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    二氧化碳催化加氢制烯烃的研究进展

    Progress in CO2-to-olefins conversion via hydrogenation

    • 摘要: 在全球气候变化和能源结构转型的背景下,CO2的高效转化与利用成为实现“双碳”目标的关键路径之一。烯烃作为重要的化工原料,其传统生产方式高度依赖化石资源,导致高能耗与高碳排放。因此,利用绿氢将CO2催化加氢转化为烯烃,不仅有助于减少温室气体排放,还能缓解对石化资源的依赖。基于此,系统综述了近年来CO2加氢制烯烃领域的研究进展,重点探讨了催化剂的设计和催化机理。首先,概述了CO2加氢制烯烃的主要技术路线,包括CO中间体路线和甲醇中间体路线。随后,阐述了催化剂的设计策略,包括主催化剂的选择(如铁基、钴基催化剂)、助剂的添加(如碱金属、过渡金属助剂)以及载体的优化(如金属氧化物、碳材料载体)。这些策略通过调控催化剂的电子结构、表面酸碱性以及活性位点的暴露,显著提升了CO2加氢制烯烃的催化性能。在催化机理方面,深入分析了CO中间体路线和甲醇中间体路线的反应机理。CO中间体路线涉及CO2的吸附与活化、CO的生成与扩散以及费托过程中的C-C偶联与加氢等步骤,而甲醇中间体路线则通过串联反应实现CO2到烯烃的转化,突破了Anderson-Schulz-Flory分布的限制,显著提高了低碳烯烃的选择性。最后,展望了未来CO2加氢制烯烃技术的发展方向,包括开发更高效、更稳定的催化剂体系,以及设计多级反应器或膜反应器等新型反应器,以提高反应效率。综上,综述了CO2加氢制烯烃催化剂的设计与催化机理,分析了不同技术路线和催化剂策略的优势与不足,并提出了未来研究的方向和重点。随着绿色化学和可持续发展理念的深入推广,CO2加氢制烯烃技术有望成为实现碳中和目标的重要途径之一。

       

      Abstract: Under the dual imperatives of global climate change and energy structure transition, the efficient conversion and utilization of CO2 has emerged as a pivotal pathway toward achieving the “dual carbon” goals. Olefins, as essential chemical feedstock, are traditionally produced through fossil resource-intensive processes characterized by high energy consumption and substantial carbon emissions. Consequently, the catalytic hydrogenation of CO2 to olefins using green hydrogen presents a promising strategy to mitigate greenhouse gas emissions while reducing reliance on petrochemical resources. Against this backdrop, this review systematically summarizes recent advancements in CO2 hydrogenation to olefins, with a particular focus on catalyst design and reaction mechanisms. The review begins with a comprehensive overview of the primary technical routes for CO2-to-olefins conversion, including the CO-mediated pathway and MTO pathway. Subsequently, it elaborates on catalyst design strategies, encompassing the selection of active components (e.g., Fe-based and Co-based catalysts), the incorporation of promoters (e.g., alkali metals and transition metals), and the optimization of supports (e.g., metal oxides and carbon-based materials). These strategies significantly enhance catalytic performance by modulating electronic structures, surface acid-base properties, and the exposure of active sites. Regarding reaction mechanisms, the review provides an in-depth analysis of the CO-mediated and methanol-mediated pathways. The CO-mediated route involves sequential steps such as CO2 adsorption/activation, CO formation/diffusion, and C-C coupling/hydrogenation during FTS. In contrast, the methanol-mediated pathway enables direct CO2-to-olefins conversion via a two-step process, circumventing the Anderson-Schulz-Flory distribution limitation and markedly improving selectivity toward light olefins. Finally, the review oulines future research directions, including the development of more efficient and stable catalytic systems, as well as the design of novel reactors (e.g., multi-stage or membrane reactors) to enhance process efficiency. In summary, this work systematically examines catalyst design principles and mechanistic insights in CO2 hydrogenation to olefins, critically evaluates the merits and limitations of different technical approaches, and proposes key areas for future investigation. With the growing emphasis on green chemistry and sustainable development, CO₂ hydrogenation to olefins holds significant potential as a transformative technology for achieving carbon neutrality.

       

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