Dimetal and duplex heteroatoms co-doped graphene aerogel in electrolytic CO₂ reduction to CO in aqueous electrolyte

Abstract

CO₂ electrochemical reduction (CO₂ER) is a promising alternative for the conversion of CO₂ into green and value-added chemicals. Among these chemicals, CO is an important product and platform molecule of the CO₂ER, which is always used to produce various chemicals such as methanol, aldehydes, and synthesis gas (H₂/CO). Developing efficient catalytic systems for the CO₂-to-CO, especially via the electrolytic chemical way, is highly important. In the present work, a N and P co-doped MnZn-bimetal supported 3D graphene aerogel (GA) catalyst, denoted as MnZn/N,P-3D-GA, was prepared and used for the CO₂ER to produce CO, which delivered high performance in the reaction. When the potential was -0.92 V [vs. reversible hydrogen electrode (RHE)], the Faradaic efficiency of CO (FE_CO) reached 96.6% and the current density was 12.0 mA·cm^-2. In addition, at the potential range from -0.97 to -1.12 V (vs. RHE), the obtained FE_CO was all more than 90%, indicating that the catalyst has a wide electrochemical window for the reaction. Density functional theory calculations indicated that the catalytic processes mainly involve *CO₂, *COOH, and *CO intermediates. The enhanced catalytic performance of the catalyst originated from the synergistic effect among the MnZn, N, P, and GA. The present work provides an important reference in the design and construction of catalysts using dual-metal-loaded and dual-heteroatom-modified GAs.

Keywords

CO₂ER / MnZn bimetal / CO / NP co-doping / graphene aerogel

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