X射线光电子能谱
光化学
电子转移
漫反射红外傅里叶变换
光催化
光谱学
化学
太阳能燃料
纳米片
材料科学
吸收光谱法
纳米技术
催化作用
化学工程
光学
有机化学
物理
量子力学
工程类
作者
Wangzhong Tang,Heng Cao,Peiyu Ma,Tao Ding,Shaoyun Huang,Jiajun Wang,Qunxiang Li,Xiuli Xu,Jinlong Yang
出处
期刊:Nano Letters
[American Chemical Society]
日期:2024-04-18
标识
DOI:10.1021/acs.nanolett.4c01064
摘要
Exploring high-efficiency photocatalysts for selective CO2 reduction is still challenging because of the limited charge separation and surface reactions. In this study, a noble-metal-free metallic VSe2 nanosheet was incorporated on g-C3N4 to serve as an electron capture and transfer center, activating surface active sites for highly efficient and selective CO2 photoreduction. Quasi in situ X-ray photoelectron spectroscopy (XPS), soft X-ray absorption spectroscopy (sXAS), and femtosecond transient absorption spectroscopy (fs-TAS) unveiled that VSe2 could capture electrons, which are further transferred to the surface for activating active sites. In situ diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) and density functional theory (DFT) calculations revealed a kinetically feasible process for the formation of a key intermediate and confirmed the favorable production of CO on the VSe2/PCN (protonated C3N4) photocatalyst. As an outcome, the optimized VSe2/PCN composite achieved 97% selectivity for solar-light-driven CO2 conversion to CO with a high rate of 16.3 μmol·g-1·h-1, without any sacrificial reagent or photosensitizer. This work offers new insights into the photocatalyst design toward highly efficient and selective CO2 conversion.
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