材料科学
密度泛函理论
离域电子
等离子体子
光催化
异质结
原子轨道
激发
化学物理
分子轨道
纳米颗粒
光化学
光电子学
分子
纳米技术
催化作用
计算化学
电子
化学
工程类
物理
电气工程
量子力学
有机化学
生物化学
作者
Tong Mou,Jhon Quiroz,Pedro H. C. Camargo,Bin Wang
标识
DOI:10.1021/acsami.1c21607
摘要
Localized surface plasmons generated on metallic nanostructures can be used to accelerate molecular transformations; however, the efficiency is limited by the challenge to control the energy/charge transfer at the interfaces. Here, we combine density functional theory (DFT) calculations and experiments to reveal the mechanism of nitrophenol reduction on Au nanoparticles under visible-light irradiation and propose a strategy to further enhance the reaction rates. DFT calculations show a reduced activation barrier under electronic excitation on Au(111), thus explaining the measured higher rates under visible-light irradiation. Furthermore, we propose a heterostructure with Au nanoparticles covered by a thin film of hexagonal boron nitride; the latter is used to decouple the molecular orbitals from the metal to enable charge localization in the molecule. DFT calculations show that by this electronic decoupling, the activation barrier can be lowered by a factor of five. This work thus provides a valuable strategy for optimizing catalytic efficiency in plasmonic photocatalysis.
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