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Development of mixed oxide catalyst for carbon dioxide hydrogenation to methanol.

二氧化碳加氢制甲醇混合氧化物催化剂的开发

基本信息

批准号：
22K04821
负责人：
Shrotri Abhijit
金额：
$ 2.58万
依托单位：
Hokkaido University
依托单位国家：
日本
项目类别：
Grant-in-Aid for Scientific Research (C)
财政年份：
2022
资助国家：
日本
起止时间：
2022-04-01 至 2025-03-31
项目状态：
未结题

来源：
https://kaken.nii.ac.jp/grant/KAKENHI-PROJECT-22K04821/
关键词：
Carbon dioxide hydrogenation mixed oxide catalyst methanol CO2 hydrogenation Methanol Oxide catalyst

项目摘要

The goal of this research is to develop mixed metal oxide catalyst for hydrogenation of carbon dioxide to methanol. Based on the proposal work we screened doped catalyst for stabilization of formate species and found that Co-ZrO2 binary catalyst shows high affinity for adsorption of CO2 as carbonate and its hydrogenation to adsorbed formate species. The formate species were adsorbed over the Co-Zr interface, however hydrogenation of formate to methanol was not efficient and methanol selectivity was 30 % even at high Co loading. Dual atom catalyst was prepared by doping In and Co in ZrO2 to overcome this issue. Characterization of catalyst revealed that both In and Co were atomically dispersed. Methanol selectivity increased to 65% over In-Co-ZrO2 catalyst along with increase in methanol yield. Mechanistic investigation showed that Co-Zr interfacial site facilitated the stabilization of formate and In was responsible for hydrogen dissociation for hydrogenation of formate to methanol. Methanol formation was accelerated due to the synergy between Co and In sites. Kinetic analysis showed that the order of reaction with respect to hydrogen reduced from 0.9 for binary catalyst to 0.3 for ternary catalyst indicating that hydrogen activation was promoted over the ternary catalyst.During screening of catalyst, In-TiO2 binary catalyst showed superior activity for reverse water gas shift reaction at low temperature and high pressure. These results were summarized and published in ChemCatChem journal.

本研究的目的是开发一种用于二氧化碳加氢制甲醇的混合金属氧化物催化剂。在此基础上，我们筛选了用于稳定甲酸盐物种的掺杂催化剂，发现Co-ZrO_2二元催化剂对CO_2作为碳酸盐的吸附及其加氢为吸附的甲酸盐物种表现出很高的亲和力。甲酸盐物种被吸附在Co-Zr界面上，然而甲酸盐到甲醇的氢化不是有效的，并且即使在高Co负载下甲醇选择性也为30%。为了克服这一问题，在ZrO 2中掺杂In和Co制备了双原子催化剂。催化剂的表征表明，在和Co原子分散。甲醇选择性在In-Co-ZrO 2催化剂上沿着甲醇收率的增加而增加到65%。机理研究表明，Co-Zr界面位促进了甲酸盐的稳定化，In是甲酸盐加氢制甲醇过程中氢解离的主要原因。甲醇的形成加速由于Co和In网站之间的协同作用。动力学分析表明，二元催化剂对氢的反应级数从0.9级降低到0.3级，表明三元催化剂对氢的活化有促进作用，在催化剂筛选过程中，In-TiO 2二元催化剂在低温高压下对水煤气变换反应具有良好的上级活性。这些结果被总结并发表在ChemCatChem杂志上。