Hydroxyl-Bonded Ru on Metallic TiN Surface Catalyzing CO2 Reduction with H2O by Infrared Light

被引：229

作者：

Su, Bo ^{[1
]}

Kong, Yuehua ^{[1
]}

Wang, Sibo ^{[1
]}

Zuo, Shouwei ^{[2
]}

Lin, Wei ^{[1
]}

Fang, Yuanxing ^{[1
]}

Hou, Yidong ^{[1
]}

Zhang, Guigang ^{[1
]}

Zhang, Huabin ^{[2
]}

Wang, Xinchen ^{[1
]}

机构：

[1] Fuzhou Univ, Coll Chem, State Key Lab Photocatalysis Energy & Environm, Fuzhou 350116, Peoples R China

[2] King Abdullah Univ Sci & Technol, KAUST Catalysis Ctr, Phys Sci & Engn Div, Thuwal 23955, Saudi Arabia

来源：

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY | 2023年 / 145卷 / 50期

基金：

中国国家自然科学基金; 国家重点研发计划;

关键词：

HYDROGENATION; WATER;

D O I：

10.1021/jacs.3c08311

中图分类号：

O6 [化学];

学科分类号：

0703 ;

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 O-2, 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.

引用

页码：27415 / 27423

页数：9

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