Role of hydroxyl on metal surface in hydrogenation reactions

被引:1
作者
Wang, Yong [1 ,2 ,3 ]
Wang, Ting [1 ]
Rong, Zeming [1 ]
Wang, Yue [1 ]
Qu, Jingping [1 ]
机构
[1] Dalian Univ Technol, Sch Chem Engn, State Key Lab Fine Chem, Dalian 116024, Peoples R China
[2] Tech Univ Munich, Dept Chem, Lichtenbergstr 4, D-85748 Garching, Germany
[3] Tech Univ Munich, Catalysis Res Ctr, Lichtenbergstr 4, D-85748 Garching, Germany
关键词
Hydrogenation; Nitroaromatic; Platinum -group metal; Surface hydroxyl; Hydrogen bond; Kinetic study; LIQUID-PHASE HYDROGENATION; IRIDIUM NANOPARTICLES; SELECTIVE HYDROGENATION; FINE CHEMICALS; OXIDATION; GRAPHENE; WATER; PLATINUM; ALCOHOL; OXYGEN;
D O I
10.1016/j.jcat.2023.01.028
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 important role of surface hydroxyl in metal catalysis is attracting more attentions but rarely studied for liquid-phase hydrogenation reactions. Here we report such deliberate research with two model sub-strates, p-chloronitrobenzene and cinnamaldehyde. Graphene-supported iridium nanoparticles with hydroxyl on the metal surface were prepared by hydrothermal synthesis, and the surface hydroxyl can be removed by a mild pre-reduction. The catalyst with surface hydroxyl exhibited around three times higher rate for the hydrogenation of p-chloronitrobenzene than the catalyst without hydroxyl, and an opposite trend was found for the hydrogenation of cinnamaldehyde. Kinetic study revealed that although the surface hydroxyl halved the coverage of H on iridium, it increased the rate constant by a factor of eight through reducing the reaction barrier for the hydrogenation of p-chloronitrobenzene. Theoretical calculation confirmed that the surface hydroxyl can polarize the nitro group via a weak hydrogen -bond interaction and thus facilitate its hydrogenation.CO 2023 Published by Elsevier Inc.
引用
收藏
页码:216 / 224
页数:9
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