全金属Ag@Au@M(M=Pd,Pt)等离子体光催化材料的制备及其催化机理的单颗粒光谱研究

表面等离子体光催化材料因其表面等离子体共振效应(SPR)，能有效吸收光能并产生“热电子”，是光催化领域研究热点之一。但热电子在金属到半导体的传输过程中寿命极短抑制了其有效利用，导致光能转换率较低。全金属等离子体光催化材料可同时作为吸光和催化反应中心，抑制能量耗散进而提高光能利用率。然而，该体系光吸收能力仍有待提高且机理不明确。进一步改善全金属等离子体光催化材料的光吸收和热电子利用率，并研究其物理化学过程，对表面等离子体光催化材料活性提高和发展推广具有非常重要的科学意义。本项目拟利用具有核壳结构的双金属等离子体纳米颗粒(Ag@Au)来增强光吸收，进而提高Ag@Au@M(M=Pd,Pt)全金属等离子体光催化材料的催化活性，结合单颗粒光谱技术，研究热电子产生和转移的具体物理化学过程，揭示SPR效应在光催化反应中的增强机制，最终实现光能-化学能的高效转换。

Plasmonic photocatalysts, which can effectively utilize light energy and generate "hot electrons" due to their surface plasmon resonance (SPR), is a research hotspot in the field of photocatalysis. However, the transfer of hot electrons from metal to semiconductor suppresses the efficient use of hot electrons due to their short lifetime, resulting in a low conversion rate of light energy. All-metal plasmonic photocatalysts, which can act as the absorption and catalytic reaction center simultaneously, inhibit the energy dissipation and thus improve the utilization of light energy. However, the light absorption capacity of the system still needs to be improved and the mechanism is not clear. Further enhancing the light absorption capacity and the hot electron utilization efficiency of all-metal plasmonic photocatalysts, and studying their physico-chemical processes are of great scientific significance for improving the activity of plasmonic photocatalysts and for their promotion. This project intends to utilize the bimetallic Ag@Au core-shell structure to enhance the light absorption and further improve the catalytic activity of the Ag@Au@M (M = Pd, Pt) plasmonic photocatalysts. Combined with single-particle-resolved spectroscopy, the physico-chemical processes of hot-electron generation and transfer are studied. The mechanism of plasmon-enhanced catalytic reaction is explored in detail, and finally efficient conversion of light energy-chemical energy can be achieved.