Ambient electrocatalytic N2 reduction to NH3 by metal fluorides

Peipei Li; Zaichun Liu; Tongwei Wu; Ya Zhang; Linyu Wang; Li Wang; Lei Ji; Youyu Zhang; Yonglan Luo; Ting Wang; Shanhu Liu; Yuping Wu; Meiling Liu; Xuping Sun

doi:10.1039/c9ta04706a

Ambient electrocatalytic N₂ reduction to NH₃ by metal fluorides

Peipei Li, Zaichun Liu, Tongwei Wu, Ya Zhang, Linyu Wang, Li Wang, Lei Ji, Youyu Zhang, Yonglan Luo, Ting Wang, Shanhu Liu, Yuping Wu, Meiling Liu, Xuping Sun

School of energy science and engineering

Research output: Contribution to journal › Article › peer-review

41 Scopus citations

Abstract

The high-temperature and high-pressure Haber-Bosch process for industrial NH₃ production is rather energy-intensive with heavy CO₂ emission. Electrochemical N₂ reduction in aqueous media offers an eco-friendly and sustainable alternative to ambient NH₃ synthesis with the aid of efficient electrocatalysts for the N₂ reduction reaction (NRR), but they suffer from limited current efficiency for NH₃ formation due to the unavoidable competing hydrogen evolution reaction (HER). Here, we report that LaF₃ nanoplates act as a superb NRR electrocatalyst for ambient N₂-to-NH₃ fixation with excellent selectivity due to their effective inhibition of the HER and activation of the NN triple bond. In 0.5 M LiClO₄, they achieve a high faradaic efficiency of 16.0% and a large NH₃ yield of 55.9 μg h^-1 mg_cat.^-1 at -0.45 V vs. the reversible hydrogen electrode, much higher than those of La₂O₃ (1.4%; 12.5 μg h^-1 mg_cat.^-1) and most reported aqueous-based NRR catalysts. This catalyst also shows high long-term electrochemical and structural stability. The detailed NRR mechanism is also discussed.

Original language	English
Pages (from-to)	17761-17765
Number of pages	5
Journal	Journal of Materials Chemistry A
Volume	7
Issue number	30
DOIs	https://doi.org/10.1039/c9ta04706a
State	Published - 2019

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@article{e68c25aefcfe4eb5b907b284f6a5b6ad,

title = "Ambient electrocatalytic N2 reduction to NH3 by metal fluorides",

abstract = "The high-temperature and high-pressure Haber-Bosch process for industrial NH3 production is rather energy-intensive with heavy CO2 emission. Electrochemical N2 reduction in aqueous media offers an eco-friendly and sustainable alternative to ambient NH3 synthesis with the aid of efficient electrocatalysts for the N2 reduction reaction (NRR), but they suffer from limited current efficiency for NH3 formation due to the unavoidable competing hydrogen evolution reaction (HER). Here, we report that LaF3 nanoplates act as a superb NRR electrocatalyst for ambient N2-to-NH3 fixation with excellent selectivity due to their effective inhibition of the HER and activation of the NN triple bond. In 0.5 M LiClO4, they achieve a high faradaic efficiency of 16.0% and a large NH3 yield of 55.9 μg h-1 mgcat.-1 at -0.45 V vs. the reversible hydrogen electrode, much higher than those of La2O3 (1.4%; 12.5 μg h-1 mgcat.-1) and most reported aqueous-based NRR catalysts. This catalyst also shows high long-term electrochemical and structural stability. The detailed NRR mechanism is also discussed.",

author = "Peipei Li and Zaichun Liu and Tongwei Wu and Ya Zhang and Linyu Wang and Li Wang and Lei Ji and Youyu Zhang and Yonglan Luo and Ting Wang and Shanhu Liu and Yuping Wu and Meiling Liu and Xuping Sun",

note = "Publisher Copyright: {\textcopyright} 2019 The Royal Society of Chemistry.",

year = "2019",

doi = "10.1039/c9ta04706a",

language = "英语",

volume = "7",

pages = "17761--17765",

journal = "Journal of Materials Chemistry A",

issn = "2050-7488",

publisher = "Royal Society of Chemistry",

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}

TY - JOUR

T1 - Ambient electrocatalytic N2 reduction to NH3 by metal fluorides

AU - Li, Peipei

AU - Liu, Zaichun

AU - Wu, Tongwei

AU - Zhang, Ya

AU - Wang, Linyu

AU - Wang, Li

AU - Ji, Lei

AU - Zhang, Youyu

AU - Luo, Yonglan

AU - Wang, Ting

AU - Liu, Shanhu

AU - Wu, Yuping

AU - Liu, Meiling

AU - Sun, Xuping

PY - 2019

Y1 - 2019

N2 - The high-temperature and high-pressure Haber-Bosch process for industrial NH3 production is rather energy-intensive with heavy CO2 emission. Electrochemical N2 reduction in aqueous media offers an eco-friendly and sustainable alternative to ambient NH3 synthesis with the aid of efficient electrocatalysts for the N2 reduction reaction (NRR), but they suffer from limited current efficiency for NH3 formation due to the unavoidable competing hydrogen evolution reaction (HER). Here, we report that LaF3 nanoplates act as a superb NRR electrocatalyst for ambient N2-to-NH3 fixation with excellent selectivity due to their effective inhibition of the HER and activation of the NN triple bond. In 0.5 M LiClO4, they achieve a high faradaic efficiency of 16.0% and a large NH3 yield of 55.9 μg h-1 mgcat.-1 at -0.45 V vs. the reversible hydrogen electrode, much higher than those of La2O3 (1.4%; 12.5 μg h-1 mgcat.-1) and most reported aqueous-based NRR catalysts. This catalyst also shows high long-term electrochemical and structural stability. The detailed NRR mechanism is also discussed.

AB - The high-temperature and high-pressure Haber-Bosch process for industrial NH3 production is rather energy-intensive with heavy CO2 emission. Electrochemical N2 reduction in aqueous media offers an eco-friendly and sustainable alternative to ambient NH3 synthesis with the aid of efficient electrocatalysts for the N2 reduction reaction (NRR), but they suffer from limited current efficiency for NH3 formation due to the unavoidable competing hydrogen evolution reaction (HER). Here, we report that LaF3 nanoplates act as a superb NRR electrocatalyst for ambient N2-to-NH3 fixation with excellent selectivity due to their effective inhibition of the HER and activation of the NN triple bond. In 0.5 M LiClO4, they achieve a high faradaic efficiency of 16.0% and a large NH3 yield of 55.9 μg h-1 mgcat.-1 at -0.45 V vs. the reversible hydrogen electrode, much higher than those of La2O3 (1.4%; 12.5 μg h-1 mgcat.-1) and most reported aqueous-based NRR catalysts. This catalyst also shows high long-term electrochemical and structural stability. The detailed NRR mechanism is also discussed.

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U2 - 10.1039/c9ta04706a

DO - 10.1039/c9ta04706a

M3 - 文章

AN - SCOPUS:85070099497

SN - 2050-7488

VL - 7

SP - 17761

EP - 17765

JO - Journal of Materials Chemistry A

JF - Journal of Materials Chemistry A

IS - 30

ER -

Ambient electrocatalytic N₂ reduction to NH₃ by metal fluorides

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