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Tuning excited-state electronic structure in tungsten oxide for enhanced nitrogen photooxidation as fertilizer

文献类型： 外文期刊

作者： Li, Shaoquan 1 ; Liu, Jinjia 3 ; Su, Wenli 4 ; Wang, Yi 1 ; Li, Jinhao 1 ; Ning, Chenjun 1 ; Ren, Jing 1 ; Wen, Xiaodong 3 ; Zhang, Wenkai 4 ; Tong, Yuxin 5 ; Wang, Chong 5 ; Zheng, Lirong 7 ; Zhang, Wei 8 ; O'Hare, Dermot 9 ; Zhao, Yufei 1 ; Duan, Xue 1 ;

作者机构： 1.Beijing Univ Chem Technol, State Key Lab Chem Resource Engn, Beijing 100029, Peoples R China

2.Quzhou Inst Innovat Resource Chem Engn, Quzhou, Zhejiang, Peoples R China

3.Inst Coal Chem, Chinese Acad Sci, State Key Lab Coal Convers, Taiyuan 030001, Peoples R China

4.Beijing Normal Univ, Ctr Adv Quantum Studies, Dept Phys & Appl Opt, Beijing Area Major Lab, Beijing 100875, Peoples R China

5.Inst Environm & Sustainable Dev Agr, Chinese Acad Agr Sci, Beijing 100081, Peoples R China

6.Synfuels China Co Ltd, Natl Energy Ctr Coal Clean Fuels, Beijing 101400, Peoples R China

7.Inst High Energy Phys, Chinese Acad Sci, Beijing Synchrotron Radiat Facil, Beijing 100049, Peoples R China

8.Chongqing Inst Green & Intelligent Technol, Chinese Acad Sci, Chongqing 400714, Peoples R China

9.Univ Oxford, Dept Chem, Chem Res Lab, Mansfield Rd, Oxford OX1 3TA, England

关键词： Photocatalytic nitrogen fixation; Electronic structure regulation; Tungsten oxide; Solar N-fertilizer

期刊名称：APPLIED CATALYSIS B-ENVIRONMENT AND ENERGY （ 影响因子：22.1； 五年影响因子：19.7 ）

ISSN： 0926-3373

年卷期： 2024 年 343 卷

页码：

收录情况： SCI

摘要： Nitrate (NO3-) is an important raw ingredient for fertilizer, but its conventional synthesis is restricted by high energy consumption and CO2 emissions. Though there have been some studies on photocatalytic nitrogen oxidation, the production rate of nitrate is undesirable and the excited-state charge-transfer pathway still re-mains unclear. Herein, we fabricated the V-doped W18O49 nanowires (V-W18O49) for direct nitrate synthesis from N2 photooxidation. The NO3- production rate is as high as 39.85 mu mol g-1 h-1 with exceptional catalytic stability and the photosynthetic nitrate fertilizer was employed to promote the growth of crops. Time-resolved spectroscopic results confirmed that the introduction of V doping in V-W18O49 has created new high-efficiency electron-transfer (ET) pathways from the W-O site to the V-dopant under photoirradiation, which leads to an improved pi-backdonation process that facilitates nitrogen activation. This newly formed ET channel facilitated efficient charge separation and ultrafast photogenerated carriers transfer, thus overcame the sluggish ET kinetics.

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