Au@Cu2O Core-Shell 和 Au@Cu2Se Yolk-Shell 纳米晶体作为光电化学水分解和光催化制氢的有前途的光催化剂,ACS Applied Materials & Interfaces

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Au@Cu2O Core-Shell 和 Au@Cu2Se Yolk-Shell 纳米晶体作为光电化学水分解和光催化制氢的有前途的光催化剂
ACS Applied Materials & Interfaces ( IF 8.3 ) Pub Date : 2022-08-30 , DOI: 10.1021/acsami.2c07145
Ting-Hsuan Lai, Chun-Wen Tsao, Mei-Jing Fang, Jhen-Yang Wu, Yu-Peng Chang, Yi-Hsuan Chiu, Ping-Yen Hsieh, Ming-Yu Kuo, Kao-Der Chang, Yung-Jung Hsu

在这项工作中，我们展示了 Au@Cu ₂ O 核壳和 Au@Cu ₂ Se 蛋黄壳纳米晶体在光电化学 (PEC) 水分解和光催化氢 (H ₂ ) 生产中作为光催化剂的实际用途。_{通过在 Au@Cu 2} O 核壳纳米晶体模板上进行连续离子交换反应制备样品。Au@Cu ₂ O 和 Au@Cu ₂ Se 显示出增强的电荷分离，因为 Au 核和蛋黄可以吸引来自 Cu ₂ O 和 Cu ₂ Se 壳的光激发电子。另一方面，Au 的局域表面等离子共振 (LSPR) 可以促进 Cu _{2的额外电荷载流子的产生}O和Cu ₂ Se。进行了有限差分时域模拟，以探索由 Au 的 LSPR 引起的局部电磁场的放大。用时间分辨光致发光和紫外光电子能谱检查样品的电荷转移动力学和能带排列。由于改进的界面电荷转移，Au@Cu ₂ O 和 Au@Cu ₂ Se 表现出比相应的纯对应样品显着更大的水还原光电流和更高的 H _{2生产光催化活性。}进行入射光子到电流效率测量以评估 Au 的等离子体效应对增强的光活性的贡献。相对于 Au@Cu₂ O, Au@Cu ₂ Se凭借蛋黄壳结构的结构优势更适合 PEC 水分解和光催化 H _2生产。目前工作的演示可能会为复杂的金属-半导体蛋黄-壳纳米晶体的合理设计提供启示，特别是那些包含金属硒化物的纳米晶体，用于卓越的光催化应用。

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Au@Cu2O Core–Shell and Au@Cu2Se Yolk–Shell Nanocrystals as Promising Photocatalysts in Photoelectrochemical Water Splitting and Photocatalytic Hydrogen Production

In this work, we demonstrated the practical use of Au@Cu₂O core–shell and Au@Cu₂Se yolk–shell nanocrystals as photocatalysts in photoelectrochemical (PEC) water splitting and photocatalytic hydrogen (H₂) production. The samples were prepared by conducting a sequential ion-exchange reaction on a Au@Cu₂O core–shell nanocrystal template. Au@Cu₂O and Au@Cu₂Se displayed enhanced charge separation as the Au core and yolk can attract photoexcited electrons from the Cu₂O and Cu₂Se shells. The localized surface plasmon resonance (LSPR) of Au, on the other hand, can facilitate additional charge carrier generation for Cu₂O and Cu₂Se. Finite-difference time-domain simulations were carried out to explore the amplification of the localized electromagnetic field induced by the LSPR of Au. The charge transfer dynamics and band alignment of the samples were examined with time-resolved photoluminescence and ultraviolet photoelectron spectroscopy. As a result of the improved interfacial charge transfer, Au@Cu₂O and Au@Cu₂Se exhibited a substantially larger photocurrent of water reduction and higher photocatalytic activity of H₂ production than the corresponding pure counterpart samples. Incident photon-to-current efficiency measurements were conducted to evaluate the contribution of the plasmonic effect of Au to the enhanced photoactivity. Relative to Au@Cu₂O, Au@Cu₂Se was more suited for PEC water splitting and photocatalytic H₂ production by virtue of the structural advantages of yolk–shell architectures. The demonstrations from the present work may shed light on the rational design of sophisticated metal–semiconductor yolk–shell nanocrystals, especially those comprising metal selenides, for superior photocatalytic applications.

更新日期：2022-08-30

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