Glycol assisted efficient conversion of CO2 captured from air to methanol with a heterogeneous Cu/ZnO/Al2O3 catalyst

被引:28
作者
Sen, Raktim
Koch, Christopher J.
Galvan, Vicente
Entesari, Nazanin
Goeppert, Alain
Prakash, G. K. Surya [1 ]
机构
[1] Univ Southern Calif, Loker Hydrocarbon Res Inst, Los Angeles, CA 90089 USA
关键词
Carbon capture and utilization; Renewable methanol economy; Direct air capture; Heterogeneous catalyst; Hydrogenation; Carbon neutral cycle; CARBON-DIOXIDE CAPTURE; LOW-TEMPERATURE SYNTHESIS; IN-SITU HYDROGENATION; OF-THE-ART; HOMOGENEOUS HYDROGENATION; DIMETHYL ETHER; AMINE; WATER; GAS; DEACTIVATION;
D O I
10.1016/j.jcou.2021.101762
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
A highly effective liquid phase system for hydrogenation of CO2 to methanol using a heterogeneous Cu/ZnO/Al2O3 catalyst under batch conditions was developed. Among the screened solvents, glycols were found to have a marked promoting effect on methanol formation at a relatively low temperature range of 170-200 degrees C using molecular H-2. Relative to the solventless system, ethylene glycol enhanced the CO2 conversion values by up to 120% which is close to the calculated equilibrium limit. CH3OH yields of up to 90% were achieved. The catalyst was remarkably stable and recyclable over multiple hydrogenation cycles. Furthermore, CO2 captured by alkali hydroxides as well as amines were successfully hydrogenated to CH3OH with the Cu/ZnO/Al2O3 catalyst for the first time with >90% yields. The catalytic process and the plausible reaction pathways were evaluated by control experiments, which suggest that the hydrogenation in the presence of an alcohol proceeds through the formation of formate ester as an intermediate. Finally, the integration of direct air capture (DAC) and hydrogenation of CO2 was demonstrated efficiently as a novel methanol synthesis process using the combination of heterogeneous catalysis and air as a renewable carbon source. Such scalable processes have considerable potential for synthesis of renewable methanol in an efficient and relatively cost-effective approach.
引用
收藏
页数:8
相关论文
共 50 条
[31]   Comparison of fibrous versus Cu/ZnO/Al2O3 catalyst for CO2 hydrogenation to methanol through modeling the reactor and the process flowsheet [J].
Pedro C. Dalben ;
Vanessa V. Gomes ;
Delano M. Santana ;
Silvio A. B. Vieira de Melo ;
Karen V. Pontes .
Brazilian Journal of Chemical Engineering, 2023, 40 :539-554
[32]   Direct Conversion of CO2 into Dimethyl Ether over Al2O3/Cu/ZnO Catalysts Prepared by Sequential Precipitation [J].
Jeong, Cheonwoo ;
Kim, Jinsung ;
Kim, Ji-Hyeon ;
Lee, Sunghoon ;
Bae, Jong Wook ;
Suh, Young-Woong .
CATALYSTS, 2019, 9 (06)
[33]   Cu-ZnO@Al2O3 hybrid nanoparticle with enhanced activity for catalytic CO2 conversion to methanol [J].
Thanh Truc Nguyen Hoang ;
Lin, Yu-Shih ;
Thi Nhu Huynh Le ;
Tien Khoa Le ;
Thi Kieu Xuan Huynh ;
Tsai, De-Hao .
ADVANCED POWDER TECHNOLOGY, 2021, 32 (05) :1785-1792
[34]   Enhanced CO2 Hydrogenation to Methanol on the Mesostructured Cu-ZnO/Al2O3-ZrO2 Catalyst [J].
Guo, Qing ;
Li, Shaozhong ;
Li, Jin ;
Hu, Yongke ;
Duanmu, Chuansong .
ACS APPLIED ENERGY MATERIALS, 2021, 4 (08) :8311-8321
[35]   Steam reforming of methanol over Cu/ZnO/ZrO2/Al2O3 catalyst [J].
Park, Jung Eun ;
Yim, Sun-Dae ;
Kim, Chang Soo ;
Park, Eun Duck .
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY, 2014, 39 (22) :11517-11527
[36]   Integrated Carbon Dioxide Capture and Conversion to Methanol Utilizing Tertiary Amines over a Heterogenous Cu/ZnO/Al2O3 Catalyst [J].
Suhail, Zohaib ;
Koch, Christopher J. ;
Goeppert, Alain ;
Prakash, G. K. Surya .
LANGMUIR, 2024, 40 (10) :5401-5408
[37]   Kinetic modeling of the methanol-assisted autocatalytic methanol synthesis on Cu/ZnO/Al2O3 [J].
Kortuz, Wieland ;
Leipold, Johannes ;
Kienle, Achim ;
Seidel-Morgenstern, Andreas .
CHEMICAL ENGINEERING JOURNAL, 2025, 518
[38]   Study of CO2 adsorption on a commercial CuO/ZnO/Al2O3 catalyst [J].
Smyrnioti, Maria ;
Tampaxis, Christos ;
Steriotis, Theodore ;
Ioannides, Theophilos .
CATALYSIS TODAY, 2020, 357 :495-502
[39]   Influence of Cu/Al Ratio on the Performance of Carbon-Supported Cu/ZnO/Al2O3 Catalysts for CO2 Hydrogenation to Methanol [J].
Xie, Zhong ;
Hei, Jinpei ;
Cheng, Lei ;
Li, Jing ;
Yin, Xiaojie ;
Meng, Sugang .
CATALYSTS, 2023, 13 (05)
[40]   Effect of Al-containing precursors on Cu/ZnO/Al2O3 catalyst for methanol production [J].
Zhang, Fan ;
Liu, Yuan ;
Xu, Xiaoying ;
Yang, Panpan ;
Miao, Ping ;
Zhang, Yulong ;
Sun, Qi .
FUEL PROCESSING TECHNOLOGY, 2018, 178 :148-155