Atomically Dispersed Transition Metals on Carbon Nanotubes with Ultrahigh Loading for Selective Electrochemical Carbon Dioxide Reduction |
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| Authors: | 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 |
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| Affiliation: | 1. Fuels and Energy Technology Institute and Department of Chemical Engineering, Curtin University, Perth, Western Australia, Australia;2. Australian Synchrotron, Clayton, Victoria, Australia;3. John de Laeter Centre, Curtin University, Perth, Western Australia, Australia;4. Centre for Microscopy, Characterization and Analysis (CMCA) and School of Molecular Sciences, The University of Western Australia, Perth, Western Australia, Australia;5. Advanced Carbon Division, Shenyang National Laboratory for Materials Science, Institute of Metal Research, Chinese Academy of Sciences, Shenyang, Liaoning, China;6. Materials Science and Technology Division, Oak Ridge National Laboratory, Oak Ridge, TN, USA;7. Faculty of Science, Health, Education and Engineering, University of Sunshine Coast, Maroochydore DC, Queensland, Australia;8. School of Chemistry and Molecular Biosciences, The University of Queensland, Brisbane, Queensland, Australia;9. Low‐Dimensional Material and Device Lab, Tsinghua‐Berkeley Shenzhen Institute, Tsinghua University, Shenzhen, P. R. China;10. Center of Excellence in Environmental Studies (CEES), King Abdulaziz University, Jeddah, Saudi Arabia |
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| 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. |
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| Keywords: | carbon dioxide reduction carbon monoxide single‐atom catalysts transition metals |
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