W5+–W5+ Pair Induced LSPR of W18O49 to Sensitize ZnIn2S4 for Full-Spectrum Solar-Light-Driven Photocatalytic Hydrogen Evolution,Advanced Functional Materials

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W5+–W5+ Pair Induced LSPR of W18O49 to Sensitize ZnIn2S4 for Full-Spectrum Solar-Light-Driven Photocatalytic Hydrogen Evolution
Advanced Functional Materials ( IF 18.5 ) Pub Date : 2022-06-19 , DOI: 10.1002/adfm.202203638
Yue Lu ₁ , Xiaofang Jia ₁ , Zhaoyu Ma ₁ , Yang Li ₁ , Shuai Yue _{2,

3,

4} , Xinfeng Liu _{2,

3,

4} , Junying Zhang ₁

Affiliation

The localized surface plasmon resonances (LSPR) effect makes W₁₈O₄₉ an effective visible and near-infrared (NIR) light antenna to realize full-spectrum solar-light driven photocatalysis, yet the precise origin remains elusive. Here, the LSPR originates from the localized electron confinement around lattice W⁵⁺–W⁵⁺ pairs in the unique structure of W₁₈O₄₉ by density-functional theory calculation, which gives W₁₈O₄₉ a broad absorption ranging from visible to NIR region, independent of the particle shape and size is confirmed. This unique periodic LSPR simplifies the design of W₁₈O₄₉-sensitized photocatalytic composite into enhancing the light absorbance of W₁₈O₄₉ and screening photocatalytic semiconductors with suitable energy band potentials. To this end, hierarchical-structure W₁₈O₄₉ microflowers with high absorbance have been coated with ZnIn₂S₄ nanosheets to achieve cocatalyst-free photocatalytic composite, which presents an outstanding H₂ production rate of 902.57 µmol within 3 h under simulated solar-light. Comprehensive characterizations, including ultrafast transient absorption spectroscopy, prove the injection of hot electrons from W₁₈O₄₉ to ZnIn₂S₄ and the increase of long-lived active electrons. This work clarifies the LSPR origin of oxygen-deficient semiconductors and paves the way for the search of broad-spectrum active photocatalyst.

中文翻译：

W5+–W5+ 对诱导 W18O49 的 LSPR 敏化 ZnIn2S4 用于全光谱太阳光驱动的光催化制氢

局部表面等离子体共振（LSPR）效应使W ₁₈ O ₄₉成为一种有效的可见光和近红外（NIR）光天线，可实现全光谱太阳光驱动的光催化，但确切的起源仍然难以捉摸。在这里，通过密度泛函理论计算，LSPR源于W ₁₈ O _{49独特结构中晶格W}⁵⁺ -W ⁵⁺对周围的局域电子限制，这使W ₁₈ O ₄₉具有从可见光到近红外光的广泛吸收区域，与颗粒形状和大小无关。这种独特的周期性 LSPR 简化了 W ₁₈ O _49的设计_{-敏化光催化复合材料以提高W 18} O ₄₉的吸光度并筛选具有合适能带势的光催化半导体。为此，利用ZnIn ₂ S ₄纳米片包覆具有高吸光度的分级结构W ₁₈ O ₄₉微花，实现了无助催化剂的光催化复合材料，在模拟太阳光下3 h内H ₂产率高达902.57 µmol。光。综合表征，包括超快瞬态吸收光谱，证明热电子从 W ₁₈ O ₄₉注入到 ZnIn ₂ S₄和长寿命活性电子的增加。这项工作阐明了缺氧半导体的 LSPR 起源，为寻找广谱活性光催化剂铺平了道路。

更新日期：2022-06-19

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