He Ruosong, Wang Yang, Li Meng, Liu Jianxin, Gu Yongqiang, Wang Wenhang, Liu Qiang, Tsubaki Noritatsu, Wu Mingbo
College of New Energy, State Key Laboratory of Heavy Oil Processing, China University of Petroleum (East China), Qingdao, 266580, China.
Department of Applied Chemistry, Graduate School of Engineering, University of Toyama, Gofuku 3190, Toyama, 930-8555, Japan.
Chemistry. 2023 Nov 21;29(65):e202301918. doi: 10.1002/chem.202301918. Epub 2023 Oct 11.
Even though Fe-based catalysts have been widely employed for CO hydrogenation into hydrocarbons, oxygenates, liquid fuels, etc., the precise regulation of their physicochemical properties is needed to enhance the catalytic performance. Herein, under the guidance of the traditional concept in heterogeneous catalysis-confinement effect, a core-shell structured catalyst Na-Fe O @C is constructed to boost the CO hydrogenation performance. Benefiting from the carbon-chain growth limitation, tailorable H /CO ratio on the catalytic interface, and unique electronic property that all endowed by the confinement effect, the selectivity and space-time yield of light olefins (C -C ) are as high as 47.4 % and 15.9 g mol h , respectively, which are all notably higher than that from the shell-less counterpart. The function mechanism of the confinement effect in Fe-based catalysts are clarified in detail by multiple characterization and density functional theory (DFT). This work may offer a new prospect for the rational design of CO hydrogenation catalyst.
尽管铁基催化剂已被广泛用于将CO加氢转化为烃类、含氧化合物、液体燃料等,但仍需要精确调控其物理化学性质以提高催化性能。在此,在多相催化中的传统概念——限域效应的指导下,构建了一种核壳结构催化剂Na-FeO@C以提高CO加氢性能。受益于限域效应赋予的碳链生长限制、催化界面上可调节的H/CO比以及独特的电子性质,轻质烯烃(C₂-C₄)的选择性和时空产率分别高达47.4%和15.9 g mol⁻¹ h⁻¹,均显著高于无壳对应物。通过多种表征和密度泛函理论(DFT)详细阐明了铁基催化剂中限域效应的作用机制。这项工作可能为CO加氢催化剂的合理设计提供新的前景。