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

Published

August 12, 2022

Author(s)

Soumyodip Banerjee, Justin Gorham, Maxime Siegler, Natalia Drichko, Joshua Wright, Nicholas Bedford, Sara Thoi

Abstract

Atomically dispersed heteroatom coordinated metal sites (ADMS) 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 the presence of pre-formed heteroatom coordinated molecular active sites. Herein, we demonstrate that the copper boron imidazolate cage, BIF-29(Cu) can be an ideal precursor for nitrogen coordinated single site Cu catalyst for electrocatalytic carbon dioxide reduction (CO2RR). Although the pristine material exhibited moderate methane selectivity over hydrogen evolution reaction (HER), the catalytic performance is significantly enhanced (2x enhancement, 55 % CH4 at -1.25 V vs RHE) by mild thermal activation. Our extensive spectroscopic characterizations indicate the transformation of crystalline BIF-29(Cu) into an amorphous carbonaceous material comprising isolated CuN2 sites. This work encourages the discovery of single-site electrocatalytic systems through a rational selection of molecular precursor and calcination parameters for desired electrocatalytic selectivity.

Citation

ACS Applied Energy Materials

Pub Type

Journals

Download Paper

https://doi.org/10.1021/acsaem.2c01174

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Keywords

Single site catalyst, copper, boron, coordination cage, methane electrosynthesis, atomically dispersed metal sites, carbon conversion, electrocatalysis

Citation

Banerjee, S. , Gorham, J. , Siegler, M. , Drichko, N. , Wright, J. , Bedford, N. and Thoi, S. (2022), Atomically Dispersed CuNx Sites from Thermal Activation of Boron Imidazolate Cages for Electrocatalytic Methane Generation, ACS Applied Energy Materials, [online], https://doi.org/10.1021/acsaem.2c01174, https://tsapps.nist.gov/publication/get_pdf.cfm?pub_id=933004 (Accessed April 24, 2024)