@article{Sarma:2023:10.1002/adfm.202302468,
author = {Sarma, SC and Barrio, J and Bagger, A and Pedersen, A and Gong, M and Luo, H and Wang, M and Favero, S and Zhao, C and Zhang, Q and Kucernak, A and Titirici, M and Stephens, IEL},
doi = {10.1002/adfm.202302468},
journal = {Advanced Functional Materials},
title = {Reaching the fundamental limitation in CO2 reduction to CO with single atom catalysts},
url = {http://dx.doi.org/10.1002/adfm.202302468},
volume = {33},
year = {2023}
}

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TY  - JOUR
AB  - The electrochemical CO2 reduction reaction (CO2RR) to value-added chemicals with renewable electricity is a promising method to decarbonize parts of the chemical industry. Recently, single metal atoms in nitrogen-doped carbon (MNC) have emerged as potential electrocatalysts for CO2RR to CO with high activity and faradaic efficiency, although the reaction limitation for CO2RR to CO is unclear. To understand the comparison of intrinsic activity of different MNCs, two catalysts are synthesized through a decoupled two-step synthesis approach of high temperature pyrolysis and low temperature metalation (Fe or Ni). The highly meso-porous structure results in the highest reported electrochemical active site utilization based on in situ nitrite stripping; up to 59±6% for NiNC. Ex situ X-ray absorption spectroscopy (XAS) confirms the penta-coordinated nature of the active sites. The catalysts are amongst the most active in the literature for CO2 reduction to CO. The density functional theory calculations (DFT) show that their binding to the reaction intermediates approximates to that of Au surfaces. However, it is found that the turnover frequencies (TOFs) of the most active catalysts for CO evolution converge, suggesting a fundamental ceiling to the catalytic rates.
AU  - Sarma,SC
AU  - Barrio,J
AU  - Bagger,A
AU  - Pedersen,A
AU  - Gong,M
AU  - Luo,H
AU  - Wang,M
AU  - Favero,S
AU  - Zhao,C
AU  - Zhang,Q
AU  - Kucernak,A
AU  - Titirici,M
AU  - Stephens,IEL
DO  - 10.1002/adfm.202302468
PY  - 2023///
SN  - 1616-301X
TI  - Reaching the fundamental limitation in CO2 reduction to CO with single atom catalysts
T2  - Advanced Functional Materials
UR  - http://dx.doi.org/10.1002/adfm.202302468
UR  - http://hdl.handle.net/10044/1/106151
VL  - 33
ER  - 

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