Oxidant-Free Dehydrogenation of Alcohols over Hydrotalcite-Supported Palladium Catalysts

被引:29
作者
Chen Jing [1 ,2 ]
Zhang Qinghong [1 ]
Fang Wenhao [1 ]
Wang Ye [1 ]
Wan Huilin [1 ]
机构
[1] Xiamen Univ, State Key Lab Phys Chem Solid Surfaces, Natl Engn Lab Green Chem Prod Alcohols Ethers & E, Coll Chem & Chem Engn, Xiamen 361005, Fujian, Peoples R China
[2] Chinese Acad Sci, Fujian Inst Res Struct Matter, State Key Lab Struct Chem, Fuzhou 350002, Fujian, Peoples R China
关键词
green catalysis; alcohol; dehydrogenation; hydrotalcite; palladium; nanoparticle; acid-base bifunctionality; ENVIRONMENTALLY BENIGN OXIDATION; FREE AEROBIC OXIDATION; HETEROGENEOUS CATALYSIS; SELECTIVE OXIDATION; ALLYLIC ALCOHOLS; NANOPARTICLES; NANOCLUSTERS; ALDEHYDES;
D O I
10.3724/SP.J.1088.2010.00505
中图分类号
O69 [应用化学];
学科分类号
081704 ;
摘要
Pd catalysts supported on various supports have been studied for the oxidant-free dehydrogenation of alcohols The Pd catalyst loaded on hydrotalcite (HT), which is an acid-base bifunctional support, demonstrates superior benzyl alcohol conversion and benzaldehyde selectivity Detailed studies using the Pd/HT catalyst reveal that the best performance can be obtained vet the catalyst with w(Pd) = 0 32%-0 55% The Pd/HT can be used repeatedly without significant deactivation and can efficiently catalyze the dehydrogenation of various alcohols including the substituted benzylic alcohols, 2-thiophenemethanol, all-unsaturated alcohols, and cyclic aliphatic alcohols The characterization results show that the Pd(II) species over the HT are transformed into Pd nanoparticles or nanoclusters with mean size of 2 0-2 5 nm during the reaction The highly dispersed Pd(11) species in the catalyst precursors can lead to the formation of smaller Pd nanoparticles, favoring the catalytic performance We speculate that the basicity of the catalyst may promote the activation of the O-H bond of alcohol to form a Pd-benzyl alcoholate intermediate, which undergoes beta-14 abstraction by Pd nanoparticles, and the Bronsted acid sites on the catalyst surface may facilitate the release of H-2 by the interaction with the formed hydride species on Pd nanoparticles Key words: green catalysis, alcohol, dehydrogenation, hydrotalcite; palladium. nanoparticle, acid-base bifunctionality
引用
收藏
页码:1061 / 1070
页数:10
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