Modeling Electrochemical Energy Storage at the Atomic Scale

151 Pages·2018·11.017 MB·English

by  Martin Korth

Topics in Current Chemistry Collections
Martin Korth E ditor
Modeling
Electrochemical
Energy Storage
at the Atomic
Scale
Topics in Current Chemistry Collections
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Moreinformationaboutthisseriesathttp://www.springer.com/series/14181
Martin Korth
Editor
Modeling Electrochemical
Energy Storage
at the Atomic Scale
With contributions from
Isidora Cekic-Laskovic • Mangesh I. Chaudhari • Axel Groß
Johannes Kasnatscheew • Abhishek Khetan • Dilip Krishnamurthy
Ajay Muralidharan • Kristin A. Persson • Lawrence R. Pratt
Xiaohui Qu • Nav Nidhi Rajput • Susan B. Rempe • Trevor J. Seguin
Venkatasubramanian Viswanathan • Ralf Wagner • Martin Winter
Brandon M. Wood
Editor
Martin Korth
Molecular Projects UG
Münster, Germany

Partly previously published in Top Curr Chem (Z) Volume 376 (2018)

ISSN 2367-4067
Topics in Current Chemistry Collections
ISBN 978-3-030-00592-4

Library of Congress Control Number: 2018957348

© Springer Nature Switzerland AG 2018
The chapters “Assessment of Simple Models for Molecular Simulation of Ethylene Carbonate and
Propylene Carbonate as Solvents for Electrolyte Solutions” and “Elucidating Solvation Structures for
Rational Design of Multivalent Electrolytes—A Review” are licensed under the terms of the Creative
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Contents

Preface ................................................................................................................... vii

Fundamental Challenges for Modeling Electrochemical Energy
Storage Systems at the Atomic Scale ................................................................. 1
Axel Groß: Top Curr Chem (Z) 2018, 2018:17 (23, April 2018)
https://doi.org/10.1007/s41061-018-0194-3

Interfaces and Materials in Lithium Ion Batteries: Challenges
for Theoretical Electrochemistry ....................................................................... 23
Johannes Kasnatscheew, Ralf Wagner, Martin Winter
and Isidora Cekic-Laskovic: Top Curr Chem (Z) 2018, 2018:16
(18, April 2018) https://doi.org/10.1007/s41061-018-0196-1

Assessment of Simple Models for Molecular Simulation
of Ethylene Carbonate and Propylene Carbonate as Solvents
for Electrolyte Solutions ...................................................................................... 5 3
Mangesh I. Chaudhari, Ajay Muralidharan, Lawrence R. Pratt
and Susan B. Rempe: Top Curr Chem (Z) 2018, 2018:7
(12, February 2018) https://doi.org/10.1007/s41061-018-0187-2

Elucidating Solvation Structures for Rational Design
of Multivalent Electrolytes—A Review ............................................................. 79
Nav Nidhi Rajput, Trevor J. Seguin, Brandon M. Wood, Xiaohui Qu
and Kristin A. Persson: Top Curr Chem (Z) 2018, 2018:19
(26, April 2018) https://doi.org/10.1007/s41061-018-0195-2

Towards Synergistic Electrode–Electrolyte Design Principles
for Nonaqueous Li–O batteries ......................................................................... 125
2
Abhishek Khetan, Dilip Krishnamurthy
and Venkatasubramanian Viswanathan: Top Curr Chem (Z) 2018,
2018:11 (20, March 2018) https://doi.org/10.1007/s41061-018-0188-1
v
Preface

It has become apparent that electrochemical energy storage is going to play a
central role for our energy future. Current storage devices are unfortunately not yet
as safe, cheap and efficient as we would need them to be for a quick exit from fossil
fuels. Fortunately, tremendous efforts are made both experimentally and more
recently also theoretically to understand the above mentioned problems in detail
and to work on economically viable solutions or alternatives. The challenges cannot
be overlooked, especially on the theoretical side. While more and more substances
are coming into consideration as possible electrode or electrolyte materials,
knowledge about the basic storage processes is still very limited. The complexity of
real materials is causing great problems here, but also the fact that there is no
generally applicable, black-box computational model available to treat physical
systems at the atomic scale under electrochemical conditions, i.e., including the
effect of electrolytes and electrode potentials. It has nevertheless become clear that
such methods and the knowledge we could gain from them are key for innovating
electrochemical energy storage, as any rational design of essentially redox-based
devices will require a quantum-mechanical understanding of atomic-scale structures
and reactivity.
With this publication, we present studies from five research teams who dare to
venture into the unknown of electrochemical energy storage at the atomic scale.
We start with Groß, who discusses the technical obstacles we face when applying
computational methods and especially those from quantum chemistry to electro-
chemical energy storage systems.
The second contribution gives the complementary view from a leading experi-
mental group with a focus on current battery technology and a discussion of where
help from modeling and simulation would be most welcome.
Rempe and co-workers then give us a classical mechanics view of electrolytes,
b efore Rajput et al. Persson review the current state of investigations into complex
(here multivalent) electrolytes, where theory can at least help to understand and
organize contradictory experimental results.
vii
Preface
We finish with Viswanathan and co-workers, who show us how to build a bridge
from theory to experiment with the development of design principles for new device
types (here Lithium-Oxygen batteries), keeping both electrodes and electrolyte
features in mind.
We hope that the presented contributions inspire more theoreticians to turn at
least part-time to theoretical electrochemistry, not only because of the great
importance it has for societies around the globe, but also for the intellectual
challenges it poses and last but not least for the fun of it. We also hope to have
convinced one or the other experimentalist of the value of atomic-scale theoretical
investigations into electrochemical experiments. For having made this a possibility,
we would like to thank all authors for their valuable contributions.

Dr. Martin Korth
Molecular Projects UG, Münster, Germany
viii
Top Curr Chem (Z) (2018) 376:17
https://doi.org/10.1007/s41061-018-0194-3
REVIEW
Fundamental Challenges for Modeling Electrochemical
Energy Storage Systems at the Atomic Scale
Axel Groß1,2
Received: 26 April 2017 / Accepted: 23 March 2018 / Published online: 23 April 2018
© Springer International Publishing AG, part of Springer Nature 2018
Abstract There is a strong need to improve the efficiency of electrochemical
energy storage, but progress is hampered by significant technological and scientific
challenges. This review describes the potential contribution of atomic-scale mod-
eling to the development of more efficient batteries, with a particular focus on first-
principles electronic structure calculations. Numerical and theoretical obstacles
are discussed, along with ways to overcome them, and some recent examples are
presented illustrating the insights into electrochemical energy storage that can be
gained from quantum chemical studies.
Keywords Computer simulations · Density functional theory calculations ·
Electrochemical energy storage · Batteries · Electrode–electrolyte interfaces
1 Introduction
There is in principle no need to emphasize the important role of energy storage
in the context of the energy transition towards renewable energy based on, e.g.,
solar or wind power. As these resources are volatile and not necessarily available
when they are needed, they must be efficiently stored. Furthermore, there is also
Chapter 1 was originally published as Groß, A. Top Curr Chem (Z) (2018) 376: 17. https://doi.org/10.1007/
s41061-018-0194-3.
*
Axel Groß
[email protected]
1 Helmholtz Institute Ulm (HIU) Electrochemical Energy Storage, Helmholtzstrasse 11,
89069 Ulm, Germany
2 Institute of Theoretical Chemistry, Ulm University, Albert-Einstein-Allee 11, 89069 Ulm,
Germany
Reprinted from the journal 1 1 3
Top Curr Chem (Z) (2018) 376:17
a tremendous demand for energy storage in mobile devices and applications. One
of the most efficient energy carriers is the chemical bond [1]. Chemical energy
can be stored either in fuels or in batteries.
Here we focus on the electrochemical energy storage in rechargeable batteries.
There has been enormous technological progress in improving the efficiency and
storage capacity of batteries. The widespread use of mobile devices such as cel-
lular phones or laptops would not have been possible without this progress, which
is mainly due to advances in Li–ion battery technology [2, 3]. Still, the specific
energy of today’s batteries is not sufficient to enable car driving distances compa-
rable to those of combustion energy-driven vehicles [4]. In addition, the incidents
related to short circuit induced thermal runaway failures in Li–ion batteries [5]
raises concerns about safety issues. Furthermore, global lithium resources are
limited [6], which might be addressed by developing battery chemistries based on
other charge carriers. Hence there is certainly a strong need for further improve-
ments in battery technology, even in a disruptive sense.
In spite of these technological challenges, our knowledge about the atomis-
tic structures and processes in devices for electrochemical energy storage is
still rather limited [2]. This is because it is difficult to atomically observe and
resolve these structures and processes in situ under operating conditions. Here,
a close collaboration between experiment and theory could help. However, the
theoretical description of batteries also faces severe problems, as structures and
processes from the atomistic level up to the macroscopic level need to be under-
stood, which calls for a multiscale approach. In particular, the interfaces between
the electrodes and the electrolytes are often very poorly characterized, because
experimental tools with atomic resolution often do not work at these interfaces.
Any theoretical structure determination is nearly impossible without experimen-
tal information as input [7, 8]. In addition, the microscopic description of liq-
uid electrolytes in principle requires performing statistically demanding averages
over many possible structures [9–11].
All these obstacles to an appropriate and realistic theoretical description of
electrochemical energy storage systems are very discouraging. Yet, there are
rewarding incentives to start such an effort. This field is of the highest techno-
logical and societal relevance, but there are also interesting scientific questions
that need to be addressed. And indeed, significant progress has already been
made with respect to the atomistic description of processes and structures in
batteries [12].
In this review, I will address the fundamental challenges associated with mod-
eling electrochemical energy storage systems at the atomic scale. Rather than giv-
ing a comprehensive overview of existing work in this field, I will instead focus on
particular problems that characterize the challenges, but also the possibilities, in the
theoretical description of batteries. First I will briefly reiterate the basic principles of
battery operation which sets the stage for any theoretical and numerical modeling. I
will then describe the appropriate theoretical methods that are needed for a reliable
description of structures and processes in batteries. In the main part of this  review, I
will illustrate the issues in batteries that can and cannot be addressed at the moment
with state-of-the-art theoretical methods.
1 3 2 Reprinted from the journal