Disentangling efficiency-selectivity tradeoffs for electrocatalytic ammonia synthesis

Hao Fei; Ruoqi Liu; Bilong Liu; Songhua Yang; Zhenhua Zhang; Xiangyu Meng; Feipeng Yang; Guanzhen Chen; Yunze Zhang; Siyuan Wang; Jia Lei; Ziyi Wang; Chi Zhang; Qifeng Zheng; Zhuangzhi Wu; Dezhi Wang; Furong Chen; Jian Wang

doi:10.1016/j.apcatb.2026.127047

Disentangling efficiency-selectivity tradeoffs for electrocatalytic ammonia synthesis

Hao Fei
, Ruoqi Liu
, Bilong Liu
, Songhua Yang
, Zhenhua Zhang
, Xiangyu Meng
, Feipeng Yang
, Guanzhen Chen
, Yunze Zhang
, Siyuan Wang
, Jia Lei
, Ziyi Wang
, Chi Zhang
, Qifeng Zheng
, Zhuangzhi Wu^*
, Dezhi Wang^*
, Furong Chen
, Jian Wang^*

^*Corresponding author for this work

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

2 Citations (Scopus)

Abstract

Aqueous nitrogen reduction reaction (a-NRR) offers a promising alternative to the Haber-Bosch process for ammonia synthesis, but its practical viability is hindered by the hard N₂ accessibility/activation and competitive hydrogen evolution reaction (HER). These two reactions cause a serious activity-selectivity trade-off due to their coupled competing pathways at shared active sites in conventional catalysts. Here, we propose a dual-band engineering strategy on MoS₂ to decouple active sites. We identify the Mo-d and S-p band centers as independent descriptors for a-NRR and HER activity, respectively. Through vacancy and phase engineering, we modulate dual-band overlaps to boost N₂ activation while suppressing HER, achieving a sevenfold performance enhancement. Further integration into a flow reactor yields a high NH₃ output (240.01 ± 8.46 μg h^–1 mg^–1_cat.) and Faradic efficiency (65.96 ± 2.29%), even comparable to some metal-mediated NRR and nitrate reduction systems. This work establishes a descriptor-guided framework for managing competitive reactions through active-site decoupling. © 2026 Elsevier B.V.

Original language	English
Article number	127047
Number of pages	12
Journal	Applied Catalysis B: Environment and Energy
Volume	398
Online published	1 Jun 2026
DOIs	https://doi.org/10.1016/j.apcatb.2026.127047
Publication status	Online published - 1 Jun 2026

Funding

The authors acknowledge the support from the National Natural Science Foundation of China through the projects 52302312 and 52374407, the Research Grants Council of Hong Kong through the projects ECS 21308523 and C1003–24Y, the Innovation and Technology Commission of Hong Kong through the project ITS/130/23FP and GHP/290/23SZ, the City University of Hong Kong through projects 9667262, 9610537, and 7005921, the Department of Science and Technology of Guangdong Province through project 2023B1515130004, 2024A1515013020, and 2024B1515130002, the Science, Technology and Innovation Bureau of Shenzhen Municipality (Project No. SGDX20240115110505010) under the Mainland-Hong Kong Technology Cooperation Funding Scheme, Shenzhen Fundamental Research Scheme-General Program through the project JCYJ20250604184537048.

UN SDGs

This output contributes to the following UN Sustainable Development Goals (SDGs)

SDG 7 Affordable and Clean Energy

Research Keywords

Dual-band engineering
Efficiency-selectivity trade-off
Hydrogen evolution reaction
Molybdenum disulfide
Nitrogen reduction reaction

RGC Funding Information

RGC-funded

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10.1016/j.apcatb.2026.127047

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Cite this

Fei, H., Liu, R., Liu, B., Yang, S., Zhang, Z., Meng, X., Yang, F., Chen, G., Zhang, Y., Wang, S., Lei, J., Wang, Z., Zhang, C., Zheng, Q., Wu, Z., Wang, D., Chen, F., & Wang, J. (2026). Disentangling efficiency-selectivity tradeoffs for electrocatalytic ammonia synthesis. Applied Catalysis B: Environment and Energy, 398, Article 127047. Advance online publication. https://doi.org/10.1016/j.apcatb.2026.127047

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abstract = "Aqueous nitrogen reduction reaction (a-NRR) offers a promising alternative to the Haber-Bosch process for ammonia synthesis, but its practical viability is hindered by the hard N2 accessibility/activation and competitive hydrogen evolution reaction (HER). These two reactions cause a serious activity-selectivity trade-off due to their coupled competing pathways at shared active sites in conventional catalysts. Here, we propose a dual-band engineering strategy on MoS2 to decouple active sites. We identify the Mo-d and S-p band centers as independent descriptors for a-NRR and HER activity, respectively. Through vacancy and phase engineering, we modulate dual-band overlaps to boost N2 activation while suppressing HER, achieving a sevenfold performance enhancement. Further integration into a flow reactor yields a high NH3 output (240.01 ± 8.46 μg h–1 mg–1cat.) and Faradic efficiency (65.96 ± 2.29\%), even comparable to some metal-mediated NRR and nitrate reduction systems. This work establishes a descriptor-guided framework for managing competitive reactions through active-site decoupling. {\textcopyright} 2026 Elsevier B.V.",

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language = "English",

volume = "398",

journal = "Applied Catalysis B: Environment and Energy",

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T1 - Disentangling efficiency-selectivity tradeoffs for electrocatalytic ammonia synthesis

AU - Fei, Hao

AU - Liu, Ruoqi

AU - Liu, Bilong

AU - Yang, Songhua

AU - Zhang, Zhenhua

AU - Meng, Xiangyu

AU - Yang, Feipeng

AU - Chen, Guanzhen

AU - Zhang, Yunze

AU - Wang, Siyuan

AU - Lei, Jia

AU - Wang, Ziyi

AU - Zhang, Chi

AU - Zheng, Qifeng

AU - Wu, Zhuangzhi

AU - Wang, Dezhi

AU - Chen, Furong

AU - Wang, Jian

PY - 2026/6/1

Y1 - 2026/6/1

N2 - Aqueous nitrogen reduction reaction (a-NRR) offers a promising alternative to the Haber-Bosch process for ammonia synthesis, but its practical viability is hindered by the hard N2 accessibility/activation and competitive hydrogen evolution reaction (HER). These two reactions cause a serious activity-selectivity trade-off due to their coupled competing pathways at shared active sites in conventional catalysts. Here, we propose a dual-band engineering strategy on MoS2 to decouple active sites. We identify the Mo-d and S-p band centers as independent descriptors for a-NRR and HER activity, respectively. Through vacancy and phase engineering, we modulate dual-band overlaps to boost N2 activation while suppressing HER, achieving a sevenfold performance enhancement. Further integration into a flow reactor yields a high NH3 output (240.01 ± 8.46 μg h–1 mg–1cat.) and Faradic efficiency (65.96 ± 2.29%), even comparable to some metal-mediated NRR and nitrate reduction systems. This work establishes a descriptor-guided framework for managing competitive reactions through active-site decoupling. © 2026 Elsevier B.V.

AB - Aqueous nitrogen reduction reaction (a-NRR) offers a promising alternative to the Haber-Bosch process for ammonia synthesis, but its practical viability is hindered by the hard N2 accessibility/activation and competitive hydrogen evolution reaction (HER). These two reactions cause a serious activity-selectivity trade-off due to their coupled competing pathways at shared active sites in conventional catalysts. Here, we propose a dual-band engineering strategy on MoS2 to decouple active sites. We identify the Mo-d and S-p band centers as independent descriptors for a-NRR and HER activity, respectively. Through vacancy and phase engineering, we modulate dual-band overlaps to boost N2 activation while suppressing HER, achieving a sevenfold performance enhancement. Further integration into a flow reactor yields a high NH3 output (240.01 ± 8.46 μg h–1 mg–1cat.) and Faradic efficiency (65.96 ± 2.29%), even comparable to some metal-mediated NRR and nitrate reduction systems. This work establishes a descriptor-guided framework for managing competitive reactions through active-site decoupling. © 2026 Elsevier B.V.

KW - Dual-band engineering

KW - Efficiency-selectivity trade-off

KW - Hydrogen evolution reaction

KW - Molybdenum disulfide

KW - Nitrogen reduction reaction

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ER -

Disentangling efficiency-selectivity tradeoffs for electrocatalytic ammonia synthesis

Abstract

Funding

UN SDGs

Research Keywords

RGC Funding Information

Access Output

Other Access Options

Permanent Link

Other Files and Links

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ITF: Development of Solid-State Lithium-Metal Batteries with High Safety and Energy Density

YCRG: High-performance and Long-life Anion Exchange Membrane Water Electrolysis: From Material Design to Cell Innovation

YCRG-Sub-pj: High-performance and Long-life Anion Exchange Membrane Water Electrolysis: From Material Design to Cell Innovation

Cite this

Disentangling efficiency-selectivity tradeoffs for electrocatalytic ammonia synthesis

Abstract

Funding

UN SDGs

Research Keywords

RGC Funding Information

Access Output

Other Access Options

Permanent Link

Other Files and Links

Fingerprint

Projects

ITF: Development of Solid-State Lithium-Metal Batteries with High Safety and Energy Density

YCRG: High-performance and Long-life Anion Exchange Membrane Water Electrolysis: From Material Design to Cell Innovation

YCRG-Sub-pj: High-performance and Long-life Anion Exchange Membrane Water Electrolysis: From Material Design to Cell Innovation

Cite this