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Efficient and selective H2O2 production through uranyl-assisted photocatalytic oxygen reduction reaction process in a uranium-organic framework.
- Source :
- SCIENCE CHINA Chemistry; Jul2024, Vol. 67 Issue 7, p2274-2281, 8p
- Publication Year :
- 2024
-
Abstract
- Harnessing solar energy by photocatalytically converting oxygen and water into high-value-added H<subscript>2</subscript>O<subscript>2</subscript> is a promising way of alleviating both environmental and energy issues. It is worth noting that suppressing detrimental side reactions, such as the generation of •O<subscript>2</subscript><superscript>−</superscript>, is a critical approach to enhancing H<subscript>2</subscript>O<subscript>2</subscript> production. Herein, a 2-fold interpenetrating 3D uranium-organic framework (YTU-W-1) was developed and introduced for photocatalytic H<subscript>2</subscript>O<subscript>2</subscript> production. The material demonstrates a different photocatalytic mechanism when employing uranyl as an initiator, as compared with the conventional semiconductor photocatalytic pathway involving photo-generated charge carriers. Benefiting from the strong hydrogen abstraction effect of the U≡O<superscript>•</superscript> and the direct one-step oxygen reduction pathway, YTU-W-1 exhibits enhanced photocatalytic performance for H<subscript>2</subscript>O<subscript>2</subscript> production with yield efficiency of 221 µmol h<superscript>−1</superscript> g<superscript>−1</superscript>. Furthermore, YTU-W-1 displays a high H<subscript>2</subscript>O<subscript>2</subscript> selectivity of 68%, confirmed by rotating ring-disk electrode (RRDE) measurement. DFT calculations were used to elucidate the critical role of uranyl in the photocatalytic oxygen reduction reaction for H<subscript>2</subscript>O<subscript>2</subscript> production. This research introduces an innovative approach to photo driven H<subscript>2</subscript>O<subscript>2</subscript> production, underscoring the potential for heterogeneous catalysts to engage in photocatalytic reactions independently of photo-generated charge carriers. [ABSTRACT FROM AUTHOR]
Details
- Language :
- English
- ISSN :
- 16747291
- Volume :
- 67
- Issue :
- 7
- Database :
- Complementary Index
- Journal :
- SCIENCE CHINA Chemistry
- Publication Type :
- Academic Journal
- Accession number :
- 178462859
- Full Text :
- https://doi.org/10.1007/s11426-023-1987-0