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
[41]   Correlation between the porosity of γ-Al2O3 and the performance of CuO–ZnO–Al2O3 catalysts for CO2 hydrogenation into methanol [J].
Nguyen Le-Phuc ;
Tri Van Tran ;
Phuong Ngo Thuy ;
Luong Huu Nguyen ;
Thuat Thanh Trinh .
Reaction Kinetics, Mechanisms and Catalysis, 2018, 124 :171-185
[42]   Effect of titanium on methanol synthesis from CO2 hydrogenation over Cu/γ-Al2O3 [J].
Qi, GX ;
Fei, JH ;
Zheng, XM ;
Hou, ZY .
CHINESE CHEMICAL LETTERS, 2001, 12 (06) :537-540
[43]   Methanol synthesis from CO2 hydrogenation over Cu/γ-Al2O3 catalysts modified by ZnO, ZrO2 and MgO [J].
Ren, Hong ;
Xu, Cheng-Hua ;
Zhao, Hao-Yang ;
Wang, Ya-Xue ;
Liu, Jie ;
Liu, Jian-Ying .
JOURNAL OF INDUSTRIAL AND ENGINEERING CHEMISTRY, 2015, 28 :261-267
[44]   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
[45]   For Better Industrial Cu/ZnO/Al2O3 Methanol Synthesis Catalyst: A Compositional Study [J].
Xiao, Kang ;
Wang, Qiong ;
Qi, Xingzhen ;
Zhong, Liangshu .
CATALYSIS LETTERS, 2017, 147 (06) :1581-1591
[46]   Co-Production of Methanol and Methyl Formate via Catalytic Hydrogenation of CO2 over Promoted Cu/ZnO Catalyst Supported on Al2O3 and SBA-15 [J].
Berahim, Nor Hafizah ;
Zabidi, Noor Asmawati Mohd ;
Suhaimi, Nur Amirah .
CATALYSTS, 2022, 12 (09)
[47]   Methanol Synthesis by CO2 Hydrogenation overCu/ZnO/Al2O3 Catalysts under Fluctuating Conditions [J].
Zurbel, Alexander ;
Kraft, Michael ;
Kavurucu-Schubert, Sena ;
Bertau, Martin .
CHEMIE INGENIEUR TECHNIK, 2018, 90 (05) :721-724
[48]   Enhanced catalytic performance of Zr modified CuO/ZnO/Al2O3 catalyst for methanol and DME synthesis via CO2 hydrogenation [J].
Ren, Shoujie ;
Fan, Xiao ;
Shang, Zeyu ;
Shoemaker, Weston R. ;
Ma, Lu ;
Wu, Tianpin ;
Li, Shiguang ;
Klinghoffer, Naomi B. ;
Yu, Miao ;
Liang, Xinhua .
JOURNAL OF CO2 UTILIZATION, 2020, 36 :82-95
[49]   From CO2 to Methanol on Cu/ZnO/Al2O3 Industrial Catalyst. What Do We Know about the Active Phase and the Reaction Mechanism? [J].
Pacchioni, Gianfranco .
ACS CATALYSIS, 2024, 14 (04) :2730-2745
[50]   Enhanced performance and stability of Cu/ZnO catalyst by hydrophobic treatment for low-temperature methanol synthesis from CO2 2 [J].
Wang, Fan ;
Chen, Fei ;
Guo, Xiaoyu ;
He, Yingluo ;
Gao, Weizhe ;
Yasuda, Shuhei ;
Yang, Guohui ;
Tsubaki, Noritatsu .
CATALYSIS TODAY, 2024, 425