Plasma-driven CO2 hydrogenation to CH3OH over Fe2O3/γ-Al2O3 catalyst

被引:16
作者
Meng, Shengyan [1 ]
Wu, Liang [2 ]
Liu, Miao [1 ]
Cui, Zhaolun [3 ]
Chen, Qian [1 ]
Li, Shangkun [1 ,4 ]
Yan, Jiahui [1 ]
Wang, Li [5 ]
Wang, Xinkui [1 ]
Qian, Ji [1 ]
Guo, Hongchen [1 ]
Niu, Jinhai [2 ,6 ]
Bogaerts, Annemie [4 ]
Yi, Yanhui [1 ,7 ]
机构
[1] Dalian Univ Technol, Sch Chem Engn, State Key Lab Fine Chem, Dalian, Peoples R China
[2] Dalian Nationalities Univ, Sch Phys & Mat Engn, Liaoning Key Lab Optoelect Films & Mat, Dalian, Peoples R China
[3] South China Univ Technol, Sch Elect Power Engn, Guangzhou, Peoples R China
[4] Univ Antwerp, Dept Chem, Res Grp PLASMANT, Antwerp, Belgium
[5] Dalian Maritime Univ, Coll Environm Sci & Engn, Dalian, Liaoning, Peoples R China
[6] Dalian Nationalities Univ, Sch Phys & Mat Engn, Liaoning Key Lab Optoelect Films & Mat, Dalian 116600, Peoples R China
[7] Dalian Univ Technol, Sch Chem Engn, State Key Lab Fine Chem, Dalian 116024, Peoples R China
基金
中国国家自然科学基金;
关键词
chemisorbed oxygen; CO2; hydrogenation; iron-based catalyst; methanol production; plasma catalysis; CARBON-DIOXIDE; METHANOL; CONVERSION; NANOPARTICLES; HYDROCARBONS; METHANATION; REACTIVITY; REDUCTION;
D O I
10.1002/aic.18154
中图分类号
TQ [化学工业];
学科分类号
0817 ;
摘要
We report a plasma-assisted CO2 hydrogenation to CH3OH over Fe2O3/?-Al2O3 catalysts, achieving 12% CO2 conversion and 58% CH3OH selectivity at a temperature of nearly 80 & DEG;C atm pressure. We investigated the effect of various supports and loadings of the Fe-based catalysts, as well as optimized reaction conditions. We characterized catalysts by X-ray powder diffraction (XRD), hydrogen temperature programmed reduction (H-2-TPR), CO2 and CO temperature programmed desorption (CO2/CO-TPD), high-resolution transmission electron microscopy (HRTEM), scanning transmission electron microscopy (STEM), x-ray photoelectron spectroscopy (XPS), Mossbauer, and Fourier transform infrared (FTIR). The XPS results show that the enhanced CO2 conversion and CH3OH selectivity are attributed to the chemisorbed oxygen species on Fe2O3/?-Al2O3. Furthermore, the diffuse reflectance infrared Fourier transform spectroscopy (DRIFTs) and TPD results illustrate that the catalysts with stronger CO2 adsorption capacity exhibit a higher reaction performance. In situ DRIFTS gain insight into the specific reaction pathways in the CO2/H-2 plasma. This study reveals the role of chemisorbed oxygen species as a key intermediate, and inspires to design highly efficient catalysts and expand the catalytic systems for CO2 hydrogenation to CH3OH.
引用
收藏
页数:14
相关论文
共 67 条
[1]   Unexpectedly efficient CO2 hydrogenation to higher hydrocarbons over non-doped Fe2O3 [J].
Albrecht, Matthias ;
Rodemerck, Uwe ;
Schneider, Matthias ;
Broering, Martin ;
Baabe, Dirk ;
Kondratenko, Evgenii V. .
APPLIED CATALYSIS B-ENVIRONMENTAL, 2017, 204 :119-126
[2]   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
[3]   Highly Efficient Carbon Dioxide Hydrogenation to Methanol Catalyzed by Zigzag Platinum-Cobalt Nanowires [J].
Bai, Shuxing ;
Shao, Qi ;
Feng, Yonggang ;
Bu, Lingzheng ;
Huang, Xiaoqing .
SMALL, 2017, 13 (22)
[4]   Adiabatic plasma-catalytic reactor configuration: Energy efficiency enhancement by plasma and thermal synergies on CO2 methanation [J].
Biset-Peiro, Marti ;
Mey, Ruben ;
Guilera, Jordi ;
Andreu, Teresa .
CHEMICAL ENGINEERING JOURNAL, 2020, 393
[5]   On the role of ceria in Ni-Al2O3 catalyst for CO2 plasma methanation [J].
Biset-Peiro, Marti ;
Guilera, Jordi ;
Zhang, Ting ;
Arbiol, Jordi ;
Andreu, Teresa .
APPLIED CATALYSIS A-GENERAL, 2019, 575 :223-229
[6]  
Bui M, 2018, ENERG ENVIRON SCI, V11, P1062, DOI [10.1039/c7ee02342a, 10.1039/C7EE02342A]
[7]   Nonthermal plasma (NTP) activated metal-organic frameworks (MOFs) catalyst for catalytic CO2 hydrogenation [J].
Chen, Huanhao ;
Mu, Yibing ;
Shao, Yan ;
Chansai, Sarayute ;
Xiang, Huan ;
Jiao, Yilai ;
Hardacre, Christopher ;
Fan, Xiaolei .
AICHE JOURNAL, 2020, 66 (04)
[8]   Coupling non-thermal plasma with Ni catalysts supported on BETA zeolite for catalytic CO2 methanation [J].
Chen, Huanhao ;
Mu, Yibing ;
Shao, Yan ;
Chansai, Sarayute ;
Xu, Shaojun ;
Stere, Cristina E. ;
Xiang, Huan ;
Zhang, Rongxin ;
Jiao, Yilai ;
Hardacre, Christopher ;
Fan, Xiaolei .
CATALYSIS SCIENCE & TECHNOLOGY, 2019, 9 (15) :4135-4145
[9]   Induced high selectivity methanol formation during CO2 hydrogenation over a CuBr2-modified CuZnZr catalyst [J].
Chen, Shuyao ;
Zhang, Junfeng ;
Song, Faen ;
Zhang, Qingde ;
Yang, Guohui ;
Zhang, Meng ;
Wang, Xiaoxing ;
Xie, Hongjuan ;
Tan, Yisheng .
JOURNAL OF CATALYSIS, 2020, 389 :47-59
[10]   Modification of KNO3 on the reducibility and reactivity of Fe2O3-based oxygen carriers for chemical-looping combustion of methane [J].
Cheng, Xianming ;
Li, Kongzhai ;
Wei, Yonggang ;
Zhu, Xing ;
Tian, Dong .
CANADIAN JOURNAL OF CHEMICAL ENGINEERING, 2017, 95 (08) :1569-1578