光催化
等离子体子
表面等离子共振
材料科学
载流子
光化学
异质结
光电子学
催化作用
化学
纳米技术
纳米颗粒
生物化学
作者
Jingjing Yang,Lei Li,Chong Xiao,Yi Xie
标识
DOI:10.1002/anie.202311911
摘要
Photocatalysis, particularly plasmon-mediated photocatalysis, offers a green and sustainable approach for direct nitrogen oxidation into nitrate under ambient conditions. However, the unsatisfactory photocatalytic efficiency caused by the limited localized electromagnetic field enhancement and short hot carrier lifetime of traditional plasmonic catalysts is a stumbling block to the large-scale application of plasmon photocatalytic technology. Herein, we design and demonstrate the dual-plasmonic heterojunction (Bi/Csx WO3 ) achieves efficient and selective photocatalytic N2 oxidation. The yield of NO3- over Bi/Csx WO3 (694.32 μg g-1 h-1 ) are 2.4 times that over Csx WO3 (292.12 μg g-1 h-1 ) under full-spectrum irradiation. The surface dual-plasmon resonance coupling effect generates a surge of localized electromagnetic field intensity to boost the formation efficiency and delay the self-thermalization of energetic hot carriers. Ultimately, electrons participate in the formation of ⋅O2- , while holes involve in the generation of ⋅OH and the activation of N2 . The synergistic effect of multiple reactive oxygen species drives the direct photosynthesis of NO3- , which achieves the overall-utilization of photoexcited electrons and holes in photocatalytic reaction. The concept that the dual-plasmon resonance coupling effect facilitates the directional overall-utilization of photoexcited carriers will pave a new way for the rational design of efficient photocatalytic systems.
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