Accurate descriptions of molecule-surface interactions in electrocatalytic CO2 reduction on the copper surfaces

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作者：
Zheng Chen
Zhangyun Liu
Xin Xu
机构：
[1] Fudan University,Collaborative Innovation Center of Chemistry for Energy Materials, Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials, MOE Key Laboratory of Computational Physical Sciences, Department of Chemistry
[2] Hefei National Laboratory,undefined
来源：
Nature Communications | / 14卷
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摘要：
Copper-based catalysts play a pivotal role in many industrial processes and hold a great promise for electrocatalytic CO2 reduction reaction into valuable chemicals and fuels. Towards the rational design of catalysts, the growing demand on theoretical study is seriously at odds with the low accuracy of the most widely used functionals of generalized gradient approximation. Here, we present results using a hybrid scheme that combines the doubly hybrid XYG3 functional and the periodic generalized gradient approximation, whose accuracy is validated against an experimental set on copper surfaces. A near chemical accuracy is established for this set, which, in turn, leads to a substantial improvement for the calculated equilibrium and onset potentials as against the experimental values for CO2 reduction to CO on Cu(111) and Cu(100) electrodes. We anticipate that the easy use of the hybrid scheme will boost the predictive power for accurate descriptions of molecule-surface interactions in heterogeneous catalysis.
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  • [1] Campbell CT(1987)Surface science studies of the water–gas shift reaction on a model Cu(111) catalyst J. Vac. Sci. Technol. A 5 810-813
  • [2] Koel BE(2012)The active site of methanol synthesis over Cu/ZnO/Al Science 336 893-897
  • [3] Daube KA(2014)O Science 345 546-550
  • [4] Behrens M(2017) industrial catalysts Science 355 1296-1299
  • [5] Graciani J(2019)Highly active copper-ceria and copper-ceria-titania catalysts for methanol synthesis from CO Chem. Rev. 119 7610-7672
  • [6] Kattel S(2019)Active sites for CO Nat. Energy 4 732-745
  • [7] Ramírez PJ(2010) hydrogenation to methanol on Cu/ZnO catalysts Energy Environ. Sci. 3 1311-1315
  • [8] Chen JG(2016)Progress and perspectives of electrochemical CO J. Am. Chem. Soc. 138 13802-13805
  • [9] Rodriguez JA(2019) reduction on copper in aqueous electrolyte Chem. Rev. 119 6631-6669
  • [10] Liu P(2009)Advances and challenges in understanding the electrocatalytic conversion of carbon dioxide to fuels Nat. Chem. 1 37-46
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