In:
Catalysis Science & Technology, Royal Society of Chemistry (RSC), Vol. 13, No. 2 ( 2023), p. 437-456
Abstract:
The chain growth mechanisms of Fischer–Tropsch synthesis (FTS) remain a controversial topic, especially considering the much stronger adsorption ability of CO over H 2 , 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, CH 2 , CH 3 , CO, HCO and COH) under favorable conditions, especially for CH 2 (or CH 3 ) + CO coupling mechanisms. An HCO-insertion mechanism into RCH (R = H, CH 3 , …) [HCO + CH 2 → CH 2 CHO → CH 2 CO → CH 3 CO → CH 3 C + O → CH 3 CH (+ HCO) → …] was proposed at the lowest coverage, while a CO insertion mechanism into RCH (R = H, CH 3 , …) [CO + CH 2 → CH 2 CO (CH 3 + CO) → CH 2 C + O (CH 3 CO) → CH 3 C + O → CH 3 CH (+ CO) → …] was proposed at CO pre-saturation coverage (423 K, 10 atm) on the Ru(111) surface.
Type of Medium:
Online Resource
ISSN:
2044-4753
,
2044-4761
Language:
English
Publisher:
Royal Society of Chemistry (RSC)
Publication Date:
2023
detail.hit.zdb_id:
2595090-3
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