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The synergy of in situ-generated Ni0 and Ni2P to enhance CO adsorption and protonation for selective CH4 production from photocatalytic CO2 reduction.
- Source :
- Green Chemistry; 1/7/2024, Vol. 26 Issue 1, p531-541, 11p
- Publication Year :
- 2024
-
Abstract
- The selective photocatalytic reduction of CO<subscript>2</subscript> to CH<subscript>4</subscript> remains a challenge because there is a need for not only strong adsorption sites for the intermediates, but also optimal proton-feeding sites on the photocatalyst surface. Herein, a synergistic dual-site function between in situ-generated Ni<superscript>0</superscript> and Ni<subscript>2</subscript>P on carbon nitride nanosheets (CN) for photocatalytic reduction of CO<subscript>2</subscript> to CH<subscript>4</subscript> is presented. The highest CH<subscript>4</subscript> production rate of 69.03 μmol g<superscript>−1</superscript> h<superscript>−1</superscript> is achieved on Ni<subscript>2</subscript>P/CN-0.5 in an aqueous suspension. Detailed analyses show that the promotion of CH<subscript>4</subscript> is closely correlated with the formation of Ni<superscript>0</superscript> sites due to light irradiation, which is confirmed by tracking the compositions of Ni<subscript>2</subscript>P/CN-0.5 through XPS and HRTEM characterization. Density functional theory calculations have been combined with CO-TPD and in situ FTIR spectra to reveal the synergy between in situ-generated Ni<superscript>0</superscript> sites and Ni<subscript>2</subscript>P. It shows that the Ni<superscript>0</superscript> sites can stabilize the key intermediate *CO, while the Ni<superscript>0</superscript>–Ni<subscript>2</subscript>P interface can promote *H transfer from Ni<subscript>2</subscript>P to Ni<superscript>0</superscript>. Therefore, the CO intermediates are rapidly protonated to form CHO* instead of being desorbed from the surface to produce CO, and subsequently CHO* will be converted into CH<subscript>4</subscript>. This work demonstrates a new strategy of designing highly efficient photocatalysts with synergistic catalytic sites for CO<subscript>2</subscript> conversion to hydrocarbons. [ABSTRACT FROM AUTHOR]
Details
- Language :
- English
- ISSN :
- 14639262
- Volume :
- 26
- Issue :
- 1
- Database :
- Complementary Index
- Journal :
- Green Chemistry
- Publication Type :
- Academic Journal
- Accession number :
- 174564951
- Full Text :
- https://doi.org/10.1039/d3gc03549b