摘要
人类向大气中排放的大量二氧化碳(CO_(2))造成了一系列环境问题,极大地威胁了人类的生存。CO_(2)催化加氢在众多CO_(2)减排思路中具有独特优势。将CO_(2)与氢气(H_(2))转化为高附加值的下游化学品,既可以减少大气中CO_(2)浓度,又可以生产具有经济价值的商品,具有良好的应用前景。近年来,氧化铟(In_(2)O_(3))催化剂作为一种高效的新型CO_(2)加氢制甲醇的催化剂在学界饱受关注。In_(2)O_(3)表面经过活化后会产生大量氧空位,氧空位周期性产生和湮灭组成的机制抑制了副反应的发生,将CO_(2)高选择性地加氢转化为甲醇。文献中报道In_(2)O_(3)在200~300℃时甲醇选择性接近100%,特别是在高温下仍能维持高甲醇选择性。这种高温下优异的性能使In_(2)O_(3)可被用于与沸石分子筛耦合制备催化CO_(2)加氢直接制烃类化合物的双功能催化剂。In_(2)O_(3)催化剂的缺陷在于其CO_(2)的转化率较低限制了甲醇的产率。学界目前采取了一系列策略对In_(2)O_(3)催化剂进行优化和改进。主要的策略有二:(1)将In_(2)O_(3)负载在其他氧化物载体上;(2)在In_(2)O_(3)体系中引入其他金属元素。将In_(2)O_(3)负载在其他氧化物载体上可以增加In_(2)O_(3)的分散度,增加催化剂中氧空位的含量,增强吸附CO_(2)的能力,稳定关键的表面中间物种。将In_(2)O_(3)负载在ZrO_(2)上是该策略的典型例子,它可以极大地增强催化剂的本征活性。在In_(2)O_(3)体系中引入其他金属元素可以增强H_(2)解离吸附以及H_(2)溢流的能力。文献中已经报道了在In_(2)O_(3)体系中引入Pd、Pt、Cu、Rh、Au、Co、Ni等金属,并取得了良好的效果。本文归纳了In_(2)O_(3)催化剂用于CO_(2)加氢的研究进展,分别对In_(2)O_(3)的结构、In_(2)O_(3)用于CO_(2)加氢的现状、以及新型In_(2)O_(3)基催化剂的设计与改良三个方面对In_(2)O_(3)在CO_(2)加氢中的应用进行综述,并对In_(2)O_(3)�
Alarge amount of carbon dioxide(CO_(2))emitted by humans into the atmosphere has caused many environmental problems and dramatically threatens humankind’s survival.CO_(2)catalytic hydrogenation has unique advantages among many CO_(2)reduction strategies.The conversion of CO_(2)and hydrogen(H 2)into high value-added chemicals has good prospects for application,both in reducing atmospheric CO_(2)concentrations and producing economically valuable commodities.In recent years,indium oxide(In_(2)O_(3))catalysts have received much attention in the academic community as a new and efficient catalyst for the CO_(2)hydrogenation to methanol.After activation,the In_(2)O_(3)surface generates a large number of oxygen vacancies,which are periodically generated and annihilated,that inhibit the occurrence of side reactions and hydrogenates CO_(2)to methanol with high selectivity.It was reported in the literature that In_(2)O_(3)had a methanol selectivity close to 100%at 200—300℃.Especially at higher temperatures,the relatively high methanol selectivity was still maintained.This excellent performance at high temperatures allows In_(2)O_(3)to be used in coupling with zeolite to design bifunctional catalysts for the CO_(2)catalytic hydrogenation directly to hydrocarbons.The drawback of In_(2)O_(3)catalysts is that their low CO_(2)conversion limits the methanol yield.The academic community has adopted several strategies to optimize the In_(2)O_(3)-based catalysts.There are two main strategies:(1)loading In_(2)O_(3)onto other oxide supports and(2)introducing other metal elements into the In_(2)O_(3)system.Loading In_(2)O_(3)onto other oxide supports can increase the dispersion of In_(2)O_(3)species,increase the content of oxygen vacancies,enhance the ability to adsorb CO_(2),and stabilize key intermediate species.Loading In_(2)O_(3)onto ZrO_(2) is a typical example of this strategy,which can significantly enhance the intrinsic activity of the catalyst.The introduction of other metallic elements into the In_(2)O_(3)can enhance H_
作者
李龙泰
张春杰
罗学彬
杨彬
郭利民
LI Longtai;ZHANG Chunjie;LUO Xuebin;YANG Bin;GUO Limin(School of Environmental Science and Engineering,Huazhong University of Science and Technology,Wuhan 430074,China;Shanxi Xinhua Chemical Defense Equipment Research Institute Co.,Ltd.,Taiyuan 030008,China)
出处
《材料导报》
EI
CAS
CSCD
北大核心
2021年第21期21071-21078,共8页
Materials Reports
基金
国家自然科学基金面上项目(21878116)
湖北省自然科学基金杰出青年人才项目(2019CFA070)。
关键词
二氧化碳加氢
甲醇
烃类化合物
氧化铟
氧空位
氢溢流
carbon dioxide hydrogenation
methanol
hydrocarbon
indium(Ⅲ)oxide
oxygen vacancies
hydrogen spillover
