Efficient N2 electroreduction to ammonia in an isopropanol–PBS electrolyte using NiFe2O4in situ grown on nickel foam

Chang Chen; Min Cui; Qian Wang; Penglei Cui; Cong Zhang; Qian Yang; Jujie Ren

doi:10.1039/D2YA00364C

Efficient N₂ electroreduction to ammonia in an isopropanol–PBS electrolyte using NiFe₂O₄in situ grown on nickel foam†

Chang Chen,‡^ab Min Cui,‡^a Qian Wang,

*^b Penglei Cui,^b Cong Zhang,^a Qian Yang^b and Jujie Ren*^a

Author affiliations

* Corresponding authors

^a Hebei Provincial Key Laboratory of Photoelectric Control on Surface and Interface, School of Sciences, Hebei University of Science and Technology, Shijiazhuang 050018, P. R. China
E-mail: jujieren@163.com

^b CAS Key Laboratory of Green Process and Engineering, State Key Laboratory of Multiphase Complex Systems, Beijing Key Laboratory of Ionic Liquids Clean Process, Institute of Process Engineering, Chinese Academy of Sciences, Beijing 100190, P. R. China
E-mail: wangq@ipe.ac.cn

Abstract

The electrocatalytic nitrogen reduction reaction (ENRR) can produce ammonia under environmental conditions and is considered a sustainable alternative to the traditional Haber–Bosch process. However, the ENRR is limited by the solubility of nitrogen (N₂) and the hydrogen evolution reaction (HER) of the aqueous solution. It is found that the solubility of N₂ in isopropanol at room temperature and pressure is more than ten times higher than that in an aqueous solution. In addition, K⁺ can effectively inhibit the HER. Therefore, we use the two-component electrolyte of isopropanol and phosphate buffer solution (PBS) with potassium salt to weaken the influence of low solubility of N₂ in an aqueous solution and the competitive HER. In addition, we have in situ grown NiFe₂O₄ nanoarrays on nickel foam (NiFe₂O₄/NF) as the electrocatalyst. Finally, a high ammonia yield (1.1 μg h⁻¹ cm⁻²) is achieved and the faradaic efficiency (FE) exceeds 30% at room temperature and pressure. In the end, a model of N₂ adsorption on the active (311) crystal surface of NiFe₂O₄ was established by means of density functional theory (DFT) calculations, and the activation energy required for the reaction was calculated, proving that the ENRR reported here was an alternate hydrogenation path.

Supplementary files

Article information

DOI: https://doi.org/10.1039/D2YA00364C
Article type: Paper
Submitted: 27 Dec 2022
Accepted: 02 Mar 2023
First published: 03 Mar 2023
This article is Open Access

Download Citation

Energy Adv., 2023,2, 547-555

Permissions

Request permissions

Efficient N₂ electroreduction to ammonia in an isopropanol–PBS electrolyte using NiFe₂O₄in situ grown on nickel foam

C. Chen, M. Cui, Q. Wang, P. Cui, C. Zhang, Q. Yang and J. Ren, Energy Adv., 2023, 2, 547 DOI: 10.1039/D2YA00364C

This article is licensed under a Creative Commons Attribution-NonCommercial 3.0 Unported Licence. You can use material from this article in other publications, without requesting further permission from the RSC, provided that the correct acknowledgement is given and it is not used for commercial purposes.

To request permission to reproduce material from this article in a commercial publication, please go to the Copyright Clearance Center request page.

If you are an author contributing to an RSC publication, you do not need to request permission provided correct acknowledgement is given.

If you are the author of this article, you do not need to request permission to reproduce figures and diagrams provided correct acknowledgement is given. If you want to reproduce the whole article in a third-party commercial publication (excluding your thesis/dissertation for which permission is not required) please go to the Copyright Clearance Center request page.

Energy Advances