Semimetal-triggered covalent interaction in Pt-based intermetallics for fuel-cell electrocatalysis  

作　　者：Han Cheng Renjie Gui Chen Chen Si Liu Xuemin Cao Yifan Yin Ruize Ma Wenjie Wang Tianpei Zhou Xusheng Zheng Wangsheng Chu Yi Xie Changzheng Wu 

机构地区：[1]Key Laboratory of Precision and Intelligent Chemistry,School of Chemistry and Materials Science,University of Science and Technology of China,Hefei 230029,China [2]National Synchrotron Radiation Laboratory,University of Science and Technologyof China,Hefei 230029,China [3]Chemistry Experiment Teaching Center,School of Chemistry and Materials Science,Universityof Science and Technology of China,Hefei 230029,China [4]Institute of Energy,Hefei Comprehensive National Science Center,Hefei 230026,China

出　　处：《National Science Review》2024年第8期269-276,共8页国家科学评论（英文版）

基　　金：supported by the Chinese Academy of Sciences Project for Young Scientists in Basic Research (YSBR-070);the National Natural Science Foundation of China (21925110,21890750,U2032161,12147105,22201273 and 22205226);the National Key Research and Development Program of China (2022YFA1203601);the University of Science and Technology of China (USTC)Research Funds of the Double First-Class Initiative (YD2060002004 and WK2060000047);the University Synergy Innovation Program of Anhui Province (GXXT-2022-006).

摘　　要：Platinum-based intermetallic compounds(IMCs)play a vital role as electrocatalysts in a range of energy and environmental technologies,such as proton exchange membrane fuel cells.However,the synthesis of IMCs necessitates recombination of ordered Pt-M metallic bonds with high temperature driving,which is generally accompanied by side effects for catalysts'structure and performance.In this work,we highlight that semimetal atoms can trigger covalent interactions to break the synthesis-temperature limitation of platinum-based intermetallic compounds and benefit fuel-cell electrocatalysis.Attributed to partial fllings of p-block in semimetal elements,the strong covalent interaction of d-p backbonding can benefit the recombination of ordered Pt-M metallic bonds(PtGe,PtSb and PtTe)in the synthesis process.Moreover,this covalent interaction in metallic states can further promote both electron transport and orbital fillings of active sites in fuel cells.The semimetal-Pt IMCs were obtained with a temperature 300 K lower than that needed for the synthesis of metal-Pt intermetallic compounds and reached the highest CO-tolerant oxygen reduction activity(0.794 A mg^(-1) at 0.9 V and 5.1%decay under CO poisoning)among reported electrocatalysts.We anticipate that semimetal-Pt IMCs will offer new insights for the rational design of advanced electrocatalysts for fuel cells.

关 键 词：SEMIMETALS Pt intermetallics covalent interaction oxygen reduction reaction CO tolerance fuel cells 

分 类 号：O643.3[理学—物理化学] TM91[理学—化学]