双金属片
材料科学
催化作用
费托法
化学工程
X射线光电子能谱
钴
吸附
水溶液
合金
沸石咪唑盐骨架
氧化物
金属
选择性
物理化学
金属有机骨架
有机化学
化学
冶金
工程类
作者
Jyoti Gahtori,Chelsea L. Tucker,Tuhin Suvra Khan,Camilla de Sá Codeço,Túlio C. R. Rocha,Ankur Bordoloi
标识
DOI:10.1021/acsami.2c11296
摘要
Designing new materials for selective Fischer–Tropsch synthesis (FTS) is an elegant way to enhance local feedstock utilization like biomass and waste. In this approach, we have designed a thermally and chemically stable bimetallic PtCo/NC hybrid nanocomposite catalyst derived from a zeolitic imidazolate framework (ZIF-67, which contains cobalt as a metal center) through carbonization for low-temperature (413–473 K) aqueous-phase Fischer–Tropsch synthesis (AFTS). The selectivity of the desired range of hydrocarbons is adjusted using a highly dispersed PtCo bimetallic alloy, which facilitates extraordinary reduction of a metal oxide to active species by the synergic effect under the AFTS reaction conditions. The ZIF-derived catalyst tested in this study exhibited the highest activity to date for very low temperatures (433 K) in aqueous-phase Fischer–Tropsch synthesis with CO conversion rates between 0.61 and 1.20 molCO·molCo–1·h–1. Insights of the remarkable catalyst activity were examined by in situ X-ray photoelectron spectroscopy (XPS) studies corroborated by density functional theory (DFT) calculation. The bimetallic Co3Pt (111) surface was found to be highly active for the C–C coupling reaction between surface-adsorbed C and CO, forming a CCO intermediate with a very low activation barrier (Ea = 0.37 eV), in comparison to the C–C coupling activation barrier obtained over the Co (111) surface (Ea = 0.87 eV). This unique approach and observations create a new path for developing next-generation advanced catalyst systems and processes for selective low-temperature FTS.
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