Photoactivity of amorphous and crystalline TiO2 nanotube arrays (TNA) films in gas phase CO2 reduction to methane with simultaneous H2 production

Janaina S Santos; Mohammad Fereidooni; Victor Márquez; Christian V Paz-López; Martin S Villanueva; Josephus G Buijnsters; Supareak Praserthdam; Piyasan Praserthdam

doi:10.1016/j.envres.2023.117919

Photoactivity of amorphous and crystalline TiO₂ nanotube arrays (TNA) films in gas phase CO₂ reduction to methane with simultaneous H₂ production

Environ Res. 2024 Mar 1:244:117919. doi: 10.1016/j.envres.2023.117919. Epub 2023 Dec 15.

Authors

Janaina S Santos¹, Mohammad Fereidooni¹, Victor Márquez¹, Christian V Paz-López¹, Martin S Villanueva², Josephus G Buijnsters³, Supareak Praserthdam⁴, Piyasan Praserthdam⁵

Affiliations

¹ Center of Excellence on Catalysis and Catalytic Reaction Engineering (CECC), Department of Chemical Engineering, Faculty of Engineering, Chulalongkorn University, Bangkok, 10330, Thailand.
² Facultad de Ingeniería, Benemerita Universidad Autonoma de Puebla, Apartado Postal J-39, CP, 72570, Puebla, Mexico.
³ Department of Precision and Microsystems Engineering, Research Group of Micro and Nano Engineering, Delft University of Technology, Mekelweg 2, 2628 CD, Delft, the Netherlands.
⁴ High-Performance Computing Unit, Center of Excellence on Catalysis and Catalytic Reaction Engineering (CECC-HCU), Department of Chemical Engineering, Faculty of Engineering, Chulalongkorn University, Bangkok, 10330, Thailand.
⁵ Center of Excellence on Catalysis and Catalytic Reaction Engineering (CECC), Department of Chemical Engineering, Faculty of Engineering, Chulalongkorn University, Bangkok, 10330, Thailand. Electronic address: piyasan.p@chula.ac.th.

PMID: 38103777
DOI: 10.1016/j.envres.2023.117919

Abstract

This study assessed the photoactivity of amorphous and crystalline TiO₂ nanotube arrays (TNA) films in gas phase CO₂ reduction. The TNA photocatalysts were fabricated by titanium anodization and submitted to an annealing treatment for crystallization and/or cathodic reduction to introduce Ti³⁺ and oxygen vacancies into the TiO₂ structure. The cathodic reduction demonstrated a significant effect on the generated photocurrent. The photoactivity of the four TNA catalysts in CO₂ reduction with water vapor was evaluated under UV irradiation for 3 h, where CH₄ and H₂ were detected as products. The annealed sample exhibited the best performance towards methane with a production rate of 78 μmol g_cat^-1 h^-1, followed by the amorphous film, which also exhibited an impressive formation rate of 64 μmol g_cat^-1 h^-1. The amorphous and reduced-amorphous films exhibited outstanding photoactivity regarding H₂ production (142 and 144 μmol g_cat^-1 h^-1, respectively). The annealed catalyst also revealed a good performance for H₂ production (132 μmol g_cat^-1 h^-1) and high stability up to five reaction cycles. Molecular dynamic simulations demonstrated the changes in the band structure by introducing oxygen vacancies. The topics covered in this study contribute to the Sustainable Development Goals (SDG), involving affordable and clean energy (SDG#7) and industry, innovation, and infrastructure (SDG#9).

Keywords: Amorphous titania; Anatase; CO(2) photoreduction; Hydrogen generation; Methane; TiO(2) nanotubes.

MeSH terms

Carbon Dioxide*
Methane
Nanotubes* / chemistry
Oxygen

Substances

Carbon Dioxide
Methane
Oxygen