Plasmon-Driven Reorientation of Interfacial Water for Wastewater Electrolysis with Light-Emitting Diode Illumination
Journal
Advanced Science
ISSN
2198-3844
2198-3844
Date Issued
2025-06-25
Author(s)
Che Mohamad, Nur Aqlili Riana
Chae, Kyunghee
Zhou, Qiang
Huang, Wen‐Tse
Lee, Hyun Jeong
Son, Jaehyun
Moon, Jooho
Bu, Yunfei
Gong, Feng
Kim, Jeongwon
Kim, Dong Ha
Abstract
Regulating the orientation and dynamics of interfacial water is essential for optimizing electrocatalytic reactions, yet it remains challenging due to its intrinsic disorder. Here, it is demonstrated that localized surface plasmon resonance (LSPR) on an Ir single-atom Au catalyst actively restructures the hydrogen-bond (HB) network, accelerating ammonia oxidation reaction kinetics. In situ Raman spectroscopy and density functional theory calculations reveal that plasmonic excitation shifts the HB network toward a more flexible configuration, favoring the formation of three-coordinated hydrogen-bonded water (3HB·H2O) while suppressing cation-associated species (K+·H2O). This transformation enhances the dehydrogenation process and stabilizes reaction intermediates, leading to a 28% increase in NH3 oxidation kinetics. Operando X-ray absorption spectroscopy further confirms that LSPR-driven polarization at the Ir active site compresses the Ir─O bond from 1.73 to ≈1.58 Å by generating electron vacancies, thereby accelerating deprotonation with *OH during oxidative electrolysis. Extending this principle to an LED-driven plasmon-assisted symmetric wastewater electrolyzer, achieving a 40-fold current enhancement and 94% ammonia removal efficiency over 120 h at 1 V under landfill leachate-like conditions.
Subjects
ammonia oxidation reaction
LED illumination
plasmonic
single atom
symmetric electrolyzer
Publisher
Wiley
Type
journal article