Journal
ADVANCED MATERIALS
Volume 30, Issue 13, Pages -Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/adma.201706287
Keywords
carbon dioxide reduction; carbon monoxide; single-atom catalysts; transition metals
Categories
Funding
- Australian Research Council Discovery Project Funding Scheme [DP150102044, DP150102025, DP180100568, DP180100731]
- Australian Research Council LIEF grant [LE120100026]
- ORNL's Center for Nanophase Materials Sciences - Scientific User Facilities Division of U.S. Department of Energy
- Office of Science of the U.S. Department of Energy [DE-AC02-05CH11231]
- National Science Foundation [ACI-1053575]
- National Natural Science Foundation of China [51521091]
- U.S. Department of Energy, Office of Science, Basic Energy Sciences, Materials Science and Engineering
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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 nano-particles supported on CNTs.
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