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

The slow water dissociation process in alkaline electrolyte severely limits the kinetics of HER. The orientation of H2O is well known to affect the dissociation process, but H2O orientation is hard to control because of its random distribution. Herein, an atomically asymmetric local electric field w...

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Bibliographic Details
Published in:Angewandte Chemie International Edition 2023-06, Vol.62 (26), p.e202300873-n/a
Main Authors: Cai, Chao, Liu, Kang, Zhang, Long, Li, Fangbiao, Tan, Yao, Li, Pengcheng, Wang, Yanqiu, Wang, Maoyu, Feng, Zhenxing, Motta Meira, Debora, Qu, Wenqiang, Stefancu, Andrei, Li, Wenzhang, Li, Hongmei, Fu, Junwei, Wang, Hui, Zhang, Dengsong, Cortés, Emiliano, Liu, Min
Format: Article
Language:English
Subjects:
Adsorption
Alkaline HER
Atomic Charge Distribution
Electric fields
Electricity
Hydrogen
Hydrogen bonds
Hydrogen evolution reactions
INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
Interfacial Water Orientation
Kinetics
Molecular dynamics
Orientation
Raman spectroscopy
Single-Atom Site
Skewed distributions
Water
Water Dissociation
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Summary:The slow water dissociation process in alkaline electrolyte severely limits the kinetics of HER. The orientation of H2O is well known to affect the dissociation process, but H2O 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 H2O adsorption configuration and orientation, thus optimizing its dissociation process. The electric field intensity of IrRu DSACs is over 4.00×1010 N/C. The ab initio molecular dynamics simulations combined with in situ Raman spectroscopy analysis on the adsorption behavior of H2O 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. Breaking the periodic surface of catalysts by the inclusion of single atoms can help building atomic electric fields that highly promote the hydrogen evolution reaction activity. We show here that this is achieved by modulating the interfacial water orientation and by subsequently decreasing the active sites‐hydrogen distance.
ISSN:1433-7851
1521-3773
DOI:10.1002/anie.202300873