化工进展 ›› 2019, Vol. 38 ›› Issue (11): 4956-4964.DOI: 10.16085/j.issn.1000-6613.2019-0391

• 工业催化 • 上一篇    下一篇

金属氧化物催化CO2与甲醇合成碳酸二甲酯的研究进展

王旭慧1,2(),赵金仙1,裴永丽1,任军1()   

  1. 1. 太原理工大学煤科学与技术教育部和山西省重点实验室,山西 太原 030024
    2. 山西大学动力工程系,山西;太原 030013
  • 收稿日期:2019-03-15 出版日期:2019-11-05 发布日期:2019-11-05
  • 通讯作者: 任军
  • 作者简介:王旭慧(1984—),女,博士研究生,研究方向为二氧化碳的转化利用。E-mail:xuhuidb0410@126.com
  • 基金资助:
    国家自然科学基金(21776194)

Research progress in dimethyl carbonate synthesis from carbon dioxide and methanol catalyzed by metal oxides

Xuhui WANG1,2(),Jinxian ZHAO1,Yongli PEI1,Jun REN1()   

  1. 1. Key Laboratory of Coal Science and Technology, Ministry of Education and Shanxi Province, Taiyuan University of Technology, Taiyuan 030024, Shanxi, China
    2. Department of Power Engineering, Shanxi University, Taiyuan 030013, Shanxi, China
  • Received:2019-03-15 Online:2019-11-05 Published:2019-11-05
  • Contact: Jun REN

摘要:

CO2是主要的温室气体。近年来随着工业的大力发展,CO2的排放量迅猛增加,严重影响着人类的生存环境。将CO2转化成有价值的化工产品,受到了研究领域的广泛关注。其中将CO2与产能过剩的甲醇作为原料,生产碳酸二甲酯(DMC),既能减少CO2排放,又能产生有价值的绿色产品DMC。本文简述了影响CO2转化的因素,即受热力学限制和CO2活化困难;重点介绍了具有酸碱活性中心的金属氧化物ZrO2、CeO2以及复合金属氧化物催化剂的催化性能和反应机理,并分析了影响催化活性的主要原因:表面酸碱性能决定了催化活性;进一步分析了催化剂表面的酸碱性来源于Lewis酸碱位和Br?nsted酸性位。对于开发高效的金属氧化物催化剂未来的研究方向提出了展望: 通过调控催化剂的晶相和形貌、增加氧空位和羟基官能团、掺杂碱性或者酸性物种来改变催化剂表面的酸碱性,并且向催化系统中添加脱水剂。最后指出了由于CO2分子的稳定性很难被活化,需进一步深入研究其活化CO2的机理,提高CO2的转化率。

关键词: 二氧化碳, 催化, 合成, 金属氧化物, 活性

Abstract:

CO2 is main greenhouse gas. In recent years, with the vigorous development of industry, CO2 emissions are rapidly increasing and seriously affecting our living environment.CO2 conversion into valuable chemical products has attracted extensive attention in the field of research. The synthesis of dimethyl carbonate (DMC) from CO2 and methanol can not only reduce CO2 emissions but also produce valuable green products of DMC. In this paper, the factors effecting on CO2 conversion are summarized as follows: thermodynamic constraints and difficulty in CO2 activation. The common metal oxides of ZrO2, CeO2 and composite metal oxides with acid-base active centers are significantly introduced from the catalytic performance and reaction mechanism. The main reasons of affecting the catalytic activity are analyzed, which originated from Lewis acid-base sites and Br?nsted acid sites. The future research directions for developing efficient metal oxide catalysts are proposed: adjusting the crystal phase and morphology of catalysts, increasing oxygen vacancies and hydroxyl functional groups, doping alkaline or acidic species, and adding dehydrating agents to the catalytic system. At last, it is pointed out that the stability of CO2 molecule is difficult to be activated, and the mechanism of activation of CO2 molecule should be further studied to improve the conversion of CO2.

Key words: carbon dioxide, catalysis, synthesis, metal oxides, reactivity

中图分类号: 

京ICP备12046843号-2;京公网安备 11010102001994号
版权所有 © 《化工进展》编辑部
地址:北京市东城区青年湖南街13号 邮编:100011
电子信箱:hgjz@cip.com.cn
本系统由北京玛格泰克科技发展有限公司设计开发 技术支持:support@magtech.com.cn