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Heterogeneous olefin metathesis promotion using molecular hydrogen 利用分子氢促进非均相烯烃复分解
IF 9.4 Q1 CHEMISTRY, PHYSICAL Pub Date : 2026-02-05 DOI: 10.1016/j.checat.2025.101608
Dimitri Gatzios, Toghrul Azizli, Elena M. Meza Wynkoop, Stephen Stockton, Mia Chang, Matthew M. Montemore, Lucas D. Ellis
Supported metal oxide catalysts used for olefin metathesis suffer from low conversion of metal oxide precursors to metathesis-active metal oxo-alkylidenes, which has prompted recent efforts to enhance active site populations. In this work, we show that co-flowing H2 with olefins can significantly promote olefin metathesis activity on MoOx/SiO2 and WOx/SiO2 and can rapidly regenerate activity after poisoning with H2O vapor. Molecular H2 not only aids in surface oxygen removal to activate the metal oxide but also maintains steady-state metathesis activity up to 45-fold higher than with the reacting olefin alone. Our results suggest that the presence of H2 facilitates alkylidene active site regeneration via a Mo-hydride intermediate, significantly lowering the kinetic barrier for site formation compared with recently postulated silanol-facilitated activation mechanisms. Surprisingly, we show that even bulk MoO3 powder can be promoted by H2 co-flows into a metathesis-active catalyst. Further analysis is needed to fully understand these phenomena.
用于烯烃复分解的负载型金属氧化物催化剂存在金属氧化物前体转化为催化活性金属氧烷基烷烃转化率低的问题,这促使人们最近努力提高活性位点的数量。在这项工作中,我们发现H2与烯烃共流动可以显著促进烯烃在MoOx/SiO2和WOx/SiO2上的转化活性,并且在H2O蒸汽中毒后可以迅速恢复活性。H2分子不仅有助于去除表面氧以激活金属氧化物,而且还能保持比单独反应烯烃高45倍的稳态分解活性。我们的研究结果表明,与最近假设的硅醇促进活化机制相比,H2的存在有助于通过mo -氢化物中间体再生烷基烯活性位点,显著降低了位点形成的动力学屏障。令人惊讶的是,我们发现即使是大块的MoO3粉末也可以被H2共流促进成催化活性催化剂。要充分理解这些现象,还需要进一步的分析。
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引用次数: 0
A guide to performing CO2 electrolysis in zero-gap electrolyzers 在零间隙电解槽中进行二氧化碳电解的指南
IF 9.4 Q1 CHEMISTRY, PHYSICAL Pub Date : 2026-02-05 DOI: 10.1016/j.checat.2025.101630
Maxwell Goldman
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Maxwell Goldman received his PhD in corrosion science from the University of Western Ontario in 2019. He then conducted postdoctoral research on reactive carbon capture at the University of British Columbia (2019) before joining Twelve (2020) as a senior engineer. His current research interests include advancing electrochemical CO2 conversion for manufacturing fuels and chemicals.
下载:下载高清图片(559KB)下载:下载全尺寸图片马克斯韦尔·戈德曼于2019年获得西安大略大学腐蚀科学博士学位。2019年赴英属哥伦比亚大学进行活性碳捕集博士后研究,2020年加入十二元集团,任高级工程师。他目前的研究兴趣包括推进用于制造燃料和化学品的电化学二氧化碳转化。
{"title":"A guide to performing CO2 electrolysis in zero-gap electrolyzers","authors":"Maxwell Goldman","doi":"10.1016/j.checat.2025.101630","DOIUrl":"https://doi.org/10.1016/j.checat.2025.101630","url":null,"abstract":"<span><figure><span><img alt=\"\" height=\"302\" src=\"https://ars.els-cdn.com/content/image/1-s2.0-S2667109325003690-gr1.jpg\"/><ol><li><span><span>Download: <span>Download high-res image (559KB)</span></span></span></li><li><span><span>Download: <span>Download full-size image</span></span></span></li></ol></span></figure></span>Maxwell Goldman received his PhD in corrosion science from the University of Western Ontario in 2019. He then conducted postdoctoral research on reactive carbon capture at the University of British Columbia (2019) before joining Twelve (2020) as a senior engineer. His current research interests include advancing electrochemical CO<sub>2</sub> conversion for manufacturing fuels and chemicals.","PeriodicalId":53121,"journal":{"name":"Chem Catalysis","volume":"72 1","pages":""},"PeriodicalIF":9.4,"publicationDate":"2026-02-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146122520","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
Advances in photoelectrochemical nitrate reduction for solar ammonia synthesis 太阳能合成氨中硝酸盐的光电还原研究进展
IF 9.4 Q1 CHEMISTRY, PHYSICAL Pub Date : 2026-02-03 DOI: 10.1016/j.checat.2025.101600
Yanjie Fang, Yifan Gao, Mengjie Li, Yingke Wen, Bing Shan
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引用次数: 0
Photocatalytic carbonyl alkylative amination via direct C–H functionalization 通过直接C-H官能化光催化羰基烷基化胺化
IF 9.4 Q1 CHEMISTRY, PHYSICAL Pub Date : 2026-01-28 DOI: 10.1016/j.checat.2025.101582
Vaishnavi N. Nair, Madhu Sudan Manna, Tiffany A. Brisco, Joffrey Scriven, Simon De Kreijger, Ludovic Troian-Gautier, Uttam K. Tambar
{"title":"Photocatalytic carbonyl alkylative amination via direct C–H functionalization","authors":"Vaishnavi N. Nair, Madhu Sudan Manna, Tiffany A. Brisco, Joffrey Scriven, Simon De Kreijger, Ludovic Troian-Gautier, Uttam K. Tambar","doi":"10.1016/j.checat.2025.101582","DOIUrl":"https://doi.org/10.1016/j.checat.2025.101582","url":null,"abstract":"","PeriodicalId":53121,"journal":{"name":"Chem Catalysis","volume":"55 1 1","pages":""},"PeriodicalIF":9.4,"publicationDate":"2026-01-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146072648","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
Reconstructing a stable surface on pyrite-type iridium telluride to promote the oxygen evolution reaction in acid 在黄铁矿型碲化铱上重建稳定表面以促进酸中的析氧反应
IF 9.4 Q1 CHEMISTRY, PHYSICAL Pub Date : 2026-01-23 DOI: 10.1016/j.checat.2025.101580
Ran Wang, Xingzhu Liao, Jinzhen Huang, Xinghong Zhang, Xiaofeng Li, Xianjie Wang, Bo Song
Surface reconstruction is inevitable for oxygen evolution reaction (OER) electrocatalysts. Here, we report that pyrite-type iridium telluride (Ir3Te8) can undergo favorable surface reconstruction during the OER process in acid. Compared with a IrTe2 counterpart, the relatively weak Ir–Te bonds in Ir3Te8 facilitate the formation of a Ir3Te8/IrO2-TeO2 heterojunction. Strengthened orbital interaction between the reconstructed IrO2-TeO2 layer and Ir3Te8 optimizes the electronic structure to enhance the electrocatalytic activity. As a result, the reconstructed Ir3Te8 with a stable surface achieves a low overpotential of 467.8 mV at a current density of 1 A cm−2 and maintains stability over 1,000 h at 10 mA cm−2. Although surface reconstruction is inevitable, this work demonstrates that its positive impacts can be maximized through optimization of the structural characteristics of the initial iridium telluride polymorphs to customize the reconstruction process. This highlights a design strategy for advanced OER catalysts that operate in acidic environments, including Ir-based catalysts and beyond.
析氧反应(OER)电催化剂的表面重构是不可避免的。在这里,我们报道了黄铁矿型碲化铱(Ir3Te8)在酸的OER过程中可以进行良好的表面重建。与IrTe2相比,Ir3Te8中相对较弱的Ir-Te键有助于形成Ir3Te8/IrO2-TeO2异质结。重构的IrO2-TeO2层与Ir3Te8之间的轨道相互作用增强,优化了电子结构,提高了电催化活性。结果表明,具有稳定表面的重构Ir3Te8在1 a cm−2电流密度下获得了467.8 mV的低过电位,并在10 mA cm−2电流密度下保持了1,000 h以上的稳定性。虽然表面重建是不可避免的,但这项工作表明,通过优化初始碲化铱多晶的结构特征来定制重建过程,可以最大限度地发挥其积极影响。这突出了在酸性环境中工作的高级OER催化剂的设计策略,包括ir基催化剂和其他催化剂。
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引用次数: 0
A dual CO2 fixation cycle engineered in plants boosts growth and lipid synthesis 在植物中设计的双重二氧化碳固定循环促进生长和脂质合成
IF 9.4 Q1 CHEMISTRY, PHYSICAL Pub Date : 2026-01-15 DOI: 10.1016/j.checat.2025.101609
Daniel C. Volke, Pablo I. Nikel
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引用次数: 0
Generalizing reactivity for machine-learning potentials 概括机器学习电位的反应性
IF 9.4 Q1 CHEMISTRY, PHYSICAL Pub Date : 2026-01-15 DOI: 10.1016/j.checat.2025.101572
Hao Li
In a recent Nature Catalysis paper, Hu, Xie, and co-workers present an element-based machine-learning potential trained with REICO (random exploration via “imaginary chemicals” optimization). This strategy shifts training from structure catalogs to diverse elemental interactions, yielding a general, reactive potential that enables on-the-fly simulations and a path toward replacing density functional theory (DFT) for complex systems.
在Nature Catalysis最近的一篇论文中,Hu、Xie和同事们展示了一种基于元素的机器学习潜力,这种机器学习潜力是用REICO(通过“假想化学物质”优化进行随机探索)训练的。该策略将训练从结构目录转移到各种元素相互作用上,产生了一种通用的反应电位,可以进行动态模拟,并为复杂系统取代密度泛函理论(DFT)提供了一条途径。
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引用次数: 0
Stimulus-responsive catalysts offering selectable reaction pathways in methane oxidation 刺激反应催化剂在甲烷氧化中提供可选择的反应途径
IF 9.4 Q1 CHEMISTRY, PHYSICAL Pub Date : 2026-01-15 DOI: 10.1016/j.checat.2025.101626
Sachini D. Deshapriya, Jiewei Zheng, Ken Chiang, Torben Daeneke
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引用次数: 0
Mild methods for converting PVC and polyolefin mixed waste into fuel-range hydrocarbons 将聚氯乙烯和聚烯烃混合废物转化为燃料烃类的温和方法
IF 9.4 Q1 CHEMISTRY, PHYSICAL Pub Date : 2026-01-15 DOI: 10.1016/j.checat.2025.101631
Isabel Willis, Megan E. Fieser
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引用次数: 0
Break it to make it: Rewiring bacterial metabolism for the growth-coupled biosynthesis of xanthommatin animal pigments 打破它,使它:重新布线细菌代谢的生长偶联生物合成黄质动物色素
IF 9.4 Q1 CHEMISTRY, PHYSICAL Pub Date : 2026-01-15 DOI: 10.1016/j.checat.2025.101632
Jackson T. Calhoun, Shaun M.K. McKinnie
In a recent Nature Biotechnology article, Bushin et al. elegantly rewire the metabolic machinery of a genetically tractable bacterium to intertwine its survival with the production of an exogenously introduced specialized metabolite. This “growth-coupled biosynthesis” approach resulted in impressive gram-scale titers of ommochrome animal pigments with useful biomedical applications.
在《自然生物技术》最近的一篇文章中,Bushin等人优雅地重新连接了一种遗传易感细菌的代谢机制,使其生存与外源引入的专门代谢物的产生交织在一起。这种“生长耦合生物合成”方法产生了令人印象深刻的克级共色动物色素滴度,具有有用的生物医学应用。
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引用次数: 0
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Chem Catalysis
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