Effect of surface basicity over the supported Cu-ZnO catalysts on hydrogenation of CO2 to methanol

被引：46

作者：

Guo, Tan ^{[1
]}

Guo, Qing ^{[1
]}

Li, Shaozhong ^{[1
]}

Hu, Yongke ^{[1
]}

Yun, Shan ^{[1
]}

Qian, Yunhua ^{[1
]}

机构：

[1] Huaiyin Inst Technol, Natl & Local Joint Engn Res Ctr Mineral Salt Deep, Key Lab Palygorskite Sci & Appl Technol OfJ Angsu, Huaian 223003, Peoples R China

来源：

JOURNAL OF CATALYSIS | 2022年 / 407卷

关键词：

Cu-ZnO; Surface basicity; CO2; Hydrogenation; Methanol; COPPER-CATALYSTS; ACTIVE-SITES; ZR; PERFORMANCE; ADSORPTION; INDUSTRIAL; MECHANISM; INSIGHTS;

D O I：

10.1016/j.jcat.2022.01.035

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：

CO2 hydrogenation to methanol can relieve energy shortage and weaken CO2 emission, and Cu-ZnO catalysts show excellent activity, in which the surface basicity improves conversion and selectivity, but the influence mechanism is often ignored. In this work, Cu-ZnO/Al2O3, Cu-ZnO/Al2O3-MgO and Cu-ZnO/MgO were prepared to study the effect of surface basicity on CO2 hydrogenation to methanol. It was found that MgO increased the dispersed CuO species and strengthened surface basicity, leading to higher SCu and electron density on Cu surface, respectively, which promoted CO2 conversion. Meanwhile, the surface basicity strengthened CO adsorption and weakened methanol adsorption, which greatly increased methanol selectivity. In addition, methanol adsorption on catalyst surface seriously inhibited CO2 adsorption, while the strong surface basicity greatly weakened the inhibition. Besides, the strong surface basicity inhibited the dissociation of methanol into CO species. Finally, the Cu-ZnO catalyst with strong surface basicity showed high activity and selectivity. (c) 2022 Elsevier Inc. All rights reserved.

引用

页码：312 / 321

页数：10

共 64 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]

Behrens M, 2012, SCIENCE, V336, P893, DOI [10.1126/science.1219831, 10.1126/science.12198331]

[3] Methanol Synthesis from CO2 Hydrogenation [J].

Bowker, Michael .

CHEMCATCHEM, 2019, 11 (17) :4238-4246

[4]

Buendia F., 2021, CATAL TODAY, DOI [10.1016/ j.cattod.2021.1010.1002, DOI 10.1016/J.CATTOD.2021.1010.1002]

[5] New insights on CO and CO2 hydrogenation for methanol synthesis: The key role of adsorbate-adsorbate interactions on Cu and the highly active MgO-Cu interface [J].

Cao, Ang ;

Wang, Zhenbin ;

Li, Hao ;

Elnabawy, Ahmed O. ;

Norskov, Jens K. .

JOURNAL OF CATALYSIS, 2021, 400 :325-331

[6] APPLICATIONS OF ADSORPTION MICROCALORIMETRY TO THE STUDY OF HETEROGENEOUS CATALYSIS [J].

CARDONAMARTINEZ, N ;

DUMESIC, JA .

ADVANCES IN CATALYSIS, 1992, 38 :149-244

[7] The effect of surface acidic and basic properties on the hydrogenation of lauronitrile over the supported nickel catalysts [J].

Chen, Hui ;

Xue, Mingwei ;

Hu, Shenghua ;

Shen, Jianyi .

CHEMICAL ENGINEERING JOURNAL, 2012, 181 :677-684

[8] CO2 hydrogenation to methanol over Cu catalysts supported on La-modified SBA-15: The crucial role of Cu-LaOx interfaces [J].

Chen, Kun ;

Fang, Huihuang ;

Wu, Simson ;

Liu, Xi ;

Zheng, Jianwei ;

Zhou, Song ;

Duan, Xinping ;

Zhuang, Yichao ;

Tsang, Shik Chi Edman ;

Yuan, Youzhu .

APPLIED CATALYSIS B-ENVIRONMENTAL, 2019, 251 :119-129

[9] 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

[10] The role of copper oxidation state in Cu/ZnO/Al2O3 catalysts in CO2 hydrogenation and methanol productivity [J].

Dasireddy, Venkata D. B. C. ;

Likozar, Blaz .

RENEWABLE ENERGY, 2019, 140 :452-460

← 1 2 3 4 5 6 7 →