The science and technology of ultracapacitors are reviewed for a number of electrode materials, including carbon, mixed metal oxides, and conducting polymers. More work has been done using microporous carbons than with the other materials and most of the commercially available devices use carbon electrodes and an organic electrolytes. The energy density of these devices is 3¯5 Wh/kg with a power density of 300¯500 W/kg for high efficiency (90¯95%) charge/discharges. Projections of future developments using carbon indicate that energy densities of 10 Wh/kg or higher are likely with power densities of 1¯2 kW/kg. A key problem in the fabrication of these advanced devices is the bonding of the thin electrodes to a current collector such the contact resistance is less than 0.1 cm2. Special attention is given in the paper to comparing the power density characteristics of ultracapacitors and batteries. The comparisons should be made at the same charge/discharge efficiency.

Ultracapacitors: Why, How, and Where is the Technology

As one important component of sulfur cathodes, the carbon host plays a key role in the electrochemical performance of lithium-sulfur (Li-S) batteries. In this paper, a mesoporous nitrogen-doped carbon (MPNC)-sulfur nanocomposite is reported as a novel cathode for advanced Li-S batteries. The nitrogen doping in the MPNC material can effectively promote chemical adsorption between sulfur atoms and oxygen functional groups on the carbon, as verifi ed by X-ray absorption near edge structure spectroscopy, and the mechanism by which nitrogen enables the behavior is further revealed by density functional theory calculations. Based on the advantages of the porous structure and nitrogen doping, the MPNC-sulfur cathodes show excellent cycling stability (95% retention within 100 cycles) at a high current density of 0.7 mAh cm −2 with a high sulfur loading (4.2 mg S cm −2 ) and a sulfur content (70 wt%). A high areal capacity (≈3.3 mAh cm −2 ) is demonstrated by using the novel cathode, which is crucial for the practical application of Li-S batteries. It is believed that the important role of nitrogen doping promoted chemical adsorption can be extended for development of other high performance carbon-sulfur composite cathodes for Li-S batteries.

Nitrogen-Doped Mesoporous Carbon Promoted Chemical Adsorption of Sulfur and Fabrication of High-Areal-Capacity Sulfur Cathode with Exceptional Cycling Stability for Lithium-Sulfur Batteries

Rechargeable sodium-ion batteries (SIBs), as the most promising alternative to commercial lithium-ion batteries, have received tremendous attention during the last decade. Among all the anode materials for SIBs, metal sulfides/selenides (MXs) have shown inspiring results because of their versatile material species and high theoretical capacity. They suffer from large volume expansion, however, which leads to bad cycling performance. Thus, methods such as carbon modification, nanosize design, electrolyte optimization, and cut-off voltage control are used to obtain enhanced performance. Here, recent progress on MXs is summarized in terms of arranging the crystal structure, synthesis methods, electrochemical performance, mechanisms, and kinetics. Challenges are presented and effective ways to solve the problems are proposed, and a perspective for future material design is also given. It is hoped that light is shed on the development of MXs to help finally find applications for next-generation rechargeable batteries.

Advances and Challenges in Metal Sulfides/Selenides for Next-Generation Rechargeable Sodium-Ion Batteries.

Mixed metal sulfides (MMSs) have attracted increased attention as promising electrode materials for electrochemical energy storage and conversion systems including lithium-ion batteries (LIBs), sodium-ion batteries (SIBs), hybrid supercapacitors (HSCs), metal–air batteries (MABs), and water splitting. Compared with monometal sulfides, MMSs exhibit greatly enhanced electrochemical performance, which is largely originated from their higher electronic conductivity and richer redox reactions. In this review, recent progresses in the rational design and synthesis of diverse MMS-based micro/nanostructures with controlled morphologies, sizes, and compositions for LIBs, SIBs, HSCs, MABs, and water splitting are summarized. In particular, nanostructuring, synthesis of nanocomposites with carbonaceous materials and fabrication of 3D MMS-based electrodes are demonstrated to be three effective approaches for improving the electrochemical performance of MMS-based electrode materials. Furthermore, some potential challenges as well as prospects are discussed to further advance the development of MMS-based electrode materials for next-generation electrochemical energy storage and conversion systems.

Mixed Metal Sulfides for Electrochemical Energy Storage and Conversion

Transition Metal Sulfides Based on Graphene for Electrochemical Energy Storage

Typical layered transition-metal chalcogenide materials, in particular layered molybdenum disulfide (MoS2) nanocomposites, have attracted increasing attention in recent years due to their excellent chemical and physical properties in various research fieldsHere, a general overview of synthetic MoS2 based nanocomposites via different preparation approaches and their applications in energy storage devices (Li-ion battery, Na-ion battery, and supercapacitor) is presented. The relationship between morphologies and the electrochemical performances of MoS2-based nanocomposites in the three typical and promising rechargeable systems is also discussed. Finally, perspectives on major challenges and opportunities faced by MoS2-based materials to address the practical problems of MoS2-based materials are presented.

MoS2-Based Nanocomposites for Electrochemical Energy Storage

Lithium-ion batteries, which have revolutionized portable electronics over the past three decades, were eventually recognized with the 2019 Nobel Prize in chemistry. As the energy density of current lithium-ion batteries is approaching its limit, developing new battery technologies beyond lithium-ion chemistry is significant for next-generation high energy storage. Lithium-sulfur (Li-S) batteries, which rely on the reversible redox reactions between lithium and sulfur, appears to be a promising energy storage system to take over from the conventional lithium-ion batteries for next-generation energy storage owing to their overwhelming energy density compared to the existing lithium-ion batteries today. Over the past 60 years, especially the past decade, significant academic and commercial progress has been made on Li-S batteries. From the concept of the sulfur cathode first proposed in the 1960s to the current commercial Li-S batteries used in unmanned aircraft, the story of Li-S batteries is full of breakthroughs and back tracing steps. Herein, the development and advancement of Li-S batteries in terms of sulfur-based composite cathode design, separator modification, binder improvement, electrolyte optimization, and lithium metal protection is summarized. An outlook on the future directions and prospects for Li-S batteries is also offered.

Advances in Lithium–Sulfur Batteries: From Academic Research to Commercial Viability

The deployment of high-energy-density lithium-metal batteries has been greatly impeded by Li dendrite growth and safety concerns originating from flammable liquid electrolytes. Herein, we report a stable quasi-solid-state Li metal battery with a deep eutectic solvent (DES)-based self-healing polymer (DSP) electrolyte. This electrolyte was fabricated in a facile manner by in situ copolymerization of 2-(3-(6-methyl-4-oxo-1,4-dihydropyrimidin-2-yl)ureido)ethyl methacrylate (UPyMA) and pentaerythritol tetraacrylate (PETEA) monomers in a DES-based electrolyte containing fluoroethylene carbonate (FEC) as an additive. The well-designed DSP electrolyte simultaneously possesses non-flammability, high ionic conductivity and electrochemical stability, and dendrite-free Li plating. When applied in Li metal batteries with a LiMn2 O4 cathode, the DSP electrolyte effectively suppressed manganese dissolution from the cathode and enabled high-capacity and a long lifespan at room and elevated temperatures.

Deep-Eutectic-Solvent-Based Self-Healing Polymer Electrolyte for Safe and Long-Life Lithium-Metal Batteries.

Sodium-ion batteries have been emerging as attractive technologies for large-scale electrical energy storage and conversion, owing to the natural abundance and low cost of sodium resources. However, the development of sodium-ion batteries faces tremendous challenges, which is mainly due to the difficulty to identify appropriate cathode materials and anode materials. In this review, the research progresses on cathode and anode materials for sodium-ion batteries are comprehensively reviewed. We focus on the structural considerations for cathode materials and sodium storage mechanisms for anode materials. With the worldwide effort, high-performance sodium-ion batteries will be fully developed for practical applications.

Electrode Materials for Sodium-Ion Batteries: Considerations on Crystal Structures and Sodium Storage Mechanisms

Noble metal-based materials have been intensively investigated as good additives of electrode materials for supercapacitors, since they can improve the specific capacitance, conductivity, and chemical and thermal stabilities of the electrode materials. This review carefully summarizes noble metal-based materials for high-performance supercapacitor electrodes. The advances of hybrid electrodes are then assessed to include hybrid systems of noble metal-based materials with compounds such as carbonaceous materials, metals and transition metal oxides or hydroxides. A variety of synthetic methods such as hydrothermal/solvothermal methods, polymerization, and electrodeposition methods are also discussed to prepare noble metal-based materials. This review comprehensively summarizes and evaluates the recent progress in the research on noble metal-based electrode materials for supercapacitors, including synthesis methods, electrochemical performances, and related devices.

Tianyi Wang

Papers

MoS2-Based Nanocomposites for Electrochemical Energy Storage

Advances in Lithium–Sulfur Batteries: From Academic Research to Commercial Viability

Deep-Eutectic-Solvent-Based Self-Healing Polymer Electrolyte for Safe and Long-Life Lithium-Metal Batteries.

Electrode Materials for Sodium-Ion Batteries: Considerations on Crystal Structures and Sodium Storage Mechanisms

Noble metal-based materials in high-performance supercapacitors