Lattice-Confined Ru Clusters Driving Efficient Hydrazine-Assisted Membrane-Free Hydrogen Production

Jian-Zhong Jiang; Ziyi Liu; Changsheng Chen; Zijian Li; Min Gyu Kim; Chenghao Huang; Haeseong Jang; Xien Liu; Shangguo Liu; Liqiang Hou

doi:10.1002/aenm.202504762

Lattice-Confined Ru Clusters Driving Efficient Hydrazine-Assisted Membrane-Free Hydrogen Production

Jian-Zhong Jiang (Co-first Author)
, Ziyi Liu (Co-first Author)
, Changsheng Chen (Co-first Author)
, Zijian Li^*
, Min Gyu Kim
, Chenghao Huang
, Haeseong Jang^*
, Xien Liu^*
, Shangguo Liu^*
, Liqiang Hou^*

^*Corresponding author for this work

Department of Chemistry

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

12 Citations (Scopus)

Abstract

The inherent trade-off between stable anchoring of metal clusters and sufficient exposure of active sites in supported metal catalysts critically limits their electrocatalytic efficiency. This study overcomes this limitation by synthesizing Ru clusters partially confined within the SnO₂ lattice (Ru@SnO₂) via a molten salt-assisted approach. This unique structure synergistically integrates strong metal-support interaction (SMSI) with high active site exposure. The resulting catalyst exhibits exceptional bifunctional activity in alkaline media, achieving remarkably low overpotentials of 9 mV for the hydrogen evolution reaction (HER) and −82 mV for the hydrazine oxidation reaction (HzOR) at 10 mA cm⁻². A two-electrode system utilizing this catalyst demonstrated stable operation for 1000 h. Integrated into a membrane-free electrolysis (MFE) system for HzOR-assisted hydrogen production, it requires only 0.877 V to deliver 1.0 A cm⁻², achieving a substantial 67.8% energy saving compared to conventional anion exchange membrane (AEM) electrolyzers (2.726 V). Theoretical studies reveal that lattice confinement downshifts the Ru d-band center to optimize hydrogen adsorption energy. A pronounced work function difference generates a built-in electric field that accelerates water dissociation, while an end-on bidentate N₂H₄ adsorption configuration enhances HzOR activation efficiency. © 2025 Wiley-VCH GmbH.

Original language	English
Article number	e04762
Number of pages	12
Journal	Advanced Energy Materials
Volume	16
Issue number	1
Online published	19 Nov 2025
DOIs	https://doi.org/10.1002/aenm.202504762
Publication status	Published - 7 Jan 2026

Funding

J.Z.J., Z.L., and C.C. contributed equally to this work. The authors grate-fully acknowledge the ﬁnancial support from the National Natural Sci-ence Foundation of China (22402098, 22372088, 22402099, 52371165,and 12275237), the Advanced Materials-National Science and Technol-ogy Major Project (2025ZD0617300), the Natural Science Foundation of Shandong Province of China (ZR2022QB100 and ZR2022QB163), Mate-rials/Parts Technology Development Program (RS-2024-00432627), Nano& Material Technology Development Program (RS-2025-25441577), and the Department of Science and Technology of Fuzhou city (2024-Y-017,2024-SG-003, and 2024-SG-004).

UN SDGs

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

SDG 7 Affordable and Clean Energy

Research Keywords

hydrazine oxidation
hydrogen evolution
lattice confinement
membrane-free electrolysis
theoretical calculation

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title = "Lattice-Confined Ru Clusters Driving Efficient Hydrazine-Assisted Membrane-Free Hydrogen Production",

abstract = "The inherent trade-off between stable anchoring of metal clusters and sufficient exposure of active sites in supported metal catalysts critically limits their electrocatalytic efficiency. This study overcomes this limitation by synthesizing Ru clusters partially confined within the SnO2 lattice (Ru@SnO2) via a molten salt-assisted approach. This unique structure synergistically integrates strong metal-support interaction (SMSI) with high active site exposure. The resulting catalyst exhibits exceptional bifunctional activity in alkaline media, achieving remarkably low overpotentials of 9 mV for the hydrogen evolution reaction (HER) and −82 mV for the hydrazine oxidation reaction (HzOR) at 10 mA cm−2. A two-electrode system utilizing this catalyst demonstrated stable operation for 1000 h. Integrated into a membrane-free electrolysis (MFE) system for HzOR-assisted hydrogen production, it requires only 0.877 V to deliver 1.0 A cm−2, achieving a substantial 67.8\% energy saving compared to conventional anion exchange membrane (AEM) electrolyzers (2.726 V). Theoretical studies reveal that lattice confinement downshifts the Ru d-band center to optimize hydrogen adsorption energy. A pronounced work function difference generates a built-in electric field that accelerates water dissociation, while an end-on bidentate N2H4 adsorption configuration enhances HzOR activation efficiency. {\textcopyright} 2025 Wiley-VCH GmbH.",

keywords = "hydrazine oxidation, hydrogen evolution, lattice confinement, membrane-free electrolysis, theoretical calculation",

author = "Jian-Zhong Jiang and Ziyi Liu and Changsheng Chen and Zijian Li and Kim, \{Min Gyu\} and Chenghao Huang and Haeseong Jang and Xien Liu and Shangguo Liu and Liqiang Hou",

year = "2026",

month = jan,

day = "7",

doi = "10.1002/aenm.202504762",

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Lattice-Confined Ru Clusters Driving Efficient Hydrazine-Assisted Membrane-Free Hydrogen Production. / Jiang, Jian-Zhong (Co-first Author); Liu, Ziyi (Co-first Author); Chen, Changsheng (Co-first Author) et al.
In: Advanced Energy Materials, Vol. 16, No. 1, e04762, 07.01.2026.

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

TY - JOUR

T1 - Lattice-Confined Ru Clusters Driving Efficient Hydrazine-Assisted Membrane-Free Hydrogen Production

AU - Jiang, Jian-Zhong

AU - Liu, Ziyi

AU - Chen, Changsheng

AU - Li, Zijian

AU - Kim, Min Gyu

AU - Huang, Chenghao

AU - Jang, Haeseong

AU - Liu, Xien

AU - Liu, Shangguo

AU - Hou, Liqiang

PY - 2026/1/7

Y1 - 2026/1/7

N2 - The inherent trade-off between stable anchoring of metal clusters and sufficient exposure of active sites in supported metal catalysts critically limits their electrocatalytic efficiency. This study overcomes this limitation by synthesizing Ru clusters partially confined within the SnO2 lattice (Ru@SnO2) via a molten salt-assisted approach. This unique structure synergistically integrates strong metal-support interaction (SMSI) with high active site exposure. The resulting catalyst exhibits exceptional bifunctional activity in alkaline media, achieving remarkably low overpotentials of 9 mV for the hydrogen evolution reaction (HER) and −82 mV for the hydrazine oxidation reaction (HzOR) at 10 mA cm−2. A two-electrode system utilizing this catalyst demonstrated stable operation for 1000 h. Integrated into a membrane-free electrolysis (MFE) system for HzOR-assisted hydrogen production, it requires only 0.877 V to deliver 1.0 A cm−2, achieving a substantial 67.8% energy saving compared to conventional anion exchange membrane (AEM) electrolyzers (2.726 V). Theoretical studies reveal that lattice confinement downshifts the Ru d-band center to optimize hydrogen adsorption energy. A pronounced work function difference generates a built-in electric field that accelerates water dissociation, while an end-on bidentate N2H4 adsorption configuration enhances HzOR activation efficiency. © 2025 Wiley-VCH GmbH.

AB - The inherent trade-off between stable anchoring of metal clusters and sufficient exposure of active sites in supported metal catalysts critically limits their electrocatalytic efficiency. This study overcomes this limitation by synthesizing Ru clusters partially confined within the SnO2 lattice (Ru@SnO2) via a molten salt-assisted approach. This unique structure synergistically integrates strong metal-support interaction (SMSI) with high active site exposure. The resulting catalyst exhibits exceptional bifunctional activity in alkaline media, achieving remarkably low overpotentials of 9 mV for the hydrogen evolution reaction (HER) and −82 mV for the hydrazine oxidation reaction (HzOR) at 10 mA cm−2. A two-electrode system utilizing this catalyst demonstrated stable operation for 1000 h. Integrated into a membrane-free electrolysis (MFE) system for HzOR-assisted hydrogen production, it requires only 0.877 V to deliver 1.0 A cm−2, achieving a substantial 67.8% energy saving compared to conventional anion exchange membrane (AEM) electrolyzers (2.726 V). Theoretical studies reveal that lattice confinement downshifts the Ru d-band center to optimize hydrogen adsorption energy. A pronounced work function difference generates a built-in electric field that accelerates water dissociation, while an end-on bidentate N2H4 adsorption configuration enhances HzOR activation efficiency. © 2025 Wiley-VCH GmbH.

KW - hydrazine oxidation

KW - hydrogen evolution

KW - lattice confinement

KW - membrane-free electrolysis

KW - theoretical calculation

UR - https://www.scopus.com/pages/publications/105022243129

UR - https://www.scopus.com/pages/publications/105022243129#tab=impact

U2 - 10.1002/aenm.202504762

DO - 10.1002/aenm.202504762

M3 - RGC 21 - Publication in refereed journal

SN - 1614-6832

VL - 16

JO - Advanced Energy Materials

JF - Advanced Energy Materials

IS - 1

M1 - e04762

ER -

Lattice-Confined Ru Clusters Driving Efficient Hydrazine-Assisted Membrane-Free Hydrogen Production

Abstract

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Research Keywords

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