Chem CatalysisPub Date : 2024-12-16DOI: 10.1016/j.checat.2024.101199
Min Liu, Ruofei Gao, Kang Geng, Yingda Huang, Xiaowei Zhou, Jin Yao, Bin Hu, Hongjing Li, Boxin Xue, Nanwen Li
{"title":"Highly durable alkaline water electrolyzer with branched poly(oxindole biphenylene) ion-solvating membrane","authors":"Min Liu, Ruofei Gao, Kang Geng, Yingda Huang, Xiaowei Zhou, Jin Yao, Bin Hu, Hongjing Li, Boxin Xue, Nanwen Li","doi":"10.1016/j.checat.2024.101199","DOIUrl":"https://doi.org/10.1016/j.checat.2024.101199","url":null,"abstract":"Ion-solvating membranes (ISMs) offer a novel approach for high-rate alkaline water electrolyzers (AWEs), but device durability remains a major challenge for their practical application. Herein, we first found that the oxidation stability of ISMs in electrolyzers showed a significant effect on their long-term device durability, in addition to the alkaline stability. More importantly, both the operating temperature and the voltage have been observed as crucial factors affecting the oxidative stability of ISMs. While maintaining other excellent properties, the branching polymer chain in ISMs could further enhance their oxidative stability. As a result, a highly durable AWE with branched poly(oxindole biphenylene) (POBP) ISMs operated stably for over 15,000 h at 2.26 V and 60°C, representing the longest reported lifetime for ISM-based AWEs to date. These results provide significant guidance on how to reasonably design the polymer backbone and adjust the operating conditions to prolong the membrane’s lifetime in AWEs for practical applications.","PeriodicalId":53121,"journal":{"name":"Chem Catalysis","volume":"18 1","pages":""},"PeriodicalIF":9.4,"publicationDate":"2024-12-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142825754","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 : 2024-12-13DOI: 10.1016/j.checat.2024.101197
Yingdan Cui, Yian Wang, Fei Yang, Weiwei Chen, Guimei Liu, Shangqian Zhu, Xiaoyi Qiu, Fei Xiao, Gongjin Chen, Yan Sun, Mohammad Farhadpour, Dong Su, William E. Mustain, Yoonseob Kim, Minhua Shao
{"title":"Boron-activated ruthenium nanoparticles for hydrogen oxidation reaction in anion exchange membrane fuel cells","authors":"Yingdan Cui, Yian Wang, Fei Yang, Weiwei Chen, Guimei Liu, Shangqian Zhu, Xiaoyi Qiu, Fei Xiao, Gongjin Chen, Yan Sun, Mohammad Farhadpour, Dong Su, William E. Mustain, Yoonseob Kim, Minhua Shao","doi":"10.1016/j.checat.2024.101197","DOIUrl":"https://doi.org/10.1016/j.checat.2024.101197","url":null,"abstract":"The sluggish reaction kinetics of the hydrogen oxidation reaction (HOR) in alkaline media hinders the applications of anion exchange membrane fuel cells (AEMFCs). This study focuses on developing a high-performance catalyst for alkaline HOR: namely, Ru nanoparticles with a B-doped surface supported on B-doped carbon (B-Ru/BC). It delivers an outstanding exchange current density of 0.855 mA cm<sup>−2</sup><sub>PGM</sub> normalized by an electrochemical active surface area, 3 times that of commercial Pt/C and comparable to that of commercial PtRu/C, and exhibits significantly improved CO tolerance in alkaline media. Notably, the B-Ru/BC catalyst demonstrates impressive durability and achieves a peak power density of 1.5 W cm<sup>−2</sup> in AEMFCs, surpassing commercial PtRu/C. Theoretical calculations revealed the positive effects of B doping on the enhanced activity and durability of B-Ru/BC. This research introduces an organics-free synthesis method for cost-effective B-Ru/BC catalysts, aiming to propel the commercialization of AEMFCs and contribute to the advancement of sustainable energy technologies.","PeriodicalId":53121,"journal":{"name":"Chem Catalysis","volume":"1 1","pages":""},"PeriodicalIF":9.4,"publicationDate":"2024-12-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142816416","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 : 2024-11-22DOI: 10.1016/j.checat.2024.101188
Le Wang, Zi-Hao Li, Di Wu, Rui-Tian Ge, Jia Zhou, Yin-Feng Zhang, Shu-Yu Zhang
{"title":"Organocatalytic asymmetric tandem reaction for the enantioselective synthesis of chiral oxindoles to construct CyK dyes","authors":"Le Wang, Zi-Hao Li, Di Wu, Rui-Tian Ge, Jia Zhou, Yin-Feng Zhang, Shu-Yu Zhang","doi":"10.1016/j.checat.2024.101188","DOIUrl":"https://doi.org/10.1016/j.checat.2024.101188","url":null,"abstract":"We report an efficient method for the synthesis of chiral 3-trifluoromethyl-3-hydroxy oxindoles through the asymmetric [3 + 2] cascade cyclization of simple 2-naphthylamine derivatives with ethyl trifluoropyruvate. This catalytic asymmetric strategy enables the efficient construction of a series of enantioenriched CF<sub>3</sub>-quaternary carbon oxindoles with high yields and excellent stereoselectivities. The innovative synthetic approach has been applied to the synthesis of trifluoromethylated Cy-ketone fluorescent dyes with circularly polarized luminescence (CPL) properties. <em>In situ</em> infrared and density functional theory calculations indicate that our catalytic system can overcome background reactions to achieve effective enantioselective annulation.","PeriodicalId":53121,"journal":{"name":"Chem Catalysis","volume":"254 1","pages":""},"PeriodicalIF":9.4,"publicationDate":"2024-11-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142685102","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 : 2024-11-21DOI: 10.1016/j.checat.2024.101191
Jinhai Yu, Yingdi Hao, Xiaoqiang Huang
{"title":"Repurposing type I aldolase for stereospecific radical coupling with light","authors":"Jinhai Yu, Yingdi Hao, Xiaoqiang Huang","doi":"10.1016/j.checat.2024.101191","DOIUrl":"https://doi.org/10.1016/j.checat.2024.101191","url":null,"abstract":"In a recent article published in <em>Nature</em>, Melchiorre and coworkers illuminated enzymatic iminium ions formed through the condensation of 2-deoxyribose-5-phosphate aldolase with enals, triggering photodecarboxylication in the active site, and enabling photoenzymatic stereospecific radical coupling. This elegant work broadens the reactivity of enzymes and achieves a “memory of chirality” scenario.","PeriodicalId":53121,"journal":{"name":"Chem Catalysis","volume":"36 1","pages":""},"PeriodicalIF":9.4,"publicationDate":"2024-11-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142679033","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 : 2024-11-21DOI: 10.1016/j.checat.2024.101193
Gabriel F. Costa, Raphael Nagao
{"title":"Efficient nitrate-to-ammonia conversion for circular nitrogen economy","authors":"Gabriel F. Costa, Raphael Nagao","doi":"10.1016/j.checat.2024.101193","DOIUrl":"https://doi.org/10.1016/j.checat.2024.101193","url":null,"abstract":"The development of an economically feasible system for the electrochemical treatment of nitrate-rich wastewater is hampered by the complexity of the matrices. The use of membrane-free systems can be beneficial to avoid contamination by organic impurities and dissolved salts, but their implementation is challenging considering that ammonia is susceptible to anodic oxidation. This article previews a new approach that maximizes ammonia recovery by integrating a nitrate electrochemical reduction cell with a UV-assisted stripping unit that converts over 70% of nitrate into ammonia chloride.","PeriodicalId":53121,"journal":{"name":"Chem Catalysis","volume":"253 1","pages":""},"PeriodicalIF":9.4,"publicationDate":"2024-11-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142679034","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":"Enhanced electrochemical reduction of CO2 to CO by ZnO nanorods enriched with oxygen vacancies","authors":"Zhongnan Ling, Yaoyu Yin, Xinchen Kang, Xianliang Li, Ran Duan, Shuming Zhou, Huanyan Liu, Guang Mo, Zhongjun Chen, Xuehui Wu, Rongjuan Feng, Zhonghua Wu, Buxing Han, Xueqing Xing","doi":"10.1016/j.checat.2024.101192","DOIUrl":"https://doi.org/10.1016/j.checat.2024.101192","url":null,"abstract":"The efficiency of converting CO<sub>2</sub> to other valuable chemicals via the electrochemical reduction pathway depends on the electrocatalyst. In this work, an approach to prepare the ZnO catalysts used for the CO<sub>2</sub> electrocatalytic reduction was proposed, aiming at regulating the oxygen vacancy concentration in ZnO nanorods by changing the heat treatment temperature. The results show that the faradaic efficiency of CO<sub>2</sub> reduction to CO is significantly improved. An unprecedented faradaic efficiency of 98.3% and a current density of 786.56 mA cm<sup>−2</sup> were achieved using the ZnO catalyst heat treated at 500°C. It is revealed that the oxygen vacancy concentration, combined with density functional theory, can improve the performance of the ZnO electrocatalytic reduction of carbon dioxide (CO<sub>2</sub>RR) by accelerating the activation of CO<sub>2</sub> molecules and reducing the energy barrier of CO formation. This work is helpful for the development of robust and efficient ZnO catalysts and their application in the CO<sub>2</sub>RR.","PeriodicalId":53121,"journal":{"name":"Chem Catalysis","volume":"13 1","pages":""},"PeriodicalIF":9.4,"publicationDate":"2024-11-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142679028","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 : 2024-11-21DOI: 10.1016/j.checat.2024.101186
Yifan Zeng, Dongbo Li, Pengtao Xu
{"title":"Cation effects on the alkaline oxygen reduction reaction","authors":"Yifan Zeng, Dongbo Li, Pengtao Xu","doi":"10.1016/j.checat.2024.101186","DOIUrl":"https://doi.org/10.1016/j.checat.2024.101186","url":null,"abstract":"In a recent issue of <em>ACS Energy Letters</em>, Resasco and his colleagues examine how different alkali metal cations impact the oxygen reduction reaction (ORR) over a series of metal catalysts. They conclude that a metal catalyst exhibits cation-dependent ORR rates when its potential of zero total charge is positive of the ORR potential window. Such cation effects are rationalized by considering how the cations at the interface affect the rate-determining step.","PeriodicalId":53121,"journal":{"name":"Chem Catalysis","volume":"17 1","pages":""},"PeriodicalIF":9.4,"publicationDate":"2024-11-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142679031","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 : 2024-11-21DOI: 10.1016/j.checat.2024.101190
Venkata Sai Sriram Mosali, Hanna Soucie, Xiong Peng, Ehsan Faegh, Matthew Elam, Ian Street, William E. Mustain
{"title":"Mechanistic insights into the electrochemical oxidation of acetate at noble metals","authors":"Venkata Sai Sriram Mosali, Hanna Soucie, Xiong Peng, Ehsan Faegh, Matthew Elam, Ian Street, William E. Mustain","doi":"10.1016/j.checat.2024.101190","DOIUrl":"https://doi.org/10.1016/j.checat.2024.101190","url":null,"abstract":"Electrochemical acetate oxidation (AcOR) offers a sustainable approach to produce renewable biofuels. While CO₂ formation is thermodynamically favored, acetate oxidation can also yield various products through the Kolbe and Hofer-Moest mechanisms, enabling a modulation of the products formed via partial oxidation. Given the complexity of the reaction, it is crucial to understand how different reaction conditions influence the product profile. Furthermore, this process generates methyl radicals, providing insights into methane partial oxidation. The current study explores AcOR on noble metal electrodes (Pt, Pd, Au) in a 0.5 M CH<sub>3</sub>COOK aqueous electrolyte, revealing the mechanism of product formation using potential- and time-dependent electrolysis and isotope-labeling experiments. The effect of surface chemistry, ion transport, electrolyte concentration, and electrolysis techniques on product selectivity is analyzed. Additionally, the study compares product profiles from an electrolyzer cell to those obtained from model electrodes in batch-cell setup.","PeriodicalId":53121,"journal":{"name":"Chem Catalysis","volume":"57 1","pages":""},"PeriodicalIF":9.4,"publicationDate":"2024-11-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142679032","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 : 2024-11-21DOI: 10.1016/j.checat.2024.101195
Marc Robert
{"title":"Cations in molecular electrochemical catalysis","authors":"Marc Robert","doi":"10.1016/j.checat.2024.101195","DOIUrl":"https://doi.org/10.1016/j.checat.2024.101195","url":null,"abstract":"In a recent issue of <em>Nature Catalysis</em>, Yu and Shao-Horn et al. describe the impact of cations on the electrochemical reduction of CO<sub>2</sub> to methanol with Co phthalocyanine complexes deposited onto carbon nanotubes. Their findings that the catalysis is enhanced opens wide and stimulating perspectives.","PeriodicalId":53121,"journal":{"name":"Chem Catalysis","volume":"193 1","pages":""},"PeriodicalIF":9.4,"publicationDate":"2024-11-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142679036","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":"Hydrogen dissociation and CO2 activation in cascade CO2 fixation on PdIn/TiO2 catalyst","authors":"Leilei Zhou, Ying Wang, Yinze Yang, Liyan Zhang, Jingrong Li, Tingting Xiao, Peikai Luo, Xinluona Su, Haiyang Cheng, Fengyu Zhao","doi":"10.1016/j.checat.2024.101116","DOIUrl":"https://doi.org/10.1016/j.checat.2024.101116","url":null,"abstract":"Reduction of CO<sub>2</sub> emissions and conversion of CO<sub>2</sub> to valuable chemicals is an urgent mission, as it is vital to the global environment and sustainable development. The activation of CO<sub>2</sub> is always considered to be the key step for its transformation. Herein, we verified that the activation and dissociation behavior of H<sub>2</sub> was the controlling step for CO<sub>2</sub> reduction. PdIn alloy was an active center and played a pivotal role in CO<sub>2</sub> hydrogenation to the methyl reagent of HCOO∗. H<sub>2</sub> split to active H<sup>δ−</sup> species on PdIn alloy sites. Strong nucleophilic H<sup>δ−</sup> reacted with the CO<sub>2</sub> adsorbed on oxygen defects to form ∗HCOO <em>in situ</em>. A high yield of up to 99% was achieved for the cascade fixation of CO<sub>2</sub> to valuable amines. The new insights into the activation of CO<sub>2</sub> and H<sub>2</sub> and their contributions to CO<sub>2</sub> conversion that we present will attract the attention of researchers in catalysis, synthesis, surface, and interface chemistry.","PeriodicalId":53121,"journal":{"name":"Chem Catalysis","volume":"81 1","pages":""},"PeriodicalIF":9.4,"publicationDate":"2024-11-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142679037","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}