前驱体结构及Cu含量对CuFe基催化剂CO_(2)加氢制C_(2+)醇性能的影响  

Effect of precursor structure and Cu content on performance of CuFe-based catalysts for CO_(2) hydrogenation to C_(2+)alcohol

作　　者：杨晨[1] 温月丽 王斌[2] 张倩 贾雅珍 周森森 黄伟[2,3] YANG Chen;WEN Yueli;WANG Bin;ZHANG Qian;JIA Yazhen;ZHOU Sensen;HUANG Wei(College of Environmental Science and Engineering,Taiyuan University of Technology,Taiyuan 030024,Shanxi,China;State Key Laboratory of Clean and Efficient Coal Utilization,Taiyuan University of Technology,Taiyuan 030024,Shanxi,China;Coal Conversion Technology&Engineering Co.,Ltd.,Taiyuan University of Technology,Taiyuan 030024,Shanxi,China)

机构地区：[1]太原理工大学环境科学与工程学院,山西太原030024 [2]太原理工大学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 [3]山西太原理工煤转化技术工程有限公司,山西太原030024

出　　处：《天然气化工—C1化学与化工》2022年第4期32-40,共9页Natural Gas Chemical Industry

基　　金：山西省重点研发项目(国际合作)(201803D421099);山西省留学基金委资助项目(2017-035)。

摘　　要：采用类水滑石(HTLC)的制备方法制备了CuFeMg、CuFeZn和CuFeZnMg催化剂前驱体,考察了前驱体结构以及催化剂碱性强度对CO_(2)加氢制C_(2+)醇性能的影响。结合表征结果和催化剂的活性评价数据发现,相对于类水滑石前驱体结构,碱性强度对CO_(2)加氢性能的影响更为显著,弱碱性位有利于C_(2+)醇的生成。以性能最优的CuFeZn催化剂为基础,考察了活性金属Cu含量(物质的量)对CO_(2)加氢性能的影响。结果表明,改变Cu含量会影响催化剂中活性金属的相互作用、Cu^(0)的晶粒尺寸以及Fe物种的价态。当n(Cu):n(Fe):n(Zn)=0.5:1.0:2.0时,催化剂中各物种分散均匀,Cu^(0)晶粒尺寸适宜,且低价Fe物种较多,因而表现出良好的催化性能,此时CO_(2)转化率为7.70%,总醇选择性为37.78%,C_(2+)醇占比达94.26%,C_(2+)醇的时空收率为46.08 mg/(mL·h)。CuFeMg,CuFeZn and CuFeZnMg catalyst precursors were prepared by the preparation method of hydrotalcite-like compounds(HTLC),and the effects of precursor structure and catalyst basicity on the performance of CO_(2) hydrogenation to C_(2+)alcohol were investigated.Combined with the characterization results and activity evaluation data,it is found that compared with the structure of HTLC precursor,the effect of basicity on CO_(2) hydrogenation performance is more significant,and weak basic sites are beneficial to the formation of C_(2+)alcohol.Based on the optimum CuFeZn catalyst,the influence of Cu content(amount of substance)on CO_(2) hydrogenation performance was studied.The results show that Cu content affects the interaction of active metals,grain sizes of Cu^(0) and valence of Fe species.When n(Cu):n(Fe):n(Zn)=0.5:1.0:2.0,all species in the catalyst are evenly dispersed,and Cu^(0) grain size is appropriate,and there are more low valence Fe species,so the catalyst shows good catalytic performance.At this time,CO_(2) conversion is 7.70%,and total alcohol selectivity is 37.78%,and C_(2+)alcohol accounts for 94.26%,and space-time yield of C_(2+)alcohol is 46.08 mg/(mL·h).

关 键 词：CuFe基催化剂 CO_(2)加氢 C_(2+)醇 类水滑石结构 碱性 

分 类 号：TQ223.1[化学工程—有机化工] TQ426.8[理学—物理化学] O643.3[理学—化学]