The ever-increasing energy demand motivates the pursuit of inexpensive, safe, scalable, and high-performance rechargeable batteries. Carbon materials have been intensively investigated as electrode ...materials for various batteries on account of their resource abundance, low cost, nontoxicity, and diverse electrochemistry. Taking use of the reversible donor-type cation intercalation/de-intercalation (including Li
+
, Na
+
, and K
+
) at low redox potentials, carbon materials can serve as ideal anodes for 'Rocking-Chair' alkali metal-ion batteries. Meanwhile, acceptor-type intercalation of anions into graphitic carbon materials has also been revealed to be a facile, reversible process at high redox potentials. Based on anion-intercalation graphitic carbon materials, a number of dual-ion battery and Al-ion battery technologies are experiencing booming development. In this review, we summarize the significant advances of carbon materials in terms of the porous structure, chemical composition, and interlayer spacing control. Fundamental mechanisms of carbon materials as the cation host and anion host are further revisited by elaborating the electrochemistry, intercalant effect, and intercalation form. Subsequently, the recent progress in the development of novel carbon nanostructures and carbon-derived energy storage devices is presented with particular emphasis on correlating the structures with electrochemical properties as well as assessing the device configuration, electrochemical reaction, and performance metric. Finally, perspectives on the remaining challenges are provided, which will accelerate the development of new carbon material concepts and carbon-derived battery technologies towards commercial implementation.
The development of carbon electrode materials for rechargeable batteries is reviewed from the perspective of structural features, electrochemistry, and devices.
Following a 15-year-long investigation on graphene, two-dimensional (2D) carbon-rich conjugated frameworks (CCFs) have attracted growing research interest as a new generation of multifunctional ...materials. Typical 2D CCFs include 2D π-conjugated polymers (also classified as 2D π-conjugated covalent organic frameworks) and 2D π-conjugated metal–organic frameworks, which are characterized by layer-stacked periodic frameworks with high in-plane π-conjugation. These unique structures endow 2D CCFs with regular porosities, large specific surface areas, and superior chemical stability. In addition, 2D CCFs exhibit certain notable properties (e.g., excellent electronic conductivity, designable topologies, and defined catalytic/redox-active sites), which have motivated increasing efforts to explore 2D CCFs for electrochemical energy applications. In this Perspective, the structural features and synthetic principles of 2D CCFs are briefly introduced. Moreover, we discuss recent achievements in 2D CCFs designed for various electrochemical energy conversion (electrocatalysis) and storage (supercapacitors and batteries) applications. Particular emphasis is placed on analyzing the precise structural regulation of 2D CCFs. Finally, we provide an outlook about the future development of synthetic 2D CCFs for electrochemical applications, which concerns novel monomer design, chemical methodology/strategy establishment, and a roadmap toward practical applications.
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IJS, KILJ, NUK, PNG, UL, UM
To keep pace with the increasing pursuit of portable and wearable electronics, it is urgent to develop advanced flexible power supplies. In this context, Zn‐ion batteries (ZIBs) have garnered ...increasing attention as favorable energy storage devices for flexible electronics, owing to the high capacity, low cost, abundant resources, high safety, and eco‐friendliness. Extensive efforts have been devoted to developing flexible ZIBs in the last few years. This work summarizes the recent achievements in the design, fabrication, and characterization of flexible ZIBs. Representative structures, such as sandwich and cable type, are particularly highlighted. Special emphasis is put on the novel design of electrolyte and electrode, which aims to endow reliable flexibility to the fabricated ZIBs. Moreover, current challenges and future opportunities for the development of high‐performance flexible ZIBs are also outlined.
The recent development of electrode materials, gel electrolytes, and device configurations for flexible zinc‐ion batteries (ZIBs) is reviewed. Recent progresses in flexible ZIBs are discussed by briefly categorizing into Zn–Mn based, Zn–V based, Zn–Prussian blue analog based, and the other ZIBs. The current challenges and future opportunities for the development of flexible ZIBs are also discussed.
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BFBNIB, FZAB, GIS, IJS, KILJ, NLZOH, NUK, OILJ, SBCE, SBMB, UL, UM, UPUK
Employing high-rate ion-intercalation electrodes represents a feasible way to mitigate the inherent trade-off between energy density and power density for electrochemical energy storage devices, but ...efficient approaches to boost the charge-storage kinetics of electrodes are still needed. Here, we demonstrate a water-incorporation strategy to expand the interlayer gap of α-MoO
, in which water molecules take the place of lattice oxygen of α-MoO
. Accordingly, the modified α-MoO
electrode exhibits theoretical-value-close specific capacity (963 C g
at 0.1 mV s
), greatly improved rate capability (from 4.4% to 40.2% at 100 mV s
) and boosted cycling stability (from 21 to 71% over 600 cycles). A fast-kinetics dual-ion-intercalation energy storage device is further assembled by combining the modified α-MoO
anode with an anion-intercalation graphite cathode, operating well over a wide discharge rate range. Our study sheds light on a promising design strategy of layered materials for high-kinetics charge storage.
Supercapacitors (SCs) have great promise as the state‐of‐the‐art power source in portable electronics and hybrid vehicles. The performance of SCs is largely determined by the properties of the ...electrode material, and numerous efforts have been devoted to the explorations of novel electrode materials. Recently, iron‐based materials, including Fe2O3, Fe3O4, FeOOH, FeOx, CoFe2O4, and MnFe2O4, have received considerable attention as very promising electrode materials for SCs due to their high theoretical specific capacitances, natural abundance, low cost, and non‐toxicity. However, most of these Fe‐based SC electrodes suffer from poor conductivity and/or electrochemical instability, which seriously impede their implementation as high‐performance electrodes for SCs. To settle these issues, substantial efforts have been made in improving their conductivity and cycling stability, and great processes have been achieved. Here, recent research advances in the rational design and synthesis of diverse Fe‐based nanostructured electrodes and their capacitive performance for SCs are presented. Besides, challenges and prospects of Fe‐based materials as advanced negative electrodes for SCs are also discussed.
Recent research advances in the rational design and fabrication of nanostructured iron‐based materials (e.g., single iron metal oxides/hydroxides: Fe2O3, Fe3O4, FeOOH, etc., and binary metal oxides: CoFe2O4, NiFe2O4, etc.) as advanced negative electrodes for supercapacitors is highlighted. Moreover, the current challenges and future prospects of iron‐based negative electrodes in the development of high‐performance supercapacitors are also discussed.
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FZAB, GIS, IJS, KILJ, NLZOH, NUK, OILJ, SBCE, SBMB, UL, UM, UPUK
Advanced flexible batteries with high energy density and long cycle life are an important research target. Herein, the first paradigm of a high‐performance and stable flexible rechargeable ...quasi‐solid‐state Zn–MnO2 battery is constructed by engineering MnO2 electrodes and gel electrolyte. Benefiting from a poly(3,4‐ethylenedioxythiophene) (PEDOT) buffer layer and a Mn2+‐based neutral electrolyte, the fabricated Zn–MnO2@PEDOT battery presents a remarkable capacity of 366.6 mA h g−1 and good cycling performance (83.7% after 300 cycles) in aqueous electrolyte. More importantly, when using PVA/ZnCl2/MnSO4 gel as electrolyte, the as‐fabricated quasi‐solid‐state Zn–MnO2@PEDOT battery remains highly rechargeable, maintaining more than 77.7% of its initial capacity and nearly 100% Coulombic efficiency after 300 cycles. Moreover, this flexible quasi‐solid‐state Zn–MnO2 battery achieves an admirable energy density of 504.9 W h kg−1 (33.95 mW h cm−3), together with a peak power density of 8.6 kW kg−1, substantially higher than most recently reported flexible energy‐storage devices. With the merits of impressive energy density and durability, this highly flexible rechargeable Zn–MnO2 battery opens new opportunities for powering portable and wearable electronics.
A highly flexible rechargeable quasi‐solid‐state Zn–MnO2@PEDOT battery is demonstrated for the first time. The battery affords a prominent energy density of 504.9 W h kg−1 (33.95 mW h cm−3), substantially outstripping most of the recently reported batteries and supercapacitors. Additionally, benefiting from a protective layer and modified electrolyte, such a Zn–MnO2@PEDOT battery delivers a good durability of 77.7% after 300 cycles.
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BFBNIB, FZAB, GIS, IJS, KILJ, NLZOH, NUK, OILJ, SBCE, SBMB, UL, UM, UPUK
A facile and efficient electrochemical oxidation method to directly activated carbon cloth as an excellent electrode material for supercapacitors is reported. Flexible asymmetric supercapacitor ...devices based on activated carbon cloth anodes reach a remarkable energy density and excellent long‐term durability.
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BFBNIB, FZAB, GIS, IJS, KILJ, NLZOH, NUK, OILJ, SBCE, SBMB, UL, UM, UPUK
The kinetically sluggish rate of oxygen reduction reaction (ORR) on the cathode side is one of the main bottlenecks of zinc‐air batteries (ZABs), and thus the search for an efficient and ...cost‐effective catalyst for ORR is highly pursued. Co3O4 has received ever‐growing interest as a promising ORR catalyst due to the unique advantages of low‐cost, earth abundance and decent catalytic activity. However, owing to the poor conductivity as a result of its semiconducting nature, the ORR activity of the Co3O4 catalyst is still far below the expectation. Herein, we report a controllable N‐doping strategy to significantly improve the catalytic activity of Co3O4 for ORR and demonstrate these N doped Co3O4 nanowires as an additive‐free air‐cathode for flexible solid‐state zinc‐air batteries. The results of experiments and DFT calculations reveal that the catalytic activity is promoted by the N dopant through a combined set of factors, including enhanced electronic conductivity, increased O2 adsorption strength and improved reaction kinetics. Finally, the assembly of all‐solid‐state ZABs based on the optimized cathode exhibit a high volumetric capacity of 98.1 mAh cm‐3 and outstanding flexibility. The demonstration of such flexible ZABs provides valuable insights that point the way to the redesign of emerging portable electronics.
A novel additive‐free design of the air‐cathode for flexible zinc–air batteries consists of directly growing and neatly assembling mesoporous Co3O4 nanowires on a carbon cloth. To optimize the catalytic activity of Co3O4 for the oxygen reduction reaction, a controllable N‐doping strategy is developed giving rise to enhanced electronic conductivity and increased O2 adsorption strength.
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BFBNIB, FZAB, GIS, IJS, KILJ, NLZOH, NUK, OILJ, SBCE, SBMB, UL, UM, UPUK
Currently, the main bottleneck for the widespread application of Ni–Zn batteries is their poor cycling stability as a result of the irreversibility of the Ni‐based cathode and dendrite formation of ...the Zn anode during the charging–discharging processes. Herein, a highly rechargeable, flexible, fiber‐shaped Ni–Zn battery with impressive electrochemical performance is rationally demonstrated by employing Ni–NiO heterostructured nanosheets as the cathode. Benefiting from the improved conductivity and enhanced electroactivity of the Ni–NiO heterojunction nanosheet cathode, the as‐fabricated fiber‐shaped Ni–NiO//Zn battery displays high capacity and admirable rate capability. More importantly, this Ni–NiO//Zn battery shows unprecedented cyclic durability both in aqueous (96.6% capacity retention after 10 000 cycles) and polymer (almost no capacity attenuation after 10 000 cycles at 22.2 A g−1) electrolytes. Moreover, a peak energy density of 6.6 µWh cm−2, together with a remarkable power density of 20.2 mW cm−2, is achieved by the flexible quasi‐solid‐state fiber‐shaped Ni–NiO//Zn battery, outperforming most reported fiber‐shaped energy‐storage devices. Such a novel concept of a fiber‐shaped Ni–Zn battery with impressive stability will greatly enrich the flexible energy‐storage technologies for future portable/wearable electronic applications.
An ultrastable, flexible fiber‐shaped Ni–Zn battery with impressive electrochemical performance is rationally demonstrated by employing Ni–NiO heterostructured nanosheets as the cathode. This Ni–NiO//Zn battery exhibits unprecedented cyclic durability both in aqueous (96.6% capacity retention after 10 000 cycles) and polymer (almost no capacity attenuation after 10 000 cycles at 22.2 A g−1) electrolytes.
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BFBNIB, FZAB, GIS, IJS, KILJ, NLZOH, NUK, OILJ, SBCE, SBMB, UL, UM, UPUK
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