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Promoted N[triple bond]N activation by oxygen and boosted ammonia production over Bi4O5Br2

Yuan, Chen; Lu, Zilin; Jiang, Wenjun; Ibhadon, Alex O.; Teng, Fei

Authors

Chen Yuan

Zilin Lu

Wenjun Jiang

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Dr Alex Ibhadon A.O.Ibhadon@hull.ac.uk
Reader, Catalysis and Reactor Engineering for Energy Generation and Chemical Synthesis

Fei Teng



Abstract

Nitrogen photoreduction method is recognized as a safe, environmentally friendly and sustainable technology for ammonia production. For this method, nevertheless, it is a big challenge to efficaciously activate the N[tbnd]N triple bond. In this work, we mainly investigate the activation of N[tbnd]N bond and the ammonia production reaction over Bi4O5Br2. Under an N2/O2 atmosphere, the ammonia yield reaches 122.8 ?mol L?1 over Bi4O5Br2, which is 2.55 times than that under a N2 atmosphere (34.6 ?mol L?1). Theory calculation results further verify that the activation of N[tbnd]N bond is obviously improved by the presence of oxygen. It is proposed that the presence of oxygen, as an electron transfer bridge, facilitates the activation of nitrogen, and thus accelerating nitrogen photoreduction reaction. Additionally, in the methanol/water system, the ammonia production rates of Bi4O5Br2 reaches 8597.5 ?mol g?1L?1h?1, which is 6 times higher than that in pure water (1228.5 ?mol L?1g?1h?1). We assume that methanol as a hole scavenger has efficiently prevented the oxidation of ammonia, thus significantly accelerating the nitrogen photoreduction reaction. This work demonstrates that directly using air as feed gas is a very easy and cost-effective strategy for ammonia production.

Citation

Yuan, C., Lu, Z., Jiang, W., Ibhadon, A. O., & Teng, F. (2021). Promoted N[triple bond]N activation by oxygen and boosted ammonia production over Bi4O5Br2. Molecular Catalysis, 515, Article 111913. https://doi.org/10.1016/j.mcat.2021.111913

Journal Article Type Article
Acceptance Date Sep 16, 2021
Online Publication Date Sep 25, 2021
Publication Date 2021-10
Deposit Date May 3, 2022
Journal Molecular Catalysis
Print ISSN 2468-8231
Publisher Elsevier
Peer Reviewed Peer Reviewed
Volume 515
Article Number 111913
DOI https://doi.org/10.1016/j.mcat.2021.111913
Keywords Bi4O5Br2; Solar energy; Nitrogen photoreduction; N triple bond N bond activation; Oxygen
Public URL https://hull-repository.worktribe.com/output/3850045