Chem Catalysis最新文献

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Operando fluorescence spectroscopy for evaluating the activity of fatty acid hydrogenation catalysts 荧光光谱法评价脂肪酸加氢催化剂的活性
IF 9.4
Chem Catalysis Pub Date : 2025-05-20 DOI: 10.1016/j.checat.2025.101390
Jelle W. Bos, P. Tim Prins, Joris C.L. Janssens, Ramon Oord, Thimo S. Jacobs, Robin Vogel, Matteo Monai, Eelco T.C. Vogt, Bert M. Weckhuysen
{"title":"Operando fluorescence spectroscopy for evaluating the activity of fatty acid hydrogenation catalysts","authors":"Jelle W. Bos, P. Tim Prins, Joris C.L. Janssens, Ramon Oord, Thimo S. Jacobs, Robin Vogel, Matteo Monai, Eelco T.C. Vogt, Bert M. Weckhuysen","doi":"10.1016/j.checat.2025.101390","DOIUrl":"https://doi.org/10.1016/j.checat.2025.101390","url":null,"abstract":"Here, we report for the first time on <em>operando</em> fluorescence spectroscopy for liquid-phase reaction monitoring at elevated temperature and pressure. We show that it is a powerful tool for studying the hydrogenation of branched unsaturated fatty acids with zeolite and palladium catalysts. During the reaction, fluorescent impurities reacted with the zeolite, leading to a redshift of the fluorescence spectrum, which could be suppressed by hydrogenation. A strong correlation was found between the redshift of the spectrum and the hydrogenation activity of the catalysts, which can be used as a proxy. We discovered that unsaturated fatty acids were not responsible for the redshift, but that it was likely caused by fluorophores reacting on the zeolite. Experiments using a model fluorophore showed that the feedstock fluorophores are likely polycyclic aromatic hydrocarbons. We believe that this tool can be used in industrial fatty acid hydrogenation reactors to predict the endpoint of the hydrogenation.","PeriodicalId":53121,"journal":{"name":"Chem Catalysis","volume":"234 1","pages":""},"PeriodicalIF":9.4,"publicationDate":"2025-05-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144097532","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
Differential pressure CO2 electrolysis opens the way for direct coupling to industrial processes 差压CO2电解为工业过程的直接耦合开辟了道路
IF 9.4
Chem Catalysis Pub Date : 2025-05-20 DOI: 10.1016/j.checat.2025.101393
Stephan Heuser, Lucas Hoof, Kevinjeorjios Pellumbi, Jan Niklas Oberndorf, Lennart Krämer, Dennis Blaudszun, Kai junge Puring, Michael Prokein, Nils Mölders, Andreas Kilzer, Marcus Petermann, Ulf-Peter Apfel
{"title":"Differential pressure CO2 electrolysis opens the way for direct coupling to industrial processes","authors":"Stephan Heuser, Lucas Hoof, Kevinjeorjios Pellumbi, Jan Niklas Oberndorf, Lennart Krämer, Dennis Blaudszun, Kai junge Puring, Michael Prokein, Nils Mölders, Andreas Kilzer, Marcus Petermann, Ulf-Peter Apfel","doi":"10.1016/j.checat.2025.101393","DOIUrl":"https://doi.org/10.1016/j.checat.2025.101393","url":null,"abstract":"Pressurized electrochemical carbon dioxide reduction (CO<sub>2</sub>R) offers a pathway to enhance selectivity, current density, and process integration. While elevated pressures improve CO<sub>2</sub>R performance, differential pressure operation above 10 bar between cathode and anode remains underexplored. This study introduces an innovative test facility and a continuous high-pressure reactor with a zero-gap architecture, enabling gaseous CO<sub>2</sub> electrolysis at a differential pressure of 40 bar(g). Using a bipolar membrane electrode assembly eliminates the need for CO<sub>2</sub> humidification, and using ultrapure water as the sole proton source creates a salt-free environment without acid or base additives. This setup achieved a Faraday efficiency for CO of 81% at 500 mA cm<sup>−2</sup>, efficient CO<sub>2</sub>R with a CO<sub>2</sub> excess (<em>λ</em><sub>CO2</sub>) below 4, and single-pass conversion rates up to 26% at 40 bar(g). The pressurized CO<sub>2</sub>R outlet streams have low CO<sub>2</sub> content, enabling direct integration into downstream chemical processes. This marks a key advancement toward scalable, energy-efficient industrial CO<sub>2</sub> electrolysis systems.","PeriodicalId":53121,"journal":{"name":"Chem Catalysis","volume":"31 1","pages":""},"PeriodicalIF":9.4,"publicationDate":"2025-05-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144097542","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
Carbene-mediated photocatalytic ethanol synthesis by frustrated Lewis pairs 受阻路易斯对催化卡宾介导的光催化乙醇合成
IF 9.4
Chem Catalysis Pub Date : 2025-05-15 DOI: 10.1016/j.checat.2025.101385
Linqun Yu, Song Li, Zhenyi Zhang
{"title":"Carbene-mediated photocatalytic ethanol synthesis by frustrated Lewis pairs","authors":"Linqun Yu, Song Li, Zhenyi Zhang","doi":"10.1016/j.checat.2025.101385","DOIUrl":"https://doi.org/10.1016/j.checat.2025.101385","url":null,"abstract":"Reporting in the <em>Journal of the American Chemical Society</em>, Lu Li, Chao-Jun Li, and colleagues have designed a Ga-ZnO<sub>1–x</sub> nanosheet photocatalyst with rich frustrated Lewis pair (FLP) sites. They present a green methanol-to-ethanol conversion protocol and establish a safe strategy for generating methyl carbene under mild conditions.","PeriodicalId":53121,"journal":{"name":"Chem Catalysis","volume":"13 1","pages":""},"PeriodicalIF":9.4,"publicationDate":"2025-05-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143980060","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
Boosting hole mobility in oxides via metal vacancies 通过金属空位提高氧化物的空穴迁移率
IF 9.4
Chem Catalysis Pub Date : 2025-05-15 DOI: 10.1016/j.checat.2025.101391
Fatwa F. Abdi
{"title":"Boosting hole mobility in oxides via metal vacancies","authors":"Fatwa F. Abdi","doi":"10.1016/j.checat.2025.101391","DOIUrl":"https://doi.org/10.1016/j.checat.2025.101391","url":null,"abstract":"In a recent issue of <em>Nature Catalysis</em>, Liu and co-workers introduce metal-vacancy engineering to enhance hole mobility in transition-metal oxides, significantly improving photoelectrochemical water-splitting performance. This concept is crucial to addressing the disparity between hole and electron mobility and holds strong potential for broader application in catalysis and the development of functional oxides.","PeriodicalId":53121,"journal":{"name":"Chem Catalysis","volume":"13 1","pages":""},"PeriodicalIF":9.4,"publicationDate":"2025-05-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143980063","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
Viologen-COF enables near-infrared photocatalysis via linker-to-linker charge transfer Viologen-COF通过连接体之间的电荷转移实现近红外光催化
IF 9.4
Chem Catalysis Pub Date : 2025-05-15 DOI: 10.1016/j.checat.2025.101395
Yuting Liu, Xiaokun Shi, Xin Chen, Ya Du
{"title":"Viologen-COF enables near-infrared photocatalysis via linker-to-linker charge transfer","authors":"Yuting Liu, Xiaokun Shi, Xin Chen, Ya Du","doi":"10.1016/j.checat.2025.101395","DOIUrl":"https://doi.org/10.1016/j.checat.2025.101395","url":null,"abstract":"A recent study published in the <em>Journal of the American Chemical Society</em> by Wenbin Lin and colleagues introduces a groundbreaking viologen-linked porphyrin covalent organic framework (Vio-COF) that leverages linker-to-linker charge transfer (LLCT) to achieve exceptional near-infrared (NIR) light absorption with an absorption edge extending to 998 nm.","PeriodicalId":53121,"journal":{"name":"Chem Catalysis","volume":"40 1","pages":""},"PeriodicalIF":9.4,"publicationDate":"2025-05-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143980062","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
Nitrite to amine in one pot 亚硝酸盐到胺在一个锅里
IF 9.4
Chem Catalysis Pub Date : 2025-05-15 DOI: 10.1016/j.checat.2025.101384
Chen Chen, Ning Yan
{"title":"Nitrite to amine in one pot","authors":"Chen Chen, Ning Yan","doi":"10.1016/j.checat.2025.101384","DOIUrl":"https://doi.org/10.1016/j.checat.2025.101384","url":null,"abstract":"In the <em>Journal of American Chemical Society</em>, Wang and co-workers report a one-pot C–N bond-formation strategy through NH<sub>2</sub>OH-mediated electrochemical reductive amination of carbonyls and nitrite. This elegant pathway, combining high yield and Faradaic efficiency in neutral media, opens new opportunities for designing electrocatalytic amine synthesis.","PeriodicalId":53121,"journal":{"name":"Chem Catalysis","volume":"90 1","pages":""},"PeriodicalIF":9.4,"publicationDate":"2025-05-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143980061","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
Challenges of characterizing degradation in hydrogen polymer electrolyte fuel cells 表征氢聚合物电解质燃料电池降解的挑战
IF 9.4
Chem Catalysis Pub Date : 2025-05-15 DOI: 10.1016/j.checat.2025.101387
Andrea Baricci, Elena Colombo, Andrea Mattera
{"title":"Challenges of characterizing degradation in hydrogen polymer electrolyte fuel cells","authors":"Andrea Baricci, Elena Colombo, Andrea Mattera","doi":"10.1016/j.checat.2025.101387","DOIUrl":"https://doi.org/10.1016/j.checat.2025.101387","url":null,"abstract":"In this issue of <em>Chem Catalysis</em>, Xie and colleagues investigate degradation mechanisms in polymer electrolyte membrane fuel cells (PEMFCs) and their evolution over prolonged operation. Using advanced characterization techniques, the authors analyze modifications in catalyst morphology and ionomer properties.","PeriodicalId":53121,"journal":{"name":"Chem Catalysis","volume":"122 1","pages":""},"PeriodicalIF":9.4,"publicationDate":"2025-05-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143980059","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
Waste oxidation as a pathway to energy-efficient electrochemical processes 废物氧化是实现节能电化学过程的途径
IF 9.4
Chem Catalysis Pub Date : 2025-05-14 DOI: 10.1016/j.checat.2025.101392
Emilly Cristine de Brito Dorneles, Kirsten Van Fossen, Anna Li, Magda Helena Barecka
{"title":"Waste oxidation as a pathway to energy-efficient electrochemical processes","authors":"Emilly Cristine de Brito Dorneles, Kirsten Van Fossen, Anna Li, Magda Helena Barecka","doi":"10.1016/j.checat.2025.101392","DOIUrl":"https://doi.org/10.1016/j.checat.2025.101392","url":null,"abstract":"The large-scale availability of low-carbon hydrogen is critical for achieving the net zero 2050 goal, yet researchers are questioning whether the planned expansion of the renewable energy network will be sufficient to meet this demand. In the pursuit of alternative pathways to yield hydrogen, anodic oxidation reactions (AORs) are attracting much attention from the catalysis community. However, these systems are mostly studied on a small scale, and insights into their commercial application are missing. To bridge this gap, we postulate that AOR catalysts should be further developed and tested under conditions closer to real-life applications. We defined these applications from a system-level perspective and provided a practical framework to translate complex environments into conditions that can be tested under academic wet lab limitations. The proposed framework also supports the collaboration toward developing partnering technologies (e.g., separations) needed for a large-scale hydrogen supply from AORs.","PeriodicalId":53121,"journal":{"name":"Chem Catalysis","volume":"96 1","pages":""},"PeriodicalIF":9.4,"publicationDate":"2025-05-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143946207","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
Polyaniline-supported copper nanocrystals for electrochemical CO2 reduction to methane 聚苯胺负载的铜纳米晶电化学CO2还原为甲烷
IF 9.4
Chem Catalysis Pub Date : 2025-05-12 DOI: 10.1016/j.checat.2025.101389
Rong Chen, Jing Gao, Shuangte Zhao, Hongguang Wang, Guilin Zhuang, Peter A. van Aken, Michael Grätzel, Jingshan Luo
{"title":"Polyaniline-supported copper nanocrystals for electrochemical CO2 reduction to methane","authors":"Rong Chen, Jing Gao, Shuangte Zhao, Hongguang Wang, Guilin Zhuang, Peter A. van Aken, Michael Grätzel, Jingshan Luo","doi":"10.1016/j.checat.2025.101389","DOIUrl":"https://doi.org/10.1016/j.checat.2025.101389","url":null,"abstract":"Achieving industrial electrochemical CO<sub>2</sub> reduction necessitates the strategic design of electrocatalysts with high activity, superior selectivity, and excellent stability. Herein, we developed spatially dispersed copper nanocrystals supported by polyaniline (PANI-CuNCs) for electrochemical CO<sub>2</sub> reduction, achieving a faradaic efficiency of 68.6% ± 2.2% toward methane at −300 mA cm<sup>−2</sup>. The chelation of the Cu precursor within the oxidized emeraldine base (EB) is crucial for forming isolated CuNCs. The PANI substrate facilitates proton shuttling to Cu(111) sites, enhancing methane production by promoting protonation and reducing ∗CO coverage. <em>In situ</em> Raman and theoretical calculations show that PANI improves CO<sub>2</sub> adsorption and activation by creating a hydrophilic environment, highlighting its potential for industrial CO<sub>2</sub> reduction electrocatalysis. Our work introduced a promising strategy that utilizes polymers as substrates to prepare well-dispersed NCs for electrocatalysis, highlighting the potential of such systems in advancing the field of industrial electrochemical CO<sub>2</sub> reduction.","PeriodicalId":53121,"journal":{"name":"Chem Catalysis","volume":"28 1","pages":""},"PeriodicalIF":9.4,"publicationDate":"2025-05-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143933520","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
Modular silver catalysts to elucidate the role of non-covalent interactions in asymmetric C‒H amidation reactions 模块银催化剂阐明非共价相互作用在不对称C-H酰胺化反应中的作用
IF 9.4
Chem Catalysis Pub Date : 2025-05-12 DOI: 10.1016/j.checat.2025.101388
Emily Z. Schroeder, Jed H. Kim, Yue Fu, Wentan Liu, Peng Liu, Jennifer M. Schomaker
{"title":"Modular silver catalysts to elucidate the role of non-covalent interactions in asymmetric C‒H amidation reactions","authors":"Emily Z. Schroeder, Jed H. Kim, Yue Fu, Wentan Liu, Peng Liu, Jennifer M. Schomaker","doi":"10.1016/j.checat.2025.101388","DOIUrl":"https://doi.org/10.1016/j.checat.2025.101388","url":null,"abstract":"Chiral, non-racemic amines and aminoalcohols are common structural motifs in bioactive molecules. Asymmetric nitrene transfer offers a powerful approach to prepare enantioenriched amines directly from abundant C–H bonds; however, the development of general, cost-effective catalysts supported by easily tunable ligands remains a significant challenge. Herein, we report that Ag salts coordinated with unique bis(oxazoline) ligands catalyze site- and enantioselective nitrene transfer into benzylic, allylic, and unactivated C–H bonds of carbamate esters. This method provides 1,3-aminoalcohols in high yields with enantiomeric excess (<em>ee</em>) of up to 98%. Computations were used to rationalize key features influencing the observed stereochemical outcomes. Analysis of the enantiodetermining transition states revealed that high <em>ee</em> arises from a preferred square-planar geometry at the silver nitrene and stabilizing C–H/π interactions between the ligand and substrate. These features enable broad substrate scope and high chemo-, site-, and enantioselectivity in Ag-catalyzed C–H bond amidations via nitrene transfer.","PeriodicalId":53121,"journal":{"name":"Chem Catalysis","volume":"31 1","pages":""},"PeriodicalIF":9.4,"publicationDate":"2025-05-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143933457","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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