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

被引：158

作者：

Cai, Chao ^{[1
]}

Liu, Kang ^{[1
]}

Zhang, Long ^{[1
]}

Li, Fangbiao ^{[1
]}

Tan, Yao ^{[1
]}

Li, Pengcheng ^{[1
]}

Wang, Yanqiu ^{[2
]}

Wang, Maoyu ^{[3
,4
]}

Feng, Zhenxing ^{[3
]}

Motta Meira, Debora ^{[4
]}

Qu, Wenqiang ^{[5
]}

Stefancu, Andrei ^{[6
]}

Li, Wenzhang ^{[2
]}

Li, Hongmei ^{[1
,6
]}

Fu, Junwei ^{[1
]}

Wang, Hui ^{[1
]}

Zhang, Dengsong ^{[5
]}

Cortes, Emiliano ^{[6
]}

Liu, Min ^{[1
]}

机构：

[1] Cent South Univ, Hunan Joint Int Res Ctr Carbon Dioxide Resource U, Sch Phys & Elect, Changsha 410083, Hunan, Peoples R China

[2] Cent South Univ, Sch Chem & Chem Engn, Changsha 410083, Hunan, Peoples R China

[3] Oregon State Univ, Sch Chem Biol & Environm Engn, Corvallis, OR 97331 USA

[4] Argonne Natl Lab, Xray Sci Div, Adv Photon Source, Argonne, IL 60439 USA

[5] Shanghai Univ, Coll Sci, Res Ctr Nanosci & Technol, Dept Chem,Int Joint Lab Catalyt Chem, Shanghai 200444, Peoples R China

[6] Ludwig Maximilians Univ Munchen, Fak Phys, Nanoinst Munchen, D-80539 Munich, Germany

来源：

ANGEWANDTE CHEMIE-INTERNATIONAL EDITION | 2023年 / 62卷 / 26期

关键词：

Alkaline HER; Atomic Charge Distribution; Interfacial Water Orientation; Single-Atom Site; Water Dissociation; SPECTROSCOPY; IR;

D O I：

10.1002/anie.202300873

中图分类号：

O6 [化学];

学科分类号：

0703 ;

摘要：

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 4.00x10(10) 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.

引用

页数：7

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