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.

Détails bibliographiques
Publié dans:Advanced materials (Deerfield Beach, Fla.). - 1998. - 33(2021), 35 vom: 16. Sept., Seite e2008471
Auteur principal: Chen, Cheng (Auteur)
Autres auteurs: 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: Article en ligne
Langue:English
Publié: 2021
Accès à la collection:Advanced materials (Deerfield Beach, Fla.)
Sujets:Journal Article black phosphorus reaction mechanisms single-atom catalysts zero valence
Description
Résumé:© 2021 Wiley-VCH GmbH.
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
Description:Date Revised 02.09.2021
published: Print-Electronic
Citation Status PubMed-not-MEDLINE
ISSN:1521-4095
DOI:10.1002/adma.202008471