A highly efficient Cu/ZnOx/ZrO2 catalyst for selective CO2 hydrogenation to methanol

被引:35
作者
Xu, Yanan [1 ]
Gao, Zhihong [1 ]
Peng, Li [1 ]
Liu, Kang [1 ]
Yang, Yang [1 ]
Qiu, Rongxing [1 ]
Yang, Shuliang [2 ]
Wu, Chenhao [3 ]
Jiang, Jiaheng [3 ]
Wang, Yanliang [1 ]
Tan, Wenjun [1 ,3 ]
Wang, Hongtao [1 ]
Li, Jun [1 ,4 ,5 ]
机构
[1] Xiamen Univ, Coll Chem & Chem Engn, Xiamen 361005, Peoples R China
[2] Xiamen Univ, Coll Energy, Xiamen 361102, Fujian, Peoples R China
[3] Xuchang Univ, Inst Surface Micro & Nano Mat, Coll Chem & Mat Engn, Key Lab Micronano Mat Energy Storage & Convers Hen, Xuchang 461000, Henan, Peoples R China
[4] Xiamen Univ, Natl Engn Lab Green Chem Prod Alcohols Ethers & Es, Xiamen 361005, Peoples R China
[5] Collaborat Innovat Ctr Chem Energy Mat, Xiamen 361005, Peoples R China
关键词
CO2; hydrogenation; Thermal catalysis; Metal-organic frameworks; Cu/ZnOx/ZrO2; Methanol; METAL-ORGANIC FRAMEWORKS; ZR CATALYSTS; ACTIVE-SITE; PD; NANOPARTICLES; DEACTIVATION; DEPENDENCE; REDUCTION; ZNO;
D O I
10.1016/j.jcat.2022.09.011
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 ternary Cu/ZnO/Al2O3 catalyst is usually employed for producing methanol from syngas (CO/CO2/H-2) or from CO2 hydrogenation in industry. However, this catalyst often suffers from the aggregation of Cu nanoparticles and the phase separation of Cu and ZnO. In this work, a highly efficient and stable catalyst (Cu/ZnOx/ZrO2) for CO2 hydrogenation to methanol is prepared via co-precipitation method with UiO-66 as structural template. Cu/Zn is effectively combined and encapsulated in the channels of UiO-66, which avoids the aggregation of metal particles. The ZrO2 support derived from UiO-66 enhances the interaction between the support and Cu/Zn, and thus improves the catalytic performance significantly. This catalyst shows a high space-time yield of 216.7 g((MeOH)).kg((cat))(-1).h(-1) at 260 degrees C, 4 MPa and GHSV = 12000 h(-1). Furthermore, the catalyst shows good stability over a period of 50 h on stream. The performance of Cu/ZnOx/ZrO2 is much better than that of commercial catalysts and most of catalysts previously reported. (C) 2022 Elsevier Inc. All rights reserved.
引用
收藏
页码:236 / 244
页数:9
相关论文
共 47 条
[1]   Confinement of Ultrasmall Cu/ZnOx Nanoparticles in Metal-Organic Frameworks for Selective Methanol Synthesis from Catalytic Hydrogenation of CO2 [J].
An, Bing ;
Zhang, Jingzheng ;
Cheng, Kang ;
Ji, Pengfei ;
Wang, Cheng ;
Lin, Wenbin .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2017, 139 (10) :3834-3840
[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]   Homogeneous and heterogeneous catalysts for hydrogenation of CO2 to methanol under mild conditions [J].
Bai, Shao-Tao ;
De Smet, Gilles ;
Liao, Yuhe ;
Sun, Ruiyan ;
Zhou, Cheng ;
Beller, Matthias ;
Maes, Bert U. W. ;
Sels, Bert F. .
CHEMICAL SOCIETY REVIEWS, 2021, 50 (07) :4259-4298
[4]   The changing nature of the active site of Cu-Zn-Zr catalysts for the CO2 hydrogenation reaction to methanol [J].
Bonura, G. ;
Cordaro, M. ;
Cannilla, C. ;
Arena, F. ;
Frusteri, F. .
APPLIED CATALYSIS B-ENVIRONMENTAL, 2014, 152 :152-161
[5]   Selective hydrogenation of CO2 to methanol catalyzed by Cu supported on rod-like La2O2CO3 [J].
Chen, Kun ;
Duan, Xinping ;
Fang, Huihuang ;
Liang, Xuelian ;
Yuan, Youzhu .
CATALYSIS SCIENCE & TECHNOLOGY, 2018, 8 (04) :1062-1069
[6]   Kinetics of deactivation on Cu/ZnO/Al2O3 methanol synthesis catalysts [J].
Fichtl, Matthias B. ;
Schlereth, David ;
Jacobsen, Nikolas ;
Kasatkin, Igor ;
Schumann, Julia ;
Behrens, Malte ;
Schloegl, Robert ;
Hinrichsen, Olaf .
APPLIED CATALYSIS A-GENERAL, 2015, 502 :262-270
[7]   Contrasting futures for ocean and society from different anthropogenic CO2 emissions scenarios [J].
Gattuso, J-P ;
Magnan, A. ;
Bille, R. ;
Cheung, W. W. L. ;
Howes, E. L. ;
Joos, F. ;
Allemand, D. ;
Bopp, L. ;
Cooley, S. R. ;
Eakin, C. M. ;
Hoegh-Guldberg, O. ;
Kelly, R. P. ;
Poertner, H-O ;
Rogers, A. D. ;
Baxter, J. M. ;
Laffoley, D. ;
Osborn, D. ;
Rankovic, A. ;
Rochette, J. ;
Sumaila, U. R. ;
Treyer, S. ;
Turley, C. .
SCIENCE, 2015, 349 (6243)
[8]   Effect of surface basicity over the supported Cu-ZnO catalysts on hydrogenation of CO2 to methanol [J].
Guo, Tan ;
Guo, Qing ;
Li, Shaozhong ;
Hu, Yongke ;
Yun, Shan ;
Qian, Yunhua .
JOURNAL OF CATALYSIS, 2022, 407 :312-321
[9]   The influence of La doping on the catalytic behavior of Cu/ZrO2 for methanol synthesis from CO2 hydrogenation [J].
Guo, Xiaoming ;
Mao, Dongsen ;
Lu, Guanzhong ;
Wang, Song ;
Wu, Guisheng .
JOURNAL OF MOLECULAR CATALYSIS A-CHEMICAL, 2011, 345 (1-2) :60-68
[10]   Cu@ZIF-8 derived inverse ZnO/Cu catalyst with sub-5 nm ZnO for efficient CO2 hydrogenation to methanol [J].
Hu, Bing ;
Yin, Yazhi ;
Zhong, Zixin ;
Wu, Dengdeng ;
Liu, Guoliang ;
Hong, Xinlin .
CATALYSIS SCIENCE & TECHNOLOGY, 2019, 9 (10) :2673-2681