Effect of Reflux Time on the Performance of the Cu/ZrO2 Catalyst for CO2 Hydrogenation to Methanol

被引:12
作者
Dai, Wenhua [1 ]
Meng, Xin [1 ]
Xu, Bowen [1 ]
Zhao, Rui [1 ]
Jin, Daoming [1 ]
Xu, Fan [1 ]
Yang, Dandan [1 ]
Xin, Zhong [1 ]
机构
[1] East China Univ Sci & Technol, Sch Chem Engn, Shanghai Key Lab Multiphase Mat Chem Engn, Shanghai 200237, Peoples R China
基金
中国国家自然科学基金;
关键词
CO2; hydrogenation; reflux; Cu/ZrO2; catalysts; basic site; oxygen vacancy; AMORPHOUS ZRO2; STATE; CU; ADSORPTION; INSIGHTS; SITES; ACID;
D O I
10.1021/acsaem.3c01373
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
The hydrogenation of CO2 into methanol was investigated by means of the Cu/ZrO2 catalyst to analyze the effect of reflux time on catalytic performance. A series of high-activity Cu/ZrO2 catalysts were prepared by introducing the support pretreated with ammonia reflux. The effect of reflux time on the structure and performance of all catalysts was systematically studied. Combined with various characterizations such as X-ray diffraction (XRD), N-2 physisorption, temperature-programmed reduction by H2 (H2-TPR), temperature-programmed desorption of H-2 and CO2, X-ray photoelectron spectroscopy (XPS), and transmission electron microscopy (TEM), it can be seen that the catalysts after reflux exhibited a stable amorphous structure with more medium and strong basic sites. Moreover, the proportion of defect oxygen and surface Cu+ species for Cu/ZrO2 catalysts increased, and the metal-support interaction was strengthened, which effectively increased active sites and promoted CO2 activation, and thus, the catalyst with stronger activity and better stability was obtained. The CO2 conversion dramatically increased by 4-5 times (from 5.4 to 22.1%) after reflux treatment, and the Cu/ZrO2-18h catalyst had the highest catalytic activity and a methanol space time yield of 394 g(MeOH) h-1 kg(cat)( -1) at 260 ?.
引用
收藏
页码:9417 / 9426
页数:10
相关论文
共 41 条
[1]   Solid-state interactions, adsorption sites and functionality of Cu-ZnO/ZrO2 catalysts in the CO2 hydrogenation to CH3OH [J].
Arena, Francesco ;
Italiano, Giuseppe ;
Barbera, Katia ;
Bordiga, Silvia ;
Bonura, Giuseppe ;
Spadaro, Lorenzo ;
Frusteri, Francesco .
APPLIED CATALYSIS A-GENERAL, 2008, 350 (01) :16-23
[2]   Conversion of carbon dioxide to methanol: A comprehensive review [J].
Biswal, Trinath ;
Shadangi, Krushna Prasad ;
Sarangi, Prakash Kumar ;
Srivastava, Rajesh K. .
CHEMOSPHERE, 2022, 298
[3]   The Role of the Oxygen Vacancies in the Synthesis of 1, 3-Butadiene from Ethanol [J].
Chagas, Luciano H. ;
Zonetti, Priscila C. ;
Matheus, Caio R. V. ;
Rabello, Carlos R. K. ;
Alves, Odivaldo C. ;
Appel, Lucia G. .
CHEMCATCHEM, 2019, 11 (22) :5625-5632
[4]   Insight into the Role of Cu-ZrO2 Interaction in Methanol Synthesis from CO2 Hydrogenation [J].
Chang, Xiao ;
Han, Xiaoyu ;
Pan, Yutong ;
Hao, Ziwen ;
Chen, Jiyi ;
Li, Maoshuai ;
Lv, Jing ;
Ma, Xinbin .
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH, 2022, 61 (20) :6872-6883
[5]   Hydrogen Adsorption, Dissociation, and Spillover on Ru10 Clusters Supported on Anatase TiO2 and Tetragonal ZrO2 (101) Surfaces [J].
Chen, Hsin-Yi Tiffany ;
Tosoni, Sergio ;
Pacchioni, Gianfranco .
ACS CATALYSIS, 2015, 5 (09) :5486-5495
[6]   Effect of reflux digestion treatment on the catalytic performance of Ni-CaO-ZrO2 nanocomposite catalysts for CO2 reforming of CH4 [J].
Chen, Q. J. ;
Zhang, J. ;
Jin, Q. W. ;
Pan, B. R. ;
Kong, W. B. ;
Zhao, T. J. ;
Sun, Y. H. .
CATALYSIS TODAY, 2013, 215 :251-259
[7]   The role of copper oxidation state in Cu/ZnO/Al2O3 catalysts in CO2 hydrogenation and methanol productivity [J].
Dasireddy, Venkata D. B. C. ;
Likozar, Blaz .
RENEWABLE ENERGY, 2019, 140 :452-460
[8]   Influence of modifier (Mn, La, Ce, Zr and Y) on the performance of Cu/Zn/Al catalysts via hydrotalcite-like precursors for CO2 hydrogenation to methanol [J].
Gao, Peng ;
Li, Feng ;
Zhao, Ning ;
Xiao, Fukui ;
Wei, Wei ;
Zhong, Liangshu ;
Sun, Yuhan .
APPLIED CATALYSIS A-GENERAL, 2013, 468 :442-452
[9]   Effect of reflux digestion time on MoO3/ZrO2 catalyst for sulfur-resistant CO methanation [J].
Gu, Jia ;
Xin, Zhong ;
Tao, Miao ;
Lv, Yuhao ;
Gao, Wenli ;
Si, Qian .
FUEL, 2019, 241 :129-137
[10]   New insight into the mechanism of carbon dioxide activation on copper-based catalysts: A theoretical study [J].
Ha, Nguyen Ngoc ;
Ha, Nguyen Thi Thu ;
Cam, Le Minh .
JOURNAL OF MOLECULAR GRAPHICS & MODELLING, 2021, 107