M-N-C-Supported Catalysts for Carbon Dioxide Reduction Reaction

Abstract

Electrochemical carbon dioxide reduction (CO2RR) is a promising approach to converting CO2 into value-added chemicals using renewable electricity and to ultimately reducing the dependence on fossil resources. However, achieving sufficient activity and selectivity in economically viable CO2 electrolyzers presents a great challenge for CO2RR catalysts.1 Carbons are an important and particularly suitable component of a majority of CO2RR catalysts due to their excellent electronic conductivity, relatively easily achievable high porosity and hierarchical pore structure.2, 3 Thanks to these benefits, the metal-nitrogen-carbon (M-N-C) materials, containing at least 95 at% of carbon, have attracted special interest due to their promising selectivity for CO in CO2RR.4 In particular, the Ni-N-C support has been used to improve selectivity of Cu-based CO2RR catalysts for ethylene, attributed to the enhancement of CO generation during CO2RR.5 However, a comprehensive study is still needed to understand the effect of composition and morphology of M-N-C materials as supports for CO2RR.In this presentation, we will summarize the results of our recent study that has focused on the effect of composition (e.g., different metal centers) and morphology (e.g., porosity) of M-N-C supports on the activity and selectivity of metal (e.g., Cu) nanoparticles. We will specifically concentrate on possible advantages/disadvantages of using M-N-C materials as performance enhancing supports rather than autonomous CO2RR electrocatalysts. Acknowledgement Research presented in this work was supported by the Laboratory Directed Research and Development program of Los Alamos National Laboratory under project number 20230065DR. References (1) Masel, R. I.; Liu, Z.; Yang, H.; Kaczur, J. J.; Carrillo, D.; Ren, S.; Salvatore, D.; Berlinguette, C. P. An industrial perspective on catalysts for low-temperature CO2 electrolysis. Nature Nanotechnology 2021, 16 (2), 118-128.(2) Jhong, H.-R. M.; Tornow, C. E.; Kim, C.; Verma, S.; Oberst, J. L.; Anderson, P. S.; Gewirth, A. A.; Fujigaya, T.; Nakashima, N.; Kenis, P. J. A. Gold Nanoparticles on Polymer-Wrapped Carbon Nanotubes: An Efficient and Selective Catalyst for the Electroreduction of CO2. ChemPhysChem 2017, 18 (22), 3274-3279.(3) Baturina, O. A.; Lu, Q.; Padilla, M. A.; Xin, L.; Li, W.; Serov, A.; Artyushkova, K.; Atanassov, P.; Xu, F.; Epshteyn, A.; et al. CO2 Electroreduction to Hydrocarbons on Carbon-Supported Cu Nanoparticles. ACS Catalysis 2014, 4 (10), 3682-3695.(4) Liang, S.; Huang, L.; Gao, Y.; Wang, Q.; Liu, B. Electrochemical Reduction of CO2 to CO over Transition Metal/N-Doped Carbon Catalysts: The Active Sites and Reaction Mechanism. Advanced Science 2021, 8 (24), 2102886.(5) Wang, X.; de Araújo, J. F.; Ju, W.; Bagger, A.; Schmies, H.; Kühl, S.; Rossmeisl, J.; Strasser, P. Mechanistic reaction pathways of enhanced ethylene yields during electroreduction of CO2–CO co-feeds on Cu and Cu-tandem electrocatalysts. Nature Nanotechnology 2019, 14 (11), 1063-1070.