Engineering CuZnOAl2O3 Catalyst for Enhancing CO2 Hydrogenation to Methanol

被引:0
作者
Shi, Peixiang [1 ,2 ]
Han, Jiahao [1 ]
Tian, Yuhao [1 ]
Wang, Jingjing [1 ]
Lv, Yongkang [1 ]
Li, Yanchun [1 ]
Zhang, Xinghua [2 ]
Li, Congming [1 ]
机构
[1] Taiyuan Univ Technol, Coll Chem & Chem Engn, State Key Lab Clean & Efficient Coal Utilizat, Taiyuan 030024, Peoples R China
[2] Taiyuan Univ Technol, Coll Safety & Emergency Management, Taiyuan 030024, Peoples R China
基金
中国国家自然科学基金;
关键词
CO2; methanol; CuZnOAl2O3; pretreatment; carbonate; CU-BASED CATALYSTS; COPPER NANOPARTICLES; CARBON-DIOXIDE; MECHANISM; PRETREATMENT; ADSORPTION; HYBRID; SITES;
D O I
10.3390/molecules30061350
中图分类号
Q5 [生物化学]; Q7 [分子生物学];
学科分类号
071010 ; 081704 ;
摘要
The CuZnOAl2O3 catalyst shows excellent activity and selectivity in the reaction of CO2 hydrogenation to methanol as a consequence of its controllable physicochemical properties, which is expected to offer an efficient route to renewable energy. In this study, CuZnOAl2O3 catalysts are engineered by a special pretreatment, constructing a carbonate structure on the surface of the catalyst. Compared to the unmodified catalyst, the optimized catalyst (CZA-H-C1) not only exhibits an improved methanol selectivity of 62.5% (250 degrees C and 3 MPa) but also retains a minimal degree of deactivation of 9.57% over a 100 h period. By characterizing the catalysts with XRD, TEM, XPS and in situ DRIFTS spectroscopy, it was found that the surface carbonate species on Cu-based catalysts could significantly enhance the reaction and shield the active sites. This study offers theoretical insights and practical strategies for the rational design and optimization of high-performance heterogeneous catalysts.
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页数:17
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共 59 条
[1]   Synthesis of Hierarchically Structured Hybrid Materials by Controlled Self-Assembly of Metal Organic Framework with Mesoporous Silica for CO2 Adsorption [J].
Chen, Chong ;
Li, Bingxue ;
Zhou, Lijin ;
Xia, Zefeng ;
Feng, Nengjie ;
Ding, Jing ;
Wang, Lei ;
Wan, Hui ;
Guan, Guofeng .
ACS APPLIED MATERIALS & INTERFACES, 2017, 9 (27) :23060-23071
[2]   Cu thorn-ZrO2 interfacial sites with highly dispersed copper nanoparticles derived from Cu@UiO-67 hybrid for efficient CO2 hydrogenation to methanol [J].
Chen, Guoqing ;
Yu, Jun ;
Li, Gonghui ;
Zheng, Xiang ;
Mao, Haifang ;
Mao, Dongsen .
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY, 2023, 48 (07) :2605-2616
[3]   Transmission electron microscopy characterization of colloidal copper nanoparticles and their chemical reactivity [J].
Cheng, Guangjun ;
Walker, A. R. Hight .
ANALYTICAL AND BIOANALYTICAL CHEMISTRY, 2010, 396 (03) :1057-1069
[4]   CO2 hydrogenation to methanol over Cu/ZnO/ZrO2 catalysts prepared by precipitation-reduction method [J].
Dong, Xiaosu ;
Li, Feng ;
Zhao, Ning ;
Xiao, Fukui ;
Wang, Junwei ;
Tan, Yisheng .
APPLIED CATALYSIS B-ENVIRONMENTAL, 2016, 191 :8-17
[5]   Carbon dioxide hydrogenation to methanol: Process simulation and optimization studies [J].
Francis, Angel ;
Ramyashree, M. S. ;
Priya, S. Shanmuga ;
Kumar, S. Harish ;
Sudhakar, K. ;
Fan, Wei Keen ;
Tahir, Muhammad .
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY, 2022, 47 (86) :36418-36432
[6]   Mechanistic insights into the role of zinc oxide, zirconia and ceria supports in Cu-based catalysts for CO2 hydrogenation to methanol [J].
Fulham, George J. ;
Wu, Xianyue ;
Liu, Wen ;
Marek, Ewa J. .
CHEMICAL ENGINEERING JOURNAL, 2024, 480
[7]   High-pressure advantages in stoichiometric hydrogenation of carbon dioxide to methanol [J].
Gaikwad, Rohit ;
Bansode, Atul ;
Urakawa, Atsushi .
JOURNAL OF CATALYSIS, 2016, 343 :127-132
[8]   Mechanistic Understanding and the Rational Design of Sinter-Resistant Heterogeneous Catalysts [J].
Goodman, Emmett D. ;
Schwalbe, Jay A. ;
Cargnello, Matteo .
ACS CATALYSIS, 2017, 7 (10) :7156-7173
[9]   CO2 hydrogenation to methanol over Cu/ZnO/ZrO2 catalysts prepared via a route of solid-state reaction [J].
Guo, Xiaoming ;
Mao, Dongsen ;
Lu, Guanzhong ;
Wang, Song ;
Wu, Guisheng .
CATALYSIS COMMUNICATIONS, 2011, 12 (12) :1095-1098
[10]   Mechanism of CO2conversion to methanol over Cu(110) and Cu(100) surfaces [J].
Higham, Michael D. ;
Quesne, Matthew G. ;
Catlow, C. Richard A. .
DALTON TRANSACTIONS, 2020, 49 (25) :8478-8497