In‐Plane Assembled Orthorhombic Nb2O5 Nanorod Films with High‐Rate Li+ Intercalation for High‐Performance Flexible Li‐Ion Capacitors

Organic hybrid supercapacitors that consist of a battery electrode and a capacitive electrode show greatly improved energy density, but their power density is generally limited by the poor rate capability of battery‐type electrodes. In addition, flexible organic hybrid supercapacitors are rarely reported. To address the above issues, herein an in‐plane assembled orthorhombic Nb₂O₅ nanorod film anode with high‐rate Li⁺ intercalation to develop a flexible Li‐ion hybrid capacitor (LIC) is reported. The binder‐/additive‐free film exhibits excellent rate capability (≈73% capacity retention with the rate increased from 0.5 to 20 C) and good cycling stability (>2500 times). Kinetic analyses reveal that the high rate performance is mainly attributed to the excellent in‐plane assembly of interconnected single‐crystalline Nb₂O₅ nanorods on the current collector, ensuring fast electron transport, facile Li‐ion migration in the porous film, and greatly reduced ion‐diffusion length. Using such a Nb₂O₅ film as anode and commercial activated carbon as cathode, a flexible LIC is designed. It delivers both high gravimetric and high volumetric energy/power densities (≈95.55 Wh kg^?1/5350.9 W kg^?1; 6.7 mW h cm^?3/374.63 mW cm^?3), surpassing previous typical Li‐intercalation electrode‐based LICs. Furthermore, this LIC device still keeps good electrochemical attributes even under serious bending states (30°–180°).     

Fast and Large Lithium Storage in 3D Porous VN Nanowires–Graphene Composite as a Superior Anode Toward High‐Performance Hybrid Supercapacitors

Li‐ion hybrid capacitors (LIHCs), consisting of an energy‐type redox anode and a power‐type double‐layer cathode, are attracting significant attention due to the good combination with the advantages of conventional Li‐ion batteries and supercapacitors. However, most anodes are battery‐like materials with the sluggish kinetics of Li‐ion storage, which seriously restrict the energy storage of LIHCs at the high charge/discharge rates. Herein, vanadium nitride (VN) nanowire is demonstated to have obvious pseudocapacitive characteristic of Li‐ion storage and can get further gains in energy storage through a 3D porous architecture with the assistance of conductive reduced graphene oxide (RGO). The as‐prepared 3D VN–RGO composite exhibits the large Li‐ion storage capacity and fast charge/discharge rate within a wide working widow from 0.01–3 V (vs Li/Li⁺), which could potentially boost the operating potential and the energy and power densities of LIHCs. By employing such 3D VN–RGO composite and porous carbon nanorods with a high surface area of 3343 m² g^?1 as the anode and cathode, respectively, a novel LIHCs is fabricated with an ultrahigh energy density of 162 Wh kg^?1 at 200 W kg^?1, which also remains 64 Wh kg^?1 even at a high power density of 10 kW kg^?1.     

Fe2O3 Nanoneedles on Ultrafine Nickel Nanotube Arrays as Efficient Anode for High‐Performance Asymmetric Supercapacitors

High performance of electrochemical energy storage devices depends on the smart structure engineering of electrodes, including the tailored nanoarchitectures of current collectors and subtle hybridization of active materials. To improve the anode supercapacitive performance of Fe₂O₃ for high‐voltage asymmetric supercapacitors, here, a hybrid core‐branch nanoarchitecture is proposed by integrating Fe₂O₃ nanoneedles on ultrafine Ni nanotube arrays (NiNTAs@Fe₂O₃ nanoneedles). The fabrication process employs a bottom‐up strategy via a modified template‐assisted method starting from ultrafine ZnO nanorod arrays, ensuring the formation of ultrafine Ni nanotube arrays with ultrathin tube walls. The novel developed NiNTAs@Fe₂O₃ nanoneedle electrode is demonstrated to be a highly capacitive anode (418.7 F g^?1 at 10 mV s^?1), matching well with the similarly built NiNTAs@MnO₂ nanosheet cathode. Contributed by the efficient electron collection paths and short ion diffusion paths in the uniquely designed anode and cathode, the asymmetric supercapacitors exhibit an excellent maximum energy density of 34.1 Wh kg^?1 at the power density of 3197.7 W kg^?1 in aqueous electrolyte and 32.2 Wh kg^?1 at the power density of 3199.5 W kg^?1 in quasi‐solid‐state gel electrolyte.     

Oxygen Vacancy Modulation of Bimetallic Oxynitride Anodes toward Advanced Li‐Ion Capacitors

Binary metal oxides (such as NiCo₂O₄) are regarded as attractive electrode materials for advanced energy storage devices since they offer more electrochemical activity and higher capacity than monometal oxide. However, the volume expansion and low electronic conductivity are the main bottleneck seriously hindering their application. To overcome these barriers, a novel strategy that introduces a bimetallic oxynitride layer (NiCoON) with oxygen vacancy to the surface of NiCo₂O₄ nanowires as an anode for Li‐ion capacitors (LICs) is proposed. The oxygen vacancy on the surface and the modulation of multiple valence states are investigated by the electron paramagnetic resonance, X‐ray photoelectron spectroscopy characterization, and first‐principles calculation. Benefiting from the merits of substantially improved electrical conductivity and increased concentration of active sites, the optimized NiCoON electrode delivers remarkable capacity (1855 mAh g^?1 at 0.2 A g^?1) and rate performance. The LIC device assembled by NiCoON anodes and N‐doped carbon nanowire cathodes delivers excellent rate capability, high energy density (148.5 Wh kg^?1), and outstanding power density (30 kW kg^?1). This study provides a new pathway for developing bimetallic oxides with an improved performance in electrochemical energy storage, conversion fields, and beyond.     

Understanding the Charge Storage Mechanism to Achieve High Capacity and Fast Ion Storage in Sodium‐Ion Capacitor Anodes by Using Electrospun Nitrogen‐Doped Carbon Fibers

Microporous nitrogen‐rich carbon fibers (HAT‐CNFs) are produced by electrospinning a mixture of hexaazatriphenylene‐hexacarbonitrile (HAT‐CN) and polyvinylpyrrolidone and subsequent thermal condensation. Bonding motives, electronic structure, content of nitrogen heteroatoms, porosity, and degree of carbon stacking can be controlled by the condensation temperature due to the use of the HAT‐CN with predefined nitrogen binding motives. The HAT‐CNFs show remarkable reversible capacities (395 mAh g^?1 at 0.1 A g^?1) and rate capabilities (106 mAh g^?1 at 10 A g^?1) as an anode material for sodium storage, resulting from the abundant heteroatoms, enhanced electrical conductivity, and rapid charge carrier transport in the nanoporous structure of the 1D fibers. HAT‐CNFs also serve as a series of model compounds for the investigation of the contribution of sodium storage by intercalation and reversible binding on nitrogen sites at different rates. There is an increasing contribution of intercalation to the charge storage with increasing condensation temperature which becomes less active at high rates. A hybrid sodium‐ion capacitor full cell combining HAT‐CNF as the anode and salt‐templated porous carbon as the cathode provides remarkable performance in the voltage range of 0.5–4.0 V (95 Wh kg^?1 at 0.19 kW kg^?1 and 18 Wh kg^?1 at 13 kW kg^?1).     

All‐Cellulose‐Based Quasi‐Solid‐State Sodium‐Ion Hybrid Capacitors Enabled by Structural Hierarchy

Na‐ion hybrid capacitors consisting of battery‐type anodes and capacitor‐style cathodes are attracting increasing attention on account of the abundance of sodium‐based resources as well as the potential to bridge the gap between batteries (high energy) and supercapacitors (high power). Herein, hierarchically structured carbon materials inspired by multiscale building units of cellulose from nature are assembled with cellulose‐based gel electrolytes into Na‐ion capacitors. Nonporous hard carbon anodes are obtained through the direct thermal pyrolysis of cellulose nanocrystals. Nitrogen‐doped carbon cathodes with a coral‐like hierarchically porous architecture are prepared via hydrothermal carbonization and activation of cellulose microfibrils. The reversible charge capacity of the anode is 256.9 mAh g^?1 when operating at 0.1 A g^?1 from 0 to 1.5 V versus Na⁺/Na, and the discharge capacitance of cathodes tested within 1.5 to 4.2 V versus Na⁺/Na is 212.4 F g^?1 at 0.1 A g^?1. Utilizing Na⁺ and ClO₄^? as charge carriers, the energy density of the full Na‐ion capacitor with two asymmetric carbon electrodes can reach 181 Wh kg^?1 at 250 W kg^?1, which is one of the highest energy devices reported until now. Combined with macrocellulose‐based gel electrolytes, all‐cellulose‐based quasi‐solid‐state devices are demonstrated possessing additional advantages in terms of overall sustainability.     

Empowering Metal Phosphides Anode with Catalytic Attribute toward Superior Cyclability for Lithium‐Ion Storage

Due to high capacity, moderate redox voltage, and relatively low polarization, metal phosphides (MPs) attract much attention as viable anode materials for lithium‐ion storage. However, severe capacity decay induced by the poor reversibility of discharge product (Li₃P) in these anodes suppresses their practical applications. Herein, it is first revealed that N‐doped carbon can effectively catalyze the oxidation of Li₃P by density functional theory calculations and activation experiments. By anchoring Ni₂P nanoparticles on N‐doped carbon sheets (Ni₂P@N‐C) via a facile method, an MP‐based anode rendered with a catalytic attribute is successfully fabricated for improving the reversibility of Li₃P during lithium‐ion storage. Benefiting from this design, not only can high capacity and rate performance be reached, but also an extraordinary cyclability and capacity retention be realized, which is the best among all other phosphides reported so far. By employing such a Ni₂P@N‐C composite and a commercialized active carbon as the anode and cathode, respectively, hybrid lithium‐ion capacitors can be fabricated with an ultrahigh energy density of 80 Wh kg^?1 at a power density of 12.5 kW kg^?1. This strategy of designing electrodes may be generalized to other energy storage systems whose cycling performance needs to be improved.     

A High‐Energy Li‐Ion Battery Using a Silicon‐Based Anode and a Nano‐Structured Layered Composite Cathode

High capacity electrodes based on a Si composite anode and a layered composite oxide cathode, Ni‐rich Li[Ni_0.75Co_0.1Mn_0.15]O₂, are evaluated and combined to fabricate a high energy lithium ion battery. The Si composite anode, Si/C‐IWGS (internally wired with graphene sheets), is prepared by a scalable sol–gel process. The Si/C‐IWGS anode delivers a high capacity of >800 mAh g^?1 with an excellent cycling stability of up to 200 cycles, mainly due to the small amount of graphene (～6 wt%). The cathode (Li[Ni_0.75Co_0.1Mn_0.15]O₂) is structurally optimized (Ni‐rich core and a Ni‐depleted shell with a continuous concentration gradient between the core and shell, i.e., a full concentration gradient, FCG, cathode) so as to deliver a high capacity (>200 mAh g^?1) with excellent stability at high voltage (～4.3 V). A novel lithium ion battery system based on the Si/C‐IWGS anode and FCG cathode successfully demonstrates a high energy density (240 Wh kg^?1 at least) as well as an unprecedented excellent cycling stability of up to 750 cycles between 2.7 and 4.2 V at 1C. As a result, the novel battery system is an attractive candidate for energy storage applications demanding a high energy density and long cycle life.     

Metal–Organic Framework (MOF) Derived Electrodes with Robust and Fast Lithium Storage for Li‐Ion Hybrid Capacitors

Hybrid metal–organic frameworks (MOFs) demonstrate great promise as ideal electrode materials for energy‐related applications. Herein, a well‐organized interleaved composite of graphene‐like nanosheets embedded with MnO₂ nanoparticles (MnO₂@C‐NS) using a manganese‐based MOF and employed as a promising anode material for Li‐ion hybrid capacitor (LIHC) is engineered. This unique hybrid architecture shows intriguing electrochemical properties including high reversible specific capacity 1054 mAh g^?1 (close to the theoretical capacity of MnO₂, 1232 mAh g^?1) at 0.1 A g^?1 with remarkable rate capability and cyclic stability (90% over 1000 cycles). Such a remarkable performance may be assigned to the hierarchical porous ultrathin carbon nanosheets and tightly attached MnO₂ nanoparticles, which provide structural stability and low contact resistance during repetitive lithiation/delithiation processes. Moreover, a novel LIHC is assembled using a MnO₂@C‐NS anode and MOF derived ultrathin nanoporous carbon nanosheets (derived from other potassium‐based MOFs) cathode materials. The LIHC full‐cell delivers an ultrahigh specific energy of 166 Wh kg^?1 at 550 W kg^?1 and maintained to 49.2 Wh kg^?1 even at high specific power of 3.5 kW kg^?1 as well as long cycling stability (91% over 5000 cycles). This work opens new opportunities for designing advanced MOF derived electrodes for next‐generation energy storage devices.     

Designing 3D Biomorphic Nitrogen‐Doped MoSe2/Graphene Composites toward High‐Performance Potassium‐Ion Capacitors

Potassium‐ion hybrid capacitors (KICs) reconciling the advantages of batteries and supercapacitors have stimulated growing attention for practical energy storage because of the high abundance and low cost of potassium sources. Nevertheless, daunting challenge remains for developing high‐performance potassium accommodation materials due to the large radius of potassium ions. Molybdenum diselenide (MoSe₂) has recently been recognized as a promising anode material for potassium‐ion batteries, achieving high capacity and favorable cycling stability. However, KICs based on MoSe₂ are scarcely demonstrated by far. Herein, a diatomite‐templated synthetic strategy is devised to fabricate nitrogen‐doped MoSe₂/graphene (N‐MoSe₂/G) composites with favorable pseudocapacitive potassium storage targeting a superior anode material for KICs. Benefiting from the unique biomorphic structure, high electron/K‐ion conductivity, enriched active sites, and the conspicuous pseudocapacitive effect of N‐MoSe₂/G, thus‐derived KIC full‐cell manifests high energy/power densities (maximum 119 Wh kg^?1/7212 W kg^?1), outperforming those of recently reported KIC counterparts. Furthermore, the potassium storage mechanism of N‐MoSe₂/G composite is systematically explored with the aid of first‐principles calculations in combination of in situ X‐ray diffraction and ex situ Raman spectroscopy/transmission electron microscopy/X‐ray photoelectron spectroscopy.     

Kinetics Enhanced Nitrogen‐Doped Hierarchical Porous Hollow Carbon Spheres Boosting Advanced Potassium‐Ion Hybrid Capacitors

Potassium‐ion hybrid capacitors (PIHCs) shrewdly combine a battery‐type anode and a capacitor‐type cathode, exhibiting an energy density close to that of potassium ion batteries and a comparable power density of supercapacitors. However, the rosy scenario is compromised by the sluggish kinetics in the PIHCs device. Herein, the kinetics enhanced nitrogen‐doped hierarchical porous hollow carbon spheres (NHCS) are synthesized and successfully applied to PIHCs. As for the K half‐cell, NHCS anchored with sodium alginate delivers excellent electrochemical performance. Further evaluation shows that the binder can significantly affect the potassium storage performance of NHCS by adjusting the coatability and ionic conductivity of the NHCS anode. Moreover, kinetic analysis and density functional theory calculations reveal the origin of the superior electrochemical properties of NHCS. As expected, an advanced PIHC device is assembled with a NHCS anode and an activated NHCS cathode, demonstrating an exceptionally high energy/power density (114.2 Wh kg^?1 and 8203 W kg^?1), along with a long‐life capability. The successful construction of high‐performance PIHCs in this work opens a new avenue for the development and application of PIHCs in the future.     

Electrochemically Derived Graphene‐Like Carbon Film as a Superb Substrate for High‐Performance Aqueous Zn‐Ion Batteries

3D graphene, as a light substrate for active loadings, is essential to achieve high energy density for aqueous Zn‐ion batteries, yet traditional synthesis routes are inefficient with high energy consumption. Reported here is a simplified procedure to transform the raw graphite paper directly into the graphene‐like carbon film (GCF). The electrochemically derived GCF contains a 2D–3D hybrid network with interconnected graphene sheets, and offers a highly porous structure. To realize high energy density, the Na:MnO₂/GCF cathode and Zn/GCF anode are fabricated by electrochemical deposition. The GCF‐based Zn‐ion batteries deliver a high initial discharge capacity of 381.8 mA h g^?1 at 100 mA g^?1 and a reversible capacity of 188.0 mA h g^?1 after 1000 cycles at 1000 mA g^?1. Moreover, a recorded energy density of 511.9 Wh kg^?1 is obtained at a power density of 137 W kg^?1. The electrochemical kinetics measurement reveals the high capacitive contribution of the GCF and a co‐insertion/desertion mechanism of H⁺ and Zn²⁺ ions. First‐principles calculations are also carried out to investigate the effect of Na⁺ doping on the electrochemical performance of layered δ‐MnO₂ cathodes. The results demonstrate the attractive potential of the GCF substrate in the application of the rechargeable batteries.     

An Ultrastable Nonaqueous Potassium‐Ion Hybrid Capacitor

Potassium‐ion hybrid capacitors (PIHCs) show great potential in large‐scale energy storage due to the advantages of electrochemical capacitors and potassium‐ion batteries. However, their development remains at the preliminary stage and is mainly limited by the kinetic imbalance between the two electrodes. Herein, an architecture of NbSe₂ nanosheets embedded in N, Se co‐doped carbon nanofibers (NbSe₂/NSeCNFs) as flexible, free‐standing, and binder‐free anodes for PIHCs is reported. The NbSe₂/NSeCNFs with hierarchically porous structure and N, Se co‐doping afford highly efficient channels for fast transportation of potassium ions and electrons during repeated cycling process. Furthermore, excellent electrochemical reversibility of the NbSe₂/NSeCNFs electrode is demonstrated through in situ XRD, in situ Raman, ex situ transmission electron microscopy and element mapping. Thus, PIHCs with the NbSe₂/NSeCNFs anode and active carbon cathode achieve a high energy of 145 W h kg^?1 at a current density of 50 mA g^?1, as well as an ultra‐long cycle life of over 10 000 cycles at a high current density of 2 A g^?1. These results indicate that the assembled PIHCs display great potential for applications in the field of ultra‐long cycling energy storage devices.     

Dual‐Salt Mg‐Based Batteries with Conversion Cathodes

Mg batteries as the most typical multivalent batteries are attracting increasing attention because of resource abundance, high volumetric energy density, and smooth plating/stripping of Mg anodes. However, current limitations for the progress of Mg batteries come from the lack of high voltage electrolytes and fast Mg‐insertable structure prototypes. In order to improve their energy or power density, hybrid systems combining Li‐driven cathode reaction with Mg anode process appear to be a potential solution by bypassing the aforementioned limitations. Here, FeS _x (x = 1 or 2) is employed as conversion cathode with 2–4 electron transfers to achieve a maximum energy density close to 400 Wh kg^?1, which is comparable with that of Li‐ion batteries but without serious dendrite growth and polysulphide dissolution. In situ formation of solid electrolyte interfaces on both sulfide and Mg electrodes is likely responsible for long‐life cycling and suppression of S‐species passivation at Mg anodes. Without any decoration on the cathode, electrolyte additive, or anode protection, a reversible capacity of more than 200 mAh g^?1 is still preserved for Mg/FeS₂ after 200 cycles.     

A High‐Performance Sodium‐Ion Hybrid Capacitor Constructed by Metal–Organic Framework–Derived Anode and Cathode Materials

Sodium‐ion hybrid capacitors (SIHCs) can potentially combine the virtues of high‐energy density of batteries and high‐power output as well as long cycle life of capacitors in one device. The key point of constructing a high‐performance SIHC is to couple appropriate anode and cathode materials, which can well match in capacity and kinetics behavior simultaneously. In this work, a novel SIHC, coupling a titanium dioxide/carbon nanocomposite (TiO₂/C) anode with a 3D nanoporous carbon cathode, which are both prepared from metal–organic frameworks (MOFs, MIL‐125 (Ti) and ZIF‐8, respectively), is designed and fabricated. The robust architecture and extrinsic pseudocapacitance of TiO₂/C nanocomposite contribute to the excellent cyclic stability and rate capability in half‐cell. Hierarchical 3D nanoporous carbon displays superior capacity and rate performance. Benefiting from the merits of structures and performances of anode and cathode materials, the as‐built SIHC achieves a high energy density of 142.7 W h kg^?1 and a high power output of 25 kW kg^?1 within 1–4 V, as well as an outstanding life span of 10 000 cycles with over 90% of the capacity retention. The results make it competitive in high energy and power–required electricity storage applications.     

Enhanced Ionic/Electronic Transport in Nano‐TiO2/Sheared CNT Composite Electrode for Na+ Insertion‐based Hybrid Ion‐Capacitors

Ion‐insertion capacitors show promise to bridge the gap between supercapacitors of high power densities and batteries of high energy densities. While research efforts have primarily focused on Li⁺‐based capacitors (LICs), Na⁺‐based capacitors (SICs) are theoretically cheaper and more sustainable. Owing to the larger size of Na⁺ compared to Li⁺, finding high‐rate anode materials for SICs has been challenging. Herein, an SIC anode architecture is reported consisting of TiO₂ nanoparticles anchored on a sheared‐carbon nanotubes backbone (TiO₂/SCNT). The SCNT architecture provides advantages over other carbon architectures commonly used, such as reduced graphene oxide and CNT. In a half‐cell, the TiO₂/SCNT electrode shows a capacity of 267 mAh g^?1 at a 1 C charge/discharge rate and a capacity of 136 mAh g^?1 at 10 C while maintaining 87% of initial capacity over 1000 cycles. When combined with activated carbon (AC) in a full cell, an energy density and power density of 54.9 Wh kg^?1 and 1410 W kg^?1, respectively, are achieved while retaining a 90% capacity retention over 5000 cycles. The favorable rate capability, energy and power density, and durability of the electrode is attributed to the enhanced electronic and Na⁺ conductivity of the TiO₂/SCNT architecture.     

Besides the Capacitive and Diffusion Control: Inner-Surface Controlled Bismuth Based Electrode Facilitating Potassium-Ion Energy Storage

One of the major challenges of potassium-ion hybrid capacitors (PIHCs) is to explore favorable anode materials with fast reaction kinetics to match the cathodes. Here, an “inner-surface” controlled electrochemistry mechanism based on bismuth electrode is proposed and in-depth studied, which is different from the capacitive or diffusion controlled electrode. Such inner-surface controlled electrochemistry performance gives a high K ion diffusion ability under not only room temperature (RT) but also low temperature (LT). In this study, a kind of conjunct-like bismuth nanoparticle (CBN) is fabricated to model such an advantage. The CBN anode for PIBs displays ultra-long cycling stability and excellent rate capability, especially with a reversible capacity of 212.9 mAh g⁻¹ at 30 A g⁻¹ after 5000 cycles under RT. At −20 °C, the CBN anode achieves a capacity of 191.9 mAh g⁻¹ at 10 A g⁻¹ after 10 000 cycles. Coupling with activate carbon cathode, the as-assembled PIHCs deliver high energy/power densities (111.8 Wh kg⁻¹/412.8 W kg⁻¹ and 29 Wh kg⁻¹/14 312.6 W kg⁻¹), which outperforms those of previously reported PIHCs and other hybrid capacitors. The study provides a new understanding of the energy storage mechanism for bismuth-based electrodes and accelerates the development of advancing potassium ion storage devices, especially at LT.     

Sodium Storage Behavior in Natural Graphite using Ether‐based Electrolyte Systems

This work reports that natural graphite is capable of Na insertion and extraction with a remarkable reversibility using ether‐based electrolytes. Natural graphite (the most well‐known anode material for Li–ion batteries) has been barely studied as a suitable anode for Na rechargeable batteries due to the lack of Na intercalation capability. Herein, graphite is not only capable of Na intercalation but also exhibits outstanding performance as an anode for Na ion batteries. The graphite anode delivers a reversible capacity of ≈150 mAh g^?1 with a cycle stability for 2500 cycles, and more than 75 mAh g^?1 at 10 A g^?1 despite its micrometer‐size (≈100 μm). An Na storage mechanism in graphite, where Na⁺‐solvent co‐intercalation occurs combined with partial pseudocapacitive behaviors, is revealed in detail. It is demonstrated that the electrolyte solvent species significantly affect the electrochemical properties, not only rate capability but also redox potential. The feasibility of graphite in a Na full cell is also confirmed in conjunction with the Na_1.5VPO_4.8F_0.7 cathode, delivering an energy of ≈120 Wh kg^?1 while maintaining ≈70% of the initial capacity after 250 cycles. This exceptional behavior of natural graphite promises new avenues for the development of cost‐effective and reliable Na ion batteries.     

Hetero‐Nanonet Rechargeable Paper Batteries: Toward Ultrahigh Energy Density and Origami Foldability

Forthcoming smart energy era is in strong pursuit of full‐fledged rechargeable power sources with reliable electrochemical performances and shape versatility. Here, as a naturally abundant/environmentally friendly cellulose‐mediated cell architecture strategy to address this challenging issue, a new class of hetero‐nanonet (HN) paper batteries based on 1D building blocks of cellulose nanofibrils (CNFs)/multiwall carbon nanotubes (MWNTs) is demonstrated. The HN paper batteries consist of CNF/MWNT‐intermingled heteronets embracing electrode active powders (CM electrodes) and microporous CNF separator membranes. The CNF/MWNT heteronet‐mediated material/structural uniqueness enables the construction of 3D bicontinuous electron/ion transport pathways in the CM electrodes, thus facilitating electrochemical reaction kinetics. Furthermore, the metallic current collectors‐free, CNF/MWNT heteronet architecture allows multiple stacking of CM electrodes in series, eventually leading to user‐tailored, ultrathick (i.e., high‐mass loading) electrodes far beyond those accessible with conventional battery technologies. Notably, the HN battery (multistacked LiNi_0.5Mn_1.5O₄ (cathode)/multistacked graphite (anode)) provides exceptionally high‐energy density (=226 Wh kg^?1 per cell at 400 W kg^?1 per cell), which surpasses the target value (=200 Wh kg^?1 at 400 W kg^?1) of long‐range (=300 miles) electric vehicle batteries. In addition, the heteronet‐enabled mechanical compliance of CM electrodes, in combination with readily deformable CNF separators, allows the fabrication of paper crane batteries via origami folding technique.     

LiFePO4 Particles Embedded in Fast Bifunctional Conductor rGO&C@Li3V2(PO4)3 Nanosheets as Cathodes for High‐Performance Li‐Ion Hybrid Capacitors

The sluggish kinetics of Faradaic reactions in bulk electrodes is a significant obstacle to achieve high energy and power density in energy storage devices. Herein, a composite of LiFePO₄ particles trapped in fast bifunctional conductor rGO&C@Li₃V₂(PO₄)₃ nanosheets is prepared through an in situ competitive redox reaction. The composite exhibits extraordinary rate capability (71 mAh g^?1 at 15 A g^?1) and remarkable cycling stability (0.03% decay per cycle over 1000 cycles at 10 A g^?1). Improved extrinsic pseudocapacitive contribution is the origin of fast kinetics, which endows this composite with high energy and power density, since the unique 2D nanosheets and embedded ultrafine LiFePO₄ nanoparticles can shorten the ion and electron diffusion length. Even applied to Li‐ion hybrid capacitors, the obtained devices still achieve high power density of 3.36 kW kg^?1 along with high energy density up to 77.8 Wh kg^?1. Density functional theory computations also validate that the remarkable rate performance is facilitated by the desirable ionic and electronic conductivity of the composite.