文献类型：期刊文献

中文题名：Theoretical insight into the selectivities of copper-catalyzing heterogeneous reduction of carbon dioxide

英文题名：Theoretical insight into the selectivities of copper-catalyzing heterogeneous reduction of carbon dioxide

作者：Xitong Sun Xiaoming Cao P. Hu[1,2]

机构：[1]Key Laboratory for Advanced Materials;[2] Centre for Computational Chemistry and Research Institute of Industrial Catalysis, East China University of Science and Technology, Shanghai 200237, China;

年份：2015

卷号：0

期号：4

起止页码：553

中文期刊名：中国科学：化学英文版

外文期刊名：SCIENCE CHINA Chemistry

收录：Scopus;CSCD:【CSCD2015_2016】；PubMed;

基金：This work was supported by the National Natural Science Foundation of China （21333003, 21303051）, Shanghai Natural Science Foundatio, （13ZR1453000）, and the Recruitment Program of Global Experts （B08021）.

语种：中文

中文关键词：二氧化碳;化学还原;铜催化;HCOOH;多相;密度泛函理论;甲醇合成;工业合成

外文关键词：methanol synthesis, electrocatalytic reduction of CO2, CO2 hydrogenation, selectivity

摘要：二氧化碳的化学减小(公司 < 潜水艇 class= “ a-plus-plus ” > 当它不能仅仅移开公司， 2 ) 总是引起了集中的注意 < 潜水艇 class= “ a-plus-plus ” > 是主要温室气体而且生产有用燃料的 2 。利用基于铜的催化剂的甲醇的工业合成是为公司的一个通常使用的过程 < 潜水艇 class= “ a-plus-plus ” > 2 加氢。尽管有由识别活跃地点并且优化操作温度和压力改进它的反应机制的广泛的努力，它是仍然保持完全揭开了。公司的选择<潜水艇class=“ a-plus-plus ”>在铜电极的 2 electroreduction 能主要向碳一氧化物(公司)，蚁的酸( HCOOH )，甲烷( CH <潜水艇class=“ a-plus-plus ”> 4 )或乙烯( C <潜水艇class=“ a-plus-plus ”> 2 H <潜水艇class=“ a-plus-plus ”>取决于氢的化学潜力的 4 ),由应用潜力控制了。有趣地，尽管有在两个过程作为催化剂利用金属性的铜，甲醇几乎不能电气化学地被生产。而且，机械学的研究也被执行了试图向更理想的更高的烃完成更高的选择。在这个工作，我们考察催化公司的铜的反应机制的现在的建议 < 潜水艇 class= “ a-plus-plus ” > 在工业甲醇合成和电气化学的环境的 2 减小以密度功能的理论(DFT ) 计算分别地。另外，在选择上的液体固体接口的 solvation 和电气化学的模型的模拟方法的影响被讨论并且比较。
The chemical reduction of carbon dioxide （CO2） has always drawn intensive attentions as it can not only remove CO2 which is the primary greenhouse gas but also produce useful fuels. Industrial synthesis of methanol utilizing copper-based catalysts is a commonly used process for CO2 hydrogenation. Despite extensive efforts on improving its reaction mechanism by identifying the active sites and optimizing the operating temperature and pressure, it is still remains completely unveiled. The selectivities of CO2 electroreduction at copper electrode could mainly be towards carbon monoxide （CO）, formic acid （HCOOH）, methane （CH4） or ethylene （C2H4）, which depends on the chemical potentials of hydrogen controlled by the applied potential. Interestingly, methanol could hardly be produced electrochemically despite utilizing metallic copper as catalysts in both processes. Moreover, the mechanistic researches have also been performed aiming to achieve the higher selectivity towards more desirable higher hydrocarbons. In this work, we review the present proposals of reaction mechanisms of copper catalyzing CO2 reduction in industrial methanol synthesis and electrochemical environment in terms of density functional theory （DFT） calcula- tions, respectively. In addition, the influences of the simulation methods of solvation and electrochemical model at liquid-solid interface on the selectivity are discussed and compared.