低碳化学与化工2024，Vol.49Issue(2)：10-16,7.DOI:10.12434/j.issn.2097-2547.20230234
造孔剂诱导合成FeCoCuAl催化剂及其与ZSM-5复合催化CO2加氢制高碳烃性能
Pore-forming agent induced synthesis of FeCoCuAl catalysts and their performance in hydrogenation of CO2 to high carbon hydrocarbons with ZSM-5
摘要
Abstract
CO2 hydrogenation to high-carbon hydrocarbons(C5+)is one of the important ways to synthesize high-value chemicals and fuels,which can achieve carbon emission reduction as well as help to alleviate energy pressure.K-and Na-modified FeCoCuAl catalysts were prepared by precipitation and iso-volumetric impregnation methods,and the effects of the pore-forming agent 1,3,5-benzenetricarboxylic acid(BTA)on their catalytic performance in CO2-catalyzed hydrogenation to high-carbon hydrocarbons reaction(temperature of 300℃,pressure of 2.0 MPa,n(H2):n(CO2)= 3:1 and space velocity of 3600 h-1 of feed gas,reaction for 6 h)were investigated.ZSM-5 molecular sieve was introduced into FeCoCuAl-20.0BTA catalyst(n(BTA):n(Fe)= 20.0%)to construct a series of composite catalysts and their catalytic performance in the reaction of catalytic hydrogenation of CO2 to high-carbon hydrocarbons was investigated.The physicochemical properties of the catalysts were characterized by combining N2 adsorption/desorption,X ray diffraction(XRD),H2-temperature programmed reduction(H2-TPR),CO2 temperature programmed desorption(CO2-TPD),and H2 temperature programmed desorption(CO2-TPD),and the oil-phase compositions of the products were analyzed by GC-MS.The results show that compared with FeCoCuAl catalysts,the specific surface area and pore volume of FeCoCuAl-BTA catalysts increase,and generate more surface-active species(Fe or Fe-Co alloy),which lead to better catalytic performance of FeCoCuAl-BTA catalysts in CO2 catalytic hydrogenation reaction.The CO2 conversion rate and C5+ selectivity of FeCoCuAl-20.0BTA catalyst are up to 70% and 42%,respectively,and the products generated from CO2 hydrogenation catalyzed by FeCoCuAl-20.0BTA catalyst are mainly C2～C4 products,while on the composite catalyst constructed with FeCoCuAl-20.0BTA catalyst and ZSM-5 molecular sieve in the form of mechanical mixing of particles with the mass ratio of 1.0,the C2～C4 products generated on FeCoCuAl-20.0BTA can undergo in situ chain growth,isomerization and aromatization reactions on ZSM-5 molecular sieves,which lead to the improvement of CO2 conversion rate and C5+ selectivity,reaching 79% and 66%,respectively.关键词
造孔剂/FeCoCuAl催化剂/ZSM-5/CO2加氢/高碳烃Key words
pore-forming agent/FeCoCuAl catalysts/ZSM-5/CO2 hydrogenation/high-carbon hydrocarbons分类
化学化工引用本文复制引用
赵治华,徐成华,任红,罗晶,杜磊,刘晨龙,陈雯婧,罗静..造孔剂诱导合成FeCoCuAl催化剂及其与ZSM-5复合催化CO2加氢制高碳烃性能[J].低碳化学与化工,2024,49(2):10-16,7.基金项目
四川省科技厅自然科学基金(2022NSFSC1058) （2022NSFSC1058）
四川省科技厅国际合作项目(2020YFH0133). （2020YFH0133）
