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Ti3C2Tx (T = F, OH) MXene nanosheet: a conductive 2D catalyst for ambient electrohydrogenation of N2 to NH3

Abstract

The Haber–Bosch process for industrial-scale NH3 production suffers from high energy consume and serious CO2 emission. Electrochemical N2 reduction is an attractive carbon-neutral alternative for NH3 synthesis but severely challenged by N2 activation needing efficient electrocatalysts for the N2 reduction reaction (NRR) at ambient conditions. Here, report that Ti3C2Tx (T = F, OH) MXene nanosheet (Ti3C2Tx NS) acts as a high-performance 2D NRR electrocatalyst for ambient N2-to-NH3 conversion with excellent selectivity. In 0.1 M HCl, such Ti3C2Tx NS achieves a large NH3 yield of 20.4 μg h–1 mgcat.–1 and a high Faradic efficiency of 9.3% at –0.4 V vs. reversible hydrogen electrode, with high electrochemical and structure stability. Density functional theory calculations reveal that N2 chemisorbed on Ti3C2Tx experiences an elongation/weakness of the N≡N triple bond facilitating its catalytic conversion to NH3 and the distal NRR mechanism is more favorable with the final reaction of *NH2 to NH3 as the rate-limiting step.

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Publication details

The article was received on 12 Oct 2018, accepted on 04 Nov 2018 and first published on 07 Nov 2018


Article type: Communication
DOI: 10.1039/C8TA09840A
Citation: J. Mater. Chem. A, 2018, Accepted Manuscript
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    Ti3C2Tx (T = F, OH) MXene nanosheet: a conductive 2D catalyst for ambient electrohydrogenation of N2 to NH3

    J. Zhao, L. Zhang, X. Xie, X. Li, Y. Ma, Q. Liu, W. Fang, X. Shi, G. Cui and X. Sun, J. Mater. Chem. A, 2018, Accepted Manuscript , DOI: 10.1039/C8TA09840A

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