Textile‐Based Electrochemical Energy Storage Devices

In the past few years, insensitive attentions have been drawn to wearable and flexible energy storage devices/systems along with the emergence of wearable electronics. Much progress has been achieved in developing flexible electrochemical energy storage devices with high end‐use performance. However, challenges still remain in well balancing the electrochemical properties, mechanical properties, and the processing technologies. In this review, a specific perspective on the development of textile‐based electrochemical energy storage devices (TEESDs), in which textile components and technologies are utilized to enhance the energy storage ability and mechanical properties of wearable electronic devices, is provided. The discussion focuses on the material preparation and characteristics, electrode and device fabrication strategies, electrochemical performance and metrics, wearable compatibility, and fabrication scalability of TEESDs including textile‐based supercapacitors and lithium‐ion batteries.     

Xylene‐Bridged Phosphaviologen Oligomers and Polymers as High‐Performance Electrode‐Modifiers for Li‐Ion Batteries

Lithium‐ion batteries are one of the most common forms of energy storage devices used in society today. Due to the inherent limitations of conventional Li‐ion batteries, organic materials have surfaced as potentially suitable electrode alternatives with improved performance and sustainability. Viologens and phosphaviologens in particular, are strong electron‐accepting materials with excellent kinetic properties, making them suitable candidates for battery applications. In this paper, new polymeric species of the latter moieties are reported that lead to improved electrode stability and device performance. The performance of the phosphaviologen is further enhanced through the utilization of both redox steps, allowing for good performance proof‐of‐concept hybrid organic/Li‐ion batteries. This opens the potential for more sustainable and improved battery performance for use in current energy applications.     

Hierarchical Structures Based on Two‐Dimensional Nanomaterials for Rechargeable Lithium Batteries

Two‐dimensional (2D) nanomaterials (i.e., graphene and its derivatives, transition metal oxides and transition metal dichalcogenides) are receiving a lot attention in energy storage application because of their unprecedented properties and great diversities. However, their re‐stacking or aggregation during the electrode fabrication process has greatly hindered their further developments and applications in rechargeable lithium batteries. Recently, rationally designed hierarchical structures based on 2D nanomaterials have emerged as promising candidates in rechargeable lithium battery applications. Numerous synthetic strategies have been developed to obtain hierarchical structures and high‐performance energy storage devices based on these hierarchical structure have been realized. This review summarizes the synthesis and characteristics of three styles of hierarchical architecture, namely three‐dimensional (3D) porous network nanostructures, hollow nanostructures and self‐supported nanoarrays, presents the representative applications of hierarchical structured nanomaterials as functional materials for lithium ion batteries, lithium‐sulfur batteries and lithium‐oxygen batteries, meanwhile sheds light particularly on the relationship between structure engineering and improved electrochemical performance; and provides the existing challenges and the perspectives for this fast emerging field.     

A Calcium‐Ion Hybrid Energy Storage Device with High Capacity and Long Cycling Life under Room Temperature

Ca‐ion based devices are promising candidates for next‐generation energy storage with high performance and low cost, thanks to its multielectrons, superior kinetics, as well as abundance (2500 times lithium). Because of the lack of an appropriate combination of suitable electrode materials and electrolytes, it is unsuccessful to attain a satisfactory performance on complete Ca‐ion energy storage devices. Here, the multiion reaction strategy is defined to construct a complete Ca‐ion energy storage device and a capacitor–battery hybrid mechanism is deliberately adopted. Profiting from the elaborate design, it exhibits a high reversible capacity of 92 mAh g^?1, unmatchable rate capability, and a high capacity retention of 84% over 1000 cycles under room temperature, which is the best performance of reported Ca‐based energy storage devices.     

3D Nanostructures for the Next Generation of High‐Performance Nanodevices for Electrochemical Energy Conversion and Storage

Among the different nanostructures that have been demonstrated as promising materials for various applications, 3D nanostructures have attracted significant attention as building blocks for constructing high‐performance nanodevices. Particularly over the last decade, considerable research efforts have been devoted to designing, fabricating, and evaluating 3D nanostructures as electrodes for electrochemical energy conversion and storage devices. Although remarkable progress has been achieved, the performance of electrochemical energy devices based on 3D nanostructures in terms of energy conversion efficiency, energy storage capability, and device reliability still needs to be significantly improved to meet the requirements for practical applications. Rather than simply outlining and comparing different 3D nanostructures, this article systematically summarizes the general advantages as well as the existing and future challenges of 3D nanostructures for electrochemical energy conversion and storage, focusing on photoelectrochemical water splitting, photoelectrocatalytic solar‐to‐fuels conversion from nitrogen and carbon dioxide, rechargeable metal‐ion batteries, and supercapacitors. A comprehensive understanding of these advantages and challenges shall provide valuable guidelines and enlightenments to facilitate the further development of 3D nanostructured materials, and contribute to the achieving more efficient energy conversion and storage technologies toward a sustainable energy future.     

A Particle‐Controlled,High‐Performance,Gum‐Like Electrolyte for Safe and Flexible Energy Storage Devices

Storing energy within flexible and safe materials is one of the most important goals for energy storage devices. To that end, high‐performance conformable electrolytes, which can transport ions quickly and safely, and can also effectively separate and bond strongly to the two electrodes, are of great importance. However, it is challenging to develop an electrolyte that can play these multiple roles simultaneously. Here, aiming to overcome this challenge, a particle‐based approach to the fabrication of a high‐performance, gum‐like electrolyte is described. The intriguing properties of the gum‐like electrolyte include high ionic conductivity, good mechanical properties, excellent adhesion properties, and, more importantly, thermal‐protection capability. It is shown that these significant properties are well‐controlled by the incorporation of wax particles with variable size, loading, and surface properties that can be designed through the use of an apporpriate surfactant. This provides a promising solution for high‐performance electrolytes and indicates a cost‐effective approach to fabricating multifunctional ion‐conducting materials.     

Flexible Pseudocapacitive Electrochromics via Inkjet Printing of Additive‐Free Tungsten Oxide Nanocrystal Ink

Direct inkjet printing of functional inks is an emerging and promising technique for the fabrication of electrochemical energy storage devices. Electrochromic energy devices combine electrochromic and energy storage functions, providing a rising and burgeoning technology for next‐generation intelligent power sources. However, printing such devices has, in the past, required additives or other second phase materials in order to create inks with suitable rheological properties, which can lower printed device performance. Here, tungsten oxide nanocrystal inks are formulated without any additives for the printing of high‐quality tungsten oxide thin films. This allows the assembly of novel electrochromic pseudocapacitive zinc‐ion devices, which exhibit a relatively high capacity (≈260 C g^?1 at 1 A g^?1) with good cycling stability, a high coloration efficiency, and fast switching response. These results validate the promising features of inkjet‐printed electrochromic zinc‐ion energy storage devices in a wide range of applications in flexible electronic devices, energy‐saving buildings, and intelligent systems.     

Controllable ZnMgO Electron‐Transporting Layers for Long‐Term Stable Organic Solar Cells with 8.06% Efficiency after One‐Year Storage

Currently, one main challenge in organic solar cells (OSCs) is to achieve both good stability and high power conversion efficiencies (PCEs). Here, highly efficient and long‐term stable inverted OSCs are fabricated by combining controllable ZnMgO (ZMO) cathode interfacial materials with a polymer:fullerene bulk‐heterojunction. The resulting devices based on the nanocolloid/nanoridge ZMO electron‐transporting layers (ETLs) show greatly enhanced performance compared to that of the conventional devices or control devices without ZMO or with ZnO ETLs. The ZMO‐based OSCs maintain 84%–93% of their original PCEs over 1‐year storage under ambient conditions. An initial PCE of 9.39% is achieved for the best device, and it still retains a high PCE of 8.06% after 1‐year storage, which represents a record high value for long‐term stable OSCs. The excellent performance is attributed to the enhanced electron transportation/collection, reduced interfacial energy losses, and improved stability of the nanocolloid ZMO ETL. These findings provide a promising way to develop OSCs with high efficiencies and long device lifetime towards practical applications.     

Hollow Carbon Spheres and Their Hybrid Nanomaterials in Electrochemical Energy Storage

Electrochemical energy storage is of extraordinary importance for fulfilling the utilization of renewable and sustainable energy sources. There is an increasing demand for energy storage devices with high energy and power densities, prolonged stability, safety, and low cost. In the past decade, numerous research efforts have been devoted to achieving these requirements, especially in the design of advanced electrode materials. Hollow carbon spheres (HCS) derived nanomaterials combining the advantages of 3D HCS and porous structures have been considered as alternative electrode materials for advanced energy storage applications, due to their unique features such as high surface‐to‐volume ratios, encapsulation capability, together with outstanding chemical and thermal stability. In this review, the authors first present a comprehensive overview of the synthetic strategies of HCS, and elucidate the design and synthesis of HCS‐derived nanomaterials including various types of HCS and their nanohybrids. Additionally, their significant roles as electrode materials for supercapacitors, lithium‐ion or sodium‐ion batteries, and sulfur hosts for lithium sulfur batteries are highlighted. Finally, current challenges in the synthesis of HCS and future directions in HCS‐derived nanomaterials for energy storage applications are proposed.     

Graphene‐Based Nanocomposites for Energy Storage

Since the first report of using micromechanical cleavage method to produce graphene sheets in 2004, graphene/graphene‐based nanocomposites have attracted wide attention both for fundamental aspects as well as applications in advanced energy storage and conversion systems. In comparison to other materials, graphene‐based nanostructured materials have unique 2D structure, high electronic mobility, exceptional electronic and thermal conductivities, excellent optical transmittance, good mechanical strength, and ultrahigh surface area. Therefore, they are considered as attractive materials for hydrogen (H₂) storage and high‐performance electrochemical energy storage devices, such as supercapacitors, rechargeable lithium (Li)‐ion batteries, Li–sulfur batteries, Li–air batteries, sodium (Na)‐ion batteries, Na–air batteries, zinc (Zn)–air batteries, and vanadium redox flow batteries (VRFB), etc., as they can improve the efficiency, capacity, gravimetric energy/power densities, and cycle life of these energy storage devices. In this article, recent progress reported on the synthesis and fabrication of graphene nanocomposite materials for applications in these aforementioned various energy storage systems is reviewed. Importantly, the prospects and future challenges in both scalable manufacturing and more energy storage‐related applications are discussed.     

Heteroatom‐Doped and Oxygen‐Functionalized Nanocarbons for High‐Performance Supercapacitors

Electrochemical capacitors (best known as supercapacitors) are high‐performance energy storage devices featuring higher capacity than conventional capacitors and higher power densities than batteries, and are among the key enabling technologies of the clean energy future. This review focuses on performance enhancement of carbon‐based supercapacitors by doping other elements (heteroatoms) into the nanostructured carbon electrodes. The nanocarbon materials currently exist in all dimensionalities (from 0D quantum dots to 3D bulk materials) and show good stability and other properties in diverse electrode architectures. However, relatively low energy density and high manufacturing cost impede widespread commercial applications of nanocarbon‐based supercapacitors. Heteroatom doping into the carbon matrix is one of the most promising and versatile ways to enhance the device performance, yet the mechanisms of the doping effects still remain poorly understood. Here the effects of heteroatom doping by boron, nitrogen, sulfur, phosphorus, fluorine, chlorine, silicon, and functionalizing with oxygen on the elemental composition, structure, property, and performance relationships of nanocarbon electrodes are critically examined. The limitations of doping approaches are further discussed and guidelines for reporting the performance of heteroatom doped nanocarbon electrode‐based electrochemical capacitors are proposed. The current challenges and promising future directions for clean energy applications are discussed as well.     

High‐Temperature Shock Enabled Nanomanufacturing for Energy‐Related Applications

Functional nanomaterials are playing a crucial role in the emerging field of energy‐related devices. Recently, as a novel synthesis method, high‐temperature shock (HTS), which is rapid, low cost, eco‐friendly, universal, scalable, and controllable, has provided a promising option for the rational design and synthesis of various high‐quality nanomaterials. In this report, the HTS technique, including the equipment setup and operating principle, is systematically introduced, and recent progress in the synthesis of nanomaterials for energy storage and conversion applications using this HTS method is summarized. The growth mechanisms of nanoparticles and carbonaceous nanomaterials are thoroughly discussed, followed by the summary of the characteristic advantages of the HTS strategy. A series of nanomaterials prepared by the HTS method, including carbon‐based films, metal nanoparticles and compound nanoparticles, show high performance in the diverse applications of storage energy batteries, highly active catalysts, and smart energy devices. Finally, the future perspectives and directions of HTS in nanomanufacturing for broader applications are presented.     

Partial Nitridation‐Induced Electrochemistry Enhancement of Ternary Oxide Nanosheets for Fiber Energy Storage Device

Fiber‐based power sources are receiving interest in terms of application in wearable electronic devices. Herein, fiber‐shaped all‐solid‐state asymmetric energy storage devices are fabricated based on a partially nitridized NiCo₂O₄ hybrid nanostructures on graphite fibers (GFs). The surface nitridation leads to a 3D “pearled‐veil” network structure, in which Ni–Co–N nanospheres are mounted on NiCo₂O₄ nanosheets' electrode. It is demonstrated that the hybrid materials are more potent than the pure NiCo₂O₄ in energy storage applications due to a cooperative effect between the constituents. The Ni–Co–N segments augment the pristine oxide nanosheets by enhancing both capacity and rate performance (a specific capacity of 384.75 mAh g⁻¹ at 4 A g⁻¹, and a capacity retention of 86.5% as the current is increased to 20 A g⁻¹). The whole material system has a metallic conductivity that renders high‐rate charge and discharge, and an extremely soft feature, so that it can wrap around arbitrary‐shaped holders. All‐solid‐state asymmetric device is fabricated using Ni–Co–N/NiCo₂O₄/GFs and carbon nanotubes/GFs as the electrodes. The flexible device delivers outstanding performance compared to most oxide‐based full devices. These structured hybrid materials may find applications in miniaturized foldable energy devices.     

Phase Boundary Derived Pseudocapacitance Enhanced Nickel‐Based Composites for Electrochemical Energy Storage Devices

Several strategies have been employed to improve the performance of energy storage devices through the development of new electrode materials. The construction of transition metal compound composite electrodes plays an important role in promoting the performance of energy storage devices. However, understandings of and insight into how to enhance the composites properties are rarely reported. Taking nickel‐based compounds as an example, Ni₃N@Ni₃S₂ hybrid nanosheets are reported as a high‐performance anode material for lithium‐ion batteries that delivers higher lithium storage properties than the pristine Ni₃N and Ni₃S₂ electrodes. This demonstrates that the phase boundaries between the Ni₃N and Ni₃S₂ may contribute additional lithium storage, which leads to a synergistic effect via the high pseudocapacitance contribution from the outstanding conductivity of Ni₃N and enhanced diffusion‐controlled capacity of Ni₃S₂. The use of composites prepared through sulfuration of hydrothermally annealed nickel hydroxide‐based precursor provides an enhancement of the energy storage properties. These results provide an important approach for increasing the electrochemical activity of composites by the combined effect of interfacial mismatch and pseudocapacitance, as well as understandings of the mechanism of the enhancement of the composite electrode properties.     

Mulberry Paper‐Based Supercapacitor Exhibiting High Mechanical and Chemical Toughness for Large‐Scale Energy Storage Applications

In response to the demand for flexible and sustainable energy storage devices that exhibit high electrochemical performance, a supercapacitor system is fabricated using mulberry tree‐derived paper as a substrate and Poly(3,4‐ethylenedioxythiophene)‐poly(styrenesulfonate) (PEDOT:PSS) and carbon black as the active material. The mulberry paper‐based supercapacitor system demonstrates high energy density of 29.8–39.8 Wh kg^?1 and power density of 2.8–13.9 kW kg^?1 with 90.7% retention of its initial capacity over 15 000 charge–discharge cycles. In addition, the mulberry tree fibers are known to have superior mechanical strength and toughness and the mulberry paper‐based supercapacitor; as a result, exhibit high mechanical and chemical toughness; 99% of its initial capacity is retained after 100 repeated applications of bending strains, and twisting. 94% capacity retention is observed even after exposure to HCl and H₂SO₄ acid solutions. The fabrication methodology of the mulberry‐based supercapacitor is highly scalable and could be stacked to increase the energy storage capacity, where operation of light‐emitting diode lights with a drive voltage of 12 V integrated in a wearable device is demonstrated.     

Nature‐Inspired Electrochemical Energy‐Storage Materials and Devices

Currently, tremendous efforts are being devoted to develop high‐performance electrochemical energy‐storage materials and devices. Conventional electrochemical energy‐storage systems are confronted with great challenges to achieve high energy density, long cycle‐life, excellent biocompatibility and environmental friendliness. The biological energy metabolism and storage systems have appealing merits of high efficiency, sophisticated regulation, clean and renewability, and the rational design and fabrication of advanced electrochemical energy‐storage materials and smart devices inspired by nature have made some breakthrough progresses, recently. In this review, we summarize the latest developments in the field of nature‐inspired electrochemical energy‐storage materials and devices. Specifically, the nature‐inspired exploration, preparation and modification of electrochemical energy‐storage related materials including the active materials, binders, and separators are introduced. Furthermore, nature‐inspired design and fabrication of smart energy‐storage devices such as self‐healing supercapacitors, supercapacitors with ultrahigh operating voltage, and self‐rechargeable batteries are also discussed. The review aims to provide insights and expanded research perspectives for further study in this exciting field based on our comprehensive discussions.     

Liquid–Solid Interfacial Assemblies of Soft Materials for Functional Freestanding Layered Membrane–Based Devices toward Electrochemical Energy Systems

Freestanding layered membrane–based devices have broad applications in highly efficient energy‐storage/conversion systems. The liquid–solid interface is considered as a unique yet versatile interface for constructing such layered membrane–based devices. In this review, the authors outline recent developments in the fabrication of soft materials to functionalize layered devices from the aspect of liquid–solid interfacial assembly and engineering arts. Seven liquid–solid interfacial assembly strategies, including flow‐directed, superlattice, solvent‐casting, evaporation‐induced, dip‐coating, spinning, and electrospinning assemblies, are comprehensively highlighted with a focus on their synthetic pathways, formation mechanisms, and interface engineering strategies. Meanwhile, recent representative works on layered membrane–based devices for electrochemical energy applications are presented. Finally, challenges and opportunities of this research area are highlighted in order to stimulate future developments. This review not only offers comprehensive and practical approaches to assemble liquid–solid interfaces with soft materials for various important layered electrochemical energy devices but also sheds lights on fundamental insights by thoughtful discussions on performance enhancement mechanisms of these electrochemical energy systems.     

Recent Progress in Biomass‐Derived Electrode Materials for High Volumetric Performance Supercapacitors

Tremendous efforts have been spent on the development of electrical energy storage (EES) systems with high volumetric performance in the past few years due to the evergrowing demand of miniaturized, portable electronic devices, and electric vehicles. Among all the EES devices, supercapacitors with electrode materials derived from biosources have attracted special attention due to their eco‐friendliness, natural abundance, their intrinsic porous structures as well as their renewable and sustainable features. However, the relatively low packing densities make their specific volumetric capacitance intrinsically low, which has largely limited their further application in the supercapacitors. To address these issues, various promising approaches ranging from structural manufacture to compositional design are applied and significant breakthroughs are witnessed in recent years. In this progress report, key factors influencing the volumetric performance of biomass‐derived electrode materials are systematically discussed with a particular focus spanning from fundamental to operational aspects. This work provides insights into the development of high‐volumetric‐performance biomass‐derived supercapacitors by comprehensively summarizing recent advances in the rational structural design and fabrication. Perspectives regarding the future challenges and promising research directions on the design of next‐generation EES devices are also provided.     

Layered Oxide Cathodes for Sodium‐Ion Batteries: Phase Transition,Air Stability,and Performance

The increasing demand for replacing conventional fossil fuels with clean energy or economical and sustainable energy storage drives better battery research today. Sodium‐ion batteries (SIBs) are considered as a promising alternative for grid‐scale storage applications due to their similar “rocking‐chair” sodium storage mechanism to lithium‐ion batteries, the natural abundance, and the low cost of Na resources. Searching for appropriate electrode materials with acceptable electrochemical performance is the key point for development of SIBs. Layered transition metal oxides represent one of the most fascinating electrode materials owing to their superior specific capacity, environmental benignity, and facile synthesis. However, three major challenges (irreversible phase transition, storage instability, and insufficient battery performance) are known for cathodes in SIBs. Herein, a comprehensive review on the latest advances and progresses in the exploration of layered oxides for SIBs is presented, and a detailed and deep understanding of the relationship of phase transition, air stability, and electrochemical performance in layered oxide cathodes is provided in terms of refining the structure–function–property relationship to design improved battery materials. Layered oxides will be a competitive and attractive choice as cathodes for SIBs in next‐generation energy storage devices.     

Applications of Phosphorene and Black Phosphorus in Energy Conversion and Storage Devices

The successful isolation of phosphorene (atomic layer thick black phosphorus) in 2014 has currently aroused the interest of 2D material researchers. In this review, first, the fundamentals of phosphorus allotropes, phosphorene, and black phosphorus, are briefly introduced, along with their structures, properties, and synthesis methods. Second, the readers are presented with an overview of their energy applications. Particularly in electrochemical energy storage, the large interlayer spacing (0.53 nm) in phosphorene allows the intercalation/deintercalation of larger ions as compared to its graphene counterpart. Therefore, phosphorene may possess greater potential for high electrochemical performance. In addition, the status of lithium ion batteries as well as secondary sodium ion batteries is reviewed. Next, each application for energy generation, conversion, and storage is described in detail with milestones as well as the challenges. These emerging applications include supercapacitors, photovoltaic devices, water splitting, photocatalytic hydrogenation, oxygen evolution, and thermoelectric generators. Finally the fast‐growing dynamic field of phosphorene research is summarized and perspectives on future possibilities are presented calling on the efforts of chemists, physicists, and material scientists