Please use this identifier to cite or link to this item: https://hdl.handle.net/10356/166583
Title: Ammonia electrosynthesis with a stable metal-free 2D silicon phosphide catalyst
Authors: Lv, Chade
Jia, Ning
Qian, Yumin
Wang, Shanpeng
Wang, Xuechun
Yu, Wei
Liu, Chuntai
Pan, Hongge
Zhu, Qiang
Xu, Jianwei
Tao, Xutang
Loh, Kian Ping
Xue, Can
Yan, Qingyu
Keywords: Engineering::Materials::Nanostructured materials
Issue Date: 2023
Source: Lv, C., Jia, N., Qian, Y., Wang, S., Wang, X., Yu, W., Liu, C., Pan, H., Zhu, Q., Xu, J., Tao, X., Loh, K. P., Xue, C. & Yan, Q. (2023). Ammonia electrosynthesis with a stable metal-free 2D silicon phosphide catalyst. Small, 19(10), 2205959-. https://dx.doi.org/10.1002/smll.202205959
Project: 2021-T1-002-012 
RG 65/21 
2020-T1-001-031 
A19D9a0096 
Journal: Small 
Abstract: Metal-free 2D phosphorus-based materials are emerging catalysts for ammonia (NH3 ) production through a sustainable electrochemical nitrogen reduction reaction route under ambient conditions. However, their efficiency and stability remain challenging due to the surface oxidization. Herein, a stable phosphorus-based electrocatalyst, silicon phosphide (SiP), is explored. Density functional theory calculations certify that the N2 activation can be realized on the zigzag Si sites with a dimeric end-on coordinated mode. Such sites also allow the subsequent protonation process via the alternating associative mechanism. As the proof-of-concept demonstration, both the crystalline and amorphous SiP nanosheets (denoted as C-SiP NSs and A-SiP NSs, respectively) are obtained through ultrasonic exfoliation processes, but only the crystalline one enables effective and stable electrocatalytic nitrogen reduction reaction, in terms of an NH3 yield rate of 16.12 µg h-1  mgcat. -1 and a Faradaic efficiency of 22.48% at -0.3 V versus reversible hydrogen electrode. The resistance to oxidization plays the decisive role in guaranteeing the NH3 electrosynthesis activity for C-SiP NSs. This surface stability endows C-SiP NSs with the capability to serve as appealing electrocatalysts for nitrogen reduction reactions and other promising applications.
URI: https://hdl.handle.net/10356/166583
ISSN: 1613-6810
DOI: 10.1002/smll.202205959
Schools: School of Materials Science and Engineering 
Research Centres: Institute of Material Research and Engineering, A*STAR
Rights: © 2022 Wiley-VCH GmbH. All rights reserved. This is the peer reviewed version of the following article: Lv, C., Jia, N., Qian, Y., Wang, S., Wang, X., Yu, W., Liu, C., Pan, H., Zhu, Q., Xu, J., Tao, X., Loh, K. P., Xue, C. & Yan, Q. (2023). Ammonia electrosynthesis with a stable metal-free 2D silicon phosphide catalyst. Small, 19(10), 2205959-, which has been published in final form at https://doi.org/10.1002/smll.202205959. This article may be used for non-commercial purposes in accordance with Wiley Terms and Conditions for Use of Self-Archived Versions.
Fulltext Permission: open
Fulltext Availability: With Fulltext
Appears in Collections:MSE Journal Articles

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