Understanding activity and selectivity of metal-nitrogen-doped carbon catalysts for electrochemical reduction of CO2
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Open Access
- 16 October 2017
- journal article
- research article
- Published by Springer Science and Business Media LLC in Nature Communications
- Vol. 8 (1), 1-9
- https://doi.org/10.1038/s41467-017-01035-z
Abstract
Direct electrochemical reduction of CO2 to fuels and chemicals using renewable electricity has attracted significant attention partly due to the fundamental challenges related to reactivity and selectivity, and partly due to its importance for industrial CO2-consuming gas diffusion cathodes. Here, we present advances in the understanding of trends in the CO2 to CO electrocatalysis of metal- and nitrogen-doped porous carbons containing catalytically active M–N x moieties (M = Mn, Fe, Co, Ni, Cu). We investigate their intrinsic catalytic reactivity, CO turnover frequencies, CO faradaic efficiencies and demonstrate that Fe–N–C and especially Ni–N–C catalysts rival Au- and Ag-based catalysts. We model the catalytically active M–N x moieties using density functional theory and correlate the theoretical binding energies with the experiments to give reactivity-selectivity descriptors. This gives an atomic-scale mechanistic understanding of potential-dependent CO and hydrocarbon selectivity from the M–N x moieties and it provides predictive guidelines for the rational design of selective carbon-based CO2 reduction catalysts.Keywords
This publication has 65 references indexed in Scilit:
- Theoretical Considerations on the Electroreduction of CO to C2 Species on Cu(100) ElectrodesAngewandte Chemie, 2013
- Theoretical Considerations on the Electroreduction of CO to C2 Species on Cu(100) ElectrodesAngewandte Chemie, 2013
- Structure of the catalytic sites in Fe/N/C-catalysts for O2-reduction in PEM fuel cellsPhysical Chemistry Chemical Physics, 2012
- CO2 Reduction at Low Overpotential on Cu Electrodes Resulting from the Reduction of Thick Cu2O FilmsJournal of the American Chemical Society, 2012
- New insights into the electrochemical reduction of carbon dioxide on metallic copper surfacesEnergy & Environmental Science, 2012
- Structurally Designed Synthesis of Mechanically Stable Poly(benzoxazine-co-resol)-Based Porous Carbon Monoliths and Their Application as High-Performance CO2 Capture SorbentsJournal of the American Chemical Society, 2011
- How copper catalyzes the electroreduction of carbon dioxide into hydrocarbon fuelsEnergy & Environmental Science, 2010
- Real-space grid implementation of the projector augmented wave methodPhysical Review B, 2005
- Catalysis of the Electrochemical Reduction of Carbon Dioxide by Iron(0) Porphyrins: Synergystic Effect of Weak Brönsted AcidsJournal of the American Chemical Society, 1996
- Product Selectivity Affected by Cationic Species in Electrochemical Reduction of CO2 and CO at a Cu ElectrodeBulletin of the Chemical Society of Japan, 1991