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

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

doi:10.1002/anie.202300873

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

Journal Article · Wed Mar 08 00:00:00 EST 2023 · Angewandte Chemie (International Edition)

DOI:https://doi.org/10.1002/anie.202300873· OSTI ID:2404998

Cai, Chao ^[1]; Liu, Kang ^[1]; Zhang, Long ^[1]; Li, Fangbiao ^[1]; Tan, Yao ^[1]; Li, Pengcheng ^[1]; Wang, Yanqiu ^[1]; Wang, Maoyu ^[2]; Feng, Zhenxing ^[3]; Motta Meira, Debora ^[4]; Qu, Wenqiang ^[5]; Stefancu, Andrei ^[6]; Li, Wenzhang ^[1]; Li, Hongmei ^[7]; Fu, Junwei ^[1]; Wang, Hui ^[1]; ^[5]; ^[6]; ^[1]

Central South University, Changsha (China)
Oregon State Univ., Corvallis, OR (United States); Argonne National Laboratory (ANL), Argonne, IL (United States). Advanced Photon Source (APS)
Oregon State Univ., Corvallis, OR (United States)
Argonne National Laboratory (ANL), Argonne, IL (United States). Advanced Photon Source (APS)
Univ. of Shanghai (China)
Ludwig Maximilian University of Munich (Germany)
Central South University, Changsha (China); Ludwig Maximilian University of Munich (Germany)

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.

View Accepted Manuscript (DOE)

Research Organization:: Argonne National Laboratory (ANL), Argonne, IL (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities (SUF)

Grant/Contract Number:: AC02-06CH11357

OSTI ID:: 2404998

Journal Information:: Angewandte Chemie (International Edition), Journal Name: Angewandte Chemie (International Edition) Journal Issue: 26 Vol. 62; ISSN 1433-7851

Publisher:: WileyCopyright Statement

Country of Publication:: United States

Language:: English

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Related Subjects

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
alkaline HER
atomic charge distribution
interfacial water orientation
single-atom site
water dissociation

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

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