Atomically Dispersed Transition Metals on Carbon Nanotubes with Ultrahigh Loading for Selective Electrochemical Carbon Dioxide Reduction

Yi Cheng; Shiyong Zhao; Bernt Johannessen; Jean-Pierre Veder; Martin Saunders; Matthew R Rowles; Min Cheng; Chang Liu; Matthew F Chisholm; Roland De Marco; Hui-Ming Cheng; Shi-Ze Yang; San Ping Jiang

doi:10.1002/adma.201706287

Atomically Dispersed Transition Metals on Carbon Nanotubes with Ultrahigh Loading for Selective Electrochemical Carbon Dioxide Reduction

Adv Mater. 2018 Mar;30(13):e1706287. doi: 10.1002/adma.201706287. Epub 2018 Feb 9.

Authors

Yi Cheng¹, Shiyong Zhao¹, Bernt Johannessen², Jean-Pierre Veder³, Martin Saunders⁴, Matthew R Rowles³, Min Cheng⁵, Chang Liu⁵, Matthew F Chisholm⁶, Roland De Marco^{1

7

8}, Hui-Ming Cheng^{5

9

10}, Shi-Ze Yang⁶, San Ping Jiang¹

Affiliations

¹ Fuels and Energy Technology Institute and Department of Chemical Engineering, Curtin University, Perth, Western Australia, 6102, Australia.
² Australian Synchrotron, Clayton, Victoria, 3168, Australia.
³ John de Laeter Centre, Curtin University, Perth, Western Australia, 6102, Australia.
⁴ Centre for Microscopy, Characterization and Analysis (CMCA) and School of Molecular Sciences, The University of Western Australia, Perth, Western Australia, 6009, Australia.
⁵ Advanced Carbon Division, Shenyang National Laboratory for Materials Science, Institute of Metal Research, Chinese Academy of Sciences, Shenyang, Liaoning, 110016, China.
⁶ Materials Science and Technology Division, Oak Ridge National Laboratory, Oak Ridge, TN, 37831, USA.
⁷ Faculty of Science, Health, Education and Engineering, University of Sunshine Coast, Maroochydore DC, Queensland, 4558, Australia.
⁸ School of Chemistry and Molecular Biosciences, The University of Queensland, Brisbane, Queensland, 4072, Australia.
⁹ Low-Dimensional Material and Device Lab, Tsinghua-Berkeley Shenzhen Institute, Tsinghua University, Shenzhen, 518055, P. R. China.
¹⁰ Center of Excellence in Environmental Studies (CEES), King Abdulaziz University, Jeddah, 21589, Saudi Arabia.

PMID: 29423964
DOI: 10.1002/adma.201706287

Abstract

Single-atom catalysts (SACs) are the smallest entities for catalytic reactions with projected high atomic efficiency, superior activity, and selectivity; however, practical applications of SACs suffer from a very low metal loading of 1-2 wt%. Here, a class of SACs based on atomically dispersed transition metals on nitrogen-doped carbon nanotubes (MSA-N-CNTs, where M = Ni, Co, NiCo, CoFe, and NiPt) is synthesized with an extraordinarily high metal loading, e.g., 20 wt% in the case of NiSA-N-CNTs, using a new multistep pyrolysis process. Among these materials, NiSA-N-CNTs show an excellent selectivity and activity for the electrochemical reduction of CO₂ to CO, achieving a turnover frequency (TOF) of 11.7 s^-1 at -0.55 V (vs reversible hydrogen electrode (RHE)), two orders of magnitude higher than Ni nanoparticles supported on CNTs.

Keywords: carbon dioxide reduction; carbon monoxide; single-atom catalysts; transition metals.