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作 者:高梦迪 武璐瑶 郝家荣 黄伟[1] GAO Mengdi;WU Luyao;HAO Jiarong;HUANG Wei(State Key Laboratory of Clean and Efficient Coal Utilization,College of Chemistry and Chemical Engineering,Taiyuan University of Technology,Taiyuan 030024,Shanxi,China)
机构地区:[1]太原理工大学化学与化工学院,省部共建煤基能源清洁高效利用国家重点实验室,山西太原030024
出 处:《低碳化学与化工》2024年第8期28-37,88,共11页Low-Carbon Chemistry and Chemical Engineering
基 金:国家自然科学基金(21908157)。
摘 要:随着原油储量的减少和环境问题的加剧,迫切需要寻找生产燃料和化学品的新技术。Cu基催化剂是合成气直接制乙醇和高级醇(C_(2+)醇)的重要催化剂之一,但存在目标产物选择性低的问题。采用完全液相法制备了一系列不同Al组分含量(n(Al)/n(Zn)计)的CuZnAl催化剂(Cat-Alx),结合X射线衍射、N_(2)吸/脱附和H_(2)-程序升温还原等对催化剂的物相组成、织构性质和还原性能等进行了表征。在模拟浆态床反应器中研究了Cat-Alx对CO加氢制乙醇和C_(2+)醇反应的催化性能。结果表明,Cat-Al0.8表面具有最丰富的Cu^(+)物种以及较多的氧空位,表现出相对最优的催化性能。在280℃、4 MPa和V(H_(2))/V(CO)=2/1的条件下反应24 h,Cat-Al0.8的CO转化率为18.45%,总醇选择性为30.34%,乙醇在总醇中的占比为30.19%,C_(2+)醇在总醇中的占比为48.08%。With the decrease of crude oil reserves and the aggravation of environmental problems,it is urgent to find new technologies for producing fuels and chemicals.Cu-based catalyst is one of the important catalysts for the direct synthesis of ethanol and higher alcohols(C_(2+)alcohols)from syngas,but it has the problem of low selectivity for target products.A series of CuZnAl catalysts(Cat-Alx)with different Al component contents(n(Al)/n(Zn))were prepared by the complete liquid-phase method.The phase compositions,texture properties and reduction properties of the catalysts were characterized by X-ray diffraction,N_(2) adsorption/desorption and H_(2)-programmed temperature reduction,etc.The catalytic performances of Cat-Alx for CO hydrogenation to ethanol and C_(2+)alcohols were studied in a simulated slurry bed reactor.The results show that Cat-Al0.8 has the most abundant Cu^(+)species and more oxygen vacancies on its surface,showing relatively optimal catalytic performance.Reaction under the conditions of 280℃,4 MPa and V(H_(2))/V(CO)=2/1 for 24 h,the CO conversion rate of Cat-Al0.8 is 18.45%,and the total alcohols selectivity is 30.34%,and the proportion of ethanol in the total alcohols is 30.19%,and the proportion of C_(2+)alcohols in the total alcohols is 48.08%.
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