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

Zhi Li; Yuanjun Chen; Shufang Ji; Yan Tang; Wenxing Chen; Ang Li; Jie Zhao; Yu Xiong; Yuen Wu; Yue Gong; Tao Yao; Wei Liu; Lirong Zheng; Juncai Dong; Yu Wang; Zhongbin Zhuang; Wei Xing; Chun-Ting He; Chao Peng; Weng-Chon Cheong; Qiheng Li; Maolin Zhang; Zheng Chen; Ninghua Fu; Xin Gao; Wei Zhu; Jiawei Wan; Jian Zhang; Lin Gu; Shiqiang Wei; Peijun Hu; Jun Luo; Jun Li; Chen Chen; Qing Peng; Xiangfeng Duan; Yu Huang; Xiao-Ming Chen; Dingsheng Wang; Yadong Li

doi:10.1038/s41557-020-0473-9

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

Nat Chem. 2020 Aug;12(8):764-772. doi: 10.1038/s41557-020-0473-9. Epub 2020 Jun 15.

Authors

Zhi Li^#¹, Yuanjun Chen^#¹, Shufang Ji^#¹, Yan Tang¹, Wenxing Chen¹, Ang Li², Jie Zhao³, Yu Xiong¹, Yuen Wu⁴, Yue Gong⁵, Tao Yao⁶, Wei Liu⁶, Lirong Zheng⁷, Juncai Dong⁷, Yu Wang⁸, Zhongbin Zhuang⁹, Wei Xing^{10

11}, Chun-Ting He¹², Chao Peng^{13

14}, Weng-Chon Cheong¹, Qiheng Li¹, Maolin Zhang¹, Zheng Chen¹, Ninghua Fu¹, Xin Gao¹, Wei Zhu¹, Jiawei Wan¹, Jian Zhang¹, Lin Gu⁵, Shiqiang Wei⁶, Peijun Hu^{13

14}, Jun Luo¹⁵, Jun Li¹, Chen Chen¹, Qing Peng¹, Xiangfeng Duan^{16

17}, Yu Huang^{17

18}, Xiao-Ming Chen¹², Dingsheng Wang¹⁹, Yadong Li^{20

21}

Affiliations

¹ Department of Chemistry, Tsinghua University, Beijing, China.
² Beijing Key Laboratory of Microstructure and Property of Advanced Materials, Beijing University of Technology, Beijing, China.
³ Key Laboratory for Advanced Materials and Feringa Nobel Prize Scientist Joint Research Center, Chemistry Department, School of Chemistry and Molecular Engineering, East China University of Science and Technology, Shanghai, China.
⁴ Department of Chemistry, University of Science and Technology of China, Hefei, China.
⁵ Institute of Physics, Chinese Academy of Sciences, Beijing, China.
⁶ National Synchrotron Radiation Laboratory, University of Science and Technology of China, Hefei, China.
⁷ Beijing Synchrotron Radiation Facility, Institute of High Energy Physics, Chinese Academy of Sciences, Beijing, China.
⁸ Shanghai Synchrotron Radiation Facility, Shanghai Advanced Research Institute, Chinese Academy of Sciences, Shanghai, China.
⁹ State Key Lab of Organic-Inorganic Composites and Beijing Advanced Innovation Center for Soft Matter Science and Engineering, Beijing University of Chemical Technology, Beijing, China.
¹⁰ Laboratory of Advanced Chemical Power Sources, Changchun Institute of Applied Chemistry, Chinese Academy of Sciences, Changchun, China.
¹¹ Jilin Province Key Laboratory of Low Carbon Chemical Power Sources, Changchun, China.
¹² MOE Key Laboratory of Bioinorganic and Synthetic Chemistry, School of Chemistry, Sun Yat-Sen Unversity, Guangzhou, China.
¹³ Key Laboratory for Advanced Materials, Center for Computational Chemistry and Research Institute of Industrial Catalysis, East China University of Science and Technology, Shanghai, China.
¹⁴ School of Chemistry and Chemical Engineering, Queen's University Belfast, Belfast, UK.
¹⁵ Center for Electron Microscopy, TUT-FEI Joint Laboratory, Tianjin Key Laboratory of Advanced Functional Porous Materials, Institute for New Energy Materials and Low-Carbon Technologies, School of Materials Science and Engineering, Tianjin University of Technology, Tianjin, China.
¹⁶ Department of Chemistry and Biochemistry, University of California, Los Angeles, CA, USA.
¹⁷ California NanoSystems Institute, University of California, Los Angeles, CA, USA.
¹⁸ Department of Materials Science and Engineering, University of California, Los Angeles, CA, USA.
¹⁹ Department of Chemistry, Tsinghua University, Beijing, China. wangdingsheng@mail.tsinghua.edu.cn.
²⁰ Department of Chemistry, Tsinghua University, Beijing, China. ydli@mail.tsinghua.edu.cn.
²¹ Department of Chemistry, University of Science and Technology of China, Hefei, China. ydli@mail.tsinghua.edu.cn.

^# Contributed equally.

PMID: 32541950
DOI: 10.1038/s41557-020-0473-9

Abstract

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 (M₁/CN, M = Pt, Ir, Pd, Ru, Mo, Ga, Cu, Ni, Mn). The iridium variant Ir₁/CN electrocatalyses the formic acid oxidation reaction with a mass activity of 12.9 [Formula: see text] whereas an Ir/C nanoparticle catalyst is almost inert (~4.8 × 10^-3 [Formula: see text]). The activity of Ir₁/CN is also 16 and 19 times greater than those of Pd/C and Pt/C, respectively. Furthermore, Ir₁/CN displays high tolerance to CO poisoning. First-principle density functional theory reveals that the properties of Ir₁/CN stem from the spatial isolation of iridium sites and from the modified electronic structure of iridium with respect to a conventional nanoparticle catalyst.