{"title":"zif衍生PtCu/N-DC十二面体:低铂负载下甲醇氧化活性和抗中毒能力的协同增强机制","authors":"Xue Li, Jingjia Zhang, Qianhui Li, Shuimei Yang, Chengze Wei, Feng Zhang, Zhenbo Wang","doi":"10.1016/j.apsusc.2025.163388","DOIUrl":null,"url":null,"abstract":"Preparing low-cost and high-activity methanol oxidation reaction (MOR) electrocatalysts is a key approach for renewable energy technologies. However, due to the high price and instability of platinum-based catalysts, the addition of transition metals to alloy catalysts on the basis of platinum is a prevalent strategy to improve catalytic activity and stability. Herein, we prepared a PtCu alloy catalyst that is highly dispersed on an N-doped carbon dodecahedron (PtCu/N-DC) by a simple pyrolysis method. The experiments demonstrate that the robust interaction between N-doped porous carbon support and PtCu alloy imparts strong stability to the catalyst. At the same time, there is a strong interaction between Cu atom and Pt atom, doping with Cu can adjust its surface electronic configuration of Pt, thereby improving the MOR performance of the catalyst. With a platinum loading of just 10 % compared to the 20 % in commercial Pt/C, PtCu/N-DC exhibits mass activity and specific activity that are 4.1 times and 5.8 times higher, with significant catalytic activity and a high level of resistance to carbon monoxide poisoning. Theoretical analysis indicates that the PtCu/N-DC catalyst exhibits a low energy barrier during the critical steps, which aligns with the enhanced electrocatalytic activity demonstrated in the experimental findings.","PeriodicalId":247,"journal":{"name":"Applied Surface Science","volume":"96 1","pages":""},"PeriodicalIF":6.3000,"publicationDate":"2025-05-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Zif-derived PtCu/N-DC dodecahedrons: Synergistic enhancement mechanism of methanol oxidation activity and poisoning resistance under low platinum loading\",\"authors\":\"Xue Li, Jingjia Zhang, Qianhui Li, Shuimei Yang, Chengze Wei, Feng Zhang, Zhenbo Wang\",\"doi\":\"10.1016/j.apsusc.2025.163388\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"Preparing low-cost and high-activity methanol oxidation reaction (MOR) electrocatalysts is a key approach for renewable energy technologies. However, due to the high price and instability of platinum-based catalysts, the addition of transition metals to alloy catalysts on the basis of platinum is a prevalent strategy to improve catalytic activity and stability. Herein, we prepared a PtCu alloy catalyst that is highly dispersed on an N-doped carbon dodecahedron (PtCu/N-DC) by a simple pyrolysis method. The experiments demonstrate that the robust interaction between N-doped porous carbon support and PtCu alloy imparts strong stability to the catalyst. At the same time, there is a strong interaction between Cu atom and Pt atom, doping with Cu can adjust its surface electronic configuration of Pt, thereby improving the MOR performance of the catalyst. With a platinum loading of just 10 % compared to the 20 % in commercial Pt/C, PtCu/N-DC exhibits mass activity and specific activity that are 4.1 times and 5.8 times higher, with significant catalytic activity and a high level of resistance to carbon monoxide poisoning. Theoretical analysis indicates that the PtCu/N-DC catalyst exhibits a low energy barrier during the critical steps, which aligns with the enhanced electrocatalytic activity demonstrated in the experimental findings.\",\"PeriodicalId\":247,\"journal\":{\"name\":\"Applied Surface Science\",\"volume\":\"96 1\",\"pages\":\"\"},\"PeriodicalIF\":6.3000,\"publicationDate\":\"2025-05-03\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Applied Surface Science\",\"FirstCategoryId\":\"88\",\"ListUrlMain\":\"https://doi.org/10.1016/j.apsusc.2025.163388\",\"RegionNum\":2,\"RegionCategory\":\"材料科学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q2\",\"JCRName\":\"CHEMISTRY, PHYSICAL\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Applied Surface Science","FirstCategoryId":"88","ListUrlMain":"https://doi.org/10.1016/j.apsusc.2025.163388","RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q2","JCRName":"CHEMISTRY, PHYSICAL","Score":null,"Total":0}
Zif-derived PtCu/N-DC dodecahedrons: Synergistic enhancement mechanism of methanol oxidation activity and poisoning resistance under low platinum loading
Preparing low-cost and high-activity methanol oxidation reaction (MOR) electrocatalysts is a key approach for renewable energy technologies. However, due to the high price and instability of platinum-based catalysts, the addition of transition metals to alloy catalysts on the basis of platinum is a prevalent strategy to improve catalytic activity and stability. Herein, we prepared a PtCu alloy catalyst that is highly dispersed on an N-doped carbon dodecahedron (PtCu/N-DC) by a simple pyrolysis method. The experiments demonstrate that the robust interaction between N-doped porous carbon support and PtCu alloy imparts strong stability to the catalyst. At the same time, there is a strong interaction between Cu atom and Pt atom, doping with Cu can adjust its surface electronic configuration of Pt, thereby improving the MOR performance of the catalyst. With a platinum loading of just 10 % compared to the 20 % in commercial Pt/C, PtCu/N-DC exhibits mass activity and specific activity that are 4.1 times and 5.8 times higher, with significant catalytic activity and a high level of resistance to carbon monoxide poisoning. Theoretical analysis indicates that the PtCu/N-DC catalyst exhibits a low energy barrier during the critical steps, which aligns with the enhanced electrocatalytic activity demonstrated in the experimental findings.
期刊介绍:
Applied Surface Science covers topics contributing to a better understanding of surfaces, interfaces, nanostructures and their applications. The journal is concerned with scientific research on the atomic and molecular level of material properties determined with specific surface analytical techniques and/or computational methods, as well as the processing of such structures.