低碳化学与化工2025,Vol.50Issue(1):47-53,7.DOI:10.12434/j.issn.2097-2547.20240161
活性炭负载双金属催化剂的乙醇气相羰基化反应性能研究
Study on catalytic performances of activated carbon loaded bimetallic catalysts for ethanol gas phase carbonylation reaction
摘要
Abstract
Ethanol gas phase carbonylation is a non-petroleum route for the production of propionic acid,and Ni-based catalysts supported on activated carbon are widely used in this reaction.In order to enhance the catalytic activity,a series of Ni-X(X=Fe,Cu or Ce)bimetallic catalysts were prepared by further doping Fe,Cu or Ce on the basis of Ni-based catalysts.The effects of metal dispersion and Ni0 relative content n(Ni0)/n(Ni0+Ni2++Ni3+)on the reaction performances were investigated by N2 physical adsorption/desorption,XRD,XPS,etc.The activity of Ni-X bimetallic catalysts for ethanol gas phase carbonylation was evaluated under the conditions of 250 ℃,0.1 MPa and the feedstock(n(CO)∶n(C2H5OH)∶n(C2H5I)=40∶20∶1)space velocity of 1.2 h-1.The results show that there exists a synergistic interaction between Ni species and CeO2 on the surface of the Ni-Ce bimetallic catalyst,which promotes the reduction of Ni2+to Ni0 and the appearance of more active sites on the catalyst surface,as well as inhibits the surface accumulation of Ni metal and promotes the dispersion of Ni metal.Compared with Ni-Fe and Ni-Cu bimetallic catalysts,the Ni-Ce bimetallic catalysts have the highest catalytic activity,and the ethanol conversion rate,combined selectivity of propionic acid and ethyl propionate and combined space-time yield of the catalyst at 6 h are 70.9%,28.0% and 220.4 mg/(g h),respectively.关键词
双金属催化剂/乙醇/气相羰基化/分散性/活性位点/活性炭Key words
bimetallic catalysts/ethanol/gas-phase carbonylation/dispersibility/active site/activated carbon分类
化学工程引用本文复制引用
刘鹏,王晓斌,丁传敏,孟园园,王明义,吴华帅,武爱莲,王俊文..活性炭负载双金属催化剂的乙醇气相羰基化反应性能研究[J].低碳化学与化工,2025,50(1):47-53,7.基金项目
国家自然科学基金(22308244) (22308244)
山西省自然科学基金(202203021221091,20210302123087). (202203021221091,20210302123087)