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Effective hydrogenation of carbonates to produce methanol over a ternary Cu/Zn/Al catalyst

文献类型：期刊论文

作者Li, Jiachen4,5,6,7; Wang, Liguo2,4,5,6,7; Hui, Xiang1,4,5,6,7; Zhang, Chanjuan4,5,6,7; Cao, Yan6,7; Xu, Shuang6,7; He, Peng6,7; Li, Huiquan3,4,5,6,7
刊名RSC ADVANCES
出版日期2020-03-31
卷号10期号:22页码:13083-13094
DOI10.1039/d0ra00347f
英文摘要Methanol synthesized from carbonate hydrogenation is of great importance for CO2 utilization indirectly. Herein, a series of Cu/Zn/Al heterogeneous catalysts were prepared by co-precipitation with a synchronous aging step, and were applied for hydrogenation of diethyl carbonate (DEC) to produce methanol. Furthermore, the catalysts were characterized by physicochemical methods, such as N-2 adsorption, ICP-OES, N2O titration, SEM, TEM, XRD, H-2-TPR and XPS in detail. Higher copper concentration led to a higher ratio of bulk CuOx species in the calcined samples, which resulted in different copper species distribution after the reduction process. Structure activity relationship analysis indicated that the balance of surface Cu-0 and Cu+ species influenced the formation rate of methanol. A higher proportion of Cu+ to (Cu+ + Cu-0) was conductive to methanol formation, while excessive Cu-0 site density played a negative influence on the methanol synthesized from DEC. Cu/Zn/Al with a 45.2% weight fraction of copper showed better performance with a total methanol formation rate of 131.0 mg g(cat.)(-1) h(-1). The reaction temperature and reaction time could obviously affect the reaction performance and the results suggested that 200 degrees C and 6 h were suitable. Furthermore, the long-term stability and activity of the catalyst was also studied on a fixed bed, and the yield of total methanol reached to 88.5% and the selectivity of total methanol gradually decreased to 74.0% within 200 h, which could be attributed to the detrimental influence derived from the increase of Cu-0. The reaction pathways involved in the hydrogenation of DEC process were proposed. The substance scope was also extended to other carbonates and the catalyst exhibited superior catalytic performance toward linear carbonates. This work provided insights into carbonate hydrogenation over an effective Cu/Zn/Al catalyst, which could be utilized into upgrading CO2 indirectly to produce commodity methanol under relatively mild reaction conditions.
WOS关键词MODIFIED CU/ZNO/AL2O3 CATALYSTS ; DIETHYL CARBONATE ; HIGHLY EFFICIENT ; HETEROGENEOUS HYDROGENATION ; CYCLIC CARBONATES ; CU ; CO2 ; DIOXIDE ; COPPER ; HYDROTALCITE
资助项目National Natural Science Foundation of China[21576272] ; "Transformational Technologies for Clean Energy and Demonstration", Strategic Priority Research Program of the Chinese Academy of Sciences[XDA 21030600] ; Science and Technology Service Network Initiative, Chinese Academy of Sciences[KFJ-STS-QYZD-138]
WOS研究方向Chemistry
语种英语
WOS记录号WOS:000527993500043
出版者ROYAL SOC CHEMISTRY
资助机构National Natural Science Foundation of China ; "Transformational Technologies for Clean Energy and Demonstration", Strategic Priority Research Program of the Chinese Academy of Sciences ; Science and Technology Service Network Initiative, Chinese Academy of Sciences
源URL[http://ir.ipe.ac.cn/handle/122111/40289]  
专题中国科学院过程工程研究所
通讯作者Wang, Liguo; Li, Huiquan
作者单位1.Tech Univ Denmark, Dept Chem & Biochem Engn, DK-2800 Lyngby, Denmark
2.Dalian Natl Lab Clean Energy, Dalian 116023, Peoples R China
3.Univ Chinese Acad Sci, Sch Chem Engn, Beijing 10049, Peoples R China
4.Univ Chinese Acad Sci, Sino Danish Ctr Educ & Res, Beijing 10049, Peoples R China
5.Univ Chinese Acad Sci, Sino Danish Coll, Beijing 100049, Peoples R China
6.Chinese Acad Sci, Inst Proc Engn, Natl Engn Lab Hydromet Cleaner Prod Technol, Beijing 100190, Peoples R China
7.Chinese Acad Sci, Inst Proc Engn, CAS Key Lab Green Proc & Engn, Beijing 100190, Peoples R China
推荐引用方式
GB/T 7714		 Li, Jiachen,Wang, Liguo,Hui, Xiang,et al. Effective hydrogenation of carbonates to produce methanol over a ternary Cu/Zn/Al catalyst[J]. RSC ADVANCES,2020,10(22):13083-13094.
APA Li, Jiachen.,Wang, Liguo.,Hui, Xiang.,Zhang, Chanjuan.,Cao, Yan.,...&Li, Huiquan.(2020).Effective hydrogenation of carbonates to produce methanol over a ternary Cu/Zn/Al catalyst.RSC ADVANCES,10(22),13083-13094.
MLA Li, Jiachen,et al."Effective hydrogenation of carbonates to produce methanol over a ternary Cu/Zn/Al catalyst".RSC ADVANCES 10.22(2020):13083-13094.

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来源：过程工程研究所

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