Pub Date : 2024-12-16DOI: 10.1016/j.checat.2024.101198
Ya Pan, Chunlan Qin, Ruichao Xu, Liuxin Xu, Shanshan Ruan, Xu Zhang, Kun Zheng, Xiao Han, Jinglin Yuan, Yanna Shui, Lidong Zhang, Zhihu Sun
The classic strong metal-support interaction (SMSI), characterized by the encapsulation of metal nanoparticles within suboxide layers, is a promising strategy for designing robust catalysts. However, applying this strategy to the high-temperature propane dehydrogenation (PDH) process, which is an important petrochemical process for the industrial production of propylene, is rarely reported. Herein, we demonstrate an SMSI-type PDH catalyst, composed of subnanometric Pt2In3 clusters encapsulated by an In2O3-x overlayer, exhibiting high stability and selectivity. During a 160-h on-stream test, it showed a slight activity decline (kd = 0.002 h−1) and maintained 99.5% propylene selectivity. The excellent performance is attributed to the dual role of the In2O3-x overlayer, which not only prevents the sintering of the Pt2In3 clusters but also modifies the electronic structure of Pt atoms via interfacial interaction, thus facilitating the generation and propylene desorption. Meanwhile, the Pt2In3 intermetallics disrupt large Pt ensembles and introduce electron-rich Pt atoms, suppressing side reactions and enhancing propylene desorption.
{"title":"Promoted propane dehydrogenation over Pt-In intermetallics via classic strong metal-support interaction","authors":"Ya Pan, Chunlan Qin, Ruichao Xu, Liuxin Xu, Shanshan Ruan, Xu Zhang, Kun Zheng, Xiao Han, Jinglin Yuan, Yanna Shui, Lidong Zhang, Zhihu Sun","doi":"10.1016/j.checat.2024.101198","DOIUrl":"https://doi.org/10.1016/j.checat.2024.101198","url":null,"abstract":"The classic strong metal-support interaction (SMSI), characterized by the encapsulation of metal nanoparticles within suboxide layers, is a promising strategy for designing robust catalysts. However, applying this strategy to the high-temperature propane dehydrogenation (PDH) process, which is an important petrochemical process for the industrial production of propylene, is rarely reported. Herein, we demonstrate an SMSI-type PDH catalyst, composed of subnanometric Pt<sub>2</sub>In<sub>3</sub> clusters encapsulated by an In<sub>2</sub>O<sub>3-<em>x</em></sub> overlayer, exhibiting high stability and selectivity. During a 160-h on-stream test, it showed a slight activity decline (<em>k</em><sub>d</sub> = 0.002 h<sup>−1</sup>) and maintained 99.5% propylene selectivity. The excellent performance is attributed to the dual role of the In<sub>2</sub>O<sub>3-<em>x</em></sub> overlayer, which not only prevents the sintering of the Pt<sub>2</sub>In<sub>3</sub> clusters but also modifies the electronic structure of Pt atoms via interfacial interaction, thus facilitating the generation and propylene desorption. Meanwhile, the Pt<sub>2</sub>In<sub>3</sub> intermetallics disrupt large Pt ensembles and introduce electron-rich Pt atoms, suppressing side reactions and enhancing propylene desorption.","PeriodicalId":53121,"journal":{"name":"Chem Catalysis","volume":"32 1","pages":""},"PeriodicalIF":9.4,"publicationDate":"2024-12-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142825752","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 : 2024-12-16DOI: 10.1016/j.checat.2024.101196
Haojing Zhang, Zhaoyi Jiang, Chao Wu, Shibo Xi, Jiajia Song, Xia Long, Zhichuan J. Xu, Ye Zhou
Creating highly effective electrocatalysts requires understanding how materials change under varied electrochemical conditions. While much effort has been devoted to investigating structural changes under operational conditions, deliberately exposing catalysts to non-operational potential regions to electrochemically activate the catalysts and improve the catalytic performance is an underexplored area. Enlightened by the fact that Fe species exhibit pronounced redox responses in alkaline solutions within a potential range that notably falls below the oxygen evolution reaction (OER) potential region, we propose an Fe-redox-oriented electrochemical activation approach to effectively alter the catalysts’ OER performance. This approach, involving pre-cycling catalysts within the Fe-redox-rich potential range, significantly enhances the OER performance of various Fe-containing materials. For the representative Fe3O4@NiO catalyst, this enhancement is primarily attributed to the formation of heterojunctions and a mixed Ni-Fe surface component, which results in a more favorable electronic structure for OER.
{"title":"Fe-redox-oriented electrochemical activation strategy enabling enhancement for efficient oxygen evolution reaction","authors":"Haojing Zhang, Zhaoyi Jiang, Chao Wu, Shibo Xi, Jiajia Song, Xia Long, Zhichuan J. Xu, Ye Zhou","doi":"10.1016/j.checat.2024.101196","DOIUrl":"https://doi.org/10.1016/j.checat.2024.101196","url":null,"abstract":"Creating highly effective electrocatalysts requires understanding how materials change under varied electrochemical conditions. While much effort has been devoted to investigating structural changes under operational conditions, deliberately exposing catalysts to non-operational potential regions to electrochemically activate the catalysts and improve the catalytic performance is an underexplored area. Enlightened by the fact that Fe species exhibit pronounced redox responses in alkaline solutions within a potential range that notably falls below the oxygen evolution reaction (OER) potential region, we propose an Fe-redox-oriented electrochemical activation approach to effectively alter the catalysts’ OER performance. This approach, involving pre-cycling catalysts within the Fe-redox-rich potential range, significantly enhances the OER performance of various Fe-containing materials. For the representative Fe<sub>3</sub>O<sub>4</sub>@NiO catalyst, this enhancement is primarily attributed to the formation of heterojunctions and a mixed Ni-Fe surface component, which results in a more favorable electronic structure for OER.","PeriodicalId":53121,"journal":{"name":"Chem Catalysis","volume":"148 1","pages":""},"PeriodicalIF":9.4,"publicationDate":"2024-12-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142825751","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 : 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
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.
{"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}
Pub 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
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−2PGM 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−2 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.
碱性介质中氢氧化反应（HOR）反应动力学缓慢，阻碍了阴离子交换膜燃料电池（aemfc）的应用。本研究的重点是开发一种高性能碱性HOR催化剂：即b掺杂碳（B-Ru/BC）表面掺杂的Ru纳米颗粒。经电化学活性表面积标准化后，该材料具有0.855 mA cm - 2PGM的交换电流密度，是商用Pt/C的3倍，与商用PtRu/C相当，并且在碱性介质中具有显著提高的CO耐受性。值得注意的是，B-Ru/BC催化剂表现出令人印象深刻的耐久性，在aemfc中实现了1.5 W cm−2的峰值功率密度，超过了商用PtRu/C。理论计算表明，B掺杂对B- ru /BC活性和耐久性的增强有积极作用。本研究介绍了一种低成本的无有机物合成B-Ru/BC催化剂的方法，旨在推动aemfc的商业化，并为可持续能源技术的发展做出贡献。
{"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}
Pub 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
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 CF3-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. In situ infrared and density functional theory calculations indicate that our catalytic system can overcome background reactions to achieve effective enantioselective annulation.
{"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}
Pub Date : 2024-11-21DOI: 10.1016/j.checat.2024.101191
Jinhai Yu, Yingdi Hao, Xiaoqiang Huang
In a recent article published in Nature, 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.
{"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}
Pub Date : 2024-11-21DOI: 10.1016/j.checat.2024.101193
Gabriel F. Costa, Raphael Nagao
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.
{"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}
The efficiency of converting CO2 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 CO2 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 CO2 reduction to CO is significantly improved. An unprecedented faradaic efficiency of 98.3% and a current density of 786.56 mA cm−2 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 (CO2RR) by accelerating the activation of CO2 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 CO2RR.
通过电化学还原途径将二氧化碳转化为其他有价值化学品的效率取决于电催化剂。在这项工作中，提出了一种制备用于二氧化碳电催化还原的氧化锌催化剂的方法，旨在通过改变热处理温度来调节氧化锌纳米棒中的氧空位浓度。结果表明，二氧化碳还原成一氧化碳的远红外效率显著提高。在 500°C 下热处理的氧化锌催化剂达到了前所未有的 98.3% 的法拉第效率和 786.56 mA cm-2 的电流密度。研究表明，氧空位浓度与密度泛函理论相结合，可以通过加速二氧化碳分子的活化和降低二氧化碳形成的能量障碍来改善氧化锌电催化还原二氧化碳（CO2RR）的性能。这项工作有助于开发稳健高效的氧化锌催化剂并将其应用于 CO2RR。
{"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}
Pub Date : 2024-11-21DOI: 10.1016/j.checat.2024.101186
Yifan Zeng, Dongbo Li, Pengtao Xu
In a recent issue of ACS Energy Letters, 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.
{"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}
Pub 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
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 CH3COOK 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.
{"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}
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