期刊
ACS CATALYSIS
卷 12, 期 16, 页码 10127-10140出版社
AMER CHEMICAL SOC
DOI: 10.1021/acscatal.2c01589
关键词
N-doped carbon; CO( 2 )reduction; electroreduction; thermal conversion; active center; N-oxide; reaction mechanism; DFT
资金
- European Union [862453]
- National Labo-ratory for Renewable Energy [RRF-2.3.1-21-2022-00009]
By synthesizing a set of N-C catalysts with identical morphologies and systematically changing the precursors, the study found that the CO2 reduction activity of these catalysts is correlated with the chemical composition, and the activity trend is similar in different reaction scenarios.
popular in different electrochemical and catalytic applications. Due to the structural and stoichiometric diversity of these materials, however, the role of different functional moieties is still controversial. We have synthesized a set of N-C catalysts, with identical morphologies (similar to 27 nm pore size). By systematically changing the precursors, we have varied the amount and chemical nature of N-functions on the catalyst surface. The CO2 reduction (CO2R) properties of these catalysts were tested in both electrochemical (EC) and thermal catalytic (TC) experiments (i.e., CO2 + H2 reaction). CO was the major CO2R product in all cases, while CH4 appeared as a minor product. Importantly, the CO2R activity changed with the chemical composition, and the activity trend was similar in the EC and TC scenarios. The activity was correlated with the amount of different N-functions, and a correlation was found for the -NOx species. Interestingly, the amount of this species decreased radically during EC CO2R, which was coupled with the performance decrease. The observations were rationalized by the adsorption/desorption properties of the samples, while theoretical insights indicated a similarity between the EC and TC paths.
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