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Bimetallic metal organic framework-templated synthesis of a Cu-ZnO/Al2O3 catalyst with superior methanol selectivity for CO2 hydrogenation
Molecular Catalysis ( IF 3.9 ) Pub Date : 2021-09-11 , DOI: 10.1016/j.mcat.2021.111870
Tianqinji Qi 1 , Yiming Zhao 1 , Shaoyun Chen 1 , Weizuo Li 2 , Xinwen Guo 1 , Yongchun Zhang 1 , Chunshan Song 3, 4
Affiliation  

It is highly desirable to develop inexpensive and highly selective catalyst for CO2 hydrogenation to methanol and Cu/ZnO/Al2O3 is a promising formulation. Herein, we report the design and synthesis of a Cu-ZnO/Al2O3 catalyst via a bimetallic metal organic framework (MOF)-templated strategy (termed Cu-ZnOMOF⊂Al2O3) and shed light on the role of the Cu-Zn@MOF precursor in this system for methanol synthesis. The developed Cu-ZnOMOF⊂Al2O3 exhibited high methanol selectivity (86.9%) and methanol space-time yield (407.2 gMeOH•kgcat−1•h−1) at higher CO2 conversion (9.1%) in comparison with the conventional Cu-ZnONO3/Al2O3 catalyst (79.6% and 209.0 gMeOH•kgcat−1•h−1, and 5.1%, respectively) at 240 ºC under 3.0 MPa. Spectroscopic characterization (TEM, XPS, EDX, in-situ DRIFTS) coupled with N2O chemisorption and temperature-programmed desorption of CO2 and H2 revealed that the surface of the new Cu-ZnOMOF⊂Al2O3 catalyst possesses higher Cu dispersion, surface-enriched ZnO and more Cu-ZnO interfacial sites, which leads to higher capability for CO2 and H2 adsorption and activation. These are considered to be the origin of higher methanol selectivity and enhanced activity of the catalyst prepared by the MOF-templated strategy for CO2 hydrogenation. This work offers a novel approach to optimizing Cu-ZnO/Al2O3 catalyst for CO2 hydrogenation to methanol.



中文翻译:

双金属金属有机骨架模板合成的 Cu-ZnO/Al2O3 催化剂对 CO2 加氢具有优异的甲醇选择性

开发用于将CO 2加氢成甲醇的廉价且高选择性的催化剂是非常可取的,并且Cu/ZnO/Al 2 O 3是一种有前途的配方。在此,我们报告了通过双金属金属有机骨架 (MOF) 模板化策略(称为 Cu-ZnO MOF ⊂Al 2 O 3)设计和合成的 Cu-ZnO/Al 2 O 3催化剂,并阐明了催化剂的作用。该系统中用于甲醇合成的 Cu-Zn@MOF 前驱体。所开发的Cu-ZnO MOF ⊂Al 2 O 3表现出较高的甲醇选择性(86.9%)和甲醇时空产率(407.2 g MeOH •kgcat -1 •h -1 )与传统的 Cu-ZnO NO3 /Al 2 O 3催化剂(79.6% 和 209.0 g MeOH •kg cat -1 •h -1相比,CO 2转化率更高(9.1%),和分别为 5.1%)在 240 ºC 和 3.0 MPa。结合 N 2 O 化学吸附和 CO 2和 H 2的程序升温脱附的光谱表征(TEM、XPS、EDX、原位漂移)表明,新型 Cu-ZnO MOF ⊂Al 2 O 3 的表面催化剂具有更高的Cu分散性、表面富集的ZnO和更多的Cu-ZnO界面位点,从而提高了对CO 2和H 2 的吸附和活化能力。这些被认为是通过 MOF 模板化 CO 2加氢策略制备的催化剂具有更高的甲醇选择性和增强的活性的原因。这项工作提供了一种优化用于 CO 2加氢制甲醇的Cu-ZnO/Al 2 O 3催化剂的新方法。

更新日期:2021-09-12
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