Enhancing Photocatalytic-Transfer Semi-Hydrogenation of Alkynes Over Pd/C3 N4 Through Dual Regulation of Nitrogen Defects and the Mott-Schottky Effect

© 2023 Wiley-VCH GmbH.

Bibliographische Detailangaben
Veröffentlicht in:Advanced materials (Deerfield Beach, Fla.). - 1998. - 35(2023), 41 vom: 19. Okt., Seite e2304130
1. Verfasser: Hu, Yaning (VerfasserIn)
Weitere Verfasser: Zhang, Shuo, Zhang, Zedong, Zhou, Hexin, Li, Bing, Sun, Zhiyi, Hu, Xuemin, Yang, Wenxiu, Li, Xiaoyan, Wang, Yu, Liu, Shuhu, Wang, Dingsheng, Lin, Jie, Chen, Wenxing, Wang, Shuo
Format: Online-Aufsatz
Sprache:English
Veröffentlicht: 2023
Zugriff auf das übergeordnete Werk:Advanced materials (Deerfield Beach, Fla.)
Schlagworte:Journal Article Mott-Schottky interactions Pd/C3N4 catalyst nitrogen defects photocatalysis selective transfer hydrogenation
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520 |a The selective hydrogenation of alkynes is an important reaction; however, the catalytic activity and selectivity in this reaction are generally conflicting. In this study, ultrafine Pd nanoparticles (NPs) loaded on a graphite-like C3 N4 structure with nitrogen defects (Pd/DCN) are synthesized. The resulting Pd/DCN exhibits excellent photocatalytic performance in the transfer hydrogenation of alkynes with ammonia borane. The reaction rate and selectivity of Pd/DCN are superior to those of Pd/BCN (bulk C3 N4 without nitrogen defects) under visible-light irradiation. The characterization results and density functional theory calculations show that the Mott-Schottky effect in Pd/DCN can change the electronic density of the Pd NPs, and thus enhances the hydrogenation selectivity toward phenylacetylene. After 1 h, the hydrogenation selectivity of Pd/DCN reaches 95%, surpassing that of Pd/BCN (83%). Meanwhile, nitrogen defects in the supports improve the visible-light response and accelerate the transfer and separation of photogenerated charges to enhance the catalytic activity of Pd/DCN. Therefore, Pd/DCN exhibits higher efficiency under visible light, with a turnover frequency (TOF) of 2002 min-1 . This TOF is five times that of Pd/DCN under dark conditions and 1.5 times that of Pd/BCN. This study provides new insights into the rational design of high-performance photocatalytic transfer hydrogenation catalysts 
650 4 |a Journal Article 
650 4 |a Mott-Schottky interactions 
650 4 |a Pd/C3N4 catalyst 
650 4 |a nitrogen defects 
650 4 |a photocatalysis 
650 4 |a selective transfer hydrogenation 
700 1 |a Zhang, Shuo  |e verfasserin  |4 aut 
700 1 |a Zhang, Zedong  |e verfasserin  |4 aut 
700 1 |a Zhou, Hexin  |e verfasserin  |4 aut 
700 1 |a Li, Bing  |e verfasserin  |4 aut 
700 1 |a Sun, Zhiyi  |e verfasserin  |4 aut 
700 1 |a Hu, Xuemin  |e verfasserin  |4 aut 
700 1 |a Yang, Wenxiu  |e verfasserin  |4 aut 
700 1 |a Li, Xiaoyan  |e verfasserin  |4 aut 
700 1 |a Wang, Yu  |e verfasserin  |4 aut 
700 1 |a Liu, Shuhu  |e verfasserin  |4 aut 
700 1 |a Wang, Dingsheng  |e verfasserin  |4 aut 
700 1 |a Lin, Jie  |e verfasserin  |4 aut 
700 1 |a Chen, Wenxing  |e verfasserin  |4 aut 
700 1 |a Wang, Shuo  |e verfasserin  |4 aut 
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