Tang Rui, Zhu Zhijie, Li Chaoran, Xiao Mengqi, Wu Zhiyi, Zhang Dake, Zhang Chengcheng, Xiao Yi, Chu Mingyu, Genest Alexander, Rupprechter Günther, Zhang Liang, Zhang Xiaohong, He Le
Institute of Functional Nano & Soft Materials (FUNSOM), Jiangsu Key Laboratory for Carbon-Based Functional Materials & Devices, Joint International Research Laboratory of Carbon-Based Functional Materials and Devices, Soochow University, Suzhou, Jiangsu 215123, China.
Institute of Materials Chemistry, Technische Universität, Wien, Vienna 1060, Austria.
ACS Mater Lett. 2021 Dec 6;3(12):1652-1659. doi: 10.1021/acsmaterialslett.1c00523. Epub 2021 Oct 27.
Cascade catalysis of reverse water gas shift (RWGS) and well-established CO hydrogenation holds promise for the conversion of greenhouse gas CO and renewable H into liquid hydrocarbons and methanol under mild conditions. However, it remains a big challenge to develop low-temperature RWGS catalysts with high activity, selectivity, and stability. Here, we report the design of an efficient RWGS catalyst by encapsulating ruthenium clusters with the size of 1 nm inside hollow silica shells. The spatially confined structure prevents the sintering of Ru clusters while the permeable silica layer allows the diffusion of gaseous reactants and products. This catalyst with reduced particle sizes not only inherits the excellent activity of Ru in CO hydrogenation reactions but also exhibits nearly 100% CO selectivity and superior stability at 200-500 °C. The ability to selectively produce CO from CO at relatively low temperatures paves the way for the production of value-added fuels from CO and renewable H.
逆水煤气变换（RWGS）的级联催化以及成熟的CO加氢反应有望在温和条件下将温室气体CO和可再生H转化为液态烃和甲醇。然而，开发具有高活性、选择性和稳定性的低温RWGS催化剂仍然是一个巨大的挑战。在此，我们报道了一种通过将尺寸为1nm的钌簇封装在中空二氧化硅壳内来设计高效RWGS催化剂的方法。空间受限结构可防止Ru簇烧结，而可渗透的二氧化硅层允许气态反应物和产物扩散。这种粒径减小的催化剂不仅继承了Ru在CO加氢反应中的优异活性，而且在200-500°C下表现出近100%的CO选择性和优异的稳定性。在相对较低温度下从CO中选择性生产CO的能力为从CO和可再生H生产增值燃料铺平了道路。
