文献类型：期刊文献

英文题名：Iridium single-atom catalyst on nitrogen-doped carbon for formic acid oxidation synthesized using a general host-guest strategy

作者：Li, Zhi[1];Chen, Yuanjun[1];Ji, Shufang[1];Tang, Yan[1];Chen, Wenxing[1];Li, Ang[2];Zhao, Jie[3];Xiong, Yu[1];Wu, Yuen[4];Gong, Yue[5];Yao, Tao[6];Liu, Wei[6];Zheng, Lirong[7];Dong, Juncai[7];Wang, Yu[8];Zhuang, Zhongbin[9,10];Xing, Wei[11,12];He, Chun-Ting[13];Peng, Chao[14,15,16];Cheong, Weng-Chon[1];Li, Qiheng[1];Zhang, Maolin[1];Chen, Zheng[1];Fu, Ninghua[1];Gao, Xin[1];Zhu, Wei[1];Wan, Jiawei[1];Zhang, Jian[1];Gu, Lin[5];Wei, Shiqiang[6];Hu, Peijun[14,15,16];Luo, Jun[17];Li, Jun[1];Chen, Chen[1];Peng, Qing[1];Duan, Xiangfeng[18,19];Huang, Yu[19,20];Chen, Xiao-Ming[13];Wang, Dingsheng[1];Li, Yadong[1,4]

机构：[1]Tsinghua Univ, Dept Chem, Beijing, Peoples R China;[2]Beijing Univ Technol, Beijing Key Lab Microstruct & Property Adv Mat, Beijing, Peoples R China;[3]East China Univ Sci & Technol, Sch Chem & Mol Engn, Key Lab Adv Mat & Feringa Nobel Prize Scientist, Joint Res Ctr,Chem Dept, Shanghai, Peoples R China;[4]Univ Sci & Technol China, Dept Chem, Hefei, Peoples R China;[5]Chinese Acad Sci, Inst Phys, Beijing, Peoples R China;[6]Univ Sci & Technol China, Natl Synchrotron Radiat Lab, Hefei, Peoples R China;[7]Chinese Acad Sci, Inst High Energy Phys, Beijing Synchrotron Radiat Facil, Beijing, Peoples R China;[8]Chinese Acad Sci, Shanghai Adv Res Inst, Shanghai Synchrotron Radiat Facil, Shanghai, Peoples R China;[9]Beijing Univ Chem Technol, State Key Lab Organ Inorgan Composites, Beijing, Peoples R China;[10]Beijing Univ Chem Technol, Beijing Adv Innovat Ctr Soft Matter Sci & Engn, Beijing, Peoples R China;[11]Chinese Acad Sci, Changchun Inst Appl Chem, Lab Adv Chem Power Sources, Changchun, Peoples R China;[12]Jilin Prov Key Lab Low Carbon Chem Power Sources, Changchun, Peoples R China;[13]Sun Yat Sen Unvers, MOE Key Lab Bioinorgan & Synthet Chem, Sch Chem, Guangzhou, Peoples R China;[14]East China Univ Sci & Technol, Ctr Computat Chem, Key Lab Adv Mat, Shanghai, Peoples R China;[15]East China Univ Sci & Technol, Res Inst Ind Catalysis, Shanghai, Peoples R China;[16]Queens Univ Belfast, Sch Chem & Chem Engn, Belfast, Antrim, North Ireland;[17]Tianjin Univ Technol, Inst New Energy Mat & Low Carbon Technol, Tianjin Key Lab Adv Funct Porous Mat, Ctr Electron Microscopy,TUT FEI Joint Lab,Sch Mat, Tianjin, Peoples R China;[18]Univ Calif Los Angeles, Dept Chem & Biochem, 405 Hilgard Ave, Los Angeles, CA 90024 USA;[19]Univ Calif Los Angeles, Calif NanoSyst Inst, Los Angeles, CA USA;[20]Univ Calif Los Angeles, Dept Mat Sci & Engn, Los Angeles, CA 90024 USA

年份：2020

卷号：12

期号：8

外文期刊名：NATURE CHEMISTRY

收录：;WOS:【SCI-EXPANDED(收录号:WOS:000540397300003)】；

基金：The authors thank M.F. Li (University of California at Los Angeles) who provided insight and expertise that greatly assisted the research. This work was supported by the National Key R&D Program of China (grant no. 2018YFA0702003), the National Natural Science Foundation of China (grant nos. 21890383, 21671117, 21871159) and the Beijing Municipal Science & Technology Commission (grant no. Z191100007219003).

语种：英文

摘要：Single-atom catalysts not only maximize metal atom efficiency, they also display properties that are considerably different to their more conventional nanoparticle equivalents, making them a promising family of materials to investigate. Herein we developed a general host-guest strategy to fabricate various metal single-atom catalysts on nitrogen-doped carbon (M-1/CN, M = Pt, Ir, Pd, Ru, Mo, Ga, Cu, Ni, Mn). The iridium variant Ir-1/CN electrocatalyses the formic acid oxidation reaction with a mass activity of 12.9 Amg(Ir)(-1) whereas an Ir/C nanoparticle catalyst is almost inert (similar to 4.8 x 10(-3) Amg(Ir)(-1)). The activity of Ir-1/CN is also 16 and 19 times greater than those of Pd/C and Pt/C, respectively. Furthermore, Ir-1/CN displays high tolerance to CO poisoning. First-principle density functional theory reveals that the properties of Ir-1/CN stem from the spatial isolation of iridium sites and from the modified electronic structure of iridium with respect to a conventional nanoparticle catalyst.