Interface Modification of Single Atom-Nanocluster Synergistic Sites to Break the Activity-Selectivity-Stability Trade-Off in Selective Hydrogenations

© 2025 Wiley‐VCH GmbH.

Détails bibliographiques
Publié dans:Advanced materials (Deerfield Beach, Fla.). - 1998. - 37(2025), 32 vom: 14. Aug., Seite e2503841
Auteur principal: Chen, Zemin (Auteur)
Autres auteurs: Wang, Chufei, Zhang, Boning, Li, Jianing, Wang, Dechen, Xu, Guangyue, Zhang, Junjie, Peng, Mi, Ma, Ding, Zhang, Ying
Format: Article en ligne
Langue:English
Publié: 2025
Accès à la collection:Advanced materials (Deerfield Beach, Fla.)
Sujets:Journal Article H‐spillover Interfacial modification selective hydrogenation structure‐property analysis synergistic sites
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520 |a Synergistic sites (M1+Mn) integrating single atoms (M1) and clusters (Mn) exhibit tremendous promise for overcoming linear scaling relationships. However, metal entities spatial segregation within synergistic sites impedes the overall optimization and structure-property analysis, and the support interface of the M1 and Mn sites critical for intermediate adsorption-transfer kinetics has yet unexplored. Here, for the first time, interfacial modification strategy is proposed to modulate the interface and electronic structure of M1+Mn sites. This is systematically altered that the interface of Pd1+Pdn sites from hydroxyapatite (HAP) to nitrogen-doped carbon-modified HAP (NC/HAP) and pure NC, with all sites maintaining the comparable size and content. In the semi-hydrogenation of alkynes, volcano-type correlations between Pd1+Pdn sites with varying interfaces and hydrogenation activities are observed, peaking for those supported on NC/HAP. The obtained Pd1+PdnNC/HAP exhibits superior activity for alkynol-to-enol conversion, achieving a formation rate up to 3707.7 mol molPd -1 h-1 while maintaining 97.2% selectivity. Comprehensive investigations propose d-band center of Pd1+Pdn sites with different interfaces as a descriptor to elucidate the volcano-type correlation for various selective hydrogenation reactions. Interfacial modification of Pd1+Pdn sites can optimize their electronic structure, adeptly managing substrates adsorption-desorption kinetic and interface H-spillover between segregated metal sites, thereby breaking -the activity-selectivity-stability trade-off 
650 4 |a Journal Article 
650 4 |a H‐spillover 
650 4 |a Interfacial modification 
650 4 |a selective hydrogenation 
650 4 |a structure‐property analysis 
650 4 |a synergistic sites 
700 1 |a Wang, Chufei  |e verfasserin  |4 aut 
700 1 |a Zhang, Boning  |e verfasserin  |4 aut 
700 1 |a Li, Jianing  |e verfasserin  |4 aut 
700 1 |a Wang, Dechen  |e verfasserin  |4 aut 
700 1 |a Xu, Guangyue  |e verfasserin  |4 aut 
700 1 |a Zhang, Junjie  |e verfasserin  |4 aut 
700 1 |a Peng, Mi  |e verfasserin  |4 aut 
700 1 |a Ma, Ding  |e verfasserin  |4 aut 
700 1 |a Zhang, Ying  |e verfasserin  |4 aut 
773 0 8 |i Enthalten in  |t Advanced materials (Deerfield Beach, Fla.)  |d 1998  |g 37(2025), 32 vom: 14. Aug., Seite e2503841  |w (DE-627)NLM098206397  |x 1521-4095  |7 nnas 
773 1 8 |g volume:37  |g year:2025  |g number:32  |g day:14  |g month:08  |g pages:e2503841 
856 4 0 |u http://dx.doi.org/10.1002/adma.202503841  |3 Volltext 
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