Improving selective hydrogenation of carbonyls bond in α, β-unsaturated aldehydes over Pt nanoparticles encaged within the amines-functionalized MIL-101-NH2

被引:24
|
作者
Zahid, Muhammad [1 ,2 ]
Ismail, Ahmed [1 ]
Sohail, Manzar [2 ]
Zhu, Yujun [1 ]
机构
[1] Heilongjiang Univ, Key Lab Funct Inorgan Mat Chem, Minist Educ, Harbin 150080, Peoples R China
[2] Natl Univ Sci & Technol, Sch Nat Sci, Dept Chem, Islamabad 44000, Pakistan
关键词
Pt-based catalysts; Mesoporous MOFs; Amines functionalization; Selective hydrogenation; Carbonyls bond; Unsaturated alcohols; METAL-ORGANIC FRAMEWORKS; CHEMOSELECTIVE HYDROGENATION; CINNAMALDEHYDE; CATALYSTS; PLATINUM; ALCOHOL; SITES; OXIDE;
D O I
10.1016/j.jcis.2022.08.067
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
The high selectivity in the hydrogenation reactions of alpha, beta-unsaturated aldehydes is always a demanding task. Precious Pt-based catalysts play a pivotal role in selective catalytic hydrogenation of alpha, beta-unsaturated aldehydes, but controlling the selectivity is still a great challenge. Herein, the Pt nanoparticles were encaged within the mesopores of amines (-NH2) functionalized MOFs via polyol reduction method as an efficient approach to enhance the selectivity of desired carbonyls bond reduction. The as-prepared 3-Pt/MOF-NH2(x) catalysts retained the inherent properties of MOF-NH2(x) supports such as crystallinity, surface area, pore texture, and surface acidity. Remarkably, the amines modified MOFs supported Pt-based catalysts (3-Pt/MOF-NH2(x)) improved the selective hydrogenation of carbonyls (C=O) bond in cinnamaldehyde (CAL) and Furfural (FFL) with a higher selectivity (>= 80 %) under mild conditions as compared to other reported catalysts. The improved catalytic performance for the selective hydrogenation of carbonyls (C=O) bond is credited to the nitrogen (N) heteroatom of the amines group existing in the skeleton of MOFs and somewhat to the steric effect induced by mesopores of MOFs. The N heteroatom not only helps in the high uniform dispersion and stabilization of small-sized Pt nanoparticles (approximate to 2nm) but also adjust the electron movement (electronic density) via synergistic effect resulting from the N to the vacant d-orbital of active Pt nanoparticles confined within MOFs, leading to more new interfacial electrophilic and nucleophilic sites, which are beneficial for selective hydrogenation of C=O bond. Besides, the steric effect induced by mesopores of MOFs, encaging Pt nanoparticles, can alsoenhance the selective adsorption of the C=O bond to interact with the catalyst active sites, resulting inhigher selective hydrogenation of C=O bond. (C) 2022 Elsevier Inc. All rights reserved.
引用
收藏
页码:141 / 152
页数:12
相关论文
共 1 条