4.3 Article

CO spillover on ultrathin bimetallic Rh/Rh-M nanosheets

Journal

CHEM CATALYSIS
Volume 2, Issue 7, Pages 1709-1719

Publisher

CELL PRESS
DOI: 10.1016/j.checat.2022.04.013

Keywords

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Funding

  1. National Key R&D Program of China [2020YFB1505802]
  2. Ministry of Science and Technology of the People's Republic of China [2017YFA0208200, 2016YFA0204100]
  3. National Natural Science Foundation of China [22025108, 2212100020, 51802206]
  4. Guangdong Provincial Natural Science Fund for Distinguished Young Scholars [2021B1515020081]
  5. Priority Academic Program Development of Jiangsu Higher Education Institutions (PAPD)
  6. Xiamen University
  7. Guangzhou Key Laboratory of Low Dimensional Materials and Energy Storage Devices [20195010002]
  8. National Synchrotron Radiation Research Center (NSRRC)
  9. Shanghai Synchrotron Radiation Facility (SSRF), China

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This study demonstrates a method to construct ultrathin Rh/Rh-M nanosheets and investigates the impact of CO spillover on their catalytic performance. Rh/Rh-M nanosheets with CO spillover exhibit higher activity, CO2 selectivity, and resistance to CO poisoning compared to pure Rh nanosheets.
Rh has been regarded as a promising catalyst for ethanol-oxidation reaction (EOR). Nevertheless, Rh is vulnerable to CO poisoning. In this work, we demonstrate a facile strategy for constructing a unique class of ultrathin Rh/Rh-M nanosheets, on which CO can diffuse from the Rh site to theMsite. Detailed experiments, characterizations, and theoretical simulations have been conducted to validate the CO spillover effects on Rh/Rh-M nanosheets (NSs). Moreover, the significance of the CO spillover effect has been demonstrated by catalyzing the EOR, where Rh/Rh-M NSs with CO spillover display much higher activity, higher CO2 selectivity, and stronger resistance to CO poisoning compared with pure Rh NSs. Consequently, the Faraday efficiencies (FEs) of CO2 of the optimal catalyst (e.g., Rh79Co21 NSs) are 70.3% and 75.5% at 0.7 and 0.8 VRHE, respectively, and these aremuch higher than those of Rh NSs (62.0% and 64.3% at 0.7 and 0.8 VRHE, respectively).

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