高级检索

    铜基催化剂在CO2加氢制甲醇过程中的研究现状及展望

    Research status and prospect of copper-based catalysts in the process of CO2 hydrogenation to methanol

    • 摘要: 大气中CO2含量的快速增加引发了温室效应等系列环境问题,CO2的利用对于实现“碳达峰、碳中和”的目标至关重要。催化加氢是将CO2选择性转化为有价值化学品的重要方法,其中甲醇是一种重要的化学原料,可用作合成化学品和燃料的平台分子。CO2催化加氢制甲醇的关键在于开发低成本、环保和高效的催化剂。铜基催化剂因其低成本和甲醇合成高效性而得到广泛研究,但CO2化学键稳定,温度过低时难以实现C=O键的激活和断裂,且反应过程中存在副反应和催化剂失活等问题。因此,重点阐述了CO2加氢制甲醇的r-甲酸反应机理、RWGS+CO 加氢(RWGS + CO Hydrogenation)反应机理和反式-COOH反应机理;归纳了铜基金属–载体结构及氧空位等催化剂关键性质对其选择性、稳定性和活性的影响,进一步为揭示甲酸盐反应机理的作用机制提供见解;总结了Cu/ZnO、Cu/ZrO2、Cu/ZnO/ZrO2催化剂加氢过程中CO2活化方式、反应中间体结合及反应机理;论述了制备方法对Cu基催化剂结构特点、活性位点及还原条件差异的影响,为合理设计具有高活性、选择性和稳定性的催化剂提供指导。

       

      Abstract: The rapid increase of CO2 content in the atmosphere has led to environmental problems such as the greenhouse effect. The utilization of CO2 is crucial to achieve the goal of “carbon peak, carbon neutralization”. Catalytic hydrogenation of CO2 is an important method for the selective conversion of CO2 into methanol and other valuable chemicals. Methanol is an important chemical raw material and can be used as a platform molecule for the synthesis of chemicals and fuels. The key to the catalytic hydrogenation of CO2 to methanol is to create low-cost, environmentally friendly and efficient catalysts. In general, copper-based catalysts have been widely studied due to their low cost and effective synthesis of methanol. However, the chemical bond of CO2 is stable. When the temperature is too low, the C=O bond of CO2 is difficult to activate and break, and there are side reactions and catalyst deactivation during the reaction. Focus is placed on the mechanism of r-formic acid reaction, RWGS + CO Hydro reaction mechanism and trans-COOH reaction mechanism of CO2 hydrogenation to methanol. The effects of the properties of the catalyst such as copper-based metal-support structure and oxygen vacancies on the selectivity, stability and activity of the catalyst were summarized, which further provided some insights into its role in the mechanism of formate reaction. The CO2 activation mode, reaction intermediate binding and reaction mechanism in the hydrogenation process on Cu/ZnO, Cu/ZrO2 and Cu/ZnO/ZrO2 catalysts were further summarized. The effects of preparation methods on the structural characteristics, active sites and reduction conditions of Cu-based catalysts were discussed, which provided guidance for the rational design of catalysts with high activity, selectivity and stability.

       

    /

    返回文章
    返回