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揭示化学诱导热电子传输的损耗机制。

Revealing the Loss Mechanism of Chemically-Induced Hot Electron Transport.

作者信息

Roh Yujin, Jin Yeonghoon, Jeon Beomjoon, Park Yujin, Yu Kyoungsik, Park Jeong Young

机构信息

Department of Chemistry, Korea Advanced Institute of Science and Technology (KAIST), Daejeon 34141, Republic of Korea.

School of Electrical Engineering, Korea Advanced Institute of Science and Technology (KAIST), Daejeon 34141, Republic of Korea.

出版信息

Nano Lett. 2024 Mar 20;24(11):3490-3497. doi: 10.1021/acs.nanolett.4c00330. Epub 2024 Mar 11.

DOI:10.1021/acs.nanolett.4c00330
PMID:38466136
Abstract

Hot electrons are crucial for unraveling the intrinsic relationship between chemical reactions and charge transfer in heterogeneous catalysis. Significant research focused on real-time detection of reaction-driven hot electron flow (chemicurrent) to elucidate the energy conversion mechanisms, but it remains elusive because carrier generation contributes to only part of the entire process. Here, a theoretical model for quantifying the chemicurrent yield is presented by clarifying the contributions of hot carrier losses from the internal emission and multiple reflections. The experimental chemicurrent yield verifies our model with a reliable mean free path of hot electrons, emphasizing the importance of comprehensive consideration of the transport process besides hot electron generation. Moreover, Pt nanoparticles (NPs)-decorated Au/TiO is examined, showing the role of NPs-induced carrier losses in the performance of catalytic nanodiodes. These findings are expected to contribute to understanding the hot electron detection efficiency and designing nanodiodes with enhanced hot carrier flow and catalytic activity.

摘要

热电子对于揭示多相催化中化学反应与电荷转移之间的内在关系至关重要。大量研究聚焦于反应驱动的热电子流(化学电流)的实时检测,以阐明能量转换机制,但这仍然难以实现,因为载流子的产生仅占整个过程的一部分。在此,通过阐明内部发射和多次反射导致的热载流子损失的贡献,提出了一种用于量化化学电流产率的理论模型。实验测得的化学电流产率通过可靠的热电子平均自由程验证了我们的模型,强调了除热电子产生外全面考虑传输过程的重要性。此外,对Pt纳米颗粒(NPs)修饰的Au/TiO进行了研究,展示了NPs诱导的载流子损失在催化纳米二极管性能中的作用。这些发现有望有助于理解热电子检测效率,并设计出具有增强热载流子流和催化活性的纳米二极管。

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