Crystal-phase-controlled PtSn intermetallic nanowires for efficient methanol oxidation  

作　　者：Siyu Cao Mengfan Li Zihan Guo Li Gong Yangfan Lu Wenhua Zhang Yu Ni Lei Gao Chao Ma Hongwen Huang 

机构地区：[1]College of Materials Science and Engineering,Changsha University of Science and Technology,Changsha 410114,China [2]College of Materials Science and Engineering,Hunan University,Changsha 410082,China [3]Zhejiang Provincial Engineering Research Center of Oxide Semiconductors for Environmental and Optoelectronic Applications,Institute of Wenzhou,Zhejiang University,Wenzhou 325006,China [4]State Key Laboratory of Silicon Materials,School of Materials Science and Engineering,Zhejiang University,Hangzhou 310027,China [5]Department of Chemical Physics,University of Science and Technology of China,Hefei 230026,China [6]China Power Engineering Consulting Group Co.,LTD,Beijing 100120,China [7]Shenzhen Research Institute of Hunan University,Shenzhen 518055,China

出　　处：《Science China Chemistry》2024年第12期4142-4148,共7页中国科学（化学英文版）

基　　金：supported by the National Natural Science Foundation of China(22322902,U22A20396,22211540385,22309050);the National Key Research and Development Program of China(2021YFA1502000);the Jiebang Guashuai Project of Changsha City(kq2301009);the Guangdong Basic and Applied Basic Research Foundation(2024A1515012350);the Shenzhen Science and Technology Program(JCYJ20210324120800002,JCYJ20220818100012025,JCYJ2023080712-2007015);the China Postdoctoral Science Foundation(2023T160205,2023M741118);the Postdoctoral Research Fund from Institute of Wenzhou,Zhejiang University(XMGL-KJZX-202308)。

摘　　要：Developing highly efficient Pt-based methanol oxidation reaction(MOR)catalysts is pivotal for direct methanol fuel cells.Phase engineering of nanomaterials offers a promising strategy to improve their catalytic performance,yet achieving phase modulation in one-dimensional nanowires(NWs)remains a great challenge.Herein,we report a facile and one-pot synthesis approach for the crystal-phase-controlled Pt-Sn intermetallic nanowires(NWs),realizing the crystal-phases regulation of face-centered cubic Pt_(3)Sn intermetallic NWs(FCC-Pt_(3)Sn INTNWs)and hexagonal close-packed Pt Sn intermetallic NWs(HCP-PtSn INTNWs)by adjusting the amounts of Sn precursors.Notably,the FCC-Pt_(3)Sn INTNWs exhibit high mass and specific activities of 6.4 A mg_(Pt)^(-1)and 11.8 mA cm^(-2),respectively,surpassing its counterparts,the HCP-PtSn INTNWs and commercial Pt/C catalysts.After a 10,000 s durability test,the FCC-Pt_(3)Sn INTNWs still maintain a mass activity of 5.6 A mg_(Pt)^(-1),which is 24.3 times higher than that of commercial Pt/C catalyst.This dramatic enhancement of MOR performance is primarily attributed to the phasecontrolled structure and accelerated removal of CO intermediates(CO*).Theoretical calculations and CO stripping experiments demonstrate that the FCC-Pt_(3)Sn INTNWs lower the energy barrier for converting CO*into COOH*by reducing CO*binding and enhancing OH adsorption,thus significantly improving the MOR activity,CO tolerance,and stability.

关 键 词：Pt-Sn intermetallic nanowires crystal phase methanol oxidation reaction anti-CO poisoning 

分 类 号：TB383.1[一般工业技术—材料科学与工程] TQ426[化学工程]