CuZnAl-LDHs结构调控及其催化合成气制低碳醇研究  

Study on structure regulation of CuZnAl-LDHs and their catalytic synthesis of low-carbon alcohols from syngas

作　　者：王淑媛 赵东民 尹玲玲 高志华[1] 黄伟[1] WANG Shuyuan;ZHAO Dongmin;YIN Linging;GAO Zhihua;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1-9,共9页Low-Carbon Chemistry and Chemical Engineering

基　　金：山西省科技合作交流专项(202204041101011,202304041101027);中央引导地方科技发展基金(YDZJSX20231A023)。

摘　　要：为解决Cu基催化剂在合成气制取低碳醇过程中的Cu物种分散度较低等问题,分别采用4种插层方法(共沉淀法、离子交换法、焙烧复原法和返混沉淀法)对[Cu(EDTA)]^(2-)插层ZnAl类水滑石催化剂的结构进行了调控。通过XRD、N_(2)物理吸/脱附、TEM、H_(2)-TPR和XPS等表征方法对催化剂结构进行了分析,并考察了催化剂催化CO加氢制取低碳醇的性能。结果表明,改变插层方法可以有效调控催化剂的Cu分散度、Cu比表面积和氧空位相对含量等,进而影响其催化性能。采用焙烧复原法制备的催化剂Cu分散度最高,Cu比表面积最大,氧空位相对含量最多,且Cu物种与层板上的ZnO相互作用较强,其在反应条件为温度280℃、压力4.0 MPa、反应空速2000 h^(-1)和V(H_(2)):V(CO)=1:1时表现出最优的催化性能,总醇时空收率高达17468.7 mg/(g·h)。To address the issue of low dispersion of Cu species in Cu-based catalysts used in the synthesis of low-carbon alcohols from syngas,the structures of[Cu(EDTA)]^(2-)intercalated ZnAl hydrotalcite-like catalysts were successfully adjusted by four intercalation methods,including coprecipitation,ion exchange,calcination recovery,and reprecipitation methods.The catalyst structures were characterized by XRD,N_(2) physical adsorption/desorption,TEM,H_(2)-TPR,XPS and so on,and the catalytic performances of catalysts in CO hydrogenation to low-carbon alcohols were also investigated.The results show that the Cu dispersities,Cu specific surface areas and the relative contents of oxygen vacancy are regulated by the intercalation methods,thereby affecting their catalytic performances.The catalyst prepared by calcination recovery method exhibites the highest Cu dispersity,the largest Cu specific surface area and the highest oxygen vacancy concentration.Moreover,the interaction between Cu species and ZnO on the layered is strong.This catalyst exhibites the best catalytic performance under reaction conditions of temperature 280℃,pressure 4.0 MPa,gas hourly space velocity 2000 h^(-1) and V(H_(2)):V(CO)=1:1,and the total alcohol space-time yield achieves 17468.7 mg/(g·h).

关 键 词：[Cu(EDTA)]^(2-) 类水滑石 分散度 合成气 低碳醇 

分 类 号：TQ426.6[化学工程] O643.3[理学—物理化学]