Overcoming Energy-Scaling Barriers: Efficient Ammonia Electrosynthesis on High-Entropy Alloy Catalysts

Di Yin; Bowen Li; Boxiang Gao; Mengxue Chen; Dong Chen; You Meng; Shuai Zhang; Chenxu Zhang; Quan Quan; Lijie Chen; Cheng Yang; Chun-Yuen Wong; Johnny Chung Yin Ho

doi:10.1002/adma.202415739

Overcoming Energy-Scaling Barriers: Efficient Ammonia Electrosynthesis on High-Entropy Alloy Catalysts

Di Yin, Bowen Li, Boxiang Gao, Mengxue Chen, Dong Chen, You Meng, Shuai Zhang, Chenxu Zhang, Quan Quan, Lijie Chen, Cheng Yang, Chun-Yuen Wong, Johnny Chung Yin Ho^*

^*Corresponding author for this work

Research output: Journal Publications and Reviews › RGC 21 - Publication in refereed journal › peer-review

23 Downloads (CityUHK Scholars)

Abstract

Electrochemically converting nitrate (NO₃⁻) to value-added ammonia (NH₃) is a complex process involving an eight-electron transfer and numerous intermediates, presenting a significant challenge for optimization. A multi-elemental synergy strategy to regulate the local electronic structure at the atomic level is proposed, creating a broad adsorption energy landscape in high-entropy alloy (HEA) catalysts. This approach enables optimal adsorption and desorption of various intermediates, effectively overcoming energy-scaling limitations for efficient NH₃ electrosynthesis. The HEA catalyst achieved a high Faradaic efficiency of 94.5 ± 4.3% and a yield rate of 10.2 ± 0.5 mg h⁻¹ mg_cat⁻¹. It also demonstrated remarkable stability over 250 h in an integrated three-chamber device, coupling electrocatalysis with an ammonia recovery unit for continuous NH₃ collection. This work elucidates the catalytic mechanisms of multi-functional HEA systems and offers new perspectives for optimizing multi-step reactions by circumventing adsorption-energy scaling limitations. © 2025 The Author(s). Advanced Materials published by Wiley-VCH GmbH.

Original language	English
Article number	2415739
Journal	Advanced Materials
Volume	37
Issue number	9
Online published	15 Jan 2025
DOIs	https://doi.org/10.1002/adma.202415739
Publication status	Published - 5 Mar 2025

Funding

This work was financially supported by the City University of Hong Kong (project nos. 9229138, 9231502, and 9231539).

Research Keywords

electrochemical nitrate reduction
energy-scaling limitations
high-entropy alloy

Publisher's Copyright Statement

This full text is made available under CC-BY-NC-ND 4.0. https://creativecommons.org/licenses/by-nc-nd/4.0/

Access Output

10.1002/adma.202415739

268949049.pdfFinal Published version, 4.65 MBLicence: CC BY-NC-ND

Other Access Options

Check CityUHK Library

Permanent Link

Right click to copy link

Cite this

@article{aaf5ac035c2242908d39dcd31f8224a2,

title = "Overcoming Energy-Scaling Barriers: Efficient Ammonia Electrosynthesis on High-Entropy Alloy Catalysts",

abstract = "Electrochemically converting nitrate (NO3−) to value-added ammonia (NH3) is a complex process involving an eight-electron transfer and numerous intermediates, presenting a significant challenge for optimization. A multi-elemental synergy strategy to regulate the local electronic structure at the atomic level is proposed, creating a broad adsorption energy landscape in high-entropy alloy (HEA) catalysts. This approach enables optimal adsorption and desorption of various intermediates, effectively overcoming energy-scaling limitations for efficient NH3 electrosynthesis. The HEA catalyst achieved a high Faradaic efficiency of 94.5 ± 4.3% and a yield rate of 10.2 ± 0.5 mg h−1 mgcat−1. It also demonstrated remarkable stability over 250 h in an integrated three-chamber device, coupling electrocatalysis with an ammonia recovery unit for continuous NH3 collection. This work elucidates the catalytic mechanisms of multi-functional HEA systems and offers new perspectives for optimizing multi-step reactions by circumventing adsorption-energy scaling limitations. {\textcopyright} 2025 The Author(s). Advanced Materials published by Wiley-VCH GmbH.",

keywords = "electrochemical nitrate reduction, energy-scaling limitations, high-entropy alloy",

author = "Di Yin and Bowen Li and Boxiang Gao and Mengxue Chen and Dong Chen and You Meng and Shuai Zhang and Chenxu Zhang and Quan Quan and Lijie Chen and Cheng Yang and Chun-Yuen Wong and Ho, {Johnny Chung Yin}",

year = "2025",

month = mar,

day = "5",

doi = "10.1002/adma.202415739",

language = "English",

volume = "37",

journal = "Advanced Materials",

issn = "0935-9648",

publisher = "Wiley-Blackwell",

number = "9",

}

TY - JOUR

T1 - Overcoming Energy-Scaling Barriers

T2 - Efficient Ammonia Electrosynthesis on High-Entropy Alloy Catalysts

AU - Yin, Di

AU - Li, Bowen

AU - Gao, Boxiang

AU - Chen, Mengxue

AU - Chen, Dong

AU - Meng, You

AU - Zhang, Shuai

AU - Zhang, Chenxu

AU - Quan, Quan

AU - Chen, Lijie

AU - Yang, Cheng

AU - Wong, Chun-Yuen

AU - Ho, Johnny Chung Yin

PY - 2025/3/5

Y1 - 2025/3/5

N2 - Electrochemically converting nitrate (NO3−) to value-added ammonia (NH3) is a complex process involving an eight-electron transfer and numerous intermediates, presenting a significant challenge for optimization. A multi-elemental synergy strategy to regulate the local electronic structure at the atomic level is proposed, creating a broad adsorption energy landscape in high-entropy alloy (HEA) catalysts. This approach enables optimal adsorption and desorption of various intermediates, effectively overcoming energy-scaling limitations for efficient NH3 electrosynthesis. The HEA catalyst achieved a high Faradaic efficiency of 94.5 ± 4.3% and a yield rate of 10.2 ± 0.5 mg h−1 mgcat−1. It also demonstrated remarkable stability over 250 h in an integrated three-chamber device, coupling electrocatalysis with an ammonia recovery unit for continuous NH3 collection. This work elucidates the catalytic mechanisms of multi-functional HEA systems and offers new perspectives for optimizing multi-step reactions by circumventing adsorption-energy scaling limitations. © 2025 The Author(s). Advanced Materials published by Wiley-VCH GmbH.

AB - Electrochemically converting nitrate (NO3−) to value-added ammonia (NH3) is a complex process involving an eight-electron transfer and numerous intermediates, presenting a significant challenge for optimization. A multi-elemental synergy strategy to regulate the local electronic structure at the atomic level is proposed, creating a broad adsorption energy landscape in high-entropy alloy (HEA) catalysts. This approach enables optimal adsorption and desorption of various intermediates, effectively overcoming energy-scaling limitations for efficient NH3 electrosynthesis. The HEA catalyst achieved a high Faradaic efficiency of 94.5 ± 4.3% and a yield rate of 10.2 ± 0.5 mg h−1 mgcat−1. It also demonstrated remarkable stability over 250 h in an integrated three-chamber device, coupling electrocatalysis with an ammonia recovery unit for continuous NH3 collection. This work elucidates the catalytic mechanisms of multi-functional HEA systems and offers new perspectives for optimizing multi-step reactions by circumventing adsorption-energy scaling limitations. © 2025 The Author(s). Advanced Materials published by Wiley-VCH GmbH.

KW - electrochemical nitrate reduction

KW - energy-scaling limitations

KW - high-entropy alloy

UR - http://www.scopus.com/inward/record.url?scp=85215066688&partnerID=8YFLogxK

UR - https://www.scopus.com/record/pubmetrics.uri?eid=2-s2.0-85215066688&origin=recordpage

U2 - 10.1002/adma.202415739

DO - 10.1002/adma.202415739

M3 - RGC 21 - Publication in refereed journal

SN - 0935-9648

VL - 37

JO - Advanced Materials

JF - Advanced Materials

IS - 9

M1 - 2415739

ER -

Overcoming Energy-Scaling Barriers: Efficient Ammonia Electrosynthesis on High-Entropy Alloy Catalysts

Abstract

Funding

Research Keywords

Publisher's Copyright Statement

Access Output

Other Access Options

Permanent Link

Other Files and Links

Fingerprint

DON_RMG: Atomic Memristor based on Janus 2D Ferroelectric Semiconductors - RMGS

Cite this

Overcoming Energy-Scaling Barriers: Efficient Ammonia Electrosynthesis on High-Entropy Alloy Catalysts

Abstract

Funding

Research Keywords

Publisher's Copyright Statement

Access Output

Other Access Options

Permanent Link

Other Files and Links

Fingerprint

Projects

DON_RMG: Atomic Memristor based on Janus 2D Ferroelectric Semiconductors - RMGS

Cite this