Gold-like activity copper-like selectivity of heteroatomic transition metal carbides for electrocatalytic carbon dioxide reduction reaction

Mohammadreza Esmaeilirad, Artem Baskin, Alireza Kondori, Ana Sanz-Matias, Jin Qian, Boao Song, Mahmoud Tamadoni Saray, Kamil Kucuk, Andres Ruiz Belmonte, Pablo Navarro Munoz Delgado, Junwon Park, Rahman Azari, Carlo U. Segre, Reza Shahbazian-Yassar, David Prendergast () and Mohammad Asadi ()
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Mohammadreza Esmaeilirad: Illinois Institute of Technology
Artem Baskin: Lawrence Berkeley National Laboratory
Alireza Kondori: Illinois Institute of Technology
Ana Sanz-Matias: Lawrence Berkeley National Laboratory
Jin Qian: Lawrence Berkeley National Laboratory
Boao Song: University of Illinois at Chicago
Mahmoud Tamadoni Saray: University of Illinois at Chicago
Kamil Kucuk: Illinois Institute of Technology
Andres Ruiz Belmonte: Illinois Institute of Technology
Pablo Navarro Munoz Delgado: Illinois Institute of Technology
Junwon Park: Illinois Institute of Technology
Rahman Azari: Pennsylvania State University
Carlo U. Segre: Illinois Institute of Technology
Reza Shahbazian-Yassar: University of Illinois at Chicago
David Prendergast: Lawrence Berkeley National Laboratory
Mohammad Asadi: Illinois Institute of Technology

Nature Communications, 2021, vol. 12, issue 1, 1-10

Abstract: Abstract An overarching challenge of the electrochemical carbon dioxide reduction reaction (eCO2RR) is finding an earth-abundant, highly active catalyst that selectively produces hydrocarbons at relatively low overpotentials. Here, we report the eCO2RR performance of two-dimensional transition metal carbide class of materials. Our results indicate a maximum methane (CH4) current density of −421.63 mA/cm2 and a CH4 faradic efficiency of 82.7% ± 2% for di-tungsten carbide (W2C) nanoflakes in a hybrid electrolyte of 3 M potassium hydroxide and 2 M choline-chloride. Powered by a triple junction photovoltaic cell, we demonstrate a flow electrolyzer that uses humidified CO2 to produce CH4 in a 700-h process under one sun illumination with a CO2RR energy efficiency of about 62.3% and a solar-to-fuel efficiency of 20.7%. Density functional theory calculations reveal that dissociation of water, chemisorption of CO2 and cleavage of the C-O bond—the most energy consuming elementary steps in other catalysts such as copper—become nearly spontaneous at the W2C surface. This results in instantaneous formation of adsorbed CO—an important reaction intermediate—and an unlimited source of protons near the tungsten surface sites that are the main reasons for the observed superior activity, selectivity, and small potential.

Date: 2021
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DOI: 10.1038/s41467-021-25295-y

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