A vanadium-nickel oxynitride layer for enhanced electrocatalytic nitrogen fixation in neutral media

Bin Chang; Lequan Deng; Shouzhi Wang; Dong Shi; Zizheng Ai; Hehe Jiang; Yongliang Shao; Lei Zhang; Jianxing Shen; Yongzhong Wu; Xiaopeng Hao

doi:10.1039/c9ta11378a

A vanadium-nickel oxynitride layer for enhanced electrocatalytic nitrogen fixation in neutral media

Bin Chang, Lequan Deng, Shouzhi Wang, Dong Shi, Zizheng Ai, Hehe Jiang, Yongliang Shao, Lei Zhang, Jianxing Shen, Yongzhong Wu^*, Xiaopeng Hao

^*Corresponding author for this work

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

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Abstract

The application of transition-metal oxides (TMOs) in electrocatalytic nitrogen fixation still is hindered by their sluggish reaction kinetics and weak stabilization. In this work, a vanadium-nickel oxynitride (VNiON) layer is designed and synthesized on the corresponding oxide nanosheets to solve the above crucial issues. The first-principles kinetics analyses theoretically prove that the delocalized electron environment of VNiON enhanced π backdonation, which is conducive to nitrogen absorption and activation. Experimentally, both the ammonia production rate (∼6.78 μg h^-1 cm_cat.^-2) and faradaic efficiency (∼5.57%) of VNiON are enhanced by 2-fold relative to those of its corresponding oxide under neutral conditions. Meanwhile, the stability of oxide is enormously improved by introducing a VNiON layer. The mechanism of improving the nitrogen fixation performance of oxides is investigated. This work provides a novel strategy of constructing oxides with advantageous structures for extensive electrochemical applications.

Original language	English (US)
Pages (from-to)	91-96
Number of pages	6
Journal	JOURNAL OF MATERIALS CHEMISTRY A
Volume	8
Issue number	1
DOIs	https://doi.org/10.1039/c9ta11378a
State	Published - Jan 7 2020

ASJC Scopus subject areas

General Chemistry
Renewable Energy, Sustainability and the Environment
General Materials Science

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10.1039/c9ta11378a

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title = "A vanadium-nickel oxynitride layer for enhanced electrocatalytic nitrogen fixation in neutral media",

abstract = "The application of transition-metal oxides (TMOs) in electrocatalytic nitrogen fixation still is hindered by their sluggish reaction kinetics and weak stabilization. In this work, a vanadium-nickel oxynitride (VNiON) layer is designed and synthesized on the corresponding oxide nanosheets to solve the above crucial issues. The first-principles kinetics analyses theoretically prove that the delocalized electron environment of VNiON enhanced π backdonation, which is conducive to nitrogen absorption and activation. Experimentally, both the ammonia production rate (∼6.78 μg h-1 cmcat.-2) and faradaic efficiency (∼5.57%) of VNiON are enhanced by 2-fold relative to those of its corresponding oxide under neutral conditions. Meanwhile, the stability of oxide is enormously improved by introducing a VNiON layer. The mechanism of improving the nitrogen fixation performance of oxides is investigated. This work provides a novel strategy of constructing oxides with advantageous structures for extensive electrochemical applications.",

author = "Bin Chang and Lequan Deng and Shouzhi Wang and Dong Shi and Zizheng Ai and Hehe Jiang and Yongliang Shao and Lei Zhang and Jianxing Shen and Yongzhong Wu and Xiaopeng Hao",

note = "Funding Information: This work was supported by the National Natural Science Foundation of China (Contract No. 51872162 and 11890700), and the Major Basic Program of the Natural Science Foundation of Shandong Province (Contract ZR2017ZB0317 and ZR2018MEM013). Publisher Copyright: This journal is {\textcopyright} The Royal Society of Chemistry.",

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T1 - A vanadium-nickel oxynitride layer for enhanced electrocatalytic nitrogen fixation in neutral media

AU - Chang, Bin

AU - Deng, Lequan

AU - Wang, Shouzhi

AU - Shi, Dong

AU - Ai, Zizheng

AU - Jiang, Hehe

AU - Shao, Yongliang

AU - Zhang, Lei

AU - Shen, Jianxing

AU - Wu, Yongzhong

AU - Hao, Xiaopeng

N1 - Funding Information: This work was supported by the National Natural Science Foundation of China (Contract No. 51872162 and 11890700), and the Major Basic Program of the Natural Science Foundation of Shandong Province (Contract ZR2017ZB0317 and ZR2018MEM013). Publisher Copyright: This journal is © The Royal Society of Chemistry.

PY - 2020/1/7

Y1 - 2020/1/7

N2 - The application of transition-metal oxides (TMOs) in electrocatalytic nitrogen fixation still is hindered by their sluggish reaction kinetics and weak stabilization. In this work, a vanadium-nickel oxynitride (VNiON) layer is designed and synthesized on the corresponding oxide nanosheets to solve the above crucial issues. The first-principles kinetics analyses theoretically prove that the delocalized electron environment of VNiON enhanced π backdonation, which is conducive to nitrogen absorption and activation. Experimentally, both the ammonia production rate (∼6.78 μg h-1 cmcat.-2) and faradaic efficiency (∼5.57%) of VNiON are enhanced by 2-fold relative to those of its corresponding oxide under neutral conditions. Meanwhile, the stability of oxide is enormously improved by introducing a VNiON layer. The mechanism of improving the nitrogen fixation performance of oxides is investigated. This work provides a novel strategy of constructing oxides with advantageous structures for extensive electrochemical applications.

AB - The application of transition-metal oxides (TMOs) in electrocatalytic nitrogen fixation still is hindered by their sluggish reaction kinetics and weak stabilization. In this work, a vanadium-nickel oxynitride (VNiON) layer is designed and synthesized on the corresponding oxide nanosheets to solve the above crucial issues. The first-principles kinetics analyses theoretically prove that the delocalized electron environment of VNiON enhanced π backdonation, which is conducive to nitrogen absorption and activation. Experimentally, both the ammonia production rate (∼6.78 μg h-1 cmcat.-2) and faradaic efficiency (∼5.57%) of VNiON are enhanced by 2-fold relative to those of its corresponding oxide under neutral conditions. Meanwhile, the stability of oxide is enormously improved by introducing a VNiON layer. The mechanism of improving the nitrogen fixation performance of oxides is investigated. This work provides a novel strategy of constructing oxides with advantageous structures for extensive electrochemical applications.

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A vanadium-nickel oxynitride layer for enhanced electrocatalytic nitrogen fixation in neutral media

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