Facet-dependent electrocatalysis in the HCOOH synthesis from CO2 reduction on Cu catalyst: a density functional theory study

Deok Yeon Jo, Hyung Chul Ham, Kwan Young Lee

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19 Citations (Scopus)

Abstract

Copper (Cu) has unique hydrogenation properties in the CO2 reduction reaction (CO2RR) for the synthesis of valuable hydrocarbons and alcohols such as methane, ethylene, ethanol and formic acid. Among the C1 products, formic acid (HCOOH) is chemically stable in the liquid phase at room temperature and is the simplest energy source that can be synthesized from CO2. The electrochemical CO2RR on Cu has been widely studied due to its very high selectivity toward target products and mild reaction conditions. However, electrochemistry activity can be impacted by many catalytic surface properties, including the morphology, crystallinity and surface index. Cu has a face-centered cubic (FCC) structure, and the Cu(1 1 1) surface index tends to be naturally exposed. Since the number of dangling bonds on the surface of the catalyst is different for each exposed surface, each surface activity is different, and the reaction pathway may also be different. The surface indexes of Cu(1 0 0) and (2 1 1) can be observed as a supported catalyst, and Cu(1 1 0) can be observed in a rod shape nanoparticle. Herein, we performed CO2RR over each surface and proposed an energy diagram of HCOOH formation via the COOH and HCOO intermediates using spin-polarized density functional theory. We elucidate the determining factor of catalytic activity and discuss the relationship between the coordination number/surface roughness (caused by the different surface facet) and the activity through electronic analysis of the d orbitals.

Original languageEnglish
Article number146857
JournalApplied Surface Science
Volume527
DOIs
Publication statusPublished - 2020 Oct 15

Bibliographical note

Funding Information:
This research was supported by the Hydrogen Energy Innovation Technology Development Program of the National Research Foundation of Korea (NRF) funded by the Korean government (Ministry of Science and ICT(MSIT)) (No. 2019M3E6A1104113, 2020M3E6A1043955). This work was also supported by the KIST institutional program at the Korea Institute of Science and Technology and by INHA UNIVERSITY Research Grant.

Funding Information:
This research was supported by the Hydrogen Energy Innovation Technology Development Program of the National Research Foundation of Korea (NRF) funded by the Korean government (Ministry of Science and ICT(MSIT)) (No. 2019M3E6A1104113, 2020M3E6A1043955). This work was also supported by the KIST institutional program at the Korea Institute of Science and Technology and by INHA UNIVERSITY Research Grant.

Publisher Copyright:
© 2020

Copyright:
Copyright 2020 Elsevier B.V., All rights reserved.

Keywords

  • CO reduction reaction
  • Copper
  • Density functional theory
  • Electrocatalysis
  • Formic acid
  • Surface index

ASJC Scopus subject areas

  • General Chemistry
  • Condensed Matter Physics
  • General Physics and Astronomy
  • Surfaces and Interfaces
  • Surfaces, Coatings and Films

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