Photoenhanced Electrocatalytic Hydrogen Evolution Accelerated Dominantly by the Hot Electrons from Intraband Transition rather than Interband Transition.
Photoenhanced Electrocatalytic Hydrogen Evolution Accelerated Dominantly by the Hot Electrons from Intraband Transition rather than Interband Transition.
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DOI：
10.1021/acs.jpclett.3c01051
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发表时间：
2023-06
期刊：
影响因子：
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通讯作者：
Chen Chi;Yifan Pan;M. Ni;Xin-Lei Ding;Jian Li;X. Xia
中科院分区：
文献类型：
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作者：
Chen Chi;Yifan Pan;M. Ni;Xin-Lei Ding;Jian Li;X. Xia
以太阳光为能量输入的等离子体材料催化析氢反应已成为人工光合作用的研究热点。在可见光激发下，既有带内跃迁又有带间跃迁的热载流子产生，究竟哪一种热载流子在催化反应中起主导作用还不清楚。本文研究了等离子体Au三角形纳米棱镜（AuTNP）上带内和带间跃迁的超热电子对光电催化HER的贡献。与暗反应相比，带内和带间激发下的交换电流密度分别增加了9倍和3倍，这归因于带内跃迁超热电子的高能级。通过计算有光照和无光照下的反应活化能，定量分析了两种光激发模式的超热电子对光增强电还原反应（PEER）的贡献，提出了衡量不同超热电子在不同反应中作用的通用标准。
Plasmonic materials enabling sunlight as an energy input to catalyze the hydrogen evolution reaction (HER) have become the research focus of artificial photosynthesis. Upon visible photoexcitation, there are both intraband transition and interband transition hot carriers generated, and which of them dominates the catalytic reaction remains elusive. Here, the contributions of hot electrons from intraband and interband transitions to the photoelectrocatalytic HER on plasmonic Au triangle nanoprisms (AuTNPs) have been studied. Compared with the dark reaction, the exchange current density increases by 9-fold and 3-fold under intraband and interband excitation, respectively, which is attributed to the higher energy level of intraband transition hot electrons. By calculation of the reaction activation energy with and without illumination, the contributions of the hot electrons from the two photoexcitation modes to the photoenhanced electroreduction reaction (PEER) are quantitatively analyzed, proposing the general standard to measure the effect of different hot electrons in different reactions.