A density functional theory study on how γ-Al2O3 - Boehmite transformation affects carbon evolution during aqueous-phase reaction

Tinnakorn Saelee; Phakaorn Apichoksiri; Meena Rittiruam; Chanthip Wangphon; Patcharaporn Khajondetchairit; Supareak Praserthdam; Piyasan Praserthdam

doi:10.1016/j.chemosphere.2023.139842

A density functional theory study on how γ-Al₂O₃ - Boehmite transformation affects carbon evolution during aqueous-phase reaction

Chemosphere. 2023 Nov:340:139842. doi: 10.1016/j.chemosphere.2023.139842. Epub 2023 Aug 17.

Authors

Tinnakorn Saelee¹, Phakaorn Apichoksiri¹, Meena Rittiruam², Chanthip Wangphon¹, Patcharaporn Khajondetchairit³, Supareak Praserthdam⁴, Piyasan Praserthdam⁵

Affiliations

¹ High-Performance Computing Unit (CECC-HCU), Center of Excellence on Catalysis and Catalytic Reaction Engineering (CECC), Chulalongkorn University, Bangkok, 10330, Thailand; Center of Excellence on Catalysis and Catalytic Reaction Engineering (CECC), Chulalongkorn University, Bangkok, 10330, Thailand; Saelee Group, Chulalongkorn University, Bangkok, 10330, Thailand.
² High-Performance Computing Unit (CECC-HCU), Center of Excellence on Catalysis and Catalytic Reaction Engineering (CECC), Chulalongkorn University, Bangkok, 10330, Thailand; Center of Excellence on Catalysis and Catalytic Reaction Engineering (CECC), Chulalongkorn University, Bangkok, 10330, Thailand; Rittiruam Group, Chulalongkorn University, Bangkok, 10330, Thailand.
³ High-Performance Computing Unit (CECC-HCU), Center of Excellence on Catalysis and Catalytic Reaction Engineering (CECC), Chulalongkorn University, Bangkok, 10330, Thailand; Center of Excellence on Catalysis and Catalytic Reaction Engineering (CECC), Chulalongkorn University, Bangkok, 10330, Thailand; Khajondetchairit Group, Chulalongkorn University, Bangkok, 10330, Thailand.
⁴ High-Performance Computing Unit (CECC-HCU), Center of Excellence on Catalysis and Catalytic Reaction Engineering (CECC), Chulalongkorn University, Bangkok, 10330, Thailand; Center of Excellence on Catalysis and Catalytic Reaction Engineering (CECC), Chulalongkorn University, Bangkok, 10330, Thailand. Electronic address: supareak.p@chula.ac.th.
⁵ Center of Excellence on Catalysis and Catalytic Reaction Engineering (CECC), Chulalongkorn University, Bangkok, 10330, Thailand.

PMID: 37597627
DOI: 10.1016/j.chemosphere.2023.139842

Abstract

Gamma-alumina (γ-Al₂O₃), one of the most common materials, is commercially used in many catalytic applications, including the active catalyst and support. However, the problem of fast deactivation makes the utilization of the γ-Al₂O₃ challenging. This work elucidates the mechanism of coke formation consisting of coke deposition and evolution on γ-Al₂O₃(110) surfaces in differential conditions, including; clean and hydroxylation γ-Al₂O₃(110) in terms of partial and fully hydroxylation of OH/γ-Al₂O₃(110) and AlOOH(010), respectively. We demonstrated that the γ-Al₂O₃(110) surface is proper for atomic coke deposition and dimerization in the initial state, where the presence of OH species promotes the coke evolution to higher coke, C_n (where n ≥ 3). Also, the higher coke formation thermodynamically preferred the cyclic form to the aliphatic one. The electron transfer from substrates to adsorbed coke illustrates the role of the electron donor of catalyst surfaces corresponding to the electron acceptor of adsorbed cokes.

Keywords: Coking; Cyclic coke; Density functional theory; Phase transformation; γ-Al(2)O(3).

MeSH terms

Aluminum Oxide
Carbon
Coke*
Density Functional Theory

Substances

Aluminum Oxide
aluminum oxide hydroxide
Carbon
Coke