2D-layered Ti3C2 MXenes for promoted synthesis of NH3 on P25 photocatalysts

[Display omitted] •A new co-catalyst for the photocatalytic NH3 synthesis from N2 was developed.•The generation yield of NH3 was improved to five times higher.•Three aspects functions of Ti3C2 MXenes were clearly demonstrated.•Oxygen vacancies were introduced in the composition process.•DFT calculat...

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Published in:Applied catalysis. B, Environmental Environmental, 2020-09, Vol.273, p.119054, Article 119054
Main Authors: Liao, Yuan, Qian, Jing, Xie, Gang, Han, Qing, Dang, Wenqiang, Wang, Yuanshen, Lv, Lingling, Zhao, Sen, Luo, Lei, Zhang, Wen, Jiang, Hai-Ying, Tang, Junwang
Format: Article
Language:English
Subjects:
Activation
Ammonia
Catalysts
Charge density
Chemical synthesis
Chemisorption
Co-catalyst
Electrical conductivity
Electrical resistivity
Irradiation
Light irradiation
MXenes
NH3 synthesis
P25
Photocatalysis
Photoelectric effect
Photoelectric emission
Radiation
Ti3C2 MXenes
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Summary:[Display omitted] •A new co-catalyst for the photocatalytic NH3 synthesis from N2 was developed.•The generation yield of NH3 was improved to five times higher.•Three aspects functions of Ti3C2 MXenes were clearly demonstrated.•Oxygen vacancies were introduced in the composition process.•DFT calculations were used to study the chemisorption and activation of N2. A kind of 2D-layered material, Ti3C2 MXenes, was successfully used as a new and efficient co-catalyst to improve the photocatalytic NH3 synthesis performance of P25, due to its large surface area/2D-layered structure, large electric capacity, excellent electrical conductivity and effective chemisorption/activation of N2 molecules. The generation yield of NH3 was improved by five times on the optimized sample of 6% Ti3C2 MXenes–P25 compared with pure P25 under full spectrum light irradiation, consistent with the measured both photocurrent densities and charge lifetime. The further mechanistic study showed that Ti3C2 MXenes played an important role in the separation of photogenerated electron–hole pairs by accumulating the excited electrons from the excited P25. Most importantly, Ti3C2 MXenes could dramatically improve chemisorption and activation of N2 as demonstrated by ESR spectra and DFT calculations. In addition, Ti3C2 MXenes loading on P25 could introduce oxygen vacancies in P25, also beneficial for photocatalytic NH3 synthesis. Thus this study provides an efficient and promising co-catalyst for the photocatalytic NH3 synthesis process from N2 in air
ISSN:0926-3373
1873-3883
DOI:10.1016/j.apcatb.2020.119054