Highly selective CuO-ZnO@Cu-MOR catalysts prepared by ultrafast solid processing for carbon dioxide hydrogenation to methanol

IF 4.8 3区 材料科学 Q1 CHEMISTRY, APPLIED Microporous and Mesoporous Materials Pub Date : 2024-04-19 DOI:10.1016/j.micromeso.2024.113140
Yayu Wei , Bo Peng , Yanhong Li , Run Xu , Aisheng Huang
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Abstract

The conversion of CO2 into methanol has emerged as a promising strategy for addressing climate change and optimizing the utilization of carbon resources. Conventional synthesis methods for Cu-based catalysts, such as co-precipitation, necessitate the consumption of substantial amounts of solvent and meticulous control over preparation conditions, while also being susceptible to deactivation by water during hydrogenation. Therefore, it is crucial to develop a catalyst that can be readily synthesized and exhibits outstanding performance and durability. In this study, we present an ultrafast (only 20 min), solid-phase grinding approach to fabricate CuO-ZnO@Cu-MOR catalysts for CO2 hydrogenation to methanol. The resulting catalysts were comprehensively characterized using XRD, XPS, H2-TPR, NH3-TPD, SEM, HRTEM, and In-situ-FTIR techniques. Notably, the CuO-ZnO@Cu-MOR catalysts with a distinctive capsule-like structure displayed a high catalytic performance for CO2 hydrogenation. The byproducts of methane and water produced by the CO2 hydrogenation process were able to be further converted to methanol through Cu-MOR, leading to a significant enhancement of the methanol selectivity (95.6 %) and CO2 conversion (22.8 %). Moreover, a long-term test lasting 300 h demonstrated constant catalytic performances and superior durability.

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通过超快固体加工制备的高选择性 CuO-ZnO@Cu-MOR 催化剂用于二氧化碳加氢制甲醇
将二氧化碳转化为甲醇已成为应对气候变化和优化碳资源利用的一项前景广阔的战略。铜基催化剂的传统合成方法(如共沉淀法)需要消耗大量溶剂并对制备条件进行严格控制,同时还容易在氢化过程中被水失活。因此,开发一种易于合成、性能优异且经久耐用的催化剂至关重要。在本研究中,我们介绍了一种超快速(仅需 20 分钟)固相研磨方法,用于制备 CuO-ZnO@Cu-MOR 催化剂,用于 CO2 加氢制甲醇。利用 XRD、XPS、H2-TPR、NH3-TPD、SEM、HRTEM 和原位傅立叶变换红外技术对制备的催化剂进行了全面表征。值得注意的是,具有独特胶囊状结构的 CuO-ZnO@Cu-MOR 催化剂对二氧化碳加氢具有很高的催化性能。二氧化碳加氢过程中产生的副产物甲烷和水能够通过 Cu-MOR 进一步转化为甲醇,从而显著提高了甲醇选择性(95.6%)和二氧化碳转化率(22.8%)。此外,持续 300 小时的长期测试表明,该催化剂具有稳定的催化性能和卓越的耐久性。
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来源期刊
Microporous and Mesoporous Materials
Microporous and Mesoporous Materials 化学-材料科学:综合
CiteScore
10.70
自引率
5.80%
发文量
649
审稿时长
26 days
期刊介绍: Microporous and Mesoporous Materials covers novel and significant aspects of porous solids classified as either microporous (pore size up to 2 nm) or mesoporous (pore size 2 to 50 nm). The porosity should have a specific impact on the material properties or application. Typical examples are zeolites and zeolite-like materials, pillared materials, clathrasils and clathrates, carbon molecular sieves, ordered mesoporous materials, organic/inorganic porous hybrid materials, or porous metal oxides. Both natural and synthetic porous materials are within the scope of the journal. Topics which are particularly of interest include: All aspects of natural microporous and mesoporous solids The synthesis of crystalline or amorphous porous materials The physico-chemical characterization of microporous and mesoporous solids, especially spectroscopic and microscopic The modification of microporous and mesoporous solids, for example by ion exchange or solid-state reactions All topics related to diffusion of mobile species in the pores of microporous and mesoporous materials Adsorption (and other separation techniques) using microporous or mesoporous adsorbents Catalysis by microporous and mesoporous materials Host/guest interactions Theoretical chemistry and modelling of host/guest interactions All topics related to the application of microporous and mesoporous materials in industrial catalysis, separation technology, environmental protection, electrochemistry, membranes, sensors, optical devices, etc.
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