Atomically Dispersed CuNx Sites from Thermal Activation of Boron Imidazolate Cages for Electrocatalytic Methane Generation

Banerjee, Soumyodip; Gorham, Justin M.; Beccar-Varela, Pilar; Hackbarth, Haira G.; Siegler, Maxime A.; Drichko, Natalia; Wright, Joshua T.; Bedford, Nicholas M.; Thoi, V. Sara

doi:10.1021/acsaem.2c01174

Atomically Dispersed CuN_x Sites from Thermal Activation of Boron Imidazolate Cages for Electrocatalytic Methane Generation

Journal Article · Wed Aug 24 00:00:00 EDT 2022 · ACS Applied Energy Materials

DOI:https://doi.org/10.1021/acsaem.2c01174· OSTI ID:1903197

Banerjee, Soumyodip ^[1]; ^[2]; Beccar-Varela, Pilar ^[3]; ^[4]; ^[3]; Drichko, Natalia ^[3]; Wright, Joshua T. ^[5]; ^[4]; ^[3]

Johns Hopkins Univ., Baltimore, MD (United States); Johns Hopkins University
National Inst. of Standards and Technology (NIST), Gaithersburg, MD (United States)
Johns Hopkins Univ., Baltimore, MD (United States)
Univ. of New South Wales, Sydney, NSW (Australia)
Illinois Institute of Technology, Chicago, IL (United States)

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. In this work, 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 CuN_x sites. Moreover, in situ X-ray absorbance spectroscopy indicates stable CuN_x 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.

View Accepted Manuscript (DOE)

Research Organization:: Johns Hopkins Univ., Baltimore, MD (United States); Johns Hopkins University, Baltimore, MD (United States)

Sponsoring Organization:: American Chemical Society (ACS); US Air Force Office of Scientific Research (AFOSR). Asian Office of Aerospace Research and Development (AOARD); USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: AC02-06CH11357; SC0021955

OSTI ID:: 1903197

Alternate ID(s):: OSTI ID: 2427275

Journal Information:: ACS Applied Energy Materials, Journal Name: ACS Applied Energy Materials Journal Issue: 18 Vol. 6; ISSN 2574-0962

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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Atomically Dispersed CuNx Sites from Thermal Activation of Boron Imidazolate Cages for Electrocatalytic Methane Generation

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Atomically Dispersed CuN_x Sites from Thermal Activation of Boron Imidazolate Cages for Electrocatalytic Methane Generation