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Issue 28, 2019
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Cu supported on polymeric carbon nitride for selective CO2 reduction into CH4: a combined kinetics and thermodynamics investigation

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Abstract

Metal-based cocatalysts have been widely applied in the photocatalytic CO2 reduction reaction (CO2RR) and the integration of cocatalysts/semiconductors is expected to enhance the selectivity of the catalytic reaction. Nevertheless, the type and yield of products manifest a large discrepancy even for the same cocatalyst/semiconductor photocatalytic system, which requires a comprehensive study into the reaction mechanism and product distribution in detail. Here we provide kinetics evidence that selective CO2 reduction into CH4 is realized on Cu loaded carbon nitride (Cu/CN), in comparison with that on Au species (Au/CN) which yield both CO and CH3OH. Besides, it is revealed that the adsorption/desorption thermodynamic behavior of CH3OH is a crucial factor to determine the product distribution. By the establishment of binary electron transfer channels at the interface between adsorbed CH3OH and the Cu/CN surface, intensified activation of CH3OH is accomplished, resulting in the over-all reduction of CO2 into methane. Owing to the combined kinetics and thermodynamics investigation at the atomic level, this work may provide pioneering design schemes of precisely tailored cocatalyst/semiconductor photocatalytic systems for the selective CO2RR.

Graphical abstract: Cu supported on polymeric carbon nitride for selective CO2 reduction into CH4: a combined kinetics and thermodynamics investigation

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Article information


Submitted
15 May 2019
Accepted
26 Jun 2019
First published
27 Jun 2019

J. Mater. Chem. A, 2019,7, 17014-17021
Article type
Paper

Cu supported on polymeric carbon nitride for selective CO2 reduction into CH4: a combined kinetics and thermodynamics investigation

J. Li, P. Yan, K. Li, J. You, H. Wang, W. Cui, W. Cen, Y. Chu and F. Dong, J. Mater. Chem. A, 2019, 7, 17014
DOI: 10.1039/C9TA05112K

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