期刊
CHEMICAL ENGINEERING JOURNAL
卷 443, 期 -, 页码 -出版社
ELSEVIER SCIENCE SA
DOI: 10.1016/j.cej.2022.136425
关键词
Nitrogen photofixation; Defect photocatalyst; Heterojunction; Visible light; Nitrogen activation
资金
- National Key R&D Program of China [SQ2019YFE011329]
- National Natural Science Foundation of China [21972040, 21673073]
- Innovation Program of Shanghai Municipal Education Commission [2021-01-07-00-02-E00106]
- Science and Technology Commission of Shanghai Municipality [20DZ2250400]
- Shanghai Sailing Program [22YF1410200]
- Shanghai Municipal Science and Technology Major Project [2018SHZDZX03]
- Program of Introducing Talents of Disci-pline to Universities [B20031, B16017]
Efficient visible-light-driven carbon nitride/oxygen vacancy titanium dioxide (CN-OvTiO(2)) heterojunction photocatalyst can significantly increase the ammonia production rate, making it a promising solution for green and cost-effective nitrogen fixation.
Photocatalytic nitrogen fixation is a promising and green approach for converting atmospheric nitrogen to ammonia, which has been considered as a potential way to the energy-intensive Haber-Bosch process. However, the activation of nitrogen by low-cost and visible-light-driven photocatalyst remained a grand challenge. Enlightenment from biological nitrogen fixation, multi-component systems can often achieve higher efficiency when working collaboratively. Herein, we constructed an efficient visible-light-driven carbon nitride/oxygen vacancy titanium dioxide (CN-OvTiO(2)) heterojunction photocatalyst through a solvent evaporation deposition method, in which CN serves as the light absorption and electron supply components while Ov of TiO2 serves as the active site for N-2 activation. A high-efficiency electron tandem flow mode promoting photogenerated charge directional migration from CN to Ov of TiO2 under light irradiation is revealed in this system, which is the key link coupling heterojunction and defects effects. The Ov with high electron density is the active site for nitrogen chemisorption and activation according to the revealed favorable thermodynamics of lower reaction energy and kinetics of enhanced N-2 adsorption and N-N polarization. CN-OvTiO(2) shows a high quantum yield of 0.15% at 500 nm monochromatic light and a high ammonia production rate of 34 mu mol gcat(-1) under visible light irradiation, 8.5 times higher than that of pure CN. This work deeply reveals the link and synergy mechanism of hetero-junction and defects, and is expected to advance the development of visible-light-driven and low-cost nitrogen fixation catalysts.
作者
我是这篇论文的作者
点击您的名字以认领此论文并将其添加到您的个人资料中。
推荐
暂无数据