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- Sprache: Englisch
ELECTROCERAMICS FOR HIGH PERFORMANCE SUPERCAPACITORS The book describes the state-of-the-art analyses of high-density supercapacitors. In the near future, high-energy density materials will be required to accommodate the increased demand for gadgets, hybrid cars, and massive electrical energy storage systems. Fuel cells, supercapacitors, and batteries have the highest energy densities, but traditional capacitors have gained attention for intermittent energy harvesting owing to their high energy transfer rate and quick charging/discharging capability. The large amount of electric breakdown strength and modest remnant polarization are keys to the high energy density in dielectric capacitors. Above 100??C or 212??F, polymer dielectric capacitors become unstable and begin to suffer a dielectric breakdown. Hence, dielectric ceramics are the sole viable option for high-temperature applications. This book provides a basic understanding of dielectric-based energy harvesting. After a detailed analysis of the state-of-the-art, it proceeds to explain the specific strategies to enhance energy storage features, including managing the local structure and phases assembly, raising the dielectric width, and enhancing microstructure and electrical uniformity. Also discussed is the need for novel materials with applications in high-density supercapacitors. Audience The book is designed for engineers, industrialists, physicists, scientists, and researchers who work on the applications of high-density supercapacitors.
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Veröffentlichungsjahr: 2023
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Table of Contents
Cover
Series Page
Title Page
Copyright Page
Preface
1 Lead-Free Energy Storage Ceramics
1.1 Introduction
1.2 Dielectric Capacitor and Energy Storage
1.3 Energy Storage of Dielectric Ceramics Free of Lead
1.4 Conclusion and Outlooks
Acknowledgments
References
2 Lead-Based Ceramics for High-Performance Supercapacitors
2.1 Introduction
2.2 General Idea of Ceramics for Supercapacitors
2.3 Principle Involved in Electroceramics
2.4 Lead-Based Ceramics
2.5 Characteristics of Lead-Based Ceramics
2.6 Conclusion and Perspectives
References
3 Ceramic Films for High-Performance Supercapacitors
3.1 Introduction
3.2 Energy Storage Principles
3.3 Factors Optimizing Energy Density
3.4 Ceramics for Supercapacitors
3.5 Conclusions and Outlook
References
4 Ceramic Multilayers and Films for High-Performance Supercapacitors
4.1 Introduction
4.2 Fundamentals of Energy Storage in Electroceramics
4.3 Important Factors for Maximizing Energy Density
4.4 Different Types of Electroceramics Capacitors for Energy Storage
4.5 Application of Electroceramics Supercapacitor
4.6 Conclusion
References
5 Superconductors for Energy Storage
5.1 Introduction
5.2 Low-Temperature Superconductors
5.3 High-Temperature Superconductors
5.4 Superconductors in Energy Applications
5.5 Conclusion
Acknowledgments
References
6 Key Factors for Optimizing Energy Density in High-Performance Supercapacitors
6.1 Supercapacitor
6.2 Electric Double-Layer Capacitor
6.3 Pseudo-Capacitor
6.4 Hybrid Supercapacitor
6.5 The Energy Density of Supercapacitor
6.6 Future Outlook
6.7 Conclusion
References
7 Optimization of Anti-Ferroelectrics
7.1 Introduction
7.2 Energy Storage Properties
7.3 Antiferroelectric for Energy Storage
7.4 Explosive Energy Conversion
7.5 Energy Storage and High-Power Capacitors
7.6 Thermal-Electric Energy Interconversion
7.7 Optimization
7.8 Conclusion
References
8 Super Capacitive Performance Assessment of Mixed Ferromagnetic Iron and Cobalt Oxides and Their Polymer Composites
8.1 Introduction
8.2 Ferromagnetic Electrode Materials
8.3 Mixed Ferromagnetic Iron and Cobalt Oxides
8.4 Conclusion
References
9 Transition Metal Oxides with Broaden Potential Window for High-Performance Supercapacitors
9.1 Introduction of Transition Metal Oxides (TMOs)
9.2 Redox-Based Materials
9.3 Conducting Polymers
9.4 Electroactive Metal Oxides or Transition Metal Oxides (TMOs) as Electrodes for SCs
9.5 Conclusion
References
10 Aqueous Redox-Active Electrolytes
10.1 Introduction
10.2 Electrolyte Requirements for High-Performance Supercapacitors
10.3 Effect of the Electrolyte on Supercapacitor Performance
10.4 Conclusion and Future Research Directions
References
11 Strategies for Improving Energy Storage Properties
11.1 Introduction
11.2 Result and Discussion
11.3 Energy Storage Systems Applications
11.4 Energy Storage Systems Economics
11.5 Impacts on Environment by Electricity Storage
11.6 Future Prospective
11.7 Conclusion
References
12 State-of-the-Art in Electroceramics for Energy Storage
12.1 Introduction
12.2 Electroceramics for Energy-Storing Devices
12.3 Ceramic Multilayers and Films
12.4 Ceramic Films for Energy Storage in Capacitors
12.5 Conclusion
References
13 Lead-Free Ceramics for High Performance Supercapacitors
13.1 Introduction
13.2 Ceramics
13.3 Types of Ceramic Capacitors
13.4 Overview of Ceramics for Supercapacitors
13.5 Lead-Based Ceramics
13.6 Lead-Free Ceramics
13.7 Comparison of Pb-Based Ceramics and Pb-Free Ceramics
13.8 Conclusion
References
Index
End User License Agreement
List of Illustrations
Chapter 1
Figure 1.1 Polarization of the dielectric material during the process of charging.
Figure 1.2 P-E hysteresis loops and characteristic parameters of (i) linear dielec...
Chapter 2
Figure 2.1 Representation of the electrostatic capacitor.
Chapter 3
Figure 3.1 Application of energy storage capacitors.
Figure 3.2 Schematic of an electrostatic capacitor.
Figure 3.3 Volumetric capacitance of NP V
2
O
3
/MnO
2
electrodes...
Figure 3.4 (a) Scanning electron and (b) Transmission micrographs of NiCo
2
O
4
...
Figure 3.5 CV curves of NiCo
2
O
4
with (a) 0.2 moles of Ce (b) 0.4 moles of...
Figure 3.6 (a) Charge/discharge voltage profile (b) calculated specific capacitance (c) specific...
Chapter 4
Figure 4.1 (a) Applications for energy storage capacitors for power electronics and pulse power...
Figure 4.2 Four individual P−E hysteresis loops and their energy storage characteristics:...
Figure 4.3 W
rec
of 0.2PMN−0.8PS
x
T
1−x
ceramics with...
Figure 4.4 Consequence of Zr/Ti ratio on P−E loops and energy storage properties of PLZT.
Figure 4.5 (a) Unipolar P−E loops under E
max
and (b) calculated W
rec
...
Figure 4.6 Comparison of (a) E
max
vs W
rec
; (b) ΔP vs W
rec
;
Chapter 5
Figure 5.1 Corraletion between Tc, Jc and Bc
2
[15].
Figure 5.2 Bronze powder in the tube and Internal tin processes for fabricating Nb
3
Sn.
Figure 5.3 The layered structure of cuprate based HTS.
Figure 5.4 Phase Diagram of cuprate-based superconductors [reproduced with permission from Ref. 56].
Figure 5.5 Phase diagram of Ba
1-x
K
x
Fe
2
As
2
and Ba (Fe
Figure 5.6 Schematic design of a SMES system.
Figure 5.7 Schematic diagram of the SMES unit with VSC and dc chopper.
Chapter 6
Figure 6.1 Factors affecting storage density of supercapacitor [31].
Figure 6.2 Relationship between Energy storage properties and grain size (a) Grain size vs. E
max
...
Chapter 7
Figure 7.1 The recent interest of researchers in this energy density. “ISI Web of Science” is...
Figure 7.2 A typical loop between electric field and polarization [3].
Chapter 8
Figure 8.1 Working principle of supercapacitor cations (C
+
) and anions (A
-
) in solution.
Chapter 9
Figure 9.1 (a) Measurement of CV at a scan rate of 5 mV s
-1
. (b-c) CV measurements and charging...
Figure 9.2 (a-e) CV of K
+
introduced α-MnO
2
cathode and capacitance...
Figure 9.3 (a, b) CV curves and specific capacitance of Mn
3
O
4
at varying cycling stages....
Figure 9.4 (a-b) At varying scan rates typical CV curves of Fe
3
O
4
@C, (c-d) Charging...
Figure 9.5 (a) Separate potential windows CV curves of Na
0.5
MnO
2
NWAs electrode and
Figure 9.6 Schematic illustration of Na
0.5
MnO
2
//Fe
3
O
4
@C ASC, desc...
Chapter 10
Figure 10.1 Influence of electrolyte nature on various supercapacitor characteristics (reused with permission [27]).
Figure 10.2 Classification of electrolytes for supercapacitors (reused with permission [27]).
Figure 10.3 Ionic dimension and size in water-based electrolytes as obtained by modeling (reused with permission [48]).
Chapter 11
Figure 11.1 The various components of energy storage systems linked with storage applications with dependable electric grid.
Figure 11.2 Interconnectivity and intraconnectivity of energy storage technologies.
Chapter 12
Figure 12.1 (a) dielectric breakdown strengths, (b) hysteresis loops, and (c) energy density and efficiency...
Figure 12.2 Diagram of the processing step of glass-ceramics [28].
Figure 12.3 Contrast of (a) Emax vs Wrec; (b) ΔP vs Wrec; and (c) Wrec vs η for lead-based/lead
Figure 12.4 A series of ceramic multilayers (MLs) fabrication processing steps [37].
Chapter 13
Figure 13.1 General classification of ceramics.
Figure 13.2 (a) Diagram representing construction of multilayer ceramic capacitor. (b) Ceramic disc capacitor...
Figure 13.3 Perovskite structure of (a) cubic and (b) tetragonal phases. Reproduced with permission from Ref...
List of Tables
Chapter 1
Table 1.1 Performance of energy storage of some lead-free ferroelectric ceramics.
Table 1.2 Performance of energy storage of some lead-free relaxor ferroelectric ceramics.
Table 1.3 Performance of energy storage of some lead-free antiferroelectric ceramics.
Table 1.4 Performance of energy storage of lead-free glass ceramics.
Table 1.5 Performance of energy storage of some lead-free films.
Table 1.6 Performance of energy storage of some lead-free nanocomposites.
Chapter 2
Table 2.1 Metal oxide ceramic materials for the application of the supercapacitor.
Table 2.2 Reported multi-metal oxidized ceramics materials for the application of the supercapacitor.
Chapter 3
Table 3.1 Metal oxide ceramic electrodes.
Chapter 4
Table 4.1 Overall features of commercial category ceramic materials applicable for energy storage using Electronic...
Table 4.2 Summary of energy storage properties for lead-free ceramics.
Chapter 5
Table 5.1 Various LTS materials used in energy storage applications.
Table 5.2 Various HTS materials used in energy storage applications.
Chapter 8
Table 8.1 Curie temperature of some ferro (-)/ferrimagnetic materials [30].
Table 8.2 Electrochemical performance of ternary metal oxide electrode materials in different architectural morphologies.
Table 8.3 Supercapacitive performance characteristics of mixed ternary ferromagnetic iron oxide electrode materials.
Table 8.4 Supercapacitive performance characteristics of mixed ternary ferromagnetic iron oxide – polymer comp...
Table 8.5 Supercapacitive performance characteristics of ferromagnetic mixed ternary cobalt oxide electrode materials.
Table 8.6 Supercapacitive performance of mixed ternary ferromagnetic cobalt oxide – polymer composites with...
Chapter 9
Table 9.1 Electrochemical performance under varying potential windows comparison between K+-free α-MnO...
Chapter 10
Table 10.1 Ionic sizes and their conductance values.
Table 10.2 Few significant water-based electrolytic supercapacitor devices and their output.
Chapter 12
Table 12.1 Energy storage properties of BT-based ceramics
Table 12.2 Energy storage properties of ST-based ceramics.
Table 12.3 Energy storage properties of KNN-based ceramics.
Table 12.4 Energy storage characteristics of commercially utilized MLCCs.
Chapter 13
Table 13.1 Metal oxide based ceramics for supercapacitors.
Guide
Cover Page
Series Page
Title Page
Copyright Page
Preface
Table of Contents
Begin Reading
Index
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Scrivener Publishing100 Cummings Center, Suite 541JBeverly, MA 01915-6106
Publishers at ScrivenerMartin Scrivener ([email protected])Phillip Carmical ([email protected])
Electroceramics for High Performance Supercapacitors
Edited by
Inamuddin Tariq Altalhi
and
Sayed Mohammed Adnan
This edition first published 2024 by John Wiley & Sons, Inc., 111 River Street, Hoboken, NJ 07030, USA and Scrivener Publishing LLC, 100 Cummings Center, Suite 541J, Beverly, MA 01915, USA© 2024 Scrivener Publishing LLCFor more information about Scrivener publications please visit www.scrivenerpublishing.com.
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Library of Congress Cataloging-in-Publication Data
ISBN 978-1-394-16625-1
Cover image: Pixabay.ComCover design by Russell Richardson
Preface
In the near future, high-energy density materials will be required to accommodate the increased demand for gadgets, hybrid cars, and massive electrical energy storage systems. Fuel cells, supercapacitors, and batteries have the highest energy densities, but traditional capacitors have gained attention for intermittent energy harvesting owing to their high energy transfer rate and quick charging/discharging capability. The large amount of electric breakdown strength and modest remnant polarization are keys to the high energy density in dielectric capacitors. Above 100°C or 212°F, polymer dielectric capacitors become unstable and begin to suffer a dielectric breakdown. Hence, dielectric ceramics are the sole viable option for high-temperature applications. When it comes to consumer electronics, where most capacitors are made without using lead, Pb-based ceramics materials like lanthanum-doped Pb zirconate-titanate have tremendous energy harvesting capabilities. Due to this, lead-free materials with a higher energy transfer rate capability are needed.
This book provides a basic understandings of dielectric-based energy harvesting. After a detailed analysis of the state of the art, it proceeds to explain the specific strategies to enhance energy storage features, including managing the local structure and phases assembly, raising the dielectric width, and enhancing microstructure and electrical uniformity. Also discussed is the need for novel materials with applications in high-density supercapacitors.
Chapter 1 discusses lead-free electrical energy storage systems. The characteristic features, energy storage efficiency, advantages, limitations, and outlook of various kinds of lead-free dielectric materials—such as ferroelectric ceramics, relaxor ferroelectric ceramics, antiferroelectric ceramics, glass ceramics, films, and polymer-based nanocomposites—are all covered.
Chapter 2 explores various ceramic materials, especially metal-based oxides, mixed ceramics, single- and multi-element-based ceramics, and spinal ceramics. The principle and characteristics of various types of electro-ceramics are also discussed. The development of ceramic materials for supercapacitor application and their key characteristics are highlighted, as well.
Chapter 3 is designed to be the source for ceramic materials and their applications as supercapacitors for energy storage applications. It includes the principles of energy storage devices and factors affecting the performance of supercapacitors. This section details various oxide-based ceramic materials used in supercapacitor applications with suitable examples. The primary focus is on understanding the metal oxide behavior and their performance as supercapacitor electrodes.
Chapter 4 discusses the multilayer ceramic capacitors using ferroelectric ceramics, BaTiO2, lead-based and lead-free materials. The chapter also provides information about quick charging/discharging rates and high energy density, plus other characteristics like fatigue resistance, temperature/frequency stability, lifetime dependability, production cost, and equivalent series resistance, which are all crucial for practical applications.
Chapter 5 summarizes various low- and high-temperature superconducting materials that are utilized for their magnetic energy storage applications. The magnetic storage properties have been discussed with an emphasis on their role in recent energy storage projects. The future potential is also considered, by highlighting the flaws of the current scenarios.
Chapter 6 explores the main key factors for the maximum optimization of supercapacitors for energy storage. Types of supercapacitors, such as electric double-layer capacitors and pseudo capacitors, are discussed briefly. Capacitance, specific capacitance, and energy density as key factors are discussed, as well. Optimization of energy density via pre-size, grain size, bandgap, surface, and the functional group is explained. Optimization of voltage is outlined, with positive and negative electrode materials, asymmetric supercapacitors, and battery supercapacitor hybrid devices.
Chapter 7 discusses energy storage properties, and lead-based and lead-free antiferroelectric materials that can be used for energy storage. Factors to optimize the performance of these anti-ferroelectrics are provided. Challenges faced by antiferroelectric, such as energy conversion efficiency are given thorough attention. Optimization factors, from phase engineering and grain size engineering to domain engineering, and doping, are all deliberated.
Chapter 8 examines the last decade’s research about the development of mixed ternary iron/cobalt ferromagnetic oxides and their polymer nano-composites for use as electrode materials in the fabrication of supercapacitors. The role of the main components of supercapacitors is thoroughly discussed. The remarkable effect of the architectural morphology of electrode material on the performance of supercapacitors is highlighted.
Chapter 9 discusses the importance of transition metal oxides (TMOs) as electrode materials for energy storage devices. The chapter explains how TMOs can be used in supercapacitors as electrode materials, by focusing on their morphology-dependent improvements in electrochemical capacitive properties for supercapacitors, which occurs by broadening the operating potential window to increase the energy density of the devices.
Chapter 10 summarizes the most recent developments related to supercapacitors and gives an overview of aqua-based electrolytes.
Chapter 11 outlines the latest advanced materials used for supercapacitors, batteries, pumped-hydro storage, flywheel energy storage, and super-conducting magnetic energy storage.
Chapter 12 explores various the new cutting edge electroceramics that are being used for energy storage. Among these new materials are lead-based ceramics that include relaxor ferroelectric and antiferroelectric ceramics. Lead-based materials such as PLZT, PLZ, and PLZST are discussed in the lead-based ceramics category. Lead-free ceramics are covered as well, such as barium titanate-based, strontium titanate, bismuth ferrite-based, niobate-based, and bismuth-based ceramics. Furthermore, applications of ceramic multilayers and films are deliberated. This chapter provides a wide overview of various new materials that are currently being explored in the energy storage field.
Finally, chapter 13 discusses ceramics and their potential applications. Additional, different types of ceramics, like metal oxide and spinel oxide for high-performance supercapacitors, are given thorough attention. Moreover, the chapter provides a comparison of Pb-based ceramics and Pb-free ceramics.
Our thanks go to Wiley and Scrivener Publishing for their continuous support and guidance.
Inamuddin
Department of Applied Chemistry, Zakir Husain College of Engineering and Technology, Aligarh Muslim University, Aligarh, India
Tariq Altalhi
Department of Chemistry, College of Science, Taif University, Taif, Saudi Arabia
Sayed Mohammed Adnan
Department of Chemical Engineering, Zakir Husain College of Engineering and Technology, Aligarh Muslim University, Aligarh, India
1Lead-Free Energy Storage Ceramics
Sahidul Islam1,2, Arindam Das2 and Ujjwal Mandal2*
1Department of Chemistry, Krishnath College, Berhampore, Murshidabad, West Bengal, India
2Department of Chemistry, The University of Burdwan, Golapbag, Burdwan, West Bengal, India
Abstract
With the technological advancement in various fields, there is a growing demand for electronic materials having a high power density that has provoked the fabrication of capacitors with high-energy storage capacity and features like high voltage, high frequency, high-energy density, high capacitance density, high-temperature tolerance, light-weight and non-polluting to environment. For storage of electrical energy, dielectric capacitors are regarded as a promising device as their charging–discharging process is fast and has very high-power density. The development of multilayer ceramic capacitors satisfies such demands well as compared to the electrolytic and film counterpart. In a multilayer ceramic capacitor, the equivalent series resistance is extremely low, the current handling capability is high, and is stable in high temperatures. These features are essential for the generation of clean energy, designing smart grids, 5G base stations, etc. However, the main limitation in lead-free energy capacitors arises due to low energy density. Lead is present in most of the high-energy density capacitors, thus limiting their widescale application due to environmental concerns as lead is a toxic heavy metal. The power density of dielectric capacitors is higher than fuel cells, Li-ion batteries, and supercapacitors. However, their lower-energy density hinders their commercialization. The energy storage density can largely be enhanced in the dielectric/ferroelectric capacitors.
Keywords: Dielectric capacitors, ferroelectric capacitors, lead-free energy storage
1.1 Introduction
With the evolution of economic society, the crisis of fossil energy resources is emerging along with the increase of environmental pollution and climate change [1, 2]. This leads to the emphasis on the essence of renewable and clean energy sources like water, wind, thermal and solar energy [3, 4]. Thus, an increasing demand is there on devices capable of storing energy like fuel cells, batteries, electrochemical supercapacitors, supercapacitors made of dielectric parallel plates, etc. [5–8]. Among these energy storage systems, the devices having high-energy density are batteries and fuel cells (10–300 W-h/kg and 200–1000 W-h/kg, respectively) but the power density of these storage systems is low (below 500 W/kg). The slow movement of charge carriers in these systems creates a limitation in their applications in high-power systems [9, 10]. In supercapacitors, the energy density is moderate (0.04 to 30 W-h/kg) and the power density is quite high (101 to 106 W/kg) but the long charge-discharge process (order of seconds) sets the main limitation in these storage systems [11, 12]. Contrarily in dielectric capacitors, the charge–discharge process is fast (~ns) and power density is reasonably high (~108 W/kg), which is sufficient to meet the required criteria in high-power electronic components in devices like space crafts, satellites, defibrillators used for medical purpose, hybrid electric vehicles, electronic weapons, etc. [13, 14]. However, in dielectric capacitors, the major limitation is attributed to the low-energy density as compared to batteries, fuel cells, and electrochemical capacitors [15, 16]. In pulsed power systems and power electronics, dielectric capacitors occupy almost one-fourth of the size and mass [17]. Hence, in dielectric capacitors, the development of novel dielectric material is necessary to increase the power density significantly. To obtain this, researchers have given many efforts with the materials like lead magnesium niobate-lead titanate, lead lanthanum zirconate titanate, lead lanthanum zirconate stannate titanate, etc. as these materials have higher-energy density as compared to other dielectrics [18–20]. However, the use of lead in these materials sets the major drawbacks in their application as lead is a toxic heavy metal that pollutes the environment and endangers the health of living creatures, including human beings [21]. This drives the search for materials capable to store energy and free of lead.
In recent times, progress in the development of ceramics and dielectric materials free of lead, polymer-based composites, and various films happened to a considerable extent [22, 23]. In the sustainable energy program, energy storage plays an important role as this can enhance the more efficient use of energy from renewable energy sources, stabilize the energy market, and take the matter of environmental impact into account [24]. Designing capacitors renders such quality greatly as their power density is high and the charge/discharge process is fast as compared to the batteries [25]. Although the energy-storing capacity of dielectrics is less as compared to Li batteries, fuel cells, and supercapacitors, their use is proposed in high-power applications, such as defibrillators, power electronics, detonators, etc [26–28]. Recently, a great effort is given by researchers across the globe for developing materials having a dielectric constant very high and an energy storage capacity very large. In recent times, for lead-free antiferroelectric films, the reported recoverable energy density (50 J cm−3) is found to be very high at room temperature [29, 30]. Moreover, the energy density (39 J cm−3) and thermal stability of some lead-based materials are good even though the temperature increases up to 200°C [30, 31]. However, lead-based material is harmful to human beings and the environment at large. Thus, there is a limitation on the applicability of lead-based materials for energy storage. The research on lead-free materials is extremely important and is done on so many materials and found promising results for some materials like Hf0.3Zr0.7O3 thin film (ηreco=40 Joule cm−3 and η=50% at room temperature) [32, 33]. A very high value of η (=81%) and ηreco (=37 J cm−3) is obtained for 0.88BaTiO3–0.12Bi(MgTiO3) film at room temperature [34]. Although there is considerable progress in the research of lead-free materials for the storage of energy, it was found that the performance of lead-free materials is much poor as compared to that of lead-based materials. Hence, the achievement of high performance on lead-free materials is the main aim of the researchers to meet the requirement for large-scale applications in power converters, portable power electronics, and DC link capacitors [35]. Previously it was reported that materials having high piezoelectric coefficient and dielectric constant are suitable for good energy storage capacitors [36]. The performance of ferroelectric or dielectric multilayer capacitors is higher as compared to single-layer capacitors [37, 38].
1.2 Dielectric Capacitor and Energy Storage
A typical dielectric capacitor is made of two parallelly placed electrodes sandwiching the dielectric material between them. The energy storage capacity is quantified by the capacitance, as represented mathematically,
C, ε0, εr here represents capacitance, permittivity in a vacuum and relative permittivity (also known as dielectric constant), respectively. A and d represent overlapping areas and distance between the two parallelly placed plates [39, 40]. On applying the electric field between the two plates, the orientation of the dipoles of the dielectric material occurs in the direction of the applied electric field, thus in the two plates, the charge is induced and charging happens. The process of charging is stopped when the generated potential difference between the two plates due to the accumulation of charge (±Q) becomes equal to the voltage applied externally and the storing of the electric field occurs. Another way of mathematical representation of capacitance (C) is,
While charging, the total stored energy W can be expressed as [39, 40],
Hence, the energy storage in unit volume i.e., the energy density of the dielectric material can be expressed as,
where is the externally applied electric field, δ represents the charge density on the surface and D represents electrical displacement. The dielectric constant for linear dielectric materials (such as glass, and mica) remains unchanged with the change of electric field applied externally, hence the calculation of energy storage density (J) could be done as,
It is clear from equation (1.5), the density of energy storage linearly varies as a function of the square of the applied electric field and direly to the relative permittivity of the medium. However, the dielectric constant for non-linear dielectric materials is changed with the applied electric field, hence equation (1.5) is not applicable. The extent of electrical displacement in the dielectric materials having large dielectric constant becomes almost near to the polarization. Equation (1.4) in these cases takes the form:
Here, spontaneous polarization and maximum polarization of dielectric material are represented by P and Pmax [39–42]. It is evident from equation (1.6), the confined area between vertical axes and hysteresis loop in the process of charging represents the energy density (J). In Figure 1.1 (3), Polarization-Electric field diagrams i.e. hysteresis loops (represented by P-E diagrams) have been shown in the cases of linear dielectric materials (like, Al2O3), ferroelectric (FE) materials (like, PbZrxTi1-xO3), relaxor ferroelectric (RFE) materials (like, xPb(Mg1/3Nb2/3)O3-(1-x)PbTiO3) and antiferroelectric (AFE) materials (like, PbZrO3). The releasing of all the stored energy is not possible as there is energy loss (Jloss) due to electric hysteresis in the process of charging. The enclosed area between vertical axes and hysteresis loops during the process of discharging represents the recoverable energy storage density (Jrec) [43].
Figure 1.1 Polarization of the dielectric material during the process of charging.
The mathematical representation of energy efficiency (η) is,
From equation (1.7) and diagram (1.3), it is clear that a high value of electric field breakdown strength (BDS), the large value of maximum polarization, small remnant polarization, and slim P-E hysteresis loops imply the high value of Jrec and η. In linear dielectrics, the BDS and energy loss for the materials are low but as their maximum polarization is small, their application in the high-energy storage system is not suitable [40].
1.3 Energy Storage of Dielectric Ceramics Free of Lead
(i) Energy storage and ferroelectric ceramics free of lead (Figure 1.2)
The spontaneous polarization of ferroelectric material occurs within a certain range of temperatures even in the absence of an applied external electric field [44]. Above curie temperature, this spontaneous polarization disappears and a transition from ferroelectric to paraelectric occurs and linear dielectric behavior of the materials is observed [45]. One such ferroelectric material is BaTiO3 (BT) which undergoes spontaneous polarization to large extent assisting in high-energy storage density. However, its large extent of remnant polarization decreases the energy efficiency resulting in the generation of thermal energy that decreases the service life of the device [46, 47]. One of the feasible ways of tailoring the energy storage performance in ferroelectric material is doping [48]. The property of storage of energy of BaTiO3 ceramics is significantly increased if Ba2+ and Ti4+ ions are substituted with equivalent ions (that may be even hetero valent) [49]. The substitution of Ba2+ with Ca2+ or Sr2+ and the substitution of Ti4+ with Zr4+ decreases the remnant polarization, thus energy density and efficiency increase [50]. One such example is Ba0.70Ca0.30TiO3 (BCT), having moderate energy efficiency of 60% (density of energy is 1.41 J cm3 which is convertible) and it is 40% higher as compared to BaTiO3 [51]. The remnant polarization and energy loss in the case of BCT are less and have 4+ a slimmer P-E hysteresis loop as compared to BaTiO3. It is because Zr4+ has a fixed valence state whereas Ti is multivalent (Ti3+ and Ti4+). The electron conduction between Ti3+ and Ti4+ can be decreased by doping Zr4+, hence there is a decrease in energy loss [52–55]. In Zr4+ doped BaTiO3 ceramics (BaZr0.1Ti0.9O3), Zhang et al. have shown that at the appropriate sintering temperature, the quality of dielectric material becomes good and the capacity of energy storage become high (Dielectric constant: 2998, energy density: 0.5 J cm3, dielectric loss: 0.007) [56]. By sol-gel method, Scott et al. synthesized the ceramics [(BaZr0.2Ti0.8)O3]1-x- [(Ba0.7Ca0.3)TiO3]x (BZT-BCT, x = 0.10, 0.15, 0.20) doped with ca2+ and Zr2+ which has improved energy storage capacity (when x=0.10, the reported energy density is 0.6 J cm3 which is dischargeable). The reason for this improvement is the increased Pmax and reduced Pr [57]. Apart from low rampant polarization and high maximum polarization, the other parameter which plays a crucial role to achieve dielectric material with excellent energy storage is high BDS [58]. The large BDS can be obtained by improving the quality of FE ceramics i.e., ceramics with uniform and fine particle grain size and low porosity [59]. From the study of Jin et al., it was established that the grain size of Ba0.4Sr0.6TiO3 ceramics is reduced to 0.44 μm when the ceramics are sintered in the O2 atmosphere as the lack of oxygen vacancies inhibits the growth in grain size. In this ceramic material, a large value of BDS and energy storage density (16.72 kV/mm and 1.081 J cm3, respectively) and a moderate value of energy storage efficiency (73.78%) was found [60]. Surface modification in ceramics is another promising method of increasing BDS. An example of such kind of surface modification is to be found in resulting ceramics when BaTiO3 is modified by Al2O3 (i.e., A@BT) and BaTiO3 modified by B2O3–SiO2 (i.e., G@BT) [61, 62]. BDS in these two modified ceramics is found to increase by 69% and 117% on going from unmodified to modified BaTiO3 ceramics. The enhancement of BDS in G@BT as compared to that of BaTiO3 is due to a decrease in pore defect concentration. The voltage endurance in A@BT ceramics is increased as the Al2O3 coating layer act as an insulator which decreases the thermally caused breakdown that occurs due to avalanche and electron accumulation. For these ceramic materials, the density of energy storage was reported, at 2.5 and 3.2 J cm3 which are quite high compared to the density of energy (0.88 J cm3) for pure BaTiO3 [62].
Figure 1.2 P-E hysteresis loops and characteristic parameters of (i) linear dielectric (ii) ferroelectric (iii) relaxor ferroelectric and (iv) antiferroelectric materials for energy storage.
(ii) Energy storage and relaxor ferroelectric ceramics free of lead (Table 1.1)
The relaxor ferroelectric ceramics are dipolar glasses lacking a well-ordered long-range structure. Example of these type of relaxor ferroelectrics are PbMg1/3Nb2/3O3, PbSc1/2Nb1/2O3, and PbZn1/3Nb2/3O3 [68, 69]. The remnant polarization in relaxor ferroelectric materials is near zero and the P-E hysteresis loop is slim as compared to that of the ferroelectric materials, hence the energy efficiency becomes high [70]. In relaxor ferroelectrics, the diffuse phase transition can occur around dielectric maxima which renders good temperature stability [71]. Among many lead-free energy storage materials, BT-based materials have caught increasing attention as the BT materials can be converted into other ferroelectric-relaxor materials by introducing other elements in A- or B- site of it [72, 73]. The addition of Bi(Mg2/3Nb1/3)O3 (BMN) in BT leads to the conversion into the material where relaxor-like behavior was observed and high maximum energy density (1.13 J cm3) was found [74]. The introduction of Bi(Zn0.5Ti0.5)O3 (BZT) in BT as reported by Dong et al., increases the relaxor feature along with thermal stability and energy storage properties (Table 1.2) [75].
Table 1.1 Performance of energy storage of some lead-free ferroelectric ceramics.
Lead-free ferroelectric ceramics
E
(kV/cm)
J
rec
(J m
3
)
η
(%)
Reference
(Ba
0.4
Sr
0.6
)TiO
3
180
1.15
82
63
0.85(K
0.5
Na
0.5
)NbO
3
–0.15SrTiO
3
400
4.03
52
64
0.85BaTiO–0.15Bi(Mg
2/3
Nb
1/3
)O
3
140
1.13
90
65
Ba
0.4
Sr
0.6
TiO
3
–5vol%(BaO–SiO
2
–B
2
O
3
)
175
0.89
76
66
0.92(0.92Bi
0.5
Na
0.5
TiO
3
–0.08BaTiO
3
)–0.1NaNbO
3
70
0.71
66
67
Table 1.2 Performance of energy storage of some lead-free relaxor ferroelectric ceramics.
Lead-free relaxor ferroelectric ceramics
E
(kV/cm)
J
rec
(J/cm
3
)
η
(%)
Reference
0.8BaTiO
3
–0.2BiNbO
4
117
0.31
99.7
76
0.88BaTiO
3
–0.12Bi(Zn
1/2
Zr
1/2
)O
3
100
0.758
98
77
0.88BaTiO
3
–0.12Bi(Mg
1/2
Ti
1/2
)O
3
150
1.6
99.6
78
0.86BaTiO
3
–0.14Bi(Zn
1/2
Ti
1/2
)O
3
120
0.81
94
79
0.875BaTiO
3
–0.125Bi(Mg
2/3
Nb
1/3
)O
3
240
1.89
83
80
(iii) Energy storage and antiferroelectric ceramics free of lead
While spontaneous polarization occurs in ferroelectrics, the presence of antiparallel dipoles in almost equal proportion leads to the net polarization zero [81]. In presence of an appropriately high electric field, known as the field (EF) for AFE-FE phase transition, the dipoles that are anti-parallelly oriented in the AFE phase, reorient to parallel dipoles, thus AFE-FE phase transition occurs and macroscopic polarization is induced [82]. On application of electric field EA lesser than EF, FE materials are converted back into AFE materials. Hence, for antiferroelectric materials, unique double P-E loops are found leading to the large value of Jrec and η. From the I-E curve, the values of EF and EA can be found. The positive-current peak relevant to EF and negative peak-current relevant to EA is obtained by applying the positive and negative electric field, respectively [83]. The discharge rate in antiferroelectric is faster (~ns) as compared to ferroelectric as in the switching electric field EA, the FE phase is suddenly disappeared in antiferroelectric. Ferroelectrics and relaxor ferroelectrics have higher Jrec and η than antiferroelectrics [84, 85]. In the past few years, researchers have shown some interest in PbZrO3-based antiferroelectrics because of high Jrec and η. But as lead is a toxic element in its various states, the shifting of research interest to lead-free antiferroelectric materials such as AgNbO3 and (Bi0.5Nb0.5)TiO3 was very normal. Ding et al. reported 0.9 J cm3 (quite high) energy density for antiferroelectric ceramics 0.89Bi0.5Na0.5TiO3–0.06BaTiO3–0.05K0.5Na0.5NbO3 where low remnant polarization (5.4 μC/cm2) is the favorable factor [86]. From the study of Wang et al., it was found that Zr containing in the ceramics [(Bi0.5Na0.5)0.94Ba0.06] La(1-x) ZrxTiO3 lead to a slimmer hysteresis loop and AFE behavior and the combination of these two features lead to high recoverable energy density 1.58 J cm3 [87]. While emphasizing lead-free materials, AgNbO3-based materials attracted the attention of researchers recently as AFE materials have high Jrec and η. The AFE fabrics of AgNbO3 were prepared by Wei et al. by sintering at solid state with the flow of oxygen, thus achieving the dielectrics with high recoverable energy density (2.1 J cm3) but due to the poor stability of the AFE phase of AgNbO3, they have not found the double P-E loops [88]. To increase the value of Jrec, the AFE phase should be stable and EA should be high. In perovskite structure (ABO3), the phase stability can be assumed in terms of tolerance factor, t. The mathematical definition of t is [89],
Here rA and rB represent the ionic radii of cations present in A- and B-sites, respectively, rO represents, the ionic radii of the anionic oxygen atom. The stability of FE phase is seen when t>1 and the stability of AFE phase is seen when t<1. The replacement of cation (Ag+) of A site with cations having smaller size enhances the stability of AFE phase. One such example is the doping of Bi3+ ions in AgNbO3 by Tian et al. As the size of the Bi3+ ion (1.17 Å) is lesser than Ag+ ion (1.28 Å) the tolerance factor is decreased and the stability of AFE phase in the Ag0.91Bi0.03NbO3 ceramic is increased, hence, they found high Jrec value (2.6 J cm3) and η (86%) [90, 91]. So far, the largest Jrec value reported for the lead-free ceramic Ag(Nb0.85Ta0.15)O3 is 4.2 J cm3 (Table 1.3) [92].
Table 1.3 Performance of energy storage of some lead-free antiferroelectric ceramics.
Lead-free antiferroelectric ceramics
E(kV/cm)
J
loss
(J/cm
3
)
J
rec
(J/cm
3
)
η
(%)
Reference
AgNbO
3
175
3.15
2.10
40
93
Ag(Nb
0.85
Ta
0.15
)O
3
230
1.90
4.20
69
94
(Ag
0.97
Bi
0.01
)NbO
3
175
2.45
3.0
55
95
AgNbO
3
–0.1wt%MnO
2
150
2.30
2.50
52
96
0.84(Bi
0.5
Na
0.5
)TiO
3
–0.16(K
0.5
Na
0.5
)NbO
3
100
0.10
1.20
92
97
(iv) Energy storage and glass ceramics free of lead
To achieve large Jrec, the high value of BDS is important. But BDS is insufficient in lead-free ceramics due to high defect density, hence it set the limitation in their application in ceramic-based capacitors. Several factors on which BDS depends are (i) porosity, (ii) grain size, (iii) interfacial polarization, (iv) secondary phase, and (v) charge transport [98]. In the ceramic matrix, the embedding of glass increases density and reduces grain size, and the electric field is decreased across the grain boundaries, thus there is an increase in BDS. The electrical durability and wettability of B2O3–SiO2–based glass are quite good. Hence, it may be effectively added to the ceramics to increase the energy density [99]. One such example is, Wang et al. achieved higher-energy density (0.72 J cm3) at a higher electric field of 280.5 kV/cm by adding BaO–B2O3–SiO2–Na2CO3–K2CO3 into Ba0.4Sr0.6TiO3 [100]. Zhang et al. established by their research work, the introduction of 20 vol% glass (BaO–SiO2–B2O3) in Ba0.4Sr0.6TiO3 ceramic increased the BDS value to 23.9 kV/mm from 12.1 kV/mm for pure Ba0.4Sr0.6TiO3 ceramic, thus there is an enhancement of BDS by 1.9 times. The reason behind the increase of BDS is the decrease in grain size, pore size, and porosity, thus the energy density is increased [101]. From the investigation of Wang et al., it was found that the grain size and BDS of BaTiO3 are largely affected by the addition of the glass BaO–SrO–TiO2–Al2O3–SiO2–BaF2. They found that BDS is related to grain size as well as charge transport across the grain boundaries and has an inversely proportional relationship with average field strength, EGB. The electric field EGB can be defined as,
Here E is the electric field applied externally, dB represents grain size and dGB represents grain-boundary space-charge layer width. Due to the addition of glass material, dB is decreased and dGB is increased, so, the average electric field is decreased in the grain boundary space charge layer and BDS is increased [102]. Recently, upon the addition of 9 wt% Bi2O3–B2O3–SiO2 (BBS) glass with lead-free ceramics, Ba0.4Sr0.6TiO3 (BST), a higher-energy density (1.98 J cm3) and efficiency 90.57% is achieved. The BDS is increased with the increase of BBS glass content in the ceramic composition (Table 1.4) [103].
Table 1.4 Performance of energy storage of lead-free glass ceramics.
Lead-free glass ceramics
E
(kV/cm)
J
rec
(J cm
3
)
η
(%)
Reference
5% B
2
O
3
-Al
2
O
3
-SiO
2
glass doped Ba
0.85
Ca
0.15
Zr
0.1
Ti
0.9
O
3
--
1.153
75
104
(v) Storage of energy and lead-free films
The concentration of internal defects is high and BDS is low in lead-free bulk materials. Hence, there are limitations in their energy storage capacity. The defects in thin and thick films are very less as compared to bulk materials, thus BDS becomes higher, and consequently, energy density becomes higher [105]. One such example is Mn doped relaxor thin film of 0.7 (Na0.5Bi0.5)TiO3–0.3SrTiO3 developed on Pt/Ti/SiO2/Si substrate by the sol-gel method has high BDS (1894 kV/cm) and Jrec (27 J/cm3) [106]. The thin films grown by the physical method have better crystalline quality compared to the films developed by the chemical method; hence the BDS and energy storage capacity of the former are higher [107]. Using radio frequency magnetron sputtering, a high-quality thin film of epitaxial BaZr0.2Ti0.8O3 was prepared by Jia et al. by doping Nb on SrTiO3 substrate. The resulting material shows high-energy storage density (81.7%) and Jrec (30.4 J cm3) when 3MV/cm external electric field is applied. So far the largest Jrec (154 J cm3) is reported for the epitaxial lead-free relaxor thin films (Bi1/2Na1/2)0.9118La0.02Ba0.0582(Ti0.97Zr0.03)O3 (prepared by pulsed laser deposition, applying electric field 3500 kV/cm) [108]. The energy storage capacity of these films is high because of (i) the high value of BDS (ii) epitaxially, the structure is good (iii) the excellent relaxor, and (iv) the two phases, FE and AFE coexist at the vicinity of morphotropic phase boundary (MPB). Although the density of energy is high in lead-free thin films, their overall energy-storing capacity is very limited and it is because of the limited thickness. The comparatively thick films (>1 μm) can be useful for energy storage (Table 1.5) [109].
Table 1.5 Performance of energy storage of some lead-free films.
Lead-free films
E
(kV/cm)
J
rec
(J cm
3
)
η
(%)
Reference
0.95(Na
0.5
Bi
0.5
)TiO
3
–0.05SrTiO
3
(Thick film)
1965
36.1
40.80
110
(Bi
1/2
Na
1/2
)0.9118La
0.02
Ba
0.0582
(Ti
0.97
Zr
0.03
)O
3
(Epitaxical thin film)
3500
154
97.00
111
(vi) Energy storage and polymer-based nanocomposites free of lead
The ferroelectric polymers having high machinability and BDS can be useful as dielectric capacitors. An example of such a polymer is poly(vinylidene fluoride) (PVDF). However, the main limitation of these types of polymers is very low energy density due to small Pmax [112]. This problem can be overcome by proposing ceramic-polymer-based nanocomposites where the high value of maximum polarization and high value of BDS of ceramic fillers and polymer matrix, respectively get combined. But again, limitations in energy storage properties arise for two reasons (i) interfacial compatibility of an organic matrix with inorganic filler is poor, and (ii) ceramic fillers are agglomerated in the matrix of the polymer [113]. When the surface of ceramic fillers is modified, the interfacial compatibility issue is reduced. Gao et al. worked on the hydroxylation of the surface of BT with H2O2 and then they modified it with titanate coupling agent DN-101, hence the formation of nanocomposites PVDF/H2O2–DN-101–BaTiO3 (D-h-BT) occur where Pmax and BDS are larger as compared to the nanocomposites PVDF/DN-101–BaTiO3(D-B-T). In this case, an increase (3.01–4.31 J cm3) in the density of discharge energy was found [114]. An improvement in energy storage can also be done by using the core-shell structure of polymer-based nanocomposites. One example of such type is BaTiO3–SiO2 core-shell (BT@SO) filled novel PVDF-based nanocomposites where the particle size is less than 10 nm. The interface of the ultrafine nanostructure is larger than conventional 100 nm fillers, hence the polarization becomes high [115]. Apart from this, BDS also becomes high due to the presence of a strongly insulating SiO2 layer. The maximum energy density and efficiency in the case of nanocomposite with BT@SO (3 vol%) were found to be 11.5 J cm3 64%, respectively [116]. Recently, the fabrication of sandwich-structure nanocomposites and embedding them with a high BDS layer increase the electric displacement and BDS [117]. Luo et al. fabricated such type of sandwich-structured nanocomposites with the central layer of pure P(VDF-HPF) and two neighboring layers of BaTiO3-(VDF-HPF). In the sandwich-structured nanocomposites, BDS and effective electric displacement (Pmax–Pr) was found to be increased so also the density of discharge energy from 2.32 to 5.22 J cm3 Table (1.6) [118].
Table 1.6 Performance of energy storage of some lead-free nanocomposites.
Lead-free nanocomposites
E
(kV/cm)
J
rec
(J cm
3
)
η
(%)
Reference
3vol% BaTiO
3
@TiO
2
nanofibers/ (PVDF-HFP)
7977
31.2
78
119
TiO
2
nanorod arrays/PVDF
3400
10.62
70
120
10 vol% H
2
O
2
–DN-101–BaTiO
3
/PVDF
2600
4.31
47.83
121
1.4 Conclusion and Outlooks
For the practical application of lead-free dielectric capacitors, the criteria that need to be fulfilled are (i) recoverable energy density needs to be large, (ii) energy efficiency should be high, (iii) the charging and discharging process should be fast, and (iv) life span should be long. The energy efficiency and recoverable energy density of lead-free ceramics are very low as their Pr is large and BDS is low. The high-energy efficiency in the case of lead-free relaxor ceramics (ferroelectric and antiferroelectric) is because of their slim hysteresis loops, but due to small BDS, their recoverable energy density is not sufficient to be utilized practically. The recoverable energy density and energy efficiency of the lead-free thin film are quite high but due to their low volume, storing efficiency of energy become low. Similarly, the recoverable energy density is high in the case of thick films and various composites (polymer-based) but because of low efficiency in the ceramic matrix, the main limitations arise in their energy efficiency. These are the facts that good energy storage properties in lead-free materials can be achieved by increasing the BDS in lead-free ferroelectric or antiferroelectric materials, increasing the volume of thin films without affecting the BDS value, and increasing the energy efficiency in nanocomposites and thick films. In Bulk ceramics, BDS is related to the microstructure of the material which in turn is related to the grain size density of the materials. The appropriate microstructure can be achieved by monitoring the preparation and processing techniques (of ceramic powder) such as co-precipitation, spark plasma sintering, sol-gel method, etc. One important scope of improvement in overall low energy density in thin films and small BDS in bulk ceramics is the embedding of an alternating layer of conductive metal electrodes parallelly. In polymer-based nanocomposites, the energy efficiency and discharge energy density are high at room temperature, but in gentle conditions like that in embedded capacitors and harsh conditions like that in hybrid electric vehicles, the dissipation of energy can increase the temperature and as the melting point of polymer is low, the appropriate cooling system is required where extra energy is consumed. Thus, the development of an appropriate polymer-based capacitor is required which can function in a wide range of temperatures [122–124].
Acknowledgments
The financial support for the research along with this work was received from UGC-BSR and SERB-DST. SI is serving in the Department of Chemistry, Krishnath College with the capacity of Assistant Professor, and pursuing his research in the Chemistry Department, Burdwan University as a Ph.D. student. He thanks his colleagues and the Principal of the college for their support and encouragement in the best possible ways. UM is an Assistant Professor, serving in Chemistry Department, Burdwan University. All the authors acknowledge the Department of Chemistry, The University of Burdwan on the academic aspect.
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