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Boosting CO hydrogenation towards C2+ hydrocarbons over interfacial TiO2−x/Ni catalysts
Nature Communications ( IF 14.7 ) Pub Date : 2022-11-07 , DOI: 10.1038/s41467-022-34463-7
Ming Xu 1, 2 , Xuetao Qin 1 , Yao Xu 1 , Xiaochen Zhang 1 , Lirong Zheng 3 , Jin-Xun Liu 4 , Meng Wang 1 , Xi Liu 5, 6 , Ding Ma 1
Affiliation  

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 TiO2−x/Ni catalysts, where disordered TiO2−x overlayers immobilized onto the surface of Ni nanoparticles (~20 nm) are successfully engineered with SMSI effect. The optimal TiO2−x/Ni catalyst shows a CO conversion of ~19.8% in FischerTropsch synthesis (FTS) process under atmospheric pressure at 220 °C. More importantly, ~64.6% of the product is C2+ 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 Niδ−/TiO2−x interfacial sites, which could bind carbon atom strongly, inhibit methane formation and facilitate the C-C chain propagation, lead to the production of C2+ hydrocarbon on Ni surface.



中文翻译:

在界面 TiO2−x/Ni 催化剂上促进 CO 加氢生成 C2+ 烃

通过调节强金属-载体相互作用 (SMSI)来调整界面催化剂的几何和电子结构引起了相当大的关注。在此,我们报告了一系列 TiO 2- x /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 2- x覆盖层成功地设计为具有 SMSI 效应。最佳 TiO 2− x /Ni 催化剂在 220 °C 大气压下费-托合成 (FTS) 过程中的 CO 转化率约为 19.8% 。更重要的是,约 64.6% 的产品是 C 2+链烷烃,这与传统 Ni 催化剂的主要产物是甲烷的结果形成鲜明对比。先进的电子显微镜、多个原位光谱表征和密度泛函理论计算的组合研究表明 Ni δ− /TiO 2− x界面位点的存在,它可以强烈地结合碳原子,抑制甲烷形成并促进 CC 链传播,导致 Ni 表面产生 C 2+烃。

更新日期:2022-11-08
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