郑万彬,叶艳文,胡一鸣,汤岑,李艳明,鲁继青.用于巴豆醛液相选择性加氢的高性能Ir/TiH2催化剂[J].分子催化,2021,35(1):31-39 |
用于巴豆醛液相选择性加氢的高性能Ir/TiH2催化剂 |
High Performance Ir/TiH2 Catalysts for Liquid Phase Selective Hydrogenation of Crotonaldehyde |
投稿时间:2020-10-17 修订日期:2020-11-20 |
DOI:10.16084/j.issn1001-3555.2021.01.004 |
中文关键词: 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 |
英文关键词:α,β-unsaturated aldehyde selective hydrogenation oxygen vacancy hydrogen activation capacity particle size effect |
基金项目:国家自然科学基金(No.21773212,21643007). |
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中文摘要: |
在Ir/TiH2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/TiO2催化剂,相同反应条件下Ir/TiH2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/TiH2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/TiH2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. |
英文摘要: |
In this work, liquid phase selective hydrogenation of crotonaldehyde was carried out on a series of Ir/TiH2 catalysts, and the effect of reduction temperature on the catalytic behaviors was investigated. It was found that the Ir/TiH2 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/TiO2 catalyst. The enhanced reactivity was attributed to enriched oxygen vacancies on the TiH2 surface and the strong H activation capability of the TiH2 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. |
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