4.5 Article

Atomic alkali metal anchoring on graphdiyne as single-atom catalysts for capture and conversion of CO2 to HCOOH

Journal

MOLECULAR CATALYSIS
Volume 494, Issue -, Pages -

Publisher

ELSEVIER
DOI: 10.1016/j.mcat.2020.111142

Keywords

Graphdiyne; Alkali metal; Single-atom catalysts; CO2 electroreduction; First principles

Funding

  1. National Natural Science Foundation of China [61674053]
  2. Natural Science Foundation of Henan Province [162300410325]
  3. Program for Science & Technology Innovation Talents in Universities of Henan Province [18HASTIT030]
  4. Henan Overseas Expertise Introduction Center for Discipline Innovation [CXJD2019005]
  5. High Performance Computing Center of Henan Normal University
  6. Aid program for Science and Technology Innovative Research Team of Zhengzhou Normal University

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Carbon dioxide electrochemical reduction reaction (CO2RR) with proton-electron pair delineates an intriguing prospect for converting CO2 to useful chemicals. Here by means of first-principle computations, the geometric constructions, electronic structures, and CO2RR catalytic performance of graphdiyne with single adsorbed alkali metal atoms (AM@GDY) are systematically investigated. The calculated results validate that the AM@GDY complexes possess excellent stability. The catalytic performance is correlated with the size of alkali metal ions. The adsorption free energies of CO2 on AM@GDY surfaces show that the Li@GDY and Na@GDY can spontaneously capture CO2 molecules. The interactions between *OCHO specie and AM@GDY are stronger than that between *COOH and AM@GDY, which can promote the CO2 reduction to HCOOH. The AM@GDY complexes could efficiently convert CO2 into HCOOH with high-selectivity, and the limiting potentials are - 0.56 V on Li@GDY and - 0.16 V on Na@GDY monolayers. The present findings not only highlight the importance of AM@GDY for CO2 electroreduction but also indicate that they are potentially single-atom electrocatalysts.

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