McNeary W Wilson, Ellebracht Nathan C, Jue Melinda L, Rasmussen Mathew J, Crawford James M, Yung Matthew M, To Anh T, Pang Simon H
Catalytic Carbon Transformation and Scale-Up Center, National Renewable Energy Laboratory, Golden, Colorado 80401, United States.
Materials Science Division, Lawrence Livermore National Laboratory, Livermore, California 94550, United States.
ACS Omega. 2025 Jan 16;10(3):2364-2371. doi: 10.1021/acsomega.4c10049. eCollection 2025 Jan 28.
Reactive CO capture (RCC) is a promising strategy for process intensification of carbon capture and conversion for production of low-carbon fuels and chemicals. As state-of-the-art sorbent materials in point source and direct air capture systems, solid-supported amines are a natural choice to pair with supported CO hydrogenation catalysts (e.g., metallic nanoparticles) for developing high-capacity sorbent-catalyst materials for use in RCC. In this Perspective, we summarize the relevant literature combining solid-supported amines with metallic nanoparticles for thermocatalytic RCC and detail two of our own case studies using RCC to synthesize methane and methanol. Our observations suggest that the temperature mismatch between CO desorption and reaction, along with potential catalyst site poisoning by grafted aminosilanes, is a significant obstacle to realizing the potential of amine-based RCC materials in the decarbonization of chemical production. This stands in contrast to literature detailing successful RCC using liquid amines and solid catalysts, which may benefit from more favorable mass transfer dynamics, as well as early stage reports into RCC solid-phase amine-Pd materials, whose findings we were not able to replicate. More judicious reaction selection and synthetic design strategies to match materials with process conditions offer alternative pathways for future research.
反应性CO捕集（RCC）是一种很有前景的策略，可用于强化碳捕集与转化过程，以生产低碳燃料和化学品。作为点源和直接空气捕集系统中的先进吸附剂材料，固体负载胺是与负载型CO加氢催化剂（如金属纳米颗粒）配对的自然选择，用于开发用于RCC的高容量吸附剂-催化剂材料。在这篇展望文章中，我们总结了将固体负载胺与金属纳米颗粒结合用于热催化RCC的相关文献，并详细介绍了我们自己的两个使用RCC合成甲烷和甲醇的案例研究。我们的观察结果表明，CO解吸与反应之间的温度不匹配，以及接枝氨基硅烷可能导致的催化剂位点中毒，是实现胺基RCC材料在化学生产脱碳方面潜力的重大障碍。这与详细介绍使用液体胺和固体催化剂成功进行RCC的文献形成对比，后者可能受益于更有利的传质动力学，以及关于RCC固相胺-Pd材料的早期报告，但其结果我们无法重复。更明智地选择反应和设计合成策略，以使材料与工艺条件相匹配，为未来的研究提供了替代途径。
