Stability and Effects of Subsurface Oxygen in Oxide-Derived Cu Catalyst for CO2 Reduction

Liu, Chang; Lourenço, Maicon P.; Hedström, Svante; Cavalca, Filippo; Diaz-Morales, Oscar; Duarte, Hélio A.; Nilsson, Anders; Pettersson, Lars G. M.

doi:10.1021/acs.jpcc.7b08269

Title: Stability and Effects of Subsurface Oxygen in Oxide-Derived Cu Catalyst for CO₂ Reduction

Journal Article · 10 October 2017 · Journal of Physical Chemistry. C

DOI: https://doi.org/10.1021/acs.jpcc.7b08269 · OSTI ID:1463400

^[1]; Lourenço, Maicon P. ^[2];

^[1];

^[3];

^[1]; Duarte, Hélio A. ^[2];

^[1]; Pettersson, Lars G. M. ^[1]

Stockholm Univ., Stockholm (Sweden)
Univ. Federal de Minas Gerais (Brazil)
Stockholm Univ., Stockholm (Sweden); SLAC National Accelerator Lab., Menlo Park, CA (United States)

Here, oxide-derived copper (OD-Cu) catalysts are promising candidates for the electrochemical CO₂ reduction reaction (CO₂RR) due to the enhanced selectivity toward ethylene over methane evolution, which has been linked to the presence of subsurface oxygen (O_sb). In this work, O_sb is investigated with theoretical methods. Although O_sb is unstable in slab models, it becomes stabilized within a “manually” reduced OD-Cu nanocube model which was calculated by self-consistent charge density functional tight binding (SCC-DFTB). The results obtained with SCC-DFTB for the full nanocube were confirmed with subcluster models extracted from the nanocube, calculated with both density functional theory (DFT) and SCC-DFTB. The higher stability of O_sb in the nanocube is attributed to the disordered structure and greater flexibility. The adsorption strength of CO on Cu(100) is enhanced by O_sb withdrawing electron density from the Cu atom, resulting in reduction of the σ-repulsion. Hence, the coverage of CO may be increased, facilitating its dimerization.

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Research Organization:: SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)

Sponsoring Organization:: USDOE

Grant/Contract Number:: AC02-76SF00515; 348-2013-6723; KAW-2013.0020

OSTI ID:: 1463400

Journal Information:: Journal of Physical Chemistry. C, Vol. 121, Issue 45; ISSN 1932-7447

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 79 works

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