Real-time Characterization of the Fine Structure and Dynamics of an Electrical Double Layer at Electrode-electrolyte Interfaces

Zhang, Yanyan; Tang, Jilin; Ni, Zhigang; Zhao, Yao; Jia, Feifei; Luo, Qun; Mao, Lanqun; Zhu, Zihua; Wang, Fuyi

doi:10.1021/acs.jpclett.1c01134

Real-time Characterization of the Fine Structure and Dynamics of an Electrical Double Layer at Electrode-electrolyte Interfaces

Journal Article · Thu Jun 10 04:00:00 EDT 2021 · The Journal of Physical Chemistry Letters

DOI:https://doi.org/10.1021/acs.jpclett.1c01134· OSTI ID:1814497

Zhang, Yanyan ^[1]; Tang, Jilin ^[2]; Ni, Zhigang ^[3]; Zhao, Yao ^[2]; Jia, Feifei ^[2]; Luo, Qun ^[2]; Mao, Lanqun ^[2]; ^[4]; Wang, Fuyi ^[5]

Institute of Chemistry, Chinese Academy of Sciences
Chinese Academy of Sciences
Hangzhou Normal University
BATTELLE (PACIFIC NW LAB)
CHINESE ACADEMY OF SCIENCES

The chemisorption of species from supporting electrolytes on electrode surfaces is ubiquitous in electrochemical systems and affects the dynamics and mechanism of various electrochemical reactions. The understanding of chemical structure and property of the resulting electrical double layer is vital but limited. In this work, we operando probed the electrochemical interface between a gold electrode surface and a common supporting electrolyte, phosphate buffer, using our newly developed in situ liquid secondary ion mass spectrometry. We surprisingly found that on the positively charged gold electrode surface sodium cations were anchored in the stern layer in a partially dehydrated form by formation of compact ion pairs with the accumulated phosphate anions. The resulting strong and dense adsorption phase was further revealed to retard the electro-oxidation reaction of ascorbate. This finding addressed one major gap in the fundamental science of electrode-electrolyte interfaces that where and how the cations reside in the double layer to impose effects on electrochemical reactions, providing insights into engineering of better electrode-electrolyte interfaces in electrochemical processes.

Research Organization:: Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)

Sponsoring Organization:: USDOE

DOE Contract Number:: AC05-76RL01830

OSTI ID:: 1814497

Report Number(s):: PNNL-SA-162872

Journal Information:: The Journal of Physical Chemistry Letters, Journal Name: The Journal of Physical Chemistry Letters Journal Issue: 22 Vol. 12

Country of Publication:: United States

Language:: English

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