氧化锆作为促进剂对用于二氧化碳加氢制甲醇的铜/MOF-5 催化剂的影响

Amanda S. Mbhele , Mduduzi N. Cele , Mzamo L. Shozi , Holger B. Friedrich
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引用次数: 0

摘要

二氧化碳浓度的上升是造成严重气候变化和生态问题的主要人为因素。催化加氢将二氧化碳转化为包括甲醇在内的高附加值化学品和燃料,是实现含碳原料价值化和减少全球二氧化碳排放的极具吸引力的环保方法之一。然而,如何在保持稳定性的同时提高催化活性以获得高甲醇产率和选择性仍是一大挑战。本研究调查了不同 ZrO₂负载量对 Cu/MOF-5 催化剂的促进作用,以确定其对 CO₂ 加氢催化性能的影响。铜的负载量保持不变,而 MOF-5 载体上的 ZrO₂含量则通过浸渍方法变化。由于在 X 射线衍射图中没有检测到 ZrO₂ 的结晶相,因此发现 ZrO₂ 的添加会影响 BET 表面积,这表明存在无定形的 ZrO₂。催化结果表明,添加 ZrO₂ 提高了催化活性,CO₂ 转化率提高到 13.2%。结果表明,催化性能与活性金属的还原性之间存在相关性,而活性金属的还原性则受氧化锆含量的影响。ZrO₂ 负载量最高的催化剂性能最好,这归因于其表面积增大和还原性增强。在优化条件下(GHSV 为 1350 h-¹,温度为 200 °C,压力为 30 bar),催化剂的甲醇选择性达到了 100%。这项研究强调了氧化锆作为促进剂在提高 Cu/MOF-5 催化剂活性和选择性方面的重要作用,为设计 CO₂ 加氢的高效催化系统提供了重要的启示。
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The effect of zirconia as a promoter on Cu/MOF-5 catalysts for CO2 hydrogenation to methanol

The rise in carbon dioxide concentration is a primary anthropogenic source of severe climate change and ecological issues. Catalytic hydrogenation of CO2 into value-added chemicals and fuels including methanol is one of the attractive environmentally friendly ways to valorize carbon-containing feedstock and reduce global CO2 emissions. However, enhancing catalytic activity to achieve high methanol yield and selectivity while maintaining stability remains a major challenge. This study investigated the promotion of Cu/MOF-5 catalysts with varying loadings of ZrO₂ to determine its effects on catalytic performance in CO₂ hydrogenation. The copper loading was kept constant while the ZrO₂ content on the MOF-5 support was varied via the impregnation method. The addition of ZrO₂ was found to influence the BET surface area, suggesting the presence of amorphous ZrO₂, as its crystalline phases were not detected in x-ray diffractograms. Catalytic results demonstrated that ZrO₂ addition enhanced the catalytic activity, with increased CO₂ conversion up to 13.2 %. The results showed a correlation between catalytic performance and the reducibility of the active metal, driven by the amount of ZrO₂ present. The catalyst with the highest ZrO₂ loading exhibited the best performance, attributed to its increased surface area and enhanced reducibility. Under optimized conditions (GHSV of 1350 h⁻¹, temperature of 200 °C, and pressure of 30 bar), the catalyst achieved 100 % methanol selectivity. This study underscores the significant role of ZrO₂ as a promoter in enhancing the activity and selectivity of Cu/MOF-5 catalysts, providing critical insights into the design of efficient catalytic systems for CO₂ hydrogenation.

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来源期刊
CiteScore
8.40
自引率
0.00%
发文量
100
审稿时长
33 weeks
期刊介绍: The journal has a particular interest in publishing papers on the unique issues facing chemical engineering taking place in countries that are rich in resources but face specific technical and societal challenges, which require detailed knowledge of local conditions to address. Core topic areas are: Environmental process engineering • treatment and handling of waste and pollutants • the abatement of pollution, environmental process control • cleaner technologies • waste minimization • environmental chemical engineering • water treatment Reaction Engineering • modelling and simulation of reactors • transport phenomena within reacting systems • fluidization technology • reactor design Separation technologies • classic separations • novel separations Process and materials synthesis • novel synthesis of materials or processes, including but not limited to nanotechnology, ceramics, etc. Metallurgical process engineering and coal technology • novel developments related to the minerals beneficiation industry • coal technology Chemical engineering education • guides to good practice • novel approaches to learning • education beyond university.
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