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

共 46 条

[21] High efficacy of substrate dimensionality control in optimizing the specific capacitance and phase stability of hybridized nanostructures [J].

Park, Yeon Hu ;

Patil, Sharad B. ;

Jin, Xiaoyan ;

Hwang, Seong-Ju .

NANO ENERGY, 2023, 113

[22] Engineering Single-Atom Active Sites on Covalent Organic Frameworks for Boosting CO2 Photoreduction [J].

Ran, Lei ;

Li, Zhuwei ;

Ran, Bei ;

Cao, Jiaqi ;

Zhao, Yue ;

Shao, Teng ;

Song, Yurou ;

Leung, Michael K. H. ;

Sun, Licheng ;

Hou, Jungang .

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2022, 144 (37) :17097-17109

[23] Tunable green syngas generation from CO2 and H2O with sunlight as the only energy input [J].

Rashid, Roksana Tonny ;

Chen, Yiqing ;

Liu, Xuedong ;

Chowdhury, Faqrul Alam ;

Liu, Mingxin ;

Song, Jun ;

Mi, Zetian ;

Zhou, Baowen .

PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA, 2022, 119 (26)

[24] Dissolving Vanadium into Titanium Nitride Lattice Framework for Rational Polysulfide Regulation in Li-S Batteries [J].

Shang, Chaoqun ;

Li, Gaoran ;

Wei, Benben ;

Wang, Jiayi ;

Gao, Rui ;

Tian, Yuan ;

Chen, Qing ;

Zhang, Yongguang ;

Shui, Lingling ;

Zhou, Guofu ;

Hu, Yongfeng ;

Chen, Zhongwei ;

Wang, Xin .

ADVANCED ENERGY MATERIALS, 2021, 11 (03)

[25] Molecular-level insight into photocatalytic CO2 reduction with H2O over Au nanoparticles by interband transitions [J].

Shangguan, Wenchao ;

Liu, Qing ;

Wang, Ying ;

Sun, Ning ;

Liu, Yu ;

Zhao, Rui ;

Li, Yingxuan ;

Wang, Chuanyi ;

Zhao, Jincai .

NATURE COMMUNICATIONS, 2022, 13 (01)

[26] Atomically Dispersed Indium-Copper Dual-Metal Active Sites Promoting C-C Coupling for CO2 Photoreduction to Ethanol [J].

Shi, Hainan ;

Wang, Haozhi ;

Zhou, Yichen ;

Li, Jiahui ;

Zhai, Panlong ;

Li, Xiangyang ;

Gurzadyan, Gagik G. ;

Hou, Jungang ;

Yang, Hong ;

Guo, Xinwen .

ANGEWANDTE CHEMIE-INTERNATIONAL EDITION, 2022, 61 (40)

[27] Highly Selective Photocatalytic CO2 Methanation with Water Vapor on Single-Atom Platinum-Decorated Defective Carbon Nitride [J].

Shi, Xianjin ;

Huang, Yu ;

Bo, Yanan ;

Duan, Delong ;

Wang, Zhenyu ;

Cao, Junji ;

Zhu, Gangqiang ;

Ho, Wingkei ;

Wang, Liqin ;

Huang, Tingting ;

Xiong, Yujie .

ANGEWANDTE CHEMIE-INTERNATIONAL EDITION, 2022, 61 (27)

[28] S-Scheme Co9S8@Cd0.8Zn0.2S-DETA Hierarchical Nanocages Bearing Organic CO2 Activators for Photocatalytic Syngas Production [J].

Su, Bo ;

Zheng, Mei ;

Lin, Wei ;

Lu, Xue Feng ;

Luan, Deyan ;

Wang, Sibo ;

Lou, Xiong Wen .

ADVANCED ENERGY MATERIALS, 2023, 13 (15)

[29] Photocatalysis of water into hydrogen peroxide over an atomic Ga-N5 site [J].

Tan, Hao ;

Zhou, Peng ;

Liu, Meixian ;

Zhang, Qinghua ;

Liu, Fuyang ;

Guo, Hongyu ;

Zhou, Yin ;

Chen, Yan ;

Zeng, Lingyou ;

Gu, Lin ;

Zheng, Zhanfeng ;

Tong, Meiping ;

Guo, Shaojun .

NATURE SYNTHESIS, 2023, 2 (06) :557-563

[30] P and Cu Dual Sites on Graphitic Carbon Nitride for Photocatalytic CO2 Reduction to Hydrocarbon Fuels with High C2H6 Evolution [J].

Wang, Gang ;

Chen, Zhe ;

Wang, Tao ;

Wang, Dingsheng ;

Mao, Junjie .

ANGEWANDTE CHEMIE-INTERNATIONAL EDITION, 2022, 61 (40)

← 1 2 3 4 5 →