Atomically Dispersed Ni-N-C Catalysts for Electrochemical CO2 Reduction

Weiss, John C.; He, Yanghua; Cullen, David A.; Benavidez, Angelica; Jernigen, Jeremy David; Zhang, Hanguang; Osmieri, Luigi; Zelenay, Piotr

doi:10.1002/smll.202412162

Atomically Dispersed Ni-N-C Catalysts for Electrochemical CO₂ Reduction

Journal Article · Thu Jan 16 00:00:00 EST 2025 · Small

DOI:https://doi.org/10.1002/smll.202412162· OSTI ID:2503529

^[1]; He, Yanghua ^[1]; Cullen, David A. ^[2]; Benavidez, Angelica ^[3]; Jernigen, Jeremy David ^[1]; ^[1]; ^[1]; ^[1]

Los Alamos National Laboratory (LANL), Los Alamos, NM (United States)
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Sciences (CNMS)
Univ. of New Mexico, Albuquerque, NM (United States)

The atomic dispersion of nickel in Ni-N-C catalysts is key for the selective generation of carbon monoxide through the electrochemical carbon dioxide reduction reaction (CO₂RR). Herein, the study reports a highly selective, atomically dispersed Ni_1.0%-N-C catalyst with reduced Ni loading compared to previous reports. Extensive materials characterization fails to detect Ni crystalline phases, reveals the highest concentration of atomically dispersed Ni metal, and confirms the presence of the proposed Ni-N_x active site at this reduced loading. The catalyst shows excellent activity and selectivity toward CO generation, with a faradaic efficiency for CO generation (FE_CO) of 97% and partial current density for CO (j_co) of -9.0 mA cm^-2 at -0.9 V in an electrochemical H-type cell. CO₂RR activity and selectivity are also studied by rotating disk electrode (RDE) measurements where transport limitations can be suppressed. It is expected that the utility of these Ni-N-C catalysts will lie with tandem CO₂RR reaction schemes to multi-carbon (C₂₊) products.

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Research Organization:: Los Alamos National Laboratory (LANL), Los Alamos, NM (United States)

Sponsoring Organization:: USDOE Laboratory Directed Research and Development (LDRD) Program; USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities (SUF)

Grant/Contract Number:: 89233218CNA000001

OSTI ID:: 2503529

Alternate ID(s):: OSTI ID: 2507026

Report Number(s):: LA-UR-24-31527

Journal Information:: Small, Journal Name: Small; ISSN 1613-6810

Publisher:: WileyCopyright Statement

Country of Publication:: United States

Language:: English

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