Journal
ACS APPLIED ENERGY MATERIALS
Volume 6, Issue 18, Pages 9044-9056Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acsaem.2c01174
Keywords
single-site catalyst; copper; boron; coordination cage; methane electrosynthesis; atomically dispersed metal sites; carbon conversion; electrocatalysis
Funding
- U.S. Department of Energy (DOE), Office of Science, Office of Basic Energy Sciences, Catalysis Science program [DE-SC0021955]
- U.S. Department of Energy Office of Science User Facility
- DOE Office of Science by Argonne National Laboratory [DE-AC02-06CH11357]
- AOARD [FA2386-20-1-4048]
- ACS PRF [61764-ND10]
- William Hooper Grafflin Fellowship from the Department of Chemistry
- Office of Undergraduate Research, Scholarly and Creative Activity at Johns Hopkins University
- U.S. Department of Energy (DOE) [DE-SC0021955] Funding Source: U.S. Department of Energy (DOE)
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In this study, a copper boron imidazolate cage was discovered to be a convenient precursor for a competent catalyst with isolated Cu sites for carbon dioxide electroreduction. The methane selectivity was significantly enhanced after mild thermal activation, and stable CuNx sites were found during the reaction process.
Atomically dispersed metal sites (ADMSs) have been recognized as promising candidates for electrochemical conversion. Among a diverse range of molecular precursors for ADMS synthesis, framework materials are particularly interesting due to their high degree of tunability and control over the primary coordination sphere of the metal ions. Herein, we demonstrate that a copper boron imidazolate cage, BIF-29(Cu), is a convenient precursor for a competent catalyst with isolated Cu sites coordinated by N donors for carbon dioxide electroreduction (CO2RR). Although BIF-29(Cu) exhibited moderate methane selectivity over hydrogen evolution reaction (HER), the methane selectivity is significantly enhanced by 2 times (55% CH4 at -1.25 V vs RHE) after mild thermal activation. Extensive characterization methods indicate the transformation of crystalline BIF-29(Cu) into an amorphous carbonaceous material comprising isolated CuNx sites. Moreover, in situ X-ray absorbance spectroscopy indicates stable CuNx sites that are reduced during CO2RR. This work encourages the discovery of single-site electrocatalytic systems through a rational selection of molecular precursor and calcination parameters for promoting product selectivity.
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