Reaction-driven formation of anisotropic strains in FeTeSe nanosheets boosts low-concentration nitrate reduction to ammonia

FeM (M = Se, Te) chalcogenides have been well studied as promising magnets and superconductors, yet their potential as electrocatalysts is often considered limited due to anion dissolution and oxidation during electrochemical reactions. Here, we show that by using two-dimensional (2D) FeTeSe nanosheets, these conventionally perceived limitations can be leveraged to enable the reaction-driven in-situ generation of anisotropic in-plane tensile and out-of-plane compressive strains during the alkaline low-concentration nitrate reduction reaction (NO<sub>3</sub><sup>-</sup>RR). The reconstructed catalyst demonstrates enhanced performance, yielding ammonia with a near-unity Faradaic efficiency and a high yield rate of 42.14 ± 2.06 mg h<sup>-1</sup> mg<sub>cat</sub><sup>-1</sup>. A series of operando synchrotron-based X-ray measurements and ex-situ characterizations, alongside theoretical calculations, reveal that strain formation is ascribed to chalcogen vacancies created by partial Se/Te leaching, which facilitate the adsorption and dissociation of OH<sup>-</sup>/NO<sub>3</sub><sup>-</sup> from the electrolyte, resulting in an O(H)-doped strained lattice. Combined electrochemical and computational investigations suggest that the superior catalytic performance arises from the synergistic contributions from the exposed strained Fe sites and surface hydroxyl groups. These findings highlight the potential of 2D transition metal chalcogenides for in-situ structural engineering during electrochemical reactions to enhance catalytic activity for NO<sub>3</sub><sup>-</sup>RR and beyond.

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Publication Details

Journal
Nature Communications
Published
2025-04-15
DOI
https://doi.org/10.1038/s41467-025-58940-x
Citations
25
Primary Topic
Ammonia Synthesis and Nitrogen Reduction
Type
article
Field-Weighted Citation Impact
9.72

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article

Reaction-driven formation of anisotropic strains in FeTeSe nanosheets boosts low-concentration nitrate reduction to ammonia

Qingyu Yan, Yifan Xu, Ruihuan Duan, L. S. R. Kumara et al.
25 citations
Nature Communications
Ammonia Synthesis and Nitrogen Reduction
9.72
article

Reaction-driven formation of anisotropic strains in FeTeSe nanosheets boosts low-concentration nitrate reduction to ammonia

Qingyu Yan, Yifan Xu, Ruihuan Duan, L. S. R. Kumara, Bo Han, Man‐Fai Ng, Takeshi Watanabe, Jochi Tseng, Qiang Zhu, Mengxin Chen, Dongshuang Wu, Okkyun Seo, Jianwei Xu, Jinfeng Dong, Carmen Lee, Yue Hu, Jiawei Liu, Zheng Liu, Mingsheng Zhang
article en
25 citations

Abstract

FeM (M = Se, Te) chalcogenides have been well studied as promising magnets and superconductors, yet their potential as electrocatalysts is often considered limited due to anion dissolution and oxidation during electrochemical reactions. Here, we show that by using two-dimensional (2D) FeTeSe nanosheets, these conventionally perceived limitations can be leveraged to enable the reaction-driven in-situ generation of anisotropic in-plane tensile and out-of-plane compressive strains during the alkaline low-concentration nitrate reduction reaction (NO<sub>3</sub><sup>-</sup>RR). The reconstructed catalyst demonstrates enhanced performance, yielding ammonia with a near-unity Faradaic efficiency and a high yield rate of 42.14 ± 2.06 mg h<sup>-1</sup> mg<sub>cat</sub><sup>-1</sup>. A series of operando synchrotron-based X-ray measurements and ex-situ characterizations, alongside theoretical calculations, reveal that strain formation is ascribed to chalcogen vacancies created by partial Se/Te leaching, which facilitate the adsorption and dissociation of OH<sup>-</sup>/NO<sub>3</sub><sup>-</sup> from the electrolyte, resulting in an O(H)-doped strained lattice. Combined electrochemical and computational investigations suggest that the superior catalytic performance arises from the synergistic contributions from the exposed strained Fe sites and surface hydroxyl groups. These findings highlight the potential of 2D transition metal chalcogenides for in-situ structural engineering during electrochemical reactions to enhance catalytic activity for NO<sub>3</sub><sup>-</sup>RR and beyond.

Nature CommunicationsVol. 16(1)
Agency for Science, Technology and Research (SG), Nanyang Technological University (SG), Hong Kong University of Science and Technology (HK), Institute of High Performance Computing (SG), SPring-8 (JP), Japan Synchrotron Radiation Research Institute (JP), Institute of Materials Research and Engineering (SG), University of Hong Kong (HK)
Agency for Science, Technology and Research, Ministry of Education, India, National Supercomputing Center, Korea Institute of Science and Technology Information
Clean water and sanitation
Openalex Percentile: Top 1%
Ammonia Synthesis and Nitrogen Reduction
9.72
DOIOpen Access PDFOpenAlex
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