Institute of Nanophotonics, Jinan University, Guangzhou, 511443, China.
Institute of Photonics Technology, Jinan University, Guangzhou, 511443, China.
Nat Commun. 2022 Nov 15;13(1):6984. doi: 10.1038/s41467-022-34738-z.
Plasmonic hot carriers have the advantage of focusing, amplifying, and manipulating optical signals via electron oscillations which offers a feasible pathway to influence catalytic reactions. However, the contribution of nonmetallic hot carriers and thermal effects on the overall reactions are still unclear, and developing methods to enhance the efficiency of the catalysis is critical. Herein, we proposed a new strategy for flexibly modulating the hot electrons using a nonmetallic plasmonic heterostructure (named WO-nanowires/reduced-graphene-oxides) for isopropanol dehydration where the reaction rate was 180-fold greater than the corresponding thermocatalytic pathway. The key detail to this strategy lies in the synergetic utilization of ultraviolet light and visible-near-infrared light to enhance the hot electron generation and promote electron transfer for C-O bond cleavage during isopropanol dehydration reaction. This, in turn, results in a reduced reaction activation barrier down to 0.37 eV (compared to 1.0 eV of thermocatalysis) and a significantly improved conversion efficiency of 100% propylene from isopropanol. This work provides an additional strategy to modulate hot carrier of plasmonic semiconductors and helps guide the design of better catalytic materials and chemistries.
等离子体激元热载流子通过电子振荡具有聚焦、放大和操纵光学信号的优势，这为影响催化反应提供了一种可行的途径。然而，非金属热载流子和热效应对整体反应的贡献仍不清楚，开发提高催化效率的方法至关重要。在此，我们提出了一种新策略，通过使用非贵金属等离子体异质结构（命名为 WO 纳米线/还原氧化石墨烯）来灵活地调节热电子，用于异丙醇脱水反应，其反应速率比相应的热催化途径高 180 倍。该策略的关键细节在于协同利用紫外光和可见近红外光来增强热电子的产生，并促进异丙醇脱水反应中 C-O 键断裂的电子转移。这反过来又将反应活化能垒降低至 0.37eV（相比之下，热催化为 1.0eV），并显著提高了异丙醇到丙烯的转化率达到 100%。这项工作提供了一种调节等离子体半导体热载流子的额外策略，有助于指导更好的催化材料和化学的设计。
