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Atomically Local Electric Field Induced Interface Water Reorientation for Alkaline Hydrogen Evolution Reaction

Chao Cai, Kang Liu, Long Zhang, Fangbiao Li, Yao Tan, Pengcheng Li, Yanqiu Wang, Maoyu Wang, Zhenxing Feng, Debora Meira, Wenqiang Qu, Andrei Ştefancu, Wenzhang Li, Hongmei Li, Junwei Fu, Hui Wang, Dengsong Zhang, Emiliano Cortés, Min Liu

2023Angewandte Chemie37 citationsDOIOpen Access PDF

Abstract

Abstract The slow water dissociation process in alkaline electrolyte severely limits the kinetics of HER. The orientation of H 2 O is well known to affect the dissociation process, but H 2 O orientation is hard to control because of its random distribution. Herein, an atomically asymmetric local electric field was designed by IrRu dizygotic single‐atom sites (IrRu DSACs) to tune the H 2 O adsorption configuration and orientation, thus optimizing its dissociation process. The electric field intensity of IrRu DSACs is over 4.00×10 10 N/C. The ab initio molecular dynamics simulations combined with in situ Raman spectroscopy analysis on the adsorption behavior of H 2 O show that the M−H bond length (M=active site) is shortened at the interface due to the strong local electric field gradient and the optimized water orientation promotes the dissociation process of interfacial water. This work provides a new way to explore the role of single atomic sites in alkaline hydrogen evolution reaction.

Topics & Concepts

Dissociation (chemistry)Electric fieldChemistryMolecular dynamicsChemical physicsHydrogenAdsorptionAb initioRaman spectroscopyElectrolytePhysical chemistryComputational chemistryElectrodePhysicsQuantum mechanicsOpticsOrganic chemistryElectrocatalysts for Energy ConversionElectrochemical Analysis and ApplicationsSpectroscopy and Quantum Chemical Studies
Atomically Local Electric Field Induced Interface Water Reorientation for Alkaline Hydrogen Evolution Reaction | Litcius