Bin-Bin Feng, Ke-Ke Chang, Wan-Feng Xiong, Duan-Hui Si, Shui-Ying Gao, Hong-Fang Li, Rong Cao
{"title":"铜/镍多位点串联催化促进氧还原反应","authors":"Bin-Bin Feng, Ke-Ke Chang, Wan-Feng Xiong, Duan-Hui Si, Shui-Ying Gao, Hong-Fang Li, Rong Cao","doi":"10.1007/s40843-024-2952-2","DOIUrl":null,"url":null,"abstract":"<p>The special electronic characteristics and high atom usage efficiency of metal-nitrogen-carbon (M-N-C) materials have made them extremely attractive for oxygen reduction reactions (ORRs). However, it is inevitable that hydrogen peroxide (H<sub>2</sub>O<sub>2</sub>) will be formed <i>via</i> the two-electron pathway in ORRs. Herein, the Cu nanoparticles (NPs) have been encapsulated into Ni doped hollow mesoporous carbon spheres (Ni-HMCS) to reduce the generation of H<sub>2</sub>O<sub>2</sub> in ORR. Electrochemical tests confirm that the introduction of Cu NPs improves the ORR performance greatly. The obtained Cu/Ni-HMCS exhibits a half-wave potential of 0.82 V <i>vs.</i> reversible hydrogen electrode and a limited current density of 5.5 mA cm<sup>−2</sup>, which is comparable with the commercial Pt/C. Moreover, Cu/Ni-HMCS has been used in Zn-air battery, demonstrating a high power density of 161 mW cm<sup>−2</sup> and a long-term recharge capability (50 h at 5 mA cm<sup>−2</sup>). The theoretical calculation proposes a tandem catalysis pathway for Cu/Ni multi-sites catalysis, that is, H<sub>2</sub>O<sub>2</sub> released from the Ni–N<sub>4</sub> and Cu–N<sub>4</sub> sites migrates to the Cu (111) face, on which the captive H<sub>2</sub>O<sub>2</sub> is further reduced to H<sub>2</sub>O. This work demonstrates an interesting tandem catalytic pathway of dual-metal multi-sites for ORR, which provides an insight into the development of effective fuel cell electrocatalysts.</p>","PeriodicalId":773,"journal":{"name":"Science China Materials","volume":null,"pages":null},"PeriodicalIF":6.8000,"publicationDate":"2024-07-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Tandem catalysis of Cu/Ni multi-sites promotes oxygen reduction reaction\",\"authors\":\"Bin-Bin Feng, Ke-Ke Chang, Wan-Feng Xiong, Duan-Hui Si, Shui-Ying Gao, Hong-Fang Li, Rong Cao\",\"doi\":\"10.1007/s40843-024-2952-2\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<p>The special electronic characteristics and high atom usage efficiency of metal-nitrogen-carbon (M-N-C) materials have made them extremely attractive for oxygen reduction reactions (ORRs). However, it is inevitable that hydrogen peroxide (H<sub>2</sub>O<sub>2</sub>) will be formed <i>via</i> the two-electron pathway in ORRs. Herein, the Cu nanoparticles (NPs) have been encapsulated into Ni doped hollow mesoporous carbon spheres (Ni-HMCS) to reduce the generation of H<sub>2</sub>O<sub>2</sub> in ORR. Electrochemical tests confirm that the introduction of Cu NPs improves the ORR performance greatly. The obtained Cu/Ni-HMCS exhibits a half-wave potential of 0.82 V <i>vs.</i> reversible hydrogen electrode and a limited current density of 5.5 mA cm<sup>−2</sup>, which is comparable with the commercial Pt/C. Moreover, Cu/Ni-HMCS has been used in Zn-air battery, demonstrating a high power density of 161 mW cm<sup>−2</sup> and a long-term recharge capability (50 h at 5 mA cm<sup>−2</sup>). The theoretical calculation proposes a tandem catalysis pathway for Cu/Ni multi-sites catalysis, that is, H<sub>2</sub>O<sub>2</sub> released from the Ni–N<sub>4</sub> and Cu–N<sub>4</sub> sites migrates to the Cu (111) face, on which the captive H<sub>2</sub>O<sub>2</sub> is further reduced to H<sub>2</sub>O. This work demonstrates an interesting tandem catalytic pathway of dual-metal multi-sites for ORR, which provides an insight into the development of effective fuel cell electrocatalysts.</p>\",\"PeriodicalId\":773,\"journal\":{\"name\":\"Science China Materials\",\"volume\":null,\"pages\":null},\"PeriodicalIF\":6.8000,\"publicationDate\":\"2024-07-05\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Science China Materials\",\"FirstCategoryId\":\"88\",\"ListUrlMain\":\"https://doi.org/10.1007/s40843-024-2952-2\",\"RegionNum\":2,\"RegionCategory\":\"材料科学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q1\",\"JCRName\":\"MATERIALS SCIENCE, MULTIDISCIPLINARY\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Science China Materials","FirstCategoryId":"88","ListUrlMain":"https://doi.org/10.1007/s40843-024-2952-2","RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"MATERIALS SCIENCE, MULTIDISCIPLINARY","Score":null,"Total":0}
Tandem catalysis of Cu/Ni multi-sites promotes oxygen reduction reaction
The special electronic characteristics and high atom usage efficiency of metal-nitrogen-carbon (M-N-C) materials have made them extremely attractive for oxygen reduction reactions (ORRs). However, it is inevitable that hydrogen peroxide (H2O2) will be formed via the two-electron pathway in ORRs. Herein, the Cu nanoparticles (NPs) have been encapsulated into Ni doped hollow mesoporous carbon spheres (Ni-HMCS) to reduce the generation of H2O2 in ORR. Electrochemical tests confirm that the introduction of Cu NPs improves the ORR performance greatly. The obtained Cu/Ni-HMCS exhibits a half-wave potential of 0.82 V vs. reversible hydrogen electrode and a limited current density of 5.5 mA cm−2, which is comparable with the commercial Pt/C. Moreover, Cu/Ni-HMCS has been used in Zn-air battery, demonstrating a high power density of 161 mW cm−2 and a long-term recharge capability (50 h at 5 mA cm−2). The theoretical calculation proposes a tandem catalysis pathway for Cu/Ni multi-sites catalysis, that is, H2O2 released from the Ni–N4 and Cu–N4 sites migrates to the Cu (111) face, on which the captive H2O2 is further reduced to H2O. This work demonstrates an interesting tandem catalytic pathway of dual-metal multi-sites for ORR, which provides an insight into the development of effective fuel cell electrocatalysts.
期刊介绍:
Science China Materials (SCM) is a globally peer-reviewed journal that covers all facets of materials science. It is supervised by the Chinese Academy of Sciences and co-sponsored by the Chinese Academy of Sciences and the National Natural Science Foundation of China. The journal is jointly published monthly in both printed and electronic forms by Science China Press and Springer. The aim of SCM is to encourage communication of high-quality, innovative research results at the cutting-edge interface of materials science with chemistry, physics, biology, and engineering. It focuses on breakthroughs from around the world and aims to become a world-leading academic journal for materials science.