同晶取代法制备掺杂型催化剂及其催化合成甲醇性能  

Catalytic performance of methanol synthesis over doped catalysts prepared by isomorphous substitution method

作　　者：章敏 张华成 孔令奇 郑华艳[1] ZHANG Min;ZHANG Hua-cheng;KONG Ling-qi;ZHENG Hua-yan(Key Laboratory of Coal Science and Technology of Education Ministry and Shanxi Province,Taiyuan University of Technology,Taiyuan 030024,China)

机构地区：[1]太原理工大学煤科学与技术教育部和山西省重点实验室,山西太原030024

出　　处：《天然气化工—C1化学与化工》2020年第4期20-23,51,共5页Natural Gas Chemical Industry

基　　金：国家自然科学基金(21576179)。

摘　　要：在定向同晶取代法制备纯(Cux,Zn1-x)5(CO3)2(OH)6物相的基础上,通过掺杂Zr(NO3)4、Ce(NO3)4、Al(NO3)3等金属盐制备掺杂型催化剂,并用于合成气制甲醇反应中。结合XRD、BET、AAS以及H2-TPR表征探究了金属掺杂对前驱体物相组成及催化剂结构的影响。结果表明,采用定向同晶取代法能够制备出纯(Cux,Zn1-x)5(CO3)2(OH)6物相,但掺杂金属盐后,前驱体的物相组成不再单一,同时出现Cu2(CO3)(OH)2物相。金属掺杂后催化剂比表面积显著增加,进而提高其催化活性。其中Al、Zr同时掺杂制备的CZAl Zr-IS催化剂表现出最高的催化活性,其甲醇时空收率达到387.2 g/(kgCu·h)。On the basis of the phase-pure(Cux,Zn1-x)5(CO3)2(OH)6 prepared by oriented isomorphous substitution method,metal doped catalysts were obtained by doping different metal salts,such as Zr(NO3)4,Ce(NO3)4,Al(NO3)3,which were used in syngas-to-methanol system.The influence of metal doping on precursor phase components and catalyst structures were characterized with XRD,BET,AAS and H2-TPR.The results showed that the phase-pure(Cux,Zn1-x)5(CO3)2(OH)6 precursors could be obtained by oriented isomorphous substitution method.However,after metal doping,the phase of precursors was no longer pure,and Cu2(CO3)(OH)2 phase appeared.Doping metals could significantly increase the specific surface area of catalysts,thus improving the activity of the catalysts.CZAl Zr-IS catalyst prepared by adding both Al and Zr metals showed highest catalytic activity and the methanol space-time yield reached 387.2 g/(kgCu·h).

关 键 词：Cu/ZnO催化剂 定向同晶取代法 甲醇 合成气 

分 类 号：TQ426[化学工程]