Exploring coverage-dependent chain-growth mechanisms on Ru(111) for Fischer–Tropsch synthesis. Issue 2 (6th December 2022)

• Record Type: Journal Article
• Authors: Jiao, Yueyue; Ma, Huan; Ren, Pengju; Li, Teng; Li, Yong-Wang; Wen, Xiao-Dong; Jiao, Haijun
• Is Part Of: Catalysis science & technology. Volume 13:Issue 2(2023)
• Page Start: 437
• Page End: 456
• Publication Date: 2022-12-06
• Subjects: Catalysis -- Periodicals; 541.395
• DOI: 10.1039/d2cy01279k
• Languages: English
• ISSNs: 2044-4753

Abstract

Abstract : The chain growth mechanisms of Fischer–Tropsch synthesis (FTS) remain a controversial topic, especially considering the much stronger adsorption ability of CO over H2, resulting in CO pre-adsorption or saturation. Abstract : The chain growth mechanisms of Fischer–Tropsch synthesis (FTS) remain a controversial topic, especially considering the much stronger adsorption ability of CO over H2, resulting in CO pre-adsorption or saturation. Systematic periodic density functional theory computations (GGA-rPBE), and the analysis of ab initio atomistic thermodynamics and micro-kinetics on the Ru(111) surface revealed that the dense CO layer at a very early stage of FTS suppresses CO activation, promotes the coupling of CH x ( x = 0–3) and C1 as an insertion monomer (C1 = C, CH, CH2, CH3, CO, HCO and COH) under favorable conditions, especially for CH2 (or CH3 ) + CO coupling mechanisms. An HCO-insertion mechanism into RCH (R = H, CH3, …) [HCO + CH2 → CH2 CHO → CH2 CO → CH3 CO → CH3 C + O → CH3 CH (+ HCO) → …] was proposed at the lowest coverage, while a CO insertion mechanism into RCH (R = H, CH3, …) [CO + CH2 → CH2 CO (CH3 + CO) → CH2 C + O (CH3 CO) → CH3 C + O → CH3 CH (+ CO) → …] was proposed at CO pre-saturation coverage (423 K, 10 atm) on the Ru(111) surface.