Mg enhanced the performance of Cu/ZnO/ZrO2 for CO2 hydrogenation to methanol and the mechanism investigation

被引:16
作者
He, Qin [1 ,2 ]
Li, Zhongfu [1 ,2 ]
Li, Dong [3 ]
Ning, Fanghao [2 ]
Wang, Qunfei [1 ,2 ]
Liu, Wenqi [1 ,2 ]
Zhang, Weikun [1 ,2 ]
Cui, Yilin [1 ,2 ]
Zhang, Jingyan [1 ,2 ]
Liu, Conghua [1 ,2 ]
机构
[1] Shandong Univ Technol, Sch Mat Sci & Engn, Zibo 255000, Peoples R China
[2] Shandong Collegial Engn Res Ctr Novel Rare Earth C, Zibo 255000, Peoples R China
[3] Shenyang Normal Univ, Coll Chem & Chem Engn, Shenyang 110000, Peoples R China
基金
中国国家自然科学基金;
关键词
CO2; Cu/ZnO/ZrO2/MgO; Methanol; CU-ZNO/ZRO2; CATALYSTS; ADSORPTION; ZNO;
D O I
10.1016/j.mcat.2024.114008
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
Optimizing the microstructure of copper-based catalysts for CO2 hydrogenation to methanol is an attractive and widely reported strategy, but there are still certain barriers to improving both carbon dioxide conversion rate and methanol product selectivity. Herein, Cu/ZnO/ZrO2/MgO (CZZ(1-x)M(x)) catalysts were synthesized by co-precipitation method for CO2 hydrogenation to methanol. Furthermore, the structural features and reaction processes were systematically characterized by XRD, TEM, nitrogen adsorption/desorption, H-2-TPR, CO2-TPD and in-situ DRIFT. The results showed that Mg species optimized the microstructure of the catalyst, increased the dispersion of active species and constructed appropriate basic sites. This further enhanced the capture of reactive species and improved the CO2 hydrotreating to methanol reaction performance, which was accompanied by a simultaneous increase in CO2 conversion and methanol yield. It could be convinced that the highest space time yield (STY) of methanol (305.3 g(MeOH) kg(cat)(-1) h(-1)) was obtained at 220 degrees C, WHSV = 18,000 mL g(cat)(-1) h(-1) and 3 MPa (X-CO2 = 7.28%, S-MeOH = 71.8%) for the optimized CZZ(0.8)M(0.2) catalyst, which exhibited twice the CO2 conversion than Cu/ZnO/ZrO2. This work elaborated a scheme for the preparation of efficient methanol catalysts. providing reference for the research of CO2 hydrogenation to methanol process.
引用
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页数:12
相关论文
共 47 条
[1]   Influence of water vapor on the performance of Au/ZnO catalysts in methanol synthesis from CO2 and H2: A high-pressure kinetic and TAP reactor study [J].
Abdel-Mageed, Ali M. ;
Buesselmann, Matthias ;
Wiese, Klara ;
Fauth, Corinna ;
Behm, R. Juergen .
APPLIED CATALYSIS B-ENVIRONMENTAL, 2021, 297
[2]   Study of CuZnMOx oxides (M = Al, Zr, Ce, CeZr) for the catalytic hydrogenation of CO2 into methanol [J].
Angelo, Laetitia ;
Kobl, Kilian ;
Tejada, Leidy Marcela Martinez ;
Zimmermann, Yvan ;
Parkhomenko, Ksenia ;
Roger, Anne-Cecile .
COMPTES RENDUS CHIMIE, 2015, 18 (03) :250-260
[3]   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
[4]   Synthesis, characterization and activity pattern of Cu-ZnO/ZrO2 catalysts in the hydrogenation of carbon dioxide to methanol [J].
Arena, Francesco ;
Barbera, Katia ;
Italiano, Giuseppe ;
Bonura, Giuseppe ;
Spadaro, Lorenzo ;
Frusteri, Francesco .
JOURNAL OF CATALYSIS, 2007, 249 (02) :185-194
[5]  
Behrens M, 2012, SCIENCE, V336, P893, DOI [10.1126/science.1219831, 10.1126/science.12198331]
[6]   Bifunctional ZnO-MgO/activated carbon adsorbents boost H2S room temperature adsorption and catalytic oxidation [J].
Chao Yang ;
Wang, Yeshuang ;
Fan, Huiling ;
de Falco, Giacomo ;
Song Yang ;
Ju Shangguan ;
Bandosz, Teresa J. .
APPLIED CATALYSIS B-ENVIRONMENTAL, 2020, 266
[7]   Enhanced performance and stability of Cu/ZnO catalyst by introducing MgO for low-temperature methanol synthesis using methanol itself as catalytic promoter [J].
Chen, Fei ;
Gao, Weizhe ;
Wang, Kangzhou ;
Wang, Chengwei ;
Wu, Xuemei ;
Liu, Na ;
Guo, Xiaoyu ;
He, Yingluo ;
Zhang, Peipei ;
Yang, Guohui ;
Tsubaki, Noritatsu .
FUEL, 2022, 315
[8]   Hydrogenation of CO2 to methanol over Pd-Cu/CeO2 catalysts [J].
Choi, Eun Jeong ;
Lee, Yong Hee ;
Lee, Dae-Won ;
Moon, Dong-Ju ;
Lee, Kwan-Young .
MOLECULAR CATALYSIS, 2017, 434 :146-153
[9]   Cu/ZnO/AlOOH catalyst for methanol synthesis through CO2 hydrogenation [J].
Choi, EunGyoung ;
Song, KyoungHo ;
An, SoRa ;
Lee, KwanYoung ;
Youn, MinHyeh ;
Park, KiTae ;
Jeong, SoonKwan ;
Kim, HakJoo .
KOREAN JOURNAL OF CHEMICAL ENGINEERING, 2018, 35 (01) :73-81
[10]   Effect of Reflux Time on the Performance of the Cu/ZrO2 Catalyst for CO2 Hydrogenation to Methanol [J].
Dai, Wenhua ;
Meng, Xin ;
Xu, Bowen ;
Zhao, Rui ;
Jin, Daoming ;
Xu, Fan ;
Yang, Dandan ;
Xin, Zhong .
ACS APPLIED ENERGY MATERIALS, 2023, 6 (18) :9417-9426