Xu Ming, Qin Xuetao, Xu Yao, Zhang Xiaochen, Zheng Lirong, Liu Jin-Xun, Wang Meng, Liu Xi, Ma Ding
College of Chemistry and Molecular Engineering, Peking University, Beijing, 100871, P. R. China.
State Key Laboratory of Chemical Resource Engineering, Beijing University of Chemical Technology, Beijing, 100029, P. R. China.
Nat Commun. 2022 Nov 7;13(1):6720. doi: 10.1038/s41467-022-34463-7.
Considerable attention has been drawn to tune the geometric and electronic structure of interfacial catalysts via modulating strong metal-support interactions (SMSI). Herein, we report the construction of a series of TiO/Ni catalysts, where disordered TiO overlayers immobilized onto the surface of Ni nanoparticles (~20 nm) are successfully engineered with SMSI effect. The optimal TiO/Ni catalyst shows a CO conversion of ~19.8% in Fischer-Tropsch synthesis (FTS) process under atmospheric pressure at 220 °C. More importantly, ~64.6% of the product is C paraffins, which is in sharp contrast to the result of the conventional Ni catalyst with the main product being methane. A combination study of advanced electron microscopy, multiple in-situ spectroscopic characterizations, and density functional theory calculations indicates the presence of Ni/TiO interfacial sites, which could bind carbon atom strongly, inhibit methane formation and facilitate the C-C chain propagation, lead to the production of C hydrocarbon on Ni surface.
通过调节强金属-载体相互作用（SMSI）来调控界面催化剂的几何结构和电子结构已引起了广泛关注。在此，我们报道了一系列TiO/Ni催化剂的构建，其中固定在Ni纳米颗粒（~20 nm）表面的无序TiO覆盖层通过SMSI效应成功制备。最佳的TiO/Ni催化剂在220℃常压下的费托合成（FTS）过程中显示出约19.8%的CO转化率。更重要的是，约64.6%的产物为C链烷烃，这与以甲烷为主产物的传统Ni催化剂的结果形成鲜明对比。先进电子显微镜、多种原位光谱表征和密度泛函理论计算的联合研究表明存在Ni/TiO界面位点，该位点可强烈结合碳原子，抑制甲烷生成并促进C-C链传播，从而在Ni表面生成C烃。
