低碳化学与化工2025,Vol.50Issue(7):10-19,37,11.DOI:10.12434/j.issn.2097-2547.20240465
Al助剂含量对CoMn催化剂结构及其合成气制高碳醇催化性能的影响
Effect of Al additive contents on structure of CoMn catalysts and their catalytic performance in synthesis of higher alcohols from syngas
摘要
Abstract
Designing effective inorganic metal catalysts to improve the efficiency of syngas-to-alcohol conversion and the selectivity of higher alcohols(C5+alcohols)is critical for the development of sustainable chemistry and energy.To investigate the effect of Al additions on the structure and catalytic performance of CoMn catalysts in synthesis of higher alcohols from syngas,CoMnAl catalysts with varying Al addition quantities were produced by co-precipitation.The effects of Al doped on the structure,composition,morphology,valence state and surface chemical properties of CoMn catalysts were compared using characterization techniques such as XRD,SEM,EDX,N2 adsorption/desorption,ICP,XPS and CO/H2/NH3-TPD.The catalytic performance of CoMnAl catalysts was tested under conditions of 260℃,3.0 MPa,V(CO):V(H2):V(Ar)=80:40:30 and space velocity of 3000 h-1.The results show that when Al is doped in appropriate amounts as a structural promoter,it interacts with other metals to variable degrees,influencing the specific surface area and particle size of catalyst.As an electronic promoter,Al facilitates electron transfer with Co to form a Co-Al-O active phase,which in turn affects the reducibility and formation of oxygen defects of the catalyst,significantly enhancing its catalytic performance.In situ FT-IR characterization reveals that the reaction pathway of the CoMnAl(0.3)catalyst doped with Al additives is an aldehyde insertion process,which effectively inhibits the formation of methane in the reaction and improves the total alcohol selectivity to 42%.The percentage of higher alcohols in the total alcohols reaches 48.8%(mole fraction).By precisely controlling the Al doping amount,it is possible to effectively regulate the structure and surface oxygen defects of the catalyst,thereby enhancing the selectivity for higher alcohols in the syngas-to-alcohol process.关键词
合成气/高碳醇/Al助剂/氧缺陷Key words
syngas/higher alcohols/Al additives/oxygen defects分类
化学化工引用本文复制引用
葛浩,孙燕,孙启文..Al助剂含量对CoMn催化剂结构及其合成气制高碳醇催化性能的影响[J].低碳化学与化工,2025,50(7):10-19,37,11.基金项目
国家重点研发计划(2023YFB4103200). (2023YFB4103200)