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Hot‐Electron Photodynamics in Silver‐Containing BEA‐Type Nanozeolite Studied by Femtosecond Transient Absorption Spectroscopy
ChemPhysChem ( IF 2.3 ) Pub Date : 2020-10-20 , DOI: 10.1002/cphc.202000822
Farah Kawtharani 1, 2 , Svetlana Mintova 2 , Richard Retoux 3 , Mehran Mostafavi 4 , Guy Buntinx 1 , Vincent De Waele 1
Affiliation  

Silver cations were introduced in nanosized BEA‐type zeolite containing organic template by ion‐exchange followed by chemical reduction towards preparation of photoactive materials (Ag0‐BEA). The stabilization of highly dispersed Ag0 nanoparticles with a size of 1–2 nm in the BEA zeolite was revealed. The transient optical response of the Ag‐BEA samples upon photoexcitation at 400 nm was studied by femtosecond absorption. The photodynamic of the hot electrons was found to depend on the sample preparation. The lifetime of the hot electrons in the Ag−BEA samples containing small Ag nanoparticles (1–2 nm) is significantly shortened in comparison to bear Ag nanoparticles with a size of 10 nm. While for the larger Ag nanoparticles, the energy absorbed in the conduction band is decaying by electron‐phonon coupling into the metal lattice, the high surface‐to‐volume ratio of the small Ag nanoparticles favors the dissipation of the energy of the hot electrons from the metal nanoparticles (Ag0) towards the zeolitic micro‐environment. This finding is encouraging for further applications of Ag‐containing zeolites in photocatalysis and plasmonic chemistry.

中文翻译:

飞秒瞬态吸收光谱研究含银BEA型纳米沸石中的热电子光动力学

通过阳离子交换将银阳离子引入包含有机模板的纳米尺寸的BEA型沸石中,然后进行化学还原以制备光敏材料(Ag 0 -BEA)。高分散性Ag 0的稳定化在BEA沸石中发现了尺寸为1-2 nm的纳米颗粒。通过飞秒吸收研究了Ag-BEA样品在400 nm光激发时的瞬态光学响应。发现热电子的光动力学取决于样品的制备。与载有10 nm大小的Ag纳米颗粒相比,包含小Ag纳米颗粒(1-2 nm)的Ag-BEA样品中热电子的寿命大大缩短。对于较大的Ag纳米颗粒,由于电子声子耦合到金属晶格中而在导带中吸收的能量正在衰减,而较小的Ag纳米颗粒的高表面体积比有利于热电子能量的消散。金属纳米颗粒(Ag 0)朝着沸石微环境发展。这一发现对于在光催化和等离子体化学中进一步应用含银沸石是令人鼓舞的。
更新日期:2020-12-17
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