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🤝 共同合作論文

Capped Vapor−Liquid−Solid Growth of Vanadium-Substituted MoS₂ Ultrathin Films for Enhanced Photocatalytic Activity

以封蓋式氣-液-固成長法製備釩摻雜二硫化鉬超薄膜以提升光觸媒活性——應用於二氧化碳光觸媒還原

ACS Nano, 20 (2026) 2211–2224 (ACS Publications) | DOI: 10.1021/acsnano.5c17367
作者:Pin-Pin Huang, Mohammad Qorbani, Ying-Ti Hung, Ying-Ren Lai, Amr Sabbah, Mao-Feng Tseng, Chih-Yang Huang, Sumangaladevi Koodathil, Septia Kholimatussadiah, Mahmoud Kamal Hussien, Tzu-Hsuan Feng, Yo-Hsun Liu, Hsin Wang, Jia-Wei Lin, Chen-Hao Wang, Chih-I Wu, Michitoshi Hayashi, Kuei-Hsien Chen, and Li-Chyong Chen*

📄 英文摘要

This work reports a SiO₂-capped vapor−liquid−solid (VLS) growth method that assists in substituting vanadium into 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 as well as the growth temperature, we demonstrate control over film thickness, vanadium concentration, and film uniformity. The presence of V−Svac pairs manifests in 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. The 2D Svac-Mo₁₋ₓVₓS₂ model catalyst films exhibit stable and boosted photocatalytic CO₂ reduction to CO, specifically yielding approximately 5 times more than that of pristine MoS₂.

📄 中文摘要

本研究報告一種 SiO₂ 封蓋式氣-液-固(VLS)成長法,可將釩摻入二硫化鉬(MoS₂)超薄膜中並同時引入硫空位,形成 Svac-Mo₁₋ₓVₓS₂。透過優化固態前驅體厚度、SiO₂ 封蓋層厚度及成長溫度,成功控制了薄膜厚度、釩濃度與膜的均勻性。此 V−Svac 配對的存在帶來了多重效益:增強的硫空位濃度、V−S−Mo 原子間的電荷密度轉移、提升光吸收、螢光猝滅、晶格結構畸變、表面與 CO₂/H₂O 的高效鍵結、改進的電荷轉移/傳輸,以及合適的能帶圖。最終 2D Svac-Mo₁₋ₓVₓS₂ 模型觸媒薄膜展現了穩定且提升的光觸媒 CO₂ 還原為 CO 的活性,產率約為原始 MoS₂ 的 5 倍。

🔬 五項核心重要發現

1
SiO₂ 封蓋式 VLS 法:首創可同時達成 V 摻雜與 S 空位引入的成長方法,突破 MoS₂ 基面惰性限制。
2
∼5 倍 CO 產率提升:相較於原始 MoS₂,光觸媒 CO₂ 還原為 CO 的產率提升約五倍。
3
V−Svac 配對活性位點:V 摻雜與 S 空位形成協同配對,显著提升基面活化與電荷轉移動力學。
4
全方位光電性能提升:光吸收增強、螢光猝滅、晶格畸變、改善的電荷轉移/傳輸與合適的能帶排列。
5
缺陷-摻雜配對策略:為未來透過缺陷-摻雜配對設計高效光觸媒提供了通用方法論基礎。

📊 關鍵圖表

圖表 1:V-Svac/MoS₂ 異質結構之 TEM 影像與元素分佈圖,顯示 V、S、Mo 元素在複合觸媒中的分佈情形。
圖表 2:V-Svac/MoS₂ 複合觸媒之 CO₂ 還原性能:Faradaic efficiency 與 current density,與純 MoS₂ 及 V-Svac 基準樣品比較。