Pub Date : 2025-12-04DOI: 10.1016/j.checat.2025.101581
Carlos Enrique Torres-Méndez, Haining Tian
Access to multiple redox states in electrocatalysts is vital to enhance the activity and stability of molecular catalysts toward the production of fuels. In this work, we have developed a catalyst based on two caffeine units covalently linked to a benzothiadiazole core. This catalyst can store three electrons in a fully reversible manner. Under reductive conditions and in the presence of strong acids, this molecule forms an organic hydride donor that is electroactive toward H2 evolution at mild potentials in DMSO. Faradaic efficiency up to 92% and a turnover number up to 23 were achieved after 4 h of controlled potential electrolysis with no decomposition of the catalyst. A reaction mechanism involving a hydride transfer step is proposed based on the chemical species found under electrocatalytic conditions and density functional theory (DFT) calculations. The development of this small organic molecule is a step forward in the quest to low-cost, active, and long-term stable electrocatalysts for H2 evolution.
{"title":"Hydrogen evolution via hydride transfer by a small organic benzothiadiazole-caffeine electrocatalyst","authors":"Carlos Enrique Torres-Méndez, Haining Tian","doi":"10.1016/j.checat.2025.101581","DOIUrl":"https://doi.org/10.1016/j.checat.2025.101581","url":null,"abstract":"Access to multiple redox states in electrocatalysts is vital to enhance the activity and stability of molecular catalysts toward the production of fuels. In this work, we have developed a catalyst based on two caffeine units covalently linked to a benzothiadiazole core. This catalyst can store three electrons in a fully reversible manner. Under reductive conditions and in the presence of strong acids, this molecule forms an organic hydride donor that is electroactive toward H<sub>2</sub> evolution at mild potentials in DMSO. Faradaic efficiency up to 92% and a turnover number up to 23 were achieved after 4 h of controlled potential electrolysis with no decomposition of the catalyst. A reaction mechanism involving a hydride transfer step is proposed based on the chemical species found under electrocatalytic conditions and density functional theory (DFT) calculations. The development of this small organic molecule is a step forward in the quest to low-cost, active, and long-term stable electrocatalysts for H<sub>2</sub> evolution.","PeriodicalId":53121,"journal":{"name":"Chem Catalysis","volume":"28 1","pages":""},"PeriodicalIF":9.4,"publicationDate":"2025-12-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145689115","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}
Pub Date : 2025-11-26DOI: 10.1016/j.checat.2025.101573
Yilin Zhao, Yu Zhang, Yi Wei, Jingyi Chen, Lei Fan, Junmei Chen, Shibo Xi, Mingchuan Luo, Lei Shen, Lei Wang
We develop an energy-efficient electrolytic system that integrates synchronized cathodic and anodic reactions for the electrochemical upcycling of waste polyethylene terephthalate (PET) plastics. This process is enabled by a palladium-nickel bimetallic anodic electrocatalyst exhibiting outstanding activity and selectivity toward the oxidation of ethylene glycol (EG), a key hydrolysis product of PET, into formate. Kinetic analysis and mechanistic studies reveal that nickel incorporation into palladium enhances EG dehydrogenation, thereby improving both the selectivity and activity for formate production. Furthermore, kilogram-scale commercial PET waste plastic upcycling is demonstrated in a 100 cm2 electrolyzer, achieving a high PET conversion yield of 89.3% after 100 h of continuous operation at a current of 20 A. Overall, this work represents a significant advancement in the development of energy-efficient electrocatalytic systems for PET plastic upgrading.
{"title":"PdNi bimetallic catalyst enables efficient electrochemical upcycling of waste plastics","authors":"Yilin Zhao, Yu Zhang, Yi Wei, Jingyi Chen, Lei Fan, Junmei Chen, Shibo Xi, Mingchuan Luo, Lei Shen, Lei Wang","doi":"10.1016/j.checat.2025.101573","DOIUrl":"https://doi.org/10.1016/j.checat.2025.101573","url":null,"abstract":"We develop an energy-efficient electrolytic system that integrates synchronized cathodic and anodic reactions for the electrochemical upcycling of waste polyethylene terephthalate (PET) plastics. This process is enabled by a palladium-nickel bimetallic anodic electrocatalyst exhibiting outstanding activity and selectivity toward the oxidation of ethylene glycol (EG), a key hydrolysis product of PET, into formate. Kinetic analysis and mechanistic studies reveal that nickel incorporation into palladium enhances EG dehydrogenation, thereby improving both the selectivity and activity for formate production. Furthermore, kilogram-scale commercial PET waste plastic upcycling is demonstrated in a 100 cm<sup>2</sup> electrolyzer, achieving a high PET conversion yield of 89.3% after 100 h of continuous operation at a current of 20 A. Overall, this work represents a significant advancement in the development of energy-efficient electrocatalytic systems for PET plastic upgrading.","PeriodicalId":53121,"journal":{"name":"Chem Catalysis","volume":"47 1","pages":""},"PeriodicalIF":9.4,"publicationDate":"2025-11-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145600106","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}
Pub Date : 2025-11-25DOI: 10.1016/j.checat.2025.101571
Christoph Kubis, Jiali Liu, Klaus Neymeyr, Robert Franke, Baoxin Zhang
Cobalt carbonyls are crucial for the 100% atom-economical hydroformylation of alkenes. While traditional industrial processes require harsh conditions (100–400 bar, 100°C–250°C), our work explores catalyst performance under significantly milder, energy-efficient parameters. Using in situ Fourier transform infrared (FTIR) spectroscopy complemented by density functional theory (DFT) calculations, we present a comprehensive investigation into the stability and interconversion of the active species, HCo(CO)4, and its precursors, Co2(CO)8 and Co4(CO)12. We establish that HCo(CO)4 is stable at pressures as low as 10 bar and 120°C. For the first time, we directly monitored the catalyst’s formation from various sources, including Co4(CO)12, Co(acac)2, and Co(OAc)2. The activation mechanism of a cationic bisphosphine Co(II) precursor is also elucidated. This research provides a critical foundation for analyzing and optimizing cobalt-based catalysts, paving the way for more sustainable industrial processes.
钴羰基对于100%原子经济型烯烃氢甲酰化至关重要。虽然传统的工业过程需要苛刻的条件（100 - 400 bar, 100°C - 250°C），但我们的工作探索了催化剂在更温和、更节能的参数下的性能。利用原位傅里叶变换红外（FTIR）光谱和密度泛函理论（DFT）计算，我们对活性物质HCo(CO)4及其前体Co2(CO)8和Co4(CO)12的稳定性和相互转化进行了全面的研究。我们确定HCo(CO)4在低至10 bar和120°C的压力下是稳定的。我们首次从不同的来源，包括Co4(CO)12, CO (acac)2和CO (OAc)2，直接监测催化剂的形成。本文还阐明了阳离子二膦前体Co（II）的活化机理。这项研究为分析和优化钴基催化剂提供了重要的基础，为更可持续的工业过程铺平了道路。
{"title":"Understanding the formation and stability of cobalt-based catalysts for homogeneous carbonylation reactions","authors":"Christoph Kubis, Jiali Liu, Klaus Neymeyr, Robert Franke, Baoxin Zhang","doi":"10.1016/j.checat.2025.101571","DOIUrl":"https://doi.org/10.1016/j.checat.2025.101571","url":null,"abstract":"Cobalt carbonyls are crucial for the 100% atom-economical hydroformylation of alkenes. While traditional industrial processes require harsh conditions (100–400 bar, 100°C–250°C), our work explores catalyst performance under significantly milder, energy-efficient parameters. Using <em>in situ</em> Fourier transform infrared (FTIR) spectroscopy complemented by density functional theory (DFT) calculations, we present a comprehensive investigation into the stability and interconversion of the active species, HCo(CO)<sub>4</sub>, and its precursors, Co<sub>2</sub>(CO)<sub>8</sub> and Co<sub>4</sub>(CO)<sub>12</sub>. We establish that HCo(CO)<sub>4</sub> is stable at pressures as low as 10 bar and 120°C. For the first time, we directly monitored the catalyst’s formation from various sources, including Co<sub>4</sub>(CO)<sub>12</sub>, Co(acac)<sub>2</sub>, and Co(OAc)<sub>2</sub>. The activation mechanism of a cationic bisphosphine Co(II) precursor is also elucidated. This research provides a critical foundation for analyzing and optimizing cobalt-based catalysts, paving the way for more sustainable industrial processes.","PeriodicalId":53121,"journal":{"name":"Chem Catalysis","volume":"47 1","pages":""},"PeriodicalIF":9.4,"publicationDate":"2025-11-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145594164","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}
Pub Date : 2025-11-20DOI: 10.1016/j.checat.2025.101568
Kalen B. Laybourn, Patricia Z. Musacchio
Reporting in Nature Catalysis, Yu and colleagues have achieved an enantioselective C(sp3)–H fluorination of amides by using Pd catalysis, chiral amino-acid-derived ligands, and nucleophilic fluoride sources.
{"title":"Bringing stereoselectivity to C(sp3)–H nucleophilic fluorination","authors":"Kalen B. Laybourn, Patricia Z. Musacchio","doi":"10.1016/j.checat.2025.101568","DOIUrl":"https://doi.org/10.1016/j.checat.2025.101568","url":null,"abstract":"Reporting in <em>Nature Catalysis</em>, Yu and colleagues have achieved an enantioselective C(sp<sup>3</sup>)–H fluorination of amides by using Pd catalysis, chiral amino-acid-derived ligands, and nucleophilic fluoride sources.","PeriodicalId":53121,"journal":{"name":"Chem Catalysis","volume":"79 1","pages":""},"PeriodicalIF":9.4,"publicationDate":"2025-11-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145554865","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}
Pub Date : 2025-11-20DOI: 10.1016/j.checat.2025.101574
Jingjing Liu, Davide Ferri
In Nature Catalysis, Barth et al. elucidate how the Cu-site structure in Cu-SSZ-13 governs hydrogen cyanide (HCN) emissions during the selective catalytic reduction of nitric oxides with ammonia. They demonstrate that although Z2Cu sites cause high HCN release, ZCuOH species efficiently catalyze HCN decomposition, providing a design strategy for minimizing emissions.
{"title":"Active-site design in Cu-SSZ-13 curbs toxic hydrogen cyanide emissions","authors":"Jingjing Liu, Davide Ferri","doi":"10.1016/j.checat.2025.101574","DOIUrl":"https://doi.org/10.1016/j.checat.2025.101574","url":null,"abstract":"In <em>Nature Catalysis</em>, Barth et al. elucidate how the Cu-site structure in Cu-SSZ-13 governs hydrogen cyanide (HCN) emissions during the selective catalytic reduction of nitric oxides with ammonia. They demonstrate that although Z<sub>2</sub>Cu sites cause high HCN release, ZCuOH species efficiently catalyze HCN decomposition, providing a design strategy for minimizing emissions.","PeriodicalId":53121,"journal":{"name":"Chem Catalysis","volume":"28 1","pages":""},"PeriodicalIF":9.4,"publicationDate":"2025-11-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145554866","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}
Pub Date : 2025-11-20DOI: 10.1016/j.checat.2025.101552
Charles R. Teeples, Sidney M. Wilkerson-Hill
In the July 10 issue of Science, Nguyen et al. describe a universal method for carbene transfer reactions and an approach to quantifying the electrophilicity of electronically diverse carbene intermediates.
{"title":"A universal solution to the carbene electronics conundrum","authors":"Charles R. Teeples, Sidney M. Wilkerson-Hill","doi":"10.1016/j.checat.2025.101552","DOIUrl":"https://doi.org/10.1016/j.checat.2025.101552","url":null,"abstract":"In the July 10 issue of <em>Science</em>, Nguyen et al. describe a universal method for carbene transfer reactions and an approach to quantifying the electrophilicity of electronically diverse carbene intermediates.","PeriodicalId":53121,"journal":{"name":"Chem Catalysis","volume":"19 1","pages":""},"PeriodicalIF":9.4,"publicationDate":"2025-11-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145554869","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}
Hydrogen production through seawater electrolysis presents a promising approach to reduce the reliance on high-purity water sources required by traditional electrolysis methods. However, the process faces significant challenges—including halogen evolution, electrode corrosion, and complex seawater chemistry—that hinder long-term stability and efficiency. This perspective systematically examines recent advancements in electrocatalyst design focused on improving durability, selectivity, and resistance to corrosion in seawater environments. It also explores strategies for utilizing seawater resources effectively and co-synthesizing valuable chemicals, discussing the potential pathways for integrating seawater electrolysis into sustainable and scalable hydrogen production systems suitable for practical applications.
{"title":"Advances in durable electrocatalyst for seawater electrolysis applications","authors":"Suyang Feng, Yanhui Yu, Chongtai Wang, Peng Ling, Tianjiao Wang, Wenjuan Shi, Jing Li, Xingqi Han, Daoxiong Wu, Zhenye Kang, Yuliang Yuan, Xinlong Tian","doi":"10.1016/j.checat.2025.101551","DOIUrl":"https://doi.org/10.1016/j.checat.2025.101551","url":null,"abstract":"Hydrogen production through seawater electrolysis presents a promising approach to reduce the reliance on high-purity water sources required by traditional electrolysis methods. However, the process faces significant challenges—including halogen evolution, electrode corrosion, and complex seawater chemistry—that hinder long-term stability and efficiency. This perspective systematically examines recent advancements in electrocatalyst design focused on improving durability, selectivity, and resistance to corrosion in seawater environments. It also explores strategies for utilizing seawater resources effectively and co-synthesizing valuable chemicals, discussing the potential pathways for integrating seawater electrolysis into sustainable and scalable hydrogen production systems suitable for practical applications.","PeriodicalId":53121,"journal":{"name":"Chem Catalysis","volume":"149 1","pages":""},"PeriodicalIF":9.4,"publicationDate":"2025-11-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145554903","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}
Pub Date : 2025-11-20DOI: 10.1016/j.checat.2025.101575
Kevinjeorjios Pellumbi, Ulf-Peter Apfel
Connecting interfacial mechanisms with microenvironmental responses is key to optimizing CO2 electrolyzers. In a recent issue of Nature Catalysis, Haussener, López, and colleagues present a multiscale framework unifying atomistic, kinetic, and transport modeling, redefining the active site as a microenvironment to guide electrolyte and interface design.
{"title":"The search for a bridge across scales in CO2 electrolysis","authors":"Kevinjeorjios Pellumbi, Ulf-Peter Apfel","doi":"10.1016/j.checat.2025.101575","DOIUrl":"https://doi.org/10.1016/j.checat.2025.101575","url":null,"abstract":"Connecting interfacial mechanisms with microenvironmental responses is key to optimizing CO<sub>2</sub> electrolyzers. In a recent issue of <em>Nature Catalysis</em>, Haussener, López, and colleagues present a multiscale framework unifying atomistic, kinetic, and transport modeling, redefining the active site as a microenvironment to guide electrolyte and interface design.","PeriodicalId":53121,"journal":{"name":"Chem Catalysis","volume":"128 1","pages":""},"PeriodicalIF":9.4,"publicationDate":"2025-11-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145554867","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}
Pub Date : 2025-11-20DOI: 10.1016/j.checat.2025.101567
Jiyuan Liu, Yu Yang, Fengwang Li
A recent Nature Synthesis study reports an oxygen affinity engineering strategy that uses lead-doped copper to enhance CO–CHₓ coupling for ethanol electrosynthesis. Achieving 50% carbon efficiency, 22% energy efficiency, and 200-h stability, this work establishes a compelling design paradigm for selective, durable electrocatalysts toward sustainable ethanol production.
{"title":"Electrosynthesis of ethanol via oxygen affinity engineering","authors":"Jiyuan Liu, Yu Yang, Fengwang Li","doi":"10.1016/j.checat.2025.101567","DOIUrl":"https://doi.org/10.1016/j.checat.2025.101567","url":null,"abstract":"A recent <em>Nature Synthesis</em> study reports an oxygen affinity engineering strategy that uses lead-doped copper to enhance CO–CH<em>ₓ</em> coupling for ethanol electrosynthesis. Achieving 50% carbon efficiency, 22% energy efficiency, and 200-h stability, this work establishes a compelling design paradigm for selective, durable electrocatalysts toward sustainable ethanol production.","PeriodicalId":53121,"journal":{"name":"Chem Catalysis","volume":"32 1","pages":""},"PeriodicalIF":9.4,"publicationDate":"2025-11-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145554868","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}
Pub Date : 2025-11-19DOI: 10.1016/j.checat.2025.101577
Zihang Deng, Jeffrey N. Johnston
Zihang Deng received his PhD degree from Vanderbilt University, where his research focused on developing asymmetric organocatalyst generality and employing high-throughput screening in organocatalysis. He is currently a postdoctoral scholar at Harvard University (with Richard Liu), where he develops innovative coupling reagents for bioconjugation.Jeffrey N. Johnston is a Stevenson Professor of Chemistry at Vanderbilt University, where he leads a research program that develops new reactions and reagents for the synthesis of complex natural products and therapeutics. The integrative design of sustainable catalysts with strategic fragment-assembling schemes and the acceleration of the discovery phase in enantioselective catalysis are high priorities.
邓子航博士毕业于美国范德比尔特大学，主要研究方向为不对称有机催化剂的开发及在有机催化中的高通量筛选。他目前是哈佛大学博士后学者（与Richard Liu合作），在那里他开发了用于生物偶联的创新偶联试剂。Jeffrey N. Johnston是Vanderbilt University的史蒂文森化学教授，在那里他领导一个研究项目，开发用于合成复杂天然产物和治疗的新反应和试剂。可持续催化剂与战略性片段组装方案的整合设计和加速对映选择性催化的发现阶段是当务之急。
{"title":"Performance-enhancing asymmetric catalysis unlocks tuning without rebuilding","authors":"Zihang Deng, Jeffrey N. Johnston","doi":"10.1016/j.checat.2025.101577","DOIUrl":"https://doi.org/10.1016/j.checat.2025.101577","url":null,"abstract":"Zihang Deng received his PhD degree from Vanderbilt University, where his research focused on developing asymmetric organocatalyst generality and employing high-throughput screening in organocatalysis. He is currently a postdoctoral scholar at Harvard University (with Richard Liu), where he develops innovative coupling reagents for bioconjugation.Jeffrey N. Johnston is a Stevenson Professor of Chemistry at Vanderbilt University, where he leads a research program that develops new reactions and reagents for the synthesis of complex natural products and therapeutics. The integrative design of sustainable catalysts with strategic fragment-assembling schemes and the acceleration of the discovery phase in enantioselective catalysis are high priorities.","PeriodicalId":53121,"journal":{"name":"Chem Catalysis","volume":"132 1","pages":""},"PeriodicalIF":9.4,"publicationDate":"2025-11-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145545832","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}
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