Chem CatalysisPub Date : 2025-08-27DOI: 10.1016/j.checat.2025.101497
Maxwell Goldman, Aditya Prajapati, Nicholas R. Cross, Auston Clemens, An T. Chu, Laura Gutierrez, Michell Marufu, Eric Krall, Victoria Ehlinger, Thomas Moore, Eric B. Duoss, Sarah E. Baker, Christopher Hahn
{"title":"Designing ionomers to control water content for low-voltage ethylene production from CO2 electrolysis","authors":"Maxwell Goldman, Aditya Prajapati, Nicholas R. Cross, Auston Clemens, An T. Chu, Laura Gutierrez, Michell Marufu, Eric Krall, Victoria Ehlinger, Thomas Moore, Eric B. Duoss, Sarah E. Baker, Christopher Hahn","doi":"10.1016/j.checat.2025.101497","DOIUrl":"https://doi.org/10.1016/j.checat.2025.101497","url":null,"abstract":"Electrochemical CO<sub>2</sub> reduction (eCO<sub>2</sub>R) holds promise for decarbonizing industrial sectors by producing valuable commodities, such as ethylene. Incorporating polymer electrolyte ionomers onto Cu-based eCO<sub>2</sub>R cathodes is crucial for enhancing eCO<sub>2</sub>R efficiency. These ionomers control mass transport, surface chemistry, and water uptake at the cathode, enabling selectivity tuning toward desired C<sub>2</sub> products. Complexities and interdependence of interfacial properties have led to challenges within the field to define design properties of catalyst layer ionomers that can enhance the performance of Cu-based catalysts. Herein, we present a systematic investigation into ionomer properties and their relationship to electrochemical performance and demonstrate a 14.3% energy efficiency for ethylene selectivity at 200 mA cm<sup>−2</sup>. Through multiphysics modeling, we elucidated that the role of the water content of the ionomer is to mitigate flooding and control the local water concentration at the catalyst surface. Translating knowledge from this study will stimulate the synthesis of ionomers tailored for eCO<sub>2</sub>R.","PeriodicalId":53121,"journal":{"name":"Chem Catalysis","volume":"6 1","pages":""},"PeriodicalIF":9.4,"publicationDate":"2025-08-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144905966","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}
Chem CatalysisPub Date : 2025-08-21DOI: 10.1016/j.checat.2025.101443
Xin Wan, Jianglan Shui
{"title":"Fluorination propels Fe–N–C fuel cells to new heights","authors":"Xin Wan, Jianglan Shui","doi":"10.1016/j.checat.2025.101443","DOIUrl":"https://doi.org/10.1016/j.checat.2025.101443","url":null,"abstract":"In the June issue of <ce:italic>ACS Energy Letters</ce:italic>, Xing and co-workers report a fluorine-coordination strategy that modulates both the atomic coordination environments and macroscopic hydrophobicity of iron–nitrogen–carbon (Fe–N–C) fuel cell catalysts. This approach simultaneously enhances intrinsic activity, stability, and water management, marking a critical advancement toward affordable, high-performance, and durable proton-exchange membrane fuel cells.","PeriodicalId":53121,"journal":{"name":"Chem Catalysis","volume":"17 1","pages":"101443"},"PeriodicalIF":9.4,"publicationDate":"2025-08-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144901553","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}
Chem CatalysisPub Date : 2025-08-21DOI: 10.1016/j.checat.2025.101495
Caroline E. Paul
{"title":"Harnessing a versatile monooxygenase GorA to synthesize N-hydroxy compounds","authors":"Caroline E. Paul","doi":"10.1016/j.checat.2025.101495","DOIUrl":"https://doi.org/10.1016/j.checat.2025.101495","url":null,"abstract":"In <ce:italic>Cell Reports Physical Science</ce:italic>, Maier et al. unveil a biocatalytic approach for synthesizing <ce:italic>N</ce:italic>-hydroxy compounds by integrating the flavin-dependent monooxygenase GorA into an enzymatic cascade with the decarboxylase GorB and a formate dehydrogenase-driven cofactor recycling system. This work showcases GorA’s substrate scope and establishes a biocatalytic synthetic route for valuable <ce:italic>N</ce:italic>-hydroxy compounds.","PeriodicalId":53121,"journal":{"name":"Chem Catalysis","volume":"15 1","pages":"101495"},"PeriodicalIF":9.4,"publicationDate":"2025-08-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144901552","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}
Chem CatalysisPub Date : 2025-08-21DOI: 10.1016/j.checat.2025.101494
Zhiyuan Zhang, Jongwoo Lim
{"title":"Origin of copper catalyst reconstruction","authors":"Zhiyuan Zhang, Jongwoo Lim","doi":"10.1016/j.checat.2025.101494","DOIUrl":"https://doi.org/10.1016/j.checat.2025.101494","url":null,"abstract":"In the June 25 issue of <ce:italic>Nature Catalysis</ce:italic>, Yang et al. investigate the dynamic structural evolution of Cu-based catalysts during CO<ce:inf loc=\"post\">2</ce:inf> electroreduction. Using a suite of <ce:italic>operando</ce:italic> imaging and spectroscopic techniques, they uncover the critical role of ∗CO and Cu-CO species in driving Cu atom migration and catalyst reconstruction.","PeriodicalId":53121,"journal":{"name":"Chem Catalysis","volume":"17 1","pages":"101494"},"PeriodicalIF":9.4,"publicationDate":"2025-08-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144901554","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}
Chem CatalysisPub Date : 2025-08-21DOI: 10.1016/j.checat.2025.101496
M. Mar Díaz-Requejo, Pedro J. Pérez
{"title":"Weak interactions are crucial for better enantioselections","authors":"M. Mar Díaz-Requejo, Pedro J. Pérez","doi":"10.1016/j.checat.2025.101496","DOIUrl":"https://doi.org/10.1016/j.checat.2025.101496","url":null,"abstract":"In this issue of <ce:italic>Chem Catalysis</ce:italic>, Schomaker, Liu, and co-workers describe an enantioselective intramolecular silver-catalyzed nitrene transfer (NT) that forms chiral six-membered rings via C–H amidation. They use density functional theory (DFT) calculations to model initial experimental data, which provide crucial insights into the relevance of non-covalent interactions in enantioselection. These findings guide the design of novel ligands that enhance enantiomeric excess in the asymmetric amidation of diverse C–H bonds.","PeriodicalId":53121,"journal":{"name":"Chem Catalysis","volume":"13 1","pages":"101496"},"PeriodicalIF":9.4,"publicationDate":"2025-08-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144901550","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}
{"title":"Photothermal reforming of polylactic acid plastics into pyruvic acid with 92.8% selectivity at S-scheme Ov-BiVO4/CdS heterostructures","authors":"Xinxin Liang, Ying Tang, Yongqian Cui, Qingyun Tian, Qibing Dong, Ximing Li, Feng Yu, Jincai Zhao, Chuanyi Wang","doi":"10.1016/j.checat.2025.101490","DOIUrl":"https://doi.org/10.1016/j.checat.2025.101490","url":null,"abstract":"Reforming polylactic acid (PLA) into valuable chemicals while producing hydrogen is crucial for a circular economy. However, a significant challenge remains in the limited selectivity of its reformation products. Herein, we report on oxygen vacancy (O<sub>v</sub>)-modified S-scheme BiVO<sub>4</sub>/CdS heterostructures with favorable photothermal effects, aiming to strengthen the C<sub>α</sub>−C<sub>COOH</sub> bond and activate the α−OH of pretreated PLA for the highly selective production of pyruvic acid (PA). Compared to BiVO<sub>4</sub>@CdS, O<sub>v</sub>-BiVO<sub>4</sub>/CdS exhibits higher local charge accumulation on Bi sites, which increases the energy barrier of C<sub>α</sub>−C<sub>COOH</sub> bond cleavage from −0.34 to 0.44 eV and weakens the α−OH bonds in LA simultaneously, thus benefiting the generation of ∗CH<sub>3</sub>COCOOH intermediates. Moreover, the spontaneous photothermal effect of O<sub>v</sub>-BiVO<sub>4</sub>/CdS induced by O<sub>v</sub> promotes the desorption of PA, thereby suppressing its overoxidation. Consequently, the production rate of PA over O<sub>v</sub>-BiVO<sub>4</sub>/CdS reaches 8.92 mmol g<sup>−1</sup> h<sup>−1</sup> with a selectivity of 92.8%, representing one of the highest selectivity processes reported for plastic reforming.","PeriodicalId":53121,"journal":{"name":"Chem Catalysis","volume":"746 1","pages":""},"PeriodicalIF":9.4,"publicationDate":"2025-08-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144826028","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}
Chem CatalysisPub Date : 2025-08-13DOI: 10.1016/j.checat.2025.101491
Jiaolong Meng, Xuefeng Jiang
{"title":"Artificial-intelligence-enabled catalysis via standardized batch data","authors":"Jiaolong Meng, Xuefeng Jiang","doi":"10.1016/j.checat.2025.101491","DOIUrl":"https://doi.org/10.1016/j.checat.2025.101491","url":null,"abstract":"<span><figure><span><img alt=\"\" height=\"341\" src=\"https://ars.els-cdn.com/content/image/1-s2.0-S2667109325002295-fx1.jpg\"/><ol><li><span><span>Download: <span>Download high-res image (291KB)</span></span></span></li><li><span><span>Download: <span>Download full-size image</span></span></span></li></ol></span></figure></span><span><figure><span><img alt=\"\" height=\"339\" src=\"https://ars.els-cdn.com/content/image/1-s2.0-S2667109325002295-fx2.jpg\"/><ol><li><span><span>Download: <span>Download high-res image (389KB)</span></span></span></li><li><span><span>Download: <span>Download full-size image</span></span></span></li></ol></span></figure></span>Jiaolong Meng received his PhD in organic chemistry from East China Normal University in 2024 and continued his research there as a postdoctoral fellow under the supervision of Prof. Xuefeng Jiang. His research focuses on the application of artificial intelligence (AI) in chemistry and on strategies for plastic degradation. Xuefeng Jiang is a professor at East China Normal University. He earned his PhD in 2008 from the Shanghai Institute of Organic Chemistry, Chinese Academy of Sciences, under the supervision of Prof. Shengming Ma. From 2008 to 2011, he was a postdoctoral fellow, supervised by Prof. K.C. Nicolaou, at the Scripps Research Institute. His current research interests include organosulfur chemistry, AI in chemistry, and plastic degradation.","PeriodicalId":53121,"journal":{"name":"Chem Catalysis","volume":"105 1","pages":""},"PeriodicalIF":9.4,"publicationDate":"2025-08-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144826031","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}
{"title":"Accessing planar chiral ferrocenes via transient directing group-enabled C–H alkenylation under Pd(II) catalysis","authors":"Fangnuo Zhao, Yanze Li, Zhongkang Dong, Chen-Xu Liu, Quannan Wang, Qing Gu, Yu-Cheng Gu, Chao Zheng, Shu-Li You","doi":"10.1016/j.checat.2025.101485","DOIUrl":"https://doi.org/10.1016/j.checat.2025.101485","url":null,"abstract":"Pd-catalyzed asymmetric C–H functionalization is a privileged method for the synthesis of planar chiral ferrocenes. Previous examples under this category virtually rely on a preinstalled strong directing group. The transient directing strategy has witnessed considerable success in recent years. However, only limited examples have been reported for the synthesis of planar chiral ferrocenes. Herein, we report an asymmetric C–H alkenylation of ferrocenes with an array of electron-deficient olefins under Pd catalysis with <span>l</span>-<em>tert</em>-leucine as the transient-directing auxiliary. This reaction exhibits a wide substrate scope, and the target planar chiral ferrocenes are prepared in good yields (up to 85%) with exceptional enantioselectivity (up to >99% ee). Comprehensive mechanistic studies suggest that the storage of ring strain in a seven-membered palladacycle after C–H activation is the key to the success of our reaction design. It guarantees the migratory insertion as a kinetically feasible step that occurs in a strain-releasing manner.","PeriodicalId":53121,"journal":{"name":"Chem Catalysis","volume":"19 1","pages":""},"PeriodicalIF":9.4,"publicationDate":"2025-08-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144826034","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}
Chem CatalysisPub Date : 2025-08-13DOI: 10.1016/j.checat.2025.101487
Xiaoyu Xie, Ziyu Huo, Erin R. Crater, Robert B. Moore, Rong Tong
{"title":"Enantioselective polymerization of racemic lactide for stereocomplex poly(lactic acid)","authors":"Xiaoyu Xie, Ziyu Huo, Erin R. Crater, Robert B. Moore, Rong Tong","doi":"10.1016/j.checat.2025.101487","DOIUrl":"https://doi.org/10.1016/j.checat.2025.101487","url":null,"abstract":"Poly(lactic acid) (PLA) is a leading degradable and biocompatible polymer in the plastics industry. Stereocomplex PLA—a mixture of poly(<span>l</span>-lactic acid) and poly(<span>d</span>-lactic acid)—exhibits enhanced mechanical toughness and an elevated melting temperature compared to other PLA stereoisomers. However, the lack of highly enantioselective catalysts has prevented the single-step production of stereocomplex PLA from inexpensive racemic lactide. This work presents the discovery of chiral aluminum catalysts that are highly active for enantioselective lactide polymerization. Using a mixture of chiral catalysts with opposite enantioselectivities allowed for the single-step production of highly isotactic stereocomplex PLA from racemic lactide. The obtained stereocomplex PLA was tougher and more ductile than poly(<span>l</span>-lactic acid), stereoblock PLA, and even conventionally blended stereocomplex PLA. Computational studies revealed that the enantiocontrol exerted by the bimetallic aluminum complexes arises from dispersion interactions between the ligand and lactide within the catalyst cleft.","PeriodicalId":53121,"journal":{"name":"Chem Catalysis","volume":"79 1","pages":""},"PeriodicalIF":9.4,"publicationDate":"2025-08-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144826029","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}
Chem CatalysisPub Date : 2025-08-08DOI: 10.1016/j.checat.2025.101465
Rundong Zhao, Qiuyu Yan, Hao Lin, Lihong Yu, Le Liu, Jingyu Xi
{"title":"Dynamic pulse electrocatalysis for efficient and directed reduction of nitrate to ammonia","authors":"Rundong Zhao, Qiuyu Yan, Hao Lin, Lihong Yu, Le Liu, Jingyu Xi","doi":"10.1016/j.checat.2025.101465","DOIUrl":"https://doi.org/10.1016/j.checat.2025.101465","url":null,"abstract":"The electrochemical nitrate reduction reaction (NO<sub>3</sub>RR) presents a sustainable pathway to simultaneously address environmental nitrate (NO<sub>3</sub><sup>−</sup>) pollution and decarbonize ammonia (NH<sub>3</sub>) production. While traditional constant-potential electrocatalysis for NO<sub>3</sub>RR has been widely studied, it suffers from inherent limitations, including competing hydrogen evolution, intermediate desorption, mass transfer bottlenecks, etc. In response, pulsed electrocatalysis, as an easily operable method, enables the regulation of reaction pathways by periodically varying applied potentials and can effectively overcome the limitations of constant-potential catalysis. However, research on pulsed catalysis in NO<sub>3</sub>RR remains fragmented, lacking systematic categorization. Consequently, this review provides a comprehensive overview of pulsed NO<sub>3</sub>RR systems, encompassing fundamental testing methodologies, catalytic mechanisms, device configurations, <em>in situ</em> characterization techniques, and merits of pulsed strategy. Furthermore, the analysis outlines essential criteria for catalyst design to maximize the potential of pulsed strategy and emphasizes the need for enhanced research and refined investigations in existing pulsed NO<sub>3</sub>RR implementations.","PeriodicalId":53121,"journal":{"name":"Chem Catalysis","volume":"95 1","pages":""},"PeriodicalIF":9.4,"publicationDate":"2025-08-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144797549","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}