用于巴豆醛液相选择性加氢的高性能Ir/TiH_(2)催化剂  

High Performance Ir/TiH_(2) Catalysts for Liquid Phase Selective Hydrogenation of Crotonaldehyde

作　　者：郑万彬 叶艳文 胡一鸣 汤岑 李艳明 鲁继青 ZHENG Wan-bin;YE Yan-wen;HU Yi-ming;TANG Cen;LI Yan-ming;LU Ji-qing(Key Laboratory of the Ministry of Education for Advanced Catalysis Materials,Institute of Physical Chemistry,Jinhua 321004,China;Zhejiang Normal University Library And Information Center,Zhejiang Normal University,Jinhua 321004,China)

机构地区：[1]浙江师范大学物理化学研究所,先进催化材料教育部重点实验室,浙江金华321004 [2]浙江师范大学图文信息中心,浙江金华321004

出　　处：《分子催化》2021年第1期31-39,I0002,共10页Journal of Molecular Catalysis(China)

基　　金：国家自然科学基金(No.21773212,21643007)。

摘　　要：在Ir/TiH_(2)催化剂上进行了巴豆醛液相选择性加氢反应,并研究催化剂还原温度对其反应行为的影响.相比于Ir/TiO_(2)催化剂,相同反应条件下Ir/TiH_(2)催化剂的活性提高了2倍(80℃时巴豆醛转化率为52%),且巴豆醇选择性大幅度提高(78%).表征结果表明,Ir/TiH_(2)催化剂表面富含的氧缺位和强的H活化能力是催化剂性能提高的主要原因.此外,Ir/TiH_(2)催化剂中Ir颗粒尺寸随催化剂还原温度的升高而增大,导致其本征活性降低,表现出明显的尺寸效应.较小的颗粒尺寸有利于巴豆醛分子中C=O键加氢,从而提高了催化剂的反应性能.In this work, liquid phase selective hydrogenation of crotonaldehyde was carried out on a series of Ir/TiH_(2) catalysts, and the effect of reduction temperature on the catalytic behaviors was investigated. It was found that the Ir/TiH_(2) catalyst gave much higher activity(with a crotonaldehyde conversion of 52% at 80 ℃) and much higher selectivity to crotyl alcohol(78%), compared to a reference Ir/TiO_(2) catalyst. The enhanced reactivity was attributed to enriched oxygen vacancies on the TiH_(2) surface and the strong H activation capability of the TiH_(2) support. In addition, high temperature reduction resulted in the growth of the Ir particles and consequently declined turnover frequency. It was deduced that smaller Ir particles were favorable for the hydrogenation of C=O bond in the crotonaldehyde molecule and thus improved the activity.

关 键 词：α β-不饱和醛 选择性加氢 氧缺位 H活化能力 颗粒尺寸效应 

分 类 号：O643.32[理学—物理化学]