Nitrogen-doped phosphorene for electrocatalytic ammonia synthesis

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Xu, Guangrui
Li, Hao
Bati, Abdulaziz SR
Bat-Erdene, Munkhjargal
Nine, Md J
Losic, Dusan
Chen, Yu
Shapter, Joseph G
Batmunkh, Munkhbayar
Ma, Tianyi
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2020
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Abstract

The rapid surface oxidation of phosphorene under ambient conditions is considered to be a serious issue for many applications, but is used here as a strategy to achieve efficient heteroatom doping. Highly crystalline nitrogen-doped phosphorene (N-phosphorene) is prepared using a combination of ball milling and microwave techniques. The prepared N-doped phosphorene nanosheets showed outstanding electrocatalytic performance as a new type of non-metallic catalyst for nitrogen (N2) to ammonia (NH3) conversion, with an NH3 yield rate and faradaic efficiency (FE) of up to 18.79 μg h−1 mgCAT−1 and 21.51%, respectively, at a low overpotential (0 V) versus the reversible hydrogen electrode (RHE). Density functional theory calculations revealed that the high nitrogen reduction reaction (NRR) FEs originate from the increased hydrophobicity at the N and O doped phosphorene surfaces, which in turn hinders the competing hydrogen evolution reaction (HER) in an alkaline environment and promotes the NRR. This work not only introduces an efficient strategy to chemically functionalize 2D phosphorene, but also opens a new avenue in using N-doped phosphorene nanosheets as a metal-free catalyst.

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Journal of Materials Chemistry A

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© 2020 Royal Society of Chemistry. This is the author-manuscript version of this paper. Reproduced in accordance with the copyright policy of the publisher. Please refer to the journal website for access to the definitive, published version.

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Macromolecular and materials chemistry

Materials engineering

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Xu, G; Li, H; Bati, ASR; Bat-Erdene, M; Nine, MJ; Losic, D; Chen, Y; Shapter, JG; Batmunkh, M; Ma, T, Nitrogen-doped phosphorene for electrocatalytic ammonia synthesis, Journal of Materials Chemistry A

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