官能团修饰的UiO-66负载Rh催化剂合成及其催化CO2加氢制乙醇性能
SYNTHESIS OF FUNCTIONAL GROUP MODIFIED UiO-66 SUPPORTED Rh CATALYST AND ITS CATALYTIC PERFORMANCE FOR CO2 HYDROGENATION TO ETHANOL
郑珂 1胥月兵 1刘冰 1刘小浩1
作者信息
- 1. 江南大学化学与材料工程学院,江苏无锡 214122
- 折叠
摘要
二氧化碳(CO2)通过加氢转化为乙醇等高附加值的化学品是实现"双碳"目标的重要途径之一.制备不同官能团(—OH和—NH2)修饰的UiO-66负载Rh催化剂Rh/UiO-66,在间歇高压反应釜中评价所制备催化剂对CO2加氢制乙醇反应的催化性能,并结合X射线衍射、扫描电子显微镜、透射电子显微镜等表征方法,探究官能团改性对Rh基催化剂上CO2加氢反应性能的影响.结果表明:与Rh/UiO-66催化剂相比,经官能团修饰后催化剂的催化性能明显增强,尤其是经—NH2修饰的催化剂(Rh/UiO-66-NH2)表现出了优异的催化活性、乙醇选择性和循环稳定性;NH2修饰后,催化剂中Rh+含量明显增加,有利于稳定CO*,并促进其与CHx*发生C—C偶联和加氢反应生成乙醇;在压力为3.0 MPa、温度为250 ℃的条件下,Rh/UiO-66-NH2催化CO2加氢反应的CO2转化率为5.6％,乙醇选择性高达84.7％,且5次循环反应后催化剂性能基本不变.
Abstract
The hydrogenation of carbon dioxide(CO2)to ethanol and other value-added chemicals is one of the important routes to achieve"dual-carbon"goals.Rh-based catalysts supported on UiO-66 modified with different functional groups(—OH and—NH2)were prepared,their catalytic performance for CO2 hydrogenation was tested in a batch reactor,and the effect of functional group modification on the performance of Rh-based catalysts for CO2 hydrogenation was investigated by XRD,SEM,TEM,FT-IR,ICP,BET,TG,CO pulse,XPS and CO2-TPD.The results showed that the catalytic performance of the catalyst modified with functional groups was significantly enhanced compared with that of Rh/UiO-66 catalyst.In particular,the Rh/UiO-66-NH2 catalyst modified with—NH2 exhibited excellent catalytic activity,ethanol selectivity and catalytic stability;while the Rh+content in catalyst increased obviously after—NH2 modification,which was beneficial to the stabilization of CO*,C—C coupling and hydrogenation with CHx*were promoted to produce ethanol.At the pressure of 3.0 MPa and the temperature of 250 ℃,Rh/UiO-66-NH2 exhibited the highest catalytic activity(5.6％)and ethanol selectivity(84.7％)with basically unchanged catalytic performance after five cycles.
关键词
CO2加氢/乙醇/Rh催化剂/官能团/电子性质Key words
CO2 hydrogenation/ethanol/Rh catalyst/functional group/electronic property引用本文复制引用
基金项目
国家重点研发计划项目(2023YFB4103201)
国家自然科学基金项目(22379053)
出版年
2024
NETL
NSTL
万方数据