超临界条件下铁、钴负载氧化铝及碳催化剂上氢气还原二氧化碳的研究

Carbon Dioxide Reduction with Hydrogen on Fe, Co Supported Alumina and Carbon Catalysts under Supercritical Conditions.

作者信息

Bogdan Viktor I, Koklin Aleksey E, Kustov Alexander L, Pokusaeva Yana A, Bogdan Tatiana V, Kustov Leonid M

机构信息

N.D. Zelinsky Institute of Organic Chemistry, Leninsky Prospect, 47, 119991 Moscow, Russia.

Chemistry Department, Lomonosov Moscow State University, Leninskie Gory, 1, Bldg. 3, 119992 Moscow, Russia.

出版信息

Molecules. 2021 May 13;26(10):2883. doi: 10.3390/molecules26102883.

DOI:10.3390/molecules26102883

PMID:34068056

原文链接:https://pmc.ncbi.nlm.nih.gov/articles/PMC8152461/

Abstract

Reduction of CO with hydrogen into CO was studied for the first time on alumina-supported Co and Fe catalysts under supercritical conditions with the goal to produce either CO or CH as the target products. The extremely high selectivity towards methanation close to 100% was found for the Co/AlO catalyst, whereas the Fe/AlO system demonstrates a predominance of hydrogenation to CO with noticeable formation of ethane (up to 15%). The space-time yield can be increased by an order of magnitude by using the supercritical conditions as compared to the gas-phase reactions. Differences in the crystallographic phase features of Fe-containing catalysts cause the reverse water gas shift reaction to form carbon monoxide, whereas the reduced iron phases initiate the Fischer-Tropsch reaction to produce a mixture of hydrocarbons. Direct methanation occurs selectively on Co catalysts. No methanol formation was observed on the studied Fe- and Co-containing catalysts.

摘要

首次在超临界条件下，以氧化铝负载的钴和铁催化剂研究了用氢气将一氧化碳还原为一氧化碳的反应，目标是将一氧化碳或甲烷作为目标产物生成。发现钴/氧化铝催化剂对甲烷化的选择性极高，接近100%，而铁/氧化铝体系则表现出氢化生成一氧化碳的优势，并伴有明显的乙烷生成（高达15%）。与气相反应相比，使用超临界条件可使时空产率提高一个数量级。含铁催化剂晶体相特征的差异导致逆水煤气变换反应生成一氧化碳，而还原的铁相引发费托反应生成烃类混合物。直接甲烷化在钴催化剂上选择性发生。在所研究的含铁和含钴催化剂上均未观察到甲醇生成。