Zero-Valent Palladium Single-Atoms Catalysts Confined in Black Phosphorus for Efficient Semi-Hydrogenation

Zero-Valent Palladium Single-Atoms Catalysts Confined in Black Phosphorus for Efficient Semi-Hydrogenation

© 2021 Wiley-VCH GmbH.

Bibliographische Detailangaben
Veröffentlicht in:Advanced materials (Deerfield Beach, Fla.). - 1998. - 33(2021), 35 vom: 16. Sept., Seite e2008471
1. Verfasser: Chen, Cheng (VerfasserIn)
Weitere Verfasser: Ou, Wei, Yam, Kah-Meng, Xi, Shibo, Zhao, Xiaoxu, Chen, Si, Li, Jing, Lyu, Pin, Ma, Lu, Du, Yonghua, Yu, Wei, Fang, Hanyan, Yao, Chuanhao, Hai, Xiao, Xu, Haomin, Koh, Ming Joo, Pennycook, Stephen J, Lu, Junling, Lin, Ming, Su, Chenliang, Zhang, Chun, Lu, Jiong
Format: Online-Aufsatz
Sprache:English
Veröffentlicht: 2021
Zugriff auf das übergeordnete Werk:Advanced materials (Deerfield Beach, Fla.)
Schlagworte:Journal Article black phosphorus reaction mechanisms single-atom catalysts zero valence
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520 |a Single-atom catalysts (SACs) represent a new frontier in heterogeneous catalysis due to their remarkable catalytic properties and maximized atomic utilization. However, single atoms often bond to the support with polarized electron density and thus exhibit a high valence state, limiting their catalytic scopes in many chemical transformations. Here, it is demonstrated that 2D black phosphorus (BP) acts as giant phosphorus (P) ligand to confine a high density of single atoms (e.g., Pd1 , Pt1 ) via atomic layer deposition. Unlike other 2D materials, BP with relatively low electronegativity and buckled structure favors the strong confinement of robust zero-valent palladium SACs in the vacancy site. Metallic Pd1 /BP SAC shows a highly selective semi-hydrogenation of phenylacetylene toward styrene, distinct from metallic Pd nanoparticles that facilitate the formation of fully hydrogenated products. Density functional theory calculations reveal that Pd atom forms covalent-like bonding with adjacent P atoms, wherein H atoms tend to adsorb, aiding the dissociative adsorption of H2 . Zero-valent Pd in the confined space favors a larger energy gain for the synthesis of partially hydrogenated product over the fully hydrogenated one. This work provides a new route toward the synthesis of zero-valent SACs on BP for organic transformations 
650 4 |a Journal Article 
650 4 |a black phosphorus 
650 4 |a reaction mechanisms 
650 4 |a single-atom catalysts 
650 4 |a zero valence 
700 1 |a Ou, Wei  |e verfasserin  |4 aut 
700 1 |a Yam, Kah-Meng  |e verfasserin  |4 aut 
700 1 |a Xi, Shibo  |e verfasserin  |4 aut 
700 1 |a Zhao, Xiaoxu  |e verfasserin  |4 aut 
700 1 |a Chen, Si  |e verfasserin  |4 aut 
700 1 |a Li, Jing  |e verfasserin  |4 aut 
700 1 |a Lyu, Pin  |e verfasserin  |4 aut 
700 1 |a Ma, Lu  |e verfasserin  |4 aut 
700 1 |a Du, Yonghua  |e verfasserin  |4 aut 
700 1 |a Yu, Wei  |e verfasserin  |4 aut 
700 1 |a Fang, Hanyan  |e verfasserin  |4 aut 
700 1 |a Yao, Chuanhao  |e verfasserin  |4 aut 
700 1 |a Hai, Xiao  |e verfasserin  |4 aut 
700 1 |a Xu, Haomin  |e verfasserin  |4 aut 
700 1 |a Koh, Ming Joo  |e verfasserin  |4 aut 
700 1 |a Pennycook, Stephen J  |e verfasserin  |4 aut 
700 1 |a Lu, Junling  |e verfasserin  |4 aut 
700 1 |a Lin, Ming  |e verfasserin  |4 aut 
700 1 |a Su, Chenliang  |e verfasserin  |4 aut 
700 1 |a Zhang, Chun  |e verfasserin  |4 aut 
700 1 |a Lu, Jiong  |e verfasserin  |4 aut 
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773 1 8 |g volume:33  |g year:2021  |g number:35  |g day:16  |g month:09  |g pages:e2008471 
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