Hot Carrier-Driven Catalytic Reactions on Pt-CdSe-Pt Nanodumbbells and Pt/GaN under Light Irradiation
Hot Carrier-Driven Catalytic Reactions on Pt-CdSe-Pt Nanodumbbells and Pt/GaN under Light Irradiation
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DOI：
10.1021/nl400367m
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发表时间：
2013-03-01
期刊：
影响因子：
10.8
通讯作者：
Park, Jeong Young
中科院分区：
文献类型：
--
作者：
Kim, Sun Mi;Lee, Seon Joo;Park, Jeong Young
由金属纳米颗粒-半导体结组成的混合纳米催化剂为研究金属氧化物界面和热电子流在多相催化中的作用提供了一个有趣的平台。在这里，我们报告说，热载流子产生的光子吸收显着影响CO氧化的催化活性。我们发现，Pt-CdSe-Pt nanodumbells表现出更高的周转频率的2倍，在照射过程中的能量高于CdSe的带隙，而在裸Pt纳米粒子的周转率不依赖于光照射。我们发现，光照射下沉积在GaN衬底上的Pt纳米颗粒表现出的CO氧化的催化活性的变化，这取决于GaN的掺杂类型。我们假设半导体纳米棒或基底吸收光子后产生热电子，然后热电子注入Pt纳米颗粒，导致催化活性的变化。结果表明，在光照射过程中产生的热载流子流显着影响CO氧化的催化活性，导致潜在的应用作为一个热电子为基础的催化执行器。
Hybrid nanocatalysts consisting of metal nanoparticle-semiconductor junctions offer an interesting platform to study the role of metal oxide interfaces and hot electron flows in heterogeneous catalysis. Here, we report that hot carriers generated upon photon absorption significantly impact the catalytic activity of CO oxidation. We found that Pt-CdSe-Pt nanodumbbells exhibit a higher turnover frequency by a factor of 2 during irradiation by light with energy higher than the bandgap of CdSe, while the turnover rate on bare Pt nanoparticles did not depend on light irradiation. We found that Pt nanoparticles deposited on a GaN substrate under light irradiation exhibit changes in catalytic activity of CO oxidation that depends on the type of doping of the GaN. We suppose that hot electrons are generated upon the absorption of photons by the semiconducting nanorods or substrates, whereafter the hot electrons are injected into the Pt nanoparticles, resulting in the change in catalytic activity. The results imply that hot carrier flows generated during light irradiation significantly influence the catalytic activity of CO oxidation, leading to potential applications as a hot electron-based catalytic actuator.