化学
锡
光催化
红外线的
漫反射红外傅里叶变换
光化学
红外光谱学
密度泛函理论
傅里叶变换红外光谱
X射线吸收光谱法
金属
吸收光谱法
催化作用
无机化学
计算化学
化学工程
光学
有机化学
工程类
物理
作者
Bo Su,Yuehua Kong,Sibo Wang,Shouwei Zuo,Wei Lin,Yuanxing Fang,Yidong Hou,Guigang Zhang,Huabin Zhang,Xinchen Wang
摘要
Synchronized conversion of CO2 and H2O into hydrocarbons and oxygen via infrared-ignited photocatalysis remains a challenge. Herein, the hydroxyl-coordinated single-site Ru is anchored precisely on the metallic TiN surface by a NaBH4/NaOH reforming method to construct an infrared-responsive HO-Ru/TiN photocatalyst. Aberration-corrected high-angle annular dark-field scanning transmission electron microscopy (ac-HAADF-STEM) and X-ray absorption spectroscopy (XAS) confirm the atomic distribution of the Ru species. XAS and density functional theory (DFT) calculations unveil the formation of surface HO-RuN5–Ti Lewis pair sites, which achieves efficient CO2 polarization/activation via dual coordination with the C and O atoms of CO2 on HO-Ru/TiN. Also, implanting the Ru species on the TiN surface powerfully boosts the separation and transfer of photoinduced charges. Under infrared irradiation, the HO-Ru/TiN catalyst shows a superior CO2-to-CO transformation activity coupled with H2O oxidation to release O2, and the CO2 reduction rate can further be promoted by about 3-fold under simulated sunlight. With the key reaction intermediates determined by in situ diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) and predicted by DFT simulations, a possible photoredox mechanism of the CO2 reduction system is proposed.
科研通智能强力驱动
Strongly Powered by AbleSci AI