Enhancing Catalytic Activity and Selectivity by Plasmon-Induced Hot Carriers

iScience

Yu-Hang Li¹  Ping-Ping Fang¹  Fei-Fei Meng¹  Ye-Xiang Tong¹  Zhong-Qun Tian²  Feng Peng²  Xi-Hong Lu³  Jian-Feng Li³  Xing Chen³  Xiao-Qing Liu³  Hao Yang⁴ 

[1] Energy Conservation of Guangdong Province, School of Chemistry, Sun Yat-Sen University, Guangzhou 510275, China;Guangzhou Key Laboratory for New Energy and Green Catalysis, School of Chemistry and Chemical Engineering, Guangzhou University, Guangzhou 510006, China;;MOE Key Laboratory of Bioinorganic and Synthetic Chemistry, The Key Lab of Low-carbon Chem &State Key Laboratory of Physical Chemistry of Solid Surfaces, College of Chemistry and Chemical Engineering, Collaborative Innovation Center of Chemistry for Energy Materials (iChEM), Xiamen University, Xiamen 361005, China;

关键词: Inorganic Chemistry;    Catalysis;    Materials Science;   

DOI  :  

来源: DOAJ

【 摘 要 】

Summary: Plasmon-assisted chemical transformation holds great potential for solar energy conversion. However, simultaneous enhancement of reactivity and selectivity is still challenging and the mechanism remains mysterious. Herein, we elucidate the localized surface plasmon resonance (LSPR)-induced principles underlying the enhanced activity (∼70%) and selectivity of photoelectrocatalytic redox of nitrobenzene (NB) on Au nanoparticles. Hot carriers selectively accelerate the conversion rate from NB to phenylhydroxylamine (PHA) by ∼14% but suppress the transformation rate from PHA to nitrosobenzene (NSB) by ∼13%. By adding an electron accepter, the as-observed suppression ratio is substantially enlarged up to 43%. Our experiments, supported by in situ surface-enhanced Raman spectroscopy and density functional theory simulations, reveal such particular hot-carrier-induced selectivity is conjointly contributed by the accelerated hot electron transfer and the corresponding residual hot holes. This work will help expand the applications of renewable sunlight in the directional production of value-added chemicals under mild conditions.

【 授权许可】

Unknown