Journal of the American Chemical Society· 2025Q1
Lignin-Directed Construction of Vertical Ru/RuO 2 Electron–Bridge Interfaces for Low-Input Self-Powered Hydrazine-Water Splitting
- 85citations
- Q1SCImago
- 2025year
Short summary
A novel Ru/RuO2@HLC catalyst, constructed using lignin to direct Ru/RuO2 heterojunction formation within a carbon matrix, achieves a hydrogen evolution reaction (HER) current density of 50 mA cm–2 at a low 12 mV overpotential, surpassing commercial Pt/C and enabling self-powered hydrazine splitting with a cell voltage of only 0.14 V at 100 mA cm–2.
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Key points
- Lignin chelates with Ru3+ to direct the formation of Ru/RuO2 heterojunctions within a hierarchical lignin-derived carbon (HLC) matrix.
- A dynamic dual-center (DDC) electron bridge interface (Ru4+–O–Ru0) facilitates charge injection and lowers the free-energy barrier for hydrogen production.
- The Ru/RuO2@HLC catalyst achieves 50 mA cm–2 HER current density at 12 mV overpotential, outperforming Pt/C.
- Replacing oxygen evolution with hydrazine oxidation reduces the cell voltage to 0.14 V at 100 mA cm–2 for hydrazine splitting.
AI-generated from the title and abstract; the full text is not read.
Abstract
Hydrazine oxidation reaction (HzOR) has emerged as a promising anodic alternative to the oxygen evolution reaction (OER) for efficient hydrogen production. Nevertheless, two-electrode electrolyzers demand substantial cell voltages and uninterrupted external power, curbing scalable implementation. Herein, hydrothermally activated lignin chelates with Ru 3+ to direct the in situ formation of Ru/RuO 2 heterojunctions that, upon pyrolysis, are embedded within a hierarchical lignin-derived carbon (HLC) matrix to yield the Ru/RuO 2 @HLC catalyst. Combined spectroscopy and DFT calculation uncover a dynamic dual-center (DDC) at the interface: a Ru 4+ –O–Ru 0 electron bridge injects charge into RuO 2, while adjacent Ru undergoes reversible partial oxidation (Ru 0 ↔ Ru 3+ ) under bias. This DDC slightly elongates Ru–O and compresses Ru–Ru, enriches lattice oxygen, accelerates interfacial charge transfer, lowers the free-energy barrier of the rate-limiting *2NH → *2N step to 1.31 eV, and suppresses high-valence Ru dissolution. In 1.0 M KOH electrolyte, the as-prepared Ru/RuO 2 @HLC catalyst achieves a hydrogen evolution reaction (HER) current density of 50 mA cm –2 at an exceptionally low overpotential of 12 mV and surpasses commercial Pt/C. Replacing OER with HzOR significantly reduces the cell voltage to only 0.14 V at 100 mA cm –2 . A paired direct hydrazine fuel cell and an integrated overall hydrazine splitting deliver 2.32 mmol h –1 of hydrogen at approximately 100% Faradaic efficiency, representing one of the highest hydrogen production rates reported to date for self-powered hydrazine systems. This work provides a scalable platform for waste-to-hydrogen conversion and highlights the potential of renewable biomass ligands for constructing high-performance interfacial electrocatalysts.
The authors' abstract, as published at the source. Journal of the American Chemical Society, 2025 · DOI ↗
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Field: Renewable Energy, Sustainability and the Environment
Renewable Energy, Sustainability and the EnvironmentEnergy