Structural Basis of Ultralow Capacitances at Metal–Nonaqueous Solution Interfaces
Journal of the American Chemical Society, vol. 147, pp. 4060–4068
Abstract
Metal-nonaqueous solution interfaces, a key to many electrochemical technologies, including lithium metal batteries, are much less understood than their aqueous counterparts. Herein, on several metal-nonaqueous solution interfaces, we observe capacitances that are 2 orders of magnitude lower than the usual double-layer capacitance. Combining electrochemical impedance spectroscopy, atomic force microscopy, and physical modeling, we ascribe the ultralow capacitance to an interfacial layer of 10-100 nm above the metal surface. This nanometric layer has a Young's modulus around 2 MPa, which is much softer than typical solid-electrolyte interphase films. In addition, its AC ionic conductivity is 4-to-5 orders of magnitude lower than that of the bulk electrolyte. The temperature dependencies of the AC ionic conductivity and thickness suggest that the soft layer is formed from metal-mediated, dipole-dipole interactions of the nonaqueous solvent molecules. The observed soft layer opens new avenues of modulating battery performance via rational design of ion transport, (de)solvation, and charge transfer in this interfacial region.
Authors 9
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Nanjing Tech University · State Key Laboratory of Materials-Oriented Chemical Engineering
Affiliation as printed
Nanjing Tech University
State Key Laboratory of Materials-Oriented Chemical Engineering, College of Chemical Engineering
State Key Laboratory of Materials-Oriented Chemical Engineering, College of Chemical Engineering, Nanjing Tech University, Nanjing 211816, China
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Affiliation as printed
IET-3: Theory and Computation of Energy Materials, Forschungszentrum Jülich GmbH
Institute of Energy Technologies
Institute of Energy Technologies, IET-3: Theory and Computation of Energy Materials, Forschungszentrum Jülich GmbH, Jülich 52425, Germany
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Affiliation as printed
State Key Laboratory of Physical Chemistry of Solid Surfaces and College of Chemistry and Chemical Engineering
Xiamen University
State Key Laboratory of Physical Chemistry of Solid Surfaces and College of Chemistry and Chemical Engineering, Xiamen University, Xiamen 361005, China
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Affiliation as printed
IET-3: Theory and Computation of Energy Materials, Forschungszentrum Jülich GmbH
Institute of Energy Technologies
Institute of Energy Technologies, IET-3: Theory and Computation of Energy Materials, Forschungszentrum Jülich GmbH, Jülich 52425, Germany
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Nanjing Tech University · State Key Laboratory of Materials-Oriented Chemical Engineering
Affiliation as printed
Nanjing Tech University
State Key Laboratory of Materials-Oriented Chemical Engineering, College of Chemical Engineering
State Key Laboratory of Materials-Oriented Chemical Engineering, College of Chemical Engineering, Nanjing Tech University, Nanjing 211816, China
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Nanjing Tech University · State Key Laboratory of Materials-Oriented Chemical Engineering · Southeast University
Affiliation as printed
Key Laboratory of Energy Thermal Conversion and Control of Ministry of Education, School of Energy and Environment
Nanjing Tech University
Southeast University
State Key Laboratory of Materials-Oriented Chemical Engineering, College of Chemical Engineering
Key Laboratory of Energy Thermal Conversion and Control of Ministry of Education, School of Energy and Environment, Southeast University, Nanjing 210096, P. R. China
State Key Laboratory of Materials-Oriented Chemical Engineering, College of Chemical Engineering, Nanjing Tech University, Nanjing 211816, China
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Jiawei Yan corresponding
Affiliation as printed
State Key Laboratory of Physical Chemistry of Solid Surfaces and College of Chemistry and Chemical Engineering
Xiamen University
State Key Laboratory of Physical Chemistry of Solid Surfaces and College of Chemistry and Chemical Engineering, Xiamen University, Xiamen 361005, China
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Jun Zh. Huang corresponding Aachen Theory of Electrocatalytic Interfaces Faculty of Georesources and Materials Engineering
RWTH Aachen University · Forschungszentrum Jülich
Affiliation as printed
IET-3: Theory and Computation of Energy Materials, Forschungszentrum Jülich GmbH
Institute of Energy Technologies
RWTH Aachen University
Theory of Electrocatalytic Interfaces, Faculty of Georesources and Materials Engineering
Institute of Energy Technologies, IET-3: Theory and Computation of Energy Materials, Forschungszentrum Jülich GmbH, Jülich 52425, Germany
Theory of Electrocatalytic Interfaces, Faculty of Georesources and Materials Engineering, RWTH Aachen University, Aachen 52062, Germany
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Yuhui Chen corresponding
Nanjing Tech University · State Key Laboratory of Materials-Oriented Chemical Engineering
Affiliation as printed
Nanjing Tech University
State Key Laboratory of Materials-Oriented Chemical Engineering, College of Chemical Engineering
State Key Laboratory of Materials-Oriented Chemical Engineering, College of Chemical Engineering, Nanjing Tech University, Nanjing 211816, China
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