S1-supported Pd@CeO_(2) quasi-core@shell materials as advanced catalysts for selective hydrogenation of furfural  

作　　者：Xiang Chu Lingling Zhang Ke Wang Rui Zhang Xiao Wang Shuyan Song Hongjie Zhang 

机构地区：[1]State Key Laboratory of Rare Earth Resource Utilization,Changchun Institute of Applied Chemistry,Chinese Academy of Sciences,Changchun 130022,China [2]School of Applied Chemistry and Engineering,University of Science and Technology of China,Hefei 230026,China

出　　处：《Chinese Chemical Letters》2024年第3期493-496,共4页中国化学快报（英文版）

基　　金：supported by the financial aid from National Science and Technology Major Project of China(No.2022YFB3504000);National Natural Science Foundation of China(Nos.22020102003,22025506 and 22271274)。

摘　　要：Bare Pd metal nanoparticles invariably suffer from poor selectivity in furfural hydrogenation by forming flat configurations,with the aromatic ring of the substrate molecules parallel to the metal surface.Herein,we put forward a promising solution by using CeO_(2)as promoters to modify Pd nanoparticles for modulating the adsorption behaviors of furfural molecules.To achieve the highly-desired ultra-small Pd@CeO_(2)core@shell nanostructure,a“constrained auto-redox”synthesis is developed,in which silicalite-1 supports play the key role of providing their surface as the landing place of PdO_(x)precursors for inhibiting the overgrowth and the deformation.To the best of our knowledge,this is one of the smallest core@shell materials obtained from aqueous synthesis.When evaluated as catalysts,Pd@CeO_(2)/S-1 gives 98.9%conversion of furfural with 94.3%selectivity for furfural alcohol in 15 h,which is much better than that of Pd/S-1(88.6%conversion with 44.3%selectively).The DFT simulation reveals a strong interaction between the defects of CeO_(2)and the oxygen atom of the–CHO group in furfural molecules,which benefits the selective hydrogenation occurred in the–CHO group rather than the furan ring.

关 键 词：Core@shell PALLADIUM CERIA Auto-redox synthesis HYDROGENATION 

分 类 号：TQ251.11[化学工程—有机化工] TQ426