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Electrochemical engineering to tune active sites in alloy catalysts via surface-atom knockout 通过表面原子敲除调整合金催化剂活性位点的电化学工程
IF 9.4
Chem Catalysis Pub Date : 2024-05-16 DOI: 10.1016/j.checat.2024.100988
Xiaoyu Zhang, You Han
{"title":"Electrochemical engineering to tune active sites in alloy catalysts via surface-atom knockout","authors":"Xiaoyu Zhang, You Han","doi":"10.1016/j.checat.2024.100988","DOIUrl":"https://doi.org/10.1016/j.checat.2024.100988","url":null,"abstract":"<p>In a recent issue of <em>Proceedings of the National Academy of Sciences</em>, Qiu and co-workers report a novel strategy for promoting the precise exposure of active sites in alloy catalysts via surface-atom knockout enabled by electrochemical reaction. This is undoubtedly an important milestone for the design and synthesis of alloy catalysts and beyond.</p>","PeriodicalId":53121,"journal":{"name":"Chem Catalysis","volume":null,"pages":null},"PeriodicalIF":9.4,"publicationDate":"2024-05-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"140949916","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
Exchange energy pathway for water oxidation via multi-element synergy in electrocatalysts 通过电催化剂中的多元素协同作用实现水氧化的交换能途径
IF 9.4
Chem Catalysis Pub Date : 2024-05-16 DOI: 10.1016/j.checat.2024.100986
Jayaraman Theerthagiri, Kasiviswanathan Muthusamy, Myong Yong Choi
{"title":"Exchange energy pathway for water oxidation via multi-element synergy in electrocatalysts","authors":"Jayaraman Theerthagiri, Kasiviswanathan Muthusamy, Myong Yong Choi","doi":"10.1016/j.checat.2024.100986","DOIUrl":"https://doi.org/10.1016/j.checat.2024.100986","url":null,"abstract":"<p>In this issue of <em>Chem Catalysis</em>, Linjuan Zhang and co-workers present Fe/Ni mixed elements as efficient electrocatalysts for improving the oxygen evolution reaction (OER). Their study reveals a synergistic Ni-Fe effect that enhances the OER via exchange energy-gain mechanisms.</p>","PeriodicalId":53121,"journal":{"name":"Chem Catalysis","volume":null,"pages":null},"PeriodicalIF":9.4,"publicationDate":"2024-05-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"140949931","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
Electro-positive thinking: Catalytic dinitrogen reduction using electropositive metals 电正思维：使用电正性金属催化二氮还原
IF 9.4
Chem Catalysis Pub Date : 2024-05-16 DOI: 10.1016/j.checat.2024.101003
Samuel M. Bhutto, Louise A. Berben
{"title":"Electro-positive thinking: Catalytic dinitrogen reduction using electropositive metals","authors":"Samuel M. Bhutto, Louise A. Berben","doi":"10.1016/j.checat.2024.101003","DOIUrl":"https://doi.org/10.1016/j.checat.2024.101003","url":null,"abstract":"<p>In this issue of <em>Chem Catalysis</em>, Arnold and co-workers describe Lewis acidic f- and d-block metal complexes that are catalysts for the conversion of N<sub>2</sub> into secondary and tertiary amines. The origins of the remarkable selectivity and tunability of product formation are discussed in relation to molecular structure.</p>","PeriodicalId":53121,"journal":{"name":"Chem Catalysis","volume":null,"pages":null},"PeriodicalIF":9.4,"publicationDate":"2024-05-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"140949946","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
Synthesis of C5-boryl indoles via a borane-catalyzed cascade 通过硼烷催化级联合成 C5-硼吲哚
IF 9.4
Chem Catalysis Pub Date : 2024-05-16 DOI: 10.1016/j.checat.2024.101005
Sophia Moreen Gloria, Alexander P. Pulis
{"title":"Synthesis of C5-boryl indoles via a borane-catalyzed cascade","authors":"Sophia Moreen Gloria, Alexander P. Pulis","doi":"10.1016/j.checat.2024.101005","DOIUrl":"https://doi.org/10.1016/j.checat.2024.101005","url":null,"abstract":"<p>In this issue of <em>Chem Catalysis</em>, Zhang and co-workers report a new method for synthesizing C5-boryl indoles via a B(C<sub>6</sub>F<sub>5</sub>)<sub>3</sub>-catalyzed C–H borylation.</p>","PeriodicalId":53121,"journal":{"name":"Chem Catalysis","volume":null,"pages":null},"PeriodicalIF":9.4,"publicationDate":"2024-05-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"140949881","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
Dynamic evolution of single-atom Rh site and MoS2 support for hydrogen evolution 单原子 Rh 位点和 MoS2 支持氢进化的动态演化
IF 9.4
Chem Catalysis Pub Date : 2024-05-16 DOI: 10.1016/j.checat.2024.101002
Fei-Yang Yu, Hao Sun, Hua-Qiao Tan, Yang-Guang Li, Shuit-Tong Lee, Zhen-Hui Kang
{"title":"Dynamic evolution of single-atom Rh site and MoS2 support for hydrogen evolution","authors":"Fei-Yang Yu, Hao Sun, Hua-Qiao Tan, Yang-Guang Li, Shuit-Tong Lee, Zhen-Hui Kang","doi":"10.1016/j.checat.2024.101002","DOIUrl":"https://doi.org/10.1016/j.checat.2024.101002","url":null,"abstract":"<p>The dynamic evolution and structure-performance relationships of single-atom catalysts (SACs) under operating conditions are one of the most concerned hotspots at present. Here, we employed Anderson-type polyoxometalates as a precursor to prepare the SAC Rh-MoS<sub>2</sub>, which shows excellent hydrogen evolution reaction (HER) performance with a mass activity of 4.26 A mg<sup>−1</sup> at 100 mV. Such a result is much better than that of 20% Pt/C. Extensive experimental characterization combined with density functional theory (DFT) calculations suggest that the active site undergoes a dynamic evolution from Rh-S to Rh-S/O, while at the same time, the support is transformed from 1T MoS<sub>2</sub> to 1T-2H MoS<sub>2</sub>. It is this dynamic evolution of the catalyst structure that causes a series of changes in the activity, and eventually, a balance between catalytic activity and stability is achieved. This work offers a good research demonstration of the dynamic evolution of SACs under operating conditions and provides a new perspective on the design of SACs.</p>","PeriodicalId":53121,"journal":{"name":"Chem Catalysis","volume":null,"pages":null},"PeriodicalIF":9.4,"publicationDate":"2024-05-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"140949867","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
Ligands benefit nanocatalysis 配体有利于纳米催化
IF 9.4
Chem Catalysis Pub Date : 2024-05-16 DOI: 10.1016/j.checat.2024.100996
Rui Xu, Lingshan Liao, Shihui Zou, Linfang Lu
{"title":"Ligands benefit nanocatalysis","authors":"Rui Xu, Lingshan Liao, Shihui Zou, Linfang Lu","doi":"10.1016/j.checat.2024.100996","DOIUrl":"https://doi.org/10.1016/j.checat.2024.100996","url":null,"abstract":"<p>The ligands on the surface of nanocatalysts are generally considered to be removed before catalysis application. However, in the latest issue of <em>ACS Catalysis</em>, Abruña and co-workers have found that retaining ligands on nanocatalysts can promote the fuel cell performance by improving the film uniformity of the cathode layer.</p>","PeriodicalId":53121,"journal":{"name":"Chem Catalysis","volume":null,"pages":null},"PeriodicalIF":9.4,"publicationDate":"2024-05-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"140949886","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
Hydrogen peroxide-mediated tandem catalysis for electrifying chemical synthesis 过氧化氢介导的串联催化使化学合成电气化
IF 9.4
Chem Catalysis Pub Date : 2024-05-09 DOI: 10.1016/j.checat.2024.100997
Xinxin Li, Kaijie Wu, Sheng Chen, Bo Yuan, Jiaxuan Wang, Cheng Tang, Qiang Zhang
{"title":"Hydrogen peroxide-mediated tandem catalysis for electrifying chemical synthesis","authors":"Xinxin Li, Kaijie Wu, Sheng Chen, Bo Yuan, Jiaxuan Wang, Cheng Tang, Qiang Zhang","doi":"10.1016/j.checat.2024.100997","DOIUrl":"https://doi.org/10.1016/j.checat.2024.100997","url":null,"abstract":"<p>Hydrogen peroxide (H<sub>2</sub>O<sub>2</sub>) has gained widespread utility in green chemical synthesis. H<sub>2</sub>O<sub>2</sub>-mediated tandem catalysis combines the two-electron oxygen reduction reaction (2e<sup>–</sup> ORR) and organics oxidation, which enables the <em>in situ</em> conversion of organics and the <em>in situ</em> production/utilization of H<sub>2</sub>O<sub>2</sub> within the same system. This method not only reduces the cost of H<sub>2</sub>O<sub>2</sub> purification and transportation but also promotes in-depth research in the renewable manufacturing of high-value-added chemicals. As such, this review will encompass the critical initial discoveries guiding H<sub>2</sub>O<sub>2</sub>-mediated tandem catalysis and discuss the core contents such as the tandem mechanism, applicable substrates, and electrolysis modes. Design principles and research efforts are highlighted from the aspects of bifunctional catalyst design, multistep catalysis matching, reactor integration and innovation, and system expansion. Finally, we provide personal perspectives on the challenges in this burgeoning field and the strategies that can be employed to render tandem processes practically feasible.</p>","PeriodicalId":53121,"journal":{"name":"Chem Catalysis","volume":null,"pages":null},"PeriodicalIF":9.4,"publicationDate":"2024-05-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"140895854","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
A versatile cobalt catalyst for highly enantioselective hydrogenation of carbonyl compounds 用于羰基化合物高对映选择性氢化的多功能钴催化剂
IF 9.4
Chem Catalysis Pub Date : 2024-05-09 DOI: 10.1016/j.checat.2024.100999
Xiaoyong Du, Yao Zhang, Tilong Yang, Ye Xiao, Jian He, Lung Wa Chung, Gen-Qiang Chen, Xumu Zhang
{"title":"A versatile cobalt catalyst for highly enantioselective hydrogenation of carbonyl compounds","authors":"Xiaoyong Du, Yao Zhang, Tilong Yang, Ye Xiao, Jian He, Lung Wa Chung, Gen-Qiang Chen, Xumu Zhang","doi":"10.1016/j.checat.2024.100999","DOIUrl":"https://doi.org/10.1016/j.checat.2024.100999","url":null,"abstract":"<p>A general base metal catalytic system for asymmetric hydrogenation of different types of carbonyl compounds has rarely been reported. Here, we describe the development of a versatile Co/BPE system for the asymmetric hydrogenation of both α-ketoamides and aryl alkyl ketones that enable fast access to various chiral α-hydroxy amides and secondary alcohols in excellent yields and enantioselectivities (up to 98% yield and 99:1 enantiomeric ratio [er]) under base- and additive-free conditions. More importantly, cobalt-catalyzed diastereo- and enantioselective hydrogenation of α-substituted β-ketoamides has been achieved for the first time under a dynamic kinetic resolution (DKR) process using the same system. The synthetic potential has been demonstrated through reaction scale-up, product derivatization, and synthesis of various key intermediates for chiral drugs. Mechanistic studies support a new Co(II) instead of a Co(II)/Co(0) catalytic cycle involving hydride transfer and H<sub>2</sub> splitting processes, in which the oxidation state of cobalt remains unchanged.</p>","PeriodicalId":53121,"journal":{"name":"Chem Catalysis","volume":null,"pages":null},"PeriodicalIF":9.4,"publicationDate":"2024-05-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"140895942","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
Accelerated analysis of the electrochemical production route for biomass-derived adiponitrile 加速分析生物质衍生己二腈的电化学生产路线
IF 9.4
Chem Catalysis Pub Date : 2024-05-08 DOI: 10.1016/j.checat.2024.100998
Ricardo Mathison, Elina Rani, Meera K. Patel, Antonio Lopez Cerrato, Casey K. Bloomquist, Miguel A. Modestino
{"title":"Accelerated analysis of the electrochemical production route for biomass-derived adiponitrile","authors":"Ricardo Mathison, Elina Rani, Meera K. Patel, Antonio Lopez Cerrato, Casey K. Bloomquist, Miguel A. Modestino","doi":"10.1016/j.checat.2024.100998","DOIUrl":"https://doi.org/10.1016/j.checat.2024.100998","url":null,"abstract":"<p>The electrochemical transformation of biomass feedstocks offers a promising route for the sustainable production of fuels and chemicals, enhancing integration with renewable energy sources. Adiponitrile, a key intermediate in nylon 6,6 production, is mainly produced through thermochemical processes or methods relying on fossil fuel feedstocks. Alternatively, it can be produced through the Kolbe coupling of biomass-derived 3-cyanopropanoic acid, with its practical implementation hinging on understanding and controlling factors that dictate reaction selectivity. In this study, we establish relationships between electrolyte composition, electrochemical conditions, and performance metrics in this approach, achieving a maximum faradic efficiency of 40% toward adiponitrile at current densities up to 500 mA cm<sup>−2</sup>. Implementing a semi-autonomous high-throughput electrochemical workflow, we tested hundreds of reaction conditions, accelerating the exploration of reaction parameters. Limitations and guidelines obtained from this study apply to a range of electrochemical decarboxylation reactions, and the accelerated research approach shows potential for speeding up the development of sustainable electrochemical processes.</p>","PeriodicalId":53121,"journal":{"name":"Chem Catalysis","volume":null,"pages":null},"PeriodicalIF":9.4,"publicationDate":"2024-05-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"140888533","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
Ce-promoted Ni-NiO small ensemble constrained in an MgO catalyst for efficient hydrogen production through NH3 decomposition 氧化镁催化剂中的铈促进 Ni-NiO 小集合，通过分解 NH3 高效制氢
IF 9.4
Chem Catalysis Pub Date : 2024-05-08 DOI: 10.1016/j.checat.2024.101000
Zhaohua Wang, Xuan Tang, Maolin Wang, Yao Xu, Xuetao Qin, Lihui Zhou, Mi Peng, Sheng Dai, Ding Ma
{"title":"Ce-promoted Ni-NiO small ensemble constrained in an MgO catalyst for efficient hydrogen production through NH3 decomposition","authors":"Zhaohua Wang, Xuan Tang, Maolin Wang, Yao Xu, Xuetao Qin, Lihui Zhou, Mi Peng, Sheng Dai, Ding Ma","doi":"10.1016/j.checat.2024.101000","DOIUrl":"https://doi.org/10.1016/j.checat.2024.101000","url":null,"abstract":"<p>Ammonia is recognized for its potential in hydrogen storage and transportation. Among methods for hydrogen production from ammonia, catalytic decomposition stands out, and developing economical alternatives to noble metal catalysts like ruthenium (Ru) is crucial. Here, we report an exsolution strategy to obtain a size-constrained Ni<sup>0</sup>-NiO small ensemble on MgO that outperforms bare Ni single atoms and particles in ammonia decomposition. Adding Ce to the NiMg catalyst significantly enhances activity, doubling the hydrogen production rate to 92 mmol<sub>H2</sub> g<sub>cat</sub><sup>−1</sup> min<sup>−1</sup> at 550°C, surpassing most Ni-based catalysts. Characterization reveals the role of cerium in forming active Ni<sup>0</sup>-NiO ensembles by occupying specific sites on MgO. Cerium (Ce) also affects hydrogen and ammonia adsorption and alters reaction pathways. Our work highlights the structure control of transition metal sites and the promotion mechanism of rare-earth elements for ammonia conversion and hydrogen production reaction.</p>","PeriodicalId":53121,"journal":{"name":"Chem Catalysis","volume":null,"pages":null},"PeriodicalIF":9.4,"publicationDate":"2024-05-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"140888719","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
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