Journal
JOURNAL OF MATERIALS CHEMISTRY A
Volume 6, Issue 20, Pages 9708-9715Publisher
ROYAL SOC CHEMISTRY
DOI: 10.1039/c8ta03245a
Keywords
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Funding
- JSPS [JP16H06130, JP17J03705]
- MEXT, Japan
- CREST program [JPMJCR13L1]
- Noguchi Institute
- Murata Research Foundation
- [JP16H06441]
- [JP17H05489]
- Grants-in-Aid for Scientific Research [16H06130, 16H06441] Funding Source: KAKEN
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Hybrid photocatalysts constructed with a mononuclear Ru(ii)-complex (RuP), silver nanoparticles, and carbon nitride nanosheets (NS-C3N4) photocatalyze CO2 reduction to selectively form formate under visible light. The structure of the nanoparticulate silver species, which worked as promoters for the reaction, was characterized by X-ray diffraction, UV-VIS diffuse reflectance spectroscopy, high-resolution transmission microscopy, and X-ray absorption fine-structure spectroscopy. The silver promoters were loaded on the surface of NS-C3N4 by an impregnation method from an aqueous solution containing AgNO3 or an in situ photodeposition method. Impregnation of NS-C3N4 with 2.0wt% Ag followed by reduction with H-2 at 473 K (further modified with RuP) resulted in the highest photocatalytic activity, giving a turnover number of 5700 (based on RuP), which was the greatest value among the formate-generating hybrid systems with a mononuclear complex. While the optimized photocatalyst contained highly dispersed Ag2O-like nanoclusters as the major silver species, experimental results suggested that highly dispersed Ag-0 species are more important for enhancing CO2 reduction activity, that is, the obtained experimental results led us to conclude that there are two major factors affecting activity: one is the feature size of silver species (smaller is better), and the other is the oxidation state of silver (metallic is better).
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