"PeriodicalIF":9.4,"publicationDate":"2024-11-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142679028","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 effects on the alkaline oxygen reduction reaction 阳离子对碱性氧还原反应的影响

IF 9.4

Chem Catalysis Pub Date : 2024-11-21 DOI: 10.1016/j.checat.2024.101186

Yifan Zeng, Dongbo Li, Pengtao Xu

引用次数: 0

Mechanistic insights into the electrochemical oxidation of acetate at noble metals 贵金属醋酸盐电化学氧化的机理研究

IF 9.4

Chem Catalysis Pub Date : 2024-11-21 DOI: 10.1016/j.checat.2024.101190

Venkata Sai Sriram Mosali, Hanna Soucie, Xiong Peng, Ehsan Faegh, Matthew Elam, Ian Street, William E. Mustain

引用次数: 0

Cations in molecular electrochemical catalysis 分子电化学催化中的阳离子

IF 9.4

Chem Catalysis Pub Date : 2024-11-21 DOI: 10.1016/j.checat.2024.101195

Marc Robert

引用次数: 0

Hydrogen dissociation and CO2 activation in cascade CO2 fixation on PdIn/TiO2 catalyst PdIn/TiO2 催化剂上级联二氧化碳固定过程中的氢解离和二氧化碳活化

IF 9.4

Chem Catalysis Pub Date : 2024-11-21 DOI: 10.1016/j.checat.2024.101116

Leilei Zhou, Ying Wang, Yinze Yang, Liyan Zhang, Jingrong Li, Tingting Xiao, Peikai Luo, Xinluona Su, Haiyang Cheng, Fengyu Zhao

{"title":"Hydrogen dissociation and CO2 activation in cascade CO2 fixation on PdIn/TiO2 catalyst","authors":"Leilei Zhou, Ying Wang, Yinze Yang, Liyan Zhang, Jingrong Li, Tingting Xiao, Peikai Luo, Xinluona Su, Haiyang Cheng, Fengyu Zhao","doi":"10.1016/j.checat.2024.101116","DOIUrl":"https://doi.org/10.1016/j.checat.2024.101116","url":null,"abstract":"Reduction of CO2 emissions and conversion of CO2 to valuable chemicals is an urgent mission, as it is vital to the global environment and sustainable development. The activation of CO2 is always considered to be the key step for its transformation. Herein, we verified that the activation and dissociation behavior of H2 was the controlling step for CO2 reduction. PdIn alloy was an active center and played a pivotal role in CO2 hydrogenation to the methyl reagent of HCOO∗. H2 split to active Hδ− species on PdIn alloy sites. Strong nucleophilic Hδ− reacted with the CO2 adsorbed on oxygen defects to form ∗HCOO in situ. A high yield of up to 99% was achieved for the cascade fixation of CO2 to valuable amines. The new insights into the activation of CO2 and H2 and their contributions to CO2 conversion that we present will attract the attention of researchers in catalysis, synthesis, surface, and interface chemistry.","PeriodicalId":53121,"journal":{"name":"Chem Catalysis","volume":"81 1","pages":""},"PeriodicalIF":9.4,"publicationDate":"2024-11-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142679037","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

Radical-mediated regiodivergent C(sp3)–H functionalization of N-substituted indolines via enzymatic carbene transfer 通过酶促碳烯转移对 N-取代吲哚啉进行自由基介导的 C(sp3)-H 功能化

IF 9.4

Chem Catalysis Pub Date : 2024-11-21 DOI: 10.1016/j.checat.2024.101133

Bo M. Couture, Ru Cui, Jia-Min Chu, Zhuofan Shen, Sagar D. Khare, Yong Zhang, Rudi Fasan

{"title":"Radical-mediated regiodivergent C(sp3)–H functionalization of N-substituted indolines via enzymatic carbene transfer","authors":"Bo M. Couture, Ru Cui, Jia-Min Chu, Zhuofan Shen, Sagar D. Khare, Yong Zhang, Rudi Fasan","doi":"10.1016/j.checat.2024.101133","DOIUrl":"https://doi.org/10.1016/j.checat.2024.101133","url":null,"abstract":"Indolines are ubiquitous structural motifs occurring in pharmaceuticals and natural products. Here, we report a strategy for regio- and stereoselective C(sp3)–H functionalization of N-substituted indolines via carbene transfer chemistry mediated by engineered CYP119-based catalysts. These systems offer high enantioselectivity and high catalytic efficiency, as well as regiodivergent selectivity, furnishing an efficient and convenient route for diversification of these important scaffolds via direct C(sp3)–H functionalization. Selective functionalization of exocyclic C(sp3)–H bond in N-methyl indolines was also achieved, and a biocatalytic cascade combining enzyme-mediated α- and β-C(sp3)–H functionalization yielded a polycyclic indoline-containing motif found in drugs. Mechanistic and computational studies support a radical-mediated C–H functionalization pathway and provide insights into protein-mediated regiodivergent selectivity. Altogether, this work offers a direct and tunable strategy to access functionalized indolines as key building blocks for medicinal chemistry and natural product synthesis and provides first insights into the mechanism of P450-catalyzed C(sp3)–H carbene insertion.","PeriodicalId":53121,"journal":{"name":"Chem Catalysis","volume":"23 1","pages":""},"PeriodicalIF":9.4,"publicationDate":"2024-11-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142679038","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

Spatial effects define CO2 electrolysis systems 界定二氧化碳电解系统的空间效应

IF 9.4

Chem Catalysis Pub Date : 2024-11-21 DOI: 10.1016/j.checat.2024.101185

Siddhartha Subramanian, Hugo-Pieter Iglesias van Montfort, Thomas Burdyny

{"title":"Spatial effects define CO2 electrolysis systems","authors":"Siddhartha Subramanian, Hugo-Pieter Iglesias van Montfort, Thomas Burdyny","doi":"10.1016/j.checat.2024.101185","DOIUrl":"https://doi.org/10.1016/j.checat.2024.101185","url":null,"abstract":"CO2 electrolyzers show promise as a cleaner alternative to produce value-added chemicals. In the last decade, research has shifted from classifying CO2 reduction activity and selectivity as a catalytic property (zero-dimensional [0D]) to one that includes the complex interactions of gas, liquid, and solid species between the cathode and anode (1D). To scale CO2 electrolyzers, however, 2D and 3D spatial variations in product selectivity, activity, and stability arise due to the design of reactor components, as well as concentration variations of the reactants, intermediates, and products. Conventional “black-box” measurement protocols are then insufficient to characterize CO2 electrolyzers. Here, we discuss the critical multi-dimensional phenomena occurring inside these electrochemical systems, which impact the observed performance. Recent literature is used to demonstrate how a spatial perspective is essential for proper data interpretation, designing effective catalysts, and prolonging CO2 electrolyzer lifetimes. Researchers should then define CO2 electrolysis systems in multiple dimensions (2D and 3D).","PeriodicalId":53121,"journal":{"name":"Chem Catalysis","volume":"8 1","pages":""},"PeriodicalIF":9.4,"publicationDate":"2024-11-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142679029","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

Strong activity-based volcano-type relationship for dry reforming of methane through modulating Ni-CeO2 interaction over Ni/CeO2-SiO2 catalysts 通过调节 Ni/CeO2-SiO2 催化剂上 Ni-CeO2 的相互作用实现甲烷干转化的强活性火山型关系

IF 9.4

Chem Catalysis Pub Date : 2024-11-21 DOI: 10.1016/j.checat.2024.101189

Yufeng Li, Zhenwei Li, Nan Wang, Yajun Zha, Ke Zheng, Yuebing Xu, Bing Liu, Xiaohao Liu

{"title":"Strong activity-based volcano-type relationship for dry reforming of methane through modulating Ni-CeO2 interaction over Ni/CeO2-SiO2 catalysts","authors":"Yufeng Li, Zhenwei Li, Nan Wang, Yajun Zha, Ke Zheng, Yuebing Xu, Bing Liu, Xiaohao Liu","doi":"10.1016/j.checat.2024.101189","DOIUrl":"https://doi.org/10.1016/j.checat.2024.101189","url":null,"abstract":"The dry reforming of methane (DRM) reaction holds significance for efficient conversion of CH4 and CO2 into syngas for the subsequent production of premium fuels and high-value chemicals. However, catalyst deactivation is easily caused by carbon deposition over Ni-based catalysts. Here, we investigated the effects of ultrasmall CeO2 nano-islands on the DRM reaction and found a strong volcano-type relationship between CeO2 content and reaction activity over Ni/CeO2-SiO2 catalysts. A suitable CeO2 amount can only slightly suppress CH4 dissociation but largely promote carbon species elimination. More importantly, the presence of these CeO2 nano-islands positively affected the types and location of coke species by “carbon-phobic effect” and thus alleviated coverage of Ni active sites. As a result, a higher TOFCH4 was obtained by an increase of about 82% and a continuous 2,000-h run almost without any side reaction, and deactivation was achieved along with CO2 and CH4 conversions at about 96% and 92%, respectively.","PeriodicalId":53121,"journal":{"name":"Chem Catalysis","volume":"74 1","pages":""},"PeriodicalIF":9.4,"publicationDate":"2024-11-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142679030","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