Capped Vapor–Liquid–Solid Growth of Vanadium-Substituted Molybdenum Disulfide Ultrathin Films for Enhanced Photocatalytic Activity
Journal
ACS Nano
Series/Report No.
ACS Nano
Journal Volume
20
Journal Issue
2
Start Page
2211
End Page
2224
ISSN
1936-0851
1936-086X
Date Issued
2026-01-07
Author(s)
Huang, Pin-Pin
Qorbani, Mohammad
Hung, Ying-Ti
Lai, Ying-Ren
Sabbah, Amr
Tseng, Mao-Feng
Huang, Chih-Yang
Koodathil, Sumangaladevi
Kholimatussadiah, Septia
Hussien, Mahmoud Kamal
Feng, Tzu-Hsuan
Liu, Yo-Hsun
Wang, Hsin
Lin, Jia-Wei
Wang, Chen-Hao
Hayashi, Michitoshi
Chen, Kuei-Hsien
Chen, Li-Chyong
Abstract
The exceptional and tunable physicochemical properties of 2D transition metal dichalcogenides (TMDCs) have made them model catalysts for fundamental studies and applications. Activating the inert basal plane holds the key to utilizing wafer-scale TMDCs in artificial photosynthesis. To address this challenge, we report a SiO2-capped vapor–liquid–solid (VLS) growth method that assists in substituting vanadium into the molybdenum disulfide ultrathin film and introducing sulfur vacancies to form Svac-Mo1–xVxS2. By optimizing the thickness of solid precursors and the SiO2-capping layer (membrane layer), as well as the growth temperature, we demonstrate control over the film thickness, vanadium concentration, and film uniformity. Our results reveal the presence of the V–Svac pairs, manifesting in the enhanced Svac concentration and charge density transfer among V–S–Mo atoms, with multifaceted benefits, including increasing light absorption, photoluminescence quenching, crystal structure distortion, efficient binding of CO2 or H2O on the surface, improved charge transfer/transport, and a suitable energy band diagram. Furthermore, the 2D Svac-Mo1–xVxS2 model catalyst films, with abundant V–Svac pair active sites, exhibit a stable and boosted photocatalytic CO2 reduction to CO, specifically yielding ∼5 times more than that of pristine MoS2. Our study demonstrates the origin of V–Svac pairs in host MoS2, leading to basal plane activation. This suggests a foundation for future research on pairing dopants or alloying elements with defects for efficient photocatalyst design.
Subjects
2D materials
CO2reduction
photocatalysis
scanning electrochemical microscopy
semicondcutor
dopant−vacancy pairing
VLS growth method
Publisher
American Chemical Society (ACS)
Type
journal article