ZTIFs derived nitrogen-introduced high specific area and hierarchical porous carbon for oxygen reduction reaction

It is of great allure to construct nitrogen-doped hierarchical porous carbon to replace Pt-based catalysts for efficient ORR. Here, nitrogen-doped hierarchical porous carbon (NHPC) was prepared by carbonizing ZTIF-1 and KOH activating. The resultant NHPC4-700 catalyst exhibits a hierarchical porous structure and high specific area (2404 m² g^?1), which promoted the exposure of enough active sites as well as simultaneously enhanced the electron transfer rate, shorten the mass transfer pathway, enhanced ionic conductivity and carbon wetting. The results are capable of remarkably improving the ORR activities of carbon materials. The NHPC4-700 catalyst exhibits a great catalytic performance with onset potential at 0.90 V and limiting current density of ??6.0 mA cm^?2, which is close to commercial Pt/C electrocatalyst. Meanwhile, the NHPC4-700 catalysts had better stability and methanol resistance than that of Pt/C toward ORR. These superior electrochemical properties of the NHPC4-700 catalysts were closely related to their nitrogen-doped hierarchical porous structure and high specific area.

     

Hierarchical porous carbon obtained from directly carbonizing carex meyeriana for high-performance supercapacitors

Hierarchical porous carbon materials with high surface area are facilely prepared by directly carbonizing carex meyeriana without any extra activation procedure. The as-prepared porous carbon samples possess high Brunauer–Emmett–Teller (BET) surface areas (in the?~?518–742 m² g^?1 range) and unique hierarchical porous structure containing macropore channels and mesopores and micropores developed in the wall of macropores. These intriguing characteristics make the as-prepared hierarchical porous carbon samples a promising electrode material for supercapacitors. The capacitive performance was measured in the three-electrode system with 6 M KOH electrolyte. The hierarchical porous carbon prepared at the carbonization temperature of 1000 °C presents a high specific capacitance of 178.6 F g^?1 at a current density of 0.5 A g^?1, a good rate performance ( about 65.2% retention ratio at the current density of 20 A g^?1), and an excellent cycling stability (no obvious performance fading after 10,000 cycles). In addition, the fabricated two-electrode device achieves an energy density of 4.33 Wh kg^?1 at a high power density of 5 kW kg^?1. These results provide a green and facile method to synthesize the electrode material from biomass for high-performance supercapacitors.

     

Ruthenium doped LiMn1.5Ni0.5O4 microspheres with enhanced electrochemical performance as lithium-ion battery cathode

Ruthenium doped LiNi_0.5Mn_1.5O₄ (LNMO) microspheres has been prepared by a simple solid-state reaction process. The as-prepared sample was characterized by powder X-ray diffraction (XRD), scanning electron microscopy (SEM), energy dispersive spectroscopy (EDS), X-ray photoelectron spectroscopy (XPS) and electrochemistry performance test. The sample shows a spinel crystal structure without RuO₂ impurity phase, and Ru doped sample crystal plane spacing increases. Combined with EDS spectrum, it indicates that the Ru ion was doped in the LNMO and distributed homogeneously. The XPS also further confirm the existence of Ru ions, and Ru has no obvious influence on Ni and Mn elements. The SEM images show that all the samples are sphere-like, with many polyhedral particles attached to the surface. When doped with 4% Ru ion, many cavities appear on the surface to form a porous structure. Electrochemical analysis confirms that the Ru-doped sample exhibits better electrochemical properties regarding discharge capacity, cycle stability, and rate performance. The 4% Ru-doped sample owns an initial discharge capacity of 125 mAh g^?1 at 0.25C rate, with a capacity retention of 92% after 50 charge–discharge cycles. Moreover, at high current density (1C), Ru doped sample’s discharge capacity is 103 mAh g^?1 while the original is only 86 mAh g^?1. The excellent electrochemical properties are attributed to the Ru doping that increases the interlayer spacing and reduces the charge-transfer impedance (R_ct), which is beneficial to lithium ion-exchange.

     

One-step sonochemical synthesis of NiMn-LDH for supercapacitors and overall water splitting

Transition metals are attracting numerous interests for their substantial applications in supercapacitors and as non-noble metal electrocatalyst for overall water splitting. Herein, the NiMn layer double hydroxide (NiMn-LDH) is developed using the sonochemical route at different reaction times, which act as a multifunctional electrode for supercapacitors and overall water splitting. The capacitance of layer double hydroxide (LDH) synthesized at 4 h (NiMn-LDH-4 h) of reaction time was found to be 527 F g^?1 at 1 A g^?1, with 91.2% capacitance retention after 5,000 cycles at 2 A g^?1 in 6 M KOH. For hydrogen and oxygen evolution reactions, the NiMn-LDH-4 h electrode exhibits a standard of 10 mA cm^?2 at an overpotential of 120 mV and 296 mV, respectively, in 1 M KOH. Moreover, fabricated NiMn-LDH-4 h||NiMn-LDH-4 h electrolyzer for overall water splitting benchmarks 10 mA cm^?2 at 1.6 V. The superior electrochemical properties of the NiMn-LDH electrodes might be attributed to quick diffusion paths and enhanced redox reaction of NiMn-LDH nanosheets because of the high surface area.

     

Self-activated ‘green’ carbon nanoparticles for symmetric solid-state supercapacitors

Tuning of porosity and surface properties of nanoparticles especially on carbon-based nanomaterials, adopting a ‘greener’ or self-activation synthesis technique for electrical charge storage, is progressing. Herein, we report the self-activation of Teak wood sawdust in a nitrogen atmosphere at different activation temperatures to synthesize carbon nanoparticles. The activated carbon nanoparticles synthesized at 900 °C exhibits a maximum?~?360 m² g^?1 surface area with?~?2 nm average pore size diameter. Five electrolytes viz. KOH, KCl, Na₂SO₄, NaCl, and H₃PO₄ are used for studying the supercapacitance nature of the activated carbon nanoparticles in a 3-electrode configuration. A maximum specific capacitance of?~?208 F g^?1 @ 0.25 A g^?1 is obtained in 1 M KOH as the electrolyte. Two symmetric supercapacitors, aqueous (1 M KOH) and solid-state (PVA/KOH), are fabricated, and their performance difference is compiled. The solid-state symmetric supercapacitor performs in a wider voltage window (1.7 V) with a superior energy density of 27.1 Wh kg^?1 at a power density of 178 W kg^?1.

Graphical abstract

     

One-pot fabrication of pitch-derived soft carbon with hierarchical porous structure and rich sp2 carbon for sodium-ion battery

Soft carbons with porous structure have attracted increasing attention as attracting anode active materials for sodium-ion battery. However, the reported anode active materials are plagued by limited capacity and unsatisfying rate performance. Besides, the improvement of electrical conductivity is often performed by post treatment, which is time-consuming and high cost. Herein we report an one-pot fabrication of pitch-derived soft carbon using zinc acetate as hard templates. Zinc acetate can not only play a vital role in constructing hierarchical porous structure but also providing additional sp² carbon during carbonization, resulting in significantly enhanced sodium-ion storage capacity and improved rate performance. As anode active materials for sodium-ion battery, the as-prepared soft carbon with hierarchical porous structure, rich sp² carbon and doped N, O heteroatoms, exhibits an impressively high reversible capacity of 293 mAh g^?1 at 0.05 A g^?1 in sodium-ion half cells, good rate capability of 53 mAh g^?1 at 5 A g^?1, and high capacity retention of 92.2% after 1000 cycles at 1 A g^?1. Our strategy affords a facile way to prepare high-quality soft carbon materials as anode active materials for sodium-ion batteries.

     

Enriched energy storage capability and bi-functional ability of boron-doped graphene as efficient electrode for supercapacitors and lithium sulfur batteries

This work depicts the preparation of boron-doped graphene (BG) and its application as bi-functional electrode material for both the supercapacitors and lithium–sulfur (Li–S) battery. Structural, morphological, and elemental analyses of the prepared material were acquired via X-ray diffraction, Fourier transform infrared spectroscopy, Raman spectroscopy, Scanning electron microscopy, and X-ray photoelectron spectroscopy, respectively. BG worked well in supercapacitors as a capacitive electrode, featuring a high specific capacitance of 239 F g^?1 at a current rate of 1 A g^?1 and high capacity retention of 85% over 10,000 charge/discharge cycles with average coulombic efficiency of 99.5%. In addition, the sulfur/boron-doped graphene (SBG) binary composite was prepared via melt diffusion method and used as the positive electrode material in Li–S batteries. BG is effective polysulfide adsorbent and its sheet-like structure accommodates more content of sulfur, which restricts the shuttle effect and volume changes of active material during cycling. The SBG composite shows an initial discharge capacity of 1355 mAh g^?1, and it retains the discharge capacity of 636 mAh g^?1 over the 50 cycles. The present work demonstrates that BG is an efficient electrode material for energy storage applications.

     

Tailoring Hierarchically Porous Nitrogen‐, Sulfur‐Codoped Carbon for High‐Performance Supercapacitors and Oxygen Reduction

Heteroatom‐doped carbon materials are intensively studied in supercapacitors and fuel cells, because of their great potential for sustainably bearing on the energy crisis and environmental pollution. Although enormous efforts are put in material perfection with a hierarchically porous microstructure, the simultaneous optimization of both porous structures and surface functionalities is hard to achieve due to inevitable concurrent dopant leaching effect and structural collapse under required high pyrolysis temperature. In this study, an in situ dehalogenation polymerization and activation protocol is introduced to synthesize nitrogen‐ and sulfur‐codoped carbon materials (NS‐PCMs) with hierarchical pore distribution and abundant surface doping, which endows them with good conductivity, abundant accessible active sites, and efficient mass transport. As a result, the as‐prepared carbon materials (NS‐a‐PCM‐1000) show an excellent mass specific capacitance of 461.5 F g^?1 at a current density of 0.1 A g^?1, long cycle life (>23 k, 10 A g^?1), and high device energy and power density (17.3 Wh kg^?1, 250 W kg^?1). Significantly, NS‐a‐PCM‐1000 also exhibits one of the highest oxygen reduction reaction activities (onset potential of 1.0 V vs reversible hydrogen electrode) in alkaline media among all reported metal‐free catalysts.     

Hierarchically Porous Fe2CoSe4 Binary‐Metal Selenide for Extraordinary Rate Performance and Durable Anode of Sodium‐Ion Batteries

Owing to high energy capacities, transition metal chalcogenides have drawn significant research attention as the promising electrode materials for sodium‐ion batteries (SIBs). However, limited cycle life and inferior rate capabilities still hinder their practical application. Improvement of the intrinsic conductivity by smart choice of elemental combination along with carbon coupling of the nanostructures may result in excellence of rate capability and prolonged cycling stability. Herein, a hierarchically porous binary transition metal selenide (Fe₂CoSe₄, termed as FCSe) nanomaterial with improved intrinsic conductivity was prepared through an exclusive methodology. The hierarchically porous structure, intimate nanoparticle–carbon matrix contact, and better intrinsic conductivity result in extraordinary electrochemical performance through their synergistic effect. The synthesized FCSe exhibits excellent rate capability (816.3 mA h g^?1 at 0.5 A g^?1 and 400.2 mA h g^?1 at 32 A g^?1), extended cycle life (350 mA h g^?1 even after 5000 cycles at 4 A g^?1), and adequately high energy capacity (614.5 mA h g^?1 at 1 A g^?1 after 100 cycles) as anode material for SIBs. When further combined with lab‐made Na₃V₂(PO₄)₃/C cathode in Na‐ion full cells, FCSe presents reasonably high and stable specific capacity.     

ZIF-67/rGO/NiPc composite electrode material for high-performance asymmetric supercapacitors

In this reported study, novel multiple dimensional ZIF-67/rGO/NiPc composite materials were prepared for supercapacitors. The electrochemical test showed that the ZIF-67/rGO/NiPc electrode achieved a remarkable specific capacitance of 860 F g^?1 at a current density of 1 A g^?1, which was superior to that of the rGO/NiPc and ZIF-67/rGO electrodes. An asymmetric supercapacitor based on ZIF-67/rGO/NiPc//activated carbon exhibited a high specific capacitance of 200.67 F g^?1 and an extraordinary energy density of 62.7 Wh kg^?1 at a corresponding power density of 750 W kg^?1. In addition, the device demonstrated 94.6% capacitance retention after 5000 cycles. The assembled asymmetric supercapacitors could easily powered a green light-emitting diode. This work revealed a promising research route for the rational construction of multiple dimensioned high-performance electrodes materials for use in new energy storage devices.

     

Zeolite-templated mesocellular graphene foam with adjustable defects as highly efficient catalysts for oxygen reduction reaction

In this study, zeolite-templated mesocellular graphene foam was facilely synthesized by pyrolysis under different temperatures for oxygen reduction reaction. Investigations found that MGF can be regulated with different structure properties by controlling the pyrolysis temperature, where the MGF-900 (pyrolyzed under 900 °C) possessed a large BET specific surface area (619 m² g^?1), a hierarchically micro–meso–macroporous carbon framework, and a better balance between conductivity and active sites than the other counterparts (MGF-800 and MGF-1000). As a result, MGF-900 had the most excellent catalytic activity, the most positive onset potential of ??0.1 V and the highest current density of 5.01 mA cm^?2 among the different samples and many other reported carbon-based catalysts. More importantly, despite no heterogeneous atoms doping, the catalytic activity of MGF-900 was nearly equal to that of commercial Pt/C catalyst. Regarding tolerance and stability, MGF-900 behaved even better. Therefore, as a superior metal-free electrocatalyst, MGF-900 is proved to be well applied in highly efficient oxygen reduction reaction.

     

Design of XS2 (X = W or Mo)-Decorated VS2 Hybrid Nano-Architectures with Abundant Active Edge Sites for High-Rate Asymmetric Supercapacitors and Hydrogen Evolution Reactions

Two-dimensional layered transition metal dichalcogenides have emerged as promising materials for supercapacitors and hydrogen evolution reaction (HER) applications. Herein, the molybdenum sulfide (MoS₂)@vanadium sulfide (VS₂) and tungsten sulfide (WS₂)@VS₂ hybrid nano-architectures prepared via a facile one-step hydrothermal approach is reported. Hierarchical hybrids lead to rich exposed active edge sites, tuned porous nanopetals-decorated morphologies, and high intrinsic activity owing to the strong interfacial interaction between the two materials. Fabricated supercapacitors using MoS₂@VS₂ and WS₂@VS₂ electrodes exhibit high specific capacitances of 513 and 615 F g⁻¹, respectively, at an applied current of 2.5 A g⁻¹ by the three-electrode configuration. The asymmetric device fabricated using WS₂@VS₂ electrode exhibits a high specific capacitance of 222 F g⁻¹ at an applied current of 2.5 A g⁻¹ with the specific energy of 52 Wh kg⁻¹ at a specific power of 1 kW kg⁻¹. For HER, the WS₂@VS₂ catalyst shows noble characteristics with an overpotential of 56 mV to yield 10 mA cm⁻², a Tafel slope of 39 mV dec⁻¹, and an exchange current density of 1.73 mA cm⁻². In addition, density functional theory calculations are used to evaluate the durable heterostructure formation and adsorption of hydrogen atom on the various accessible sites of MoS₂@VS₂ and WS₂@VS₂ heterostructures.     

High-Activity Fe3C as pH-Universal Electrocatalyst for Boosting Oxygen Reduction Reaction and Zinc-Air Battery

Transition metal catalysts are regarded as one of promising alternatives to replace traditional Pt-based catalysts for oxygen reduction reaction (ORR). In this work, an efficient ORR catalyst is synthesized by confining Fe₃C nanoparticles into N, S co-doped porous carbon nanosheets (Fe₃C/N,S-CNS) via high-temperature pyrolysis, in which 5-sulfosalicylic acid (SSA) demonstrates as an ideal complexing agent for iron (ΙΙΙ) acetylacetonate while g-C₃N₄ behaves as a nitrogen source. The influence of the pyrolysis temperature on the ORR performance is strictly examined in the controlled experiments. The obtained catalyst exhibits excellent ORR performance (E_1/2 = 0.86 V; E_onset = 0.98 V) in alkaline electrolyte, coupled by exhibiting the superior catalytic activity and stability (E_1/2 = 0.83 V, E_onset = 0.95 V) to Pt/C in acidic media. In parallel, its ORR mechanism is carefully illustrated by the density functional theory (DFT) calculations, especially the role of the incorporated Fe₃C played in the catalytic process. The catalyst-assembled Zn-air battery also exhibits a much higher power density (163 mW cm^–2) and ultralong cyclic stability in the charge–discharge test for 750 h with a gap increase down to 20 mV. This study provides some constructive insights for preparation of advanced ORR catalysts in green energy conversion units correlated systems.     

“Wiring” Fe‐Nx‐Embedded Porous Carbon Framework onto 1D Nanotubes for Efficient Oxygen Reduction Reaction in Alkaline and Acidic Media

This study presents a novel metal‐organic‐framework‐engaged synthesis route based on porous tellurium nanotubes as a sacrificial template for hierarchically porous 1D carbon nanotubes. Furthermore, an ultrathin Fe‐ion‐containing polydopamine layer has been introduced to generate highly effective FeN_xC active sites into the carbon framework and to induce a high degree of graphitization. The synergistic effects between the hierarchically porous 1D carbon structure and the embedded FeN_xC active sites in the carbon framework manifest in superior catalytic activity toward oxygen reduction reaction (ORR) compared to Pt/C catalyst in both alkaline and acidic media. A rechargeable zinc‐air battery assembled in a decoupled configuration with the nonprecious pCNT@Fe@GL/CNF ORR electrode and Ni‐Fe LDH/NiF oxygen evolution reaction (OER) electrode exhibits charge–discharge overpotentials similar to the counterparts of Pt/C ORR electrode and IrO₂ OER electrode.     

Polyimide@Ketjenblack Composite: A Porous Organic Cathode for Fast Rechargeable Potassium‐Ion Batteries

Potassium‐ion batteries (PIBs) configurated by organic electrodes have been identified as a promising alternative to lithium‐ion batteries. Here, a porous organic Polyimide@Ketjenblack is demonstrated in PIBs as a cathode, which exhibits excellent performance with a large reversible capacity (143 mAh g^?1 at 100 mA g^?1), high rate capability (125 and 105 mAh g^?1 at 1000 and 5000 mA g^?1), and long cycling stability (76% capacity retention at 2000 mA g^?1 over 1000 cycles). The domination of fast capacitive‐like reaction kinetics is verified, which benefits from the porous structure synthesized using in situ polymerization. Moreover, a renewable and low‐cost full cell is demonstrated with superior rate behavior (106 mAh g^?1 at 3200 mA g^?1). This work proposes a strategy to design polymer electrodes for high‐performance organic PIBs.     

Single copper sites dispersed on hierarchically porous carbon for improving oxygen reduction reaction towards zinc-air battery

The demand for high-performance non-precious-metal electrocatalysts to replace the noble metal-based catalysts for oxygen reduction reaction(ORR)is intensively increasing.Herein,single-atomic copper sites supported on N-doped three-dimensional hierarchically porous carbon catalyst(Cu₁/NC)was prepared by coordination pyrolysis strategy.Remarkably,the Cu₁/NC-900 catalyst not only exhibits excellent ORR performance with a half-wave potential of 0.894 V(vs.RHE)in alkaline media,outperforming those of commercial Pt/C(0.851 V)and Cu nanoparticles anchored on N-doped porous carbon(CuNPs/NC-900),but also demonstrates high stability and methanol tolerance.Moreover,the Cu₁/NC-900 based Zn-air battery exhibits higher power density,rechargeability and cyclic stability than the one based on Pt/C.Both experimental and theoretical investigations demonstrated that the excellent performance of the as-obtained Cu₁/NC-900 could be attributed to the synergistic effect between copper coordinated by three N atoms active sites and the neighbouring carbon defect,resulting in elevated Cu d-band centers of Cu atoms and facilitating intermediate desorption for ORR process.This study may lead towards the development of highly efficient non-noble metal catalysts for applications in electrochemical energy conversion.     

Hierarchical 3D Cobalt‐Doped Fe3O4 Nanospheres@NG Hybrid as an Advanced Anode Material for High‐Performance Asymmetric Supercapacitors

Hierarchical nanostructure, high electrical conductivity, extraordinary specific surface area, and unique porous architecture are essential properties in energy storage and conversion studies. A new type of hierarchical 3D cobalt encapsulated Fe₃O₄ nanosphere is successfully developed on N‐graphene sheet (Co?Fe₃O₄ NS@NG) hybrid with unique nanostructure by simple, scalable, and efficient solvothermal technique. When applied as an electrode material for supercapacitors, hierarchical Co?Fe₃O₄ NS@NG hybrid shows an ultrahigh specific capacitance (775 F g^?1 at a current density of 1 A g^?1) with exceptional rate capability (475 F g^?1 at current density of 50 A g^?1), and admirable cycling performance (97.1% capacitance retention after 10 000 cycles). Furthermore, the fabricated Co?Fe₃O₄ NS@NG//CoMnO₃@NG asymmetric supercapacitor (ASC) device exhibits a high energy density of 89.1 Wh kg^?1 at power density of 0.901 kW kg^?1, and outstanding cycling performance (89.3% capacitance retention after 10 000 cycles). Such eminent electrochemical properties of the Co?Fe₃O₄ NS@NG are due to the high electrical conductivity, ultrahigh surface area, and unique porous architecture. This research first proposes hierarchical Co?Fe₃O₄ NS@NG hybrid as an ultrafast charge?discharge anode material for the ASC device, that holds great potential for the development of high‐performance energy storage devices.     

Biomass Derived N‐Doped Porous Carbon Supported Single Fe Atoms as Superior Electrocatalysts for Oxygen Reduction

Exploring sustainable and high‐performance electrocatalysts for the oxygen reduction reaction (ORR) is the crucial issue for the large‐scale application of fuel cell technology. A new strategy is demonstrated to utilize the biomass resource for the synthesis of N‐doped hierarchically porous carbon supported single‐atomic Fe (SA‐Fe/NHPC) electrocatalyst toward the ORR. Based on the confinement effect of porous carbon and high‐coordination natural iron source, SA‐Fe/NHPC, derived from the hemin‐adsorbed bio‐porphyra‐carbon by rapid heat‐treatment up to 800 °C, presents the atomic dispersion of Fe atoms in the N‐doped porous carbon. Compared with the molecular hemin and nanoparticle Fe samples, the as‐prepared SA‐Fe/NHPC exhibits a superior catalytic activity (E _1/2 = 0.87 V and J _k = 4.1 mA cm^?2, at 0.88 V), remarkable catalytic stability (≈1 mV negative shift of E _1/2, after 3000 potential cycles), and outstanding methanol‐tolerance, even much better than the state‐of‐the‐art Pt/C catalyst. The sustainable and effective strategy for utilizing biomass to achieve high‐performance single‐atom catalysts can also provide an opportunity for other catalytic applications in the atomic scale.     

Melamine-assisted synthesis of cobalt–nickel coordination polymers as electrode materials for supercapacitors

Coordination polymers (CPs) and/or metal–organic frameworks (MOFs) are new active materials for supercapacitors (SC). In this study, by solvothermal route, we conduct the melamine-assisted synthesis of bimetallic CPs (Co–Ni CPs) with controllable structures. The concentration of melamine plays an important role in the morphology of Co–Ni CPs, and the CPs can be turned from microspheres to nanorods. The Co–Ni CPs are used as electrode materials for SC. The spherical Co–Ni–CP-M exhibits the highest capacitances of 677 F g^?1 and 585 F g^?1 at current densities of 1 A g^?1 and 10 A g^?1, respectively, indicating an outstanding rate capability in a three-electrode system with 2.0 M KOH electrolyte. Furthermore, the Co–Ni–CP-M//active carbon device shows superior long-term cycling stability, i.e., approximately 92.6% of the initial capacitance can be retained after 10,000 cycles at 10 A g^?1 in 2.0 M KOH electrolyte. In addition, the asymmetric SC device achieves an excellent energy density of 28.35 W h kg^?1 at a power density of 700 W kg^?1.

Graphical abstract

     

Etching‐Assisted Crumpled Graphene Wrapped Spiky Iron Oxide Particles for High‐Performance Li‐Ion Hybrid Supercapacitor

From graphene oxide wrapped iron oxide particles with etching/reduction process, high‐performance anode and cathode materials of lithium‐ion hybrid supercapacitors are obtained in the same process with different etching conditions, which consist of partially etched crumpled graphene (CG) wrapped spiky iron oxide particles (CG@SF) for a battery‐type anode, and fully etched CG for a capacitive‐type cathode. The CG is formed along the shape of spikily etched particles, resulting in high specific surface area and electrical conductivity, thus the CG‐based cathode exhibits remarkable capacitive performance of 210 F g^?1 and excellent rate capabilities. The CG@SF can also be ideal anode materials owing to spiky and porous morphology of the particles and tightly attached crumpled graphene onto the spiky particles, which provides structural stability and low contact resistance during repetitive lithiation/delithiation processes. The CG@SF anode shows a particularly high capacitive performance of 1420 mAh g^?1 after 270 cycles, continuously increases capacity beyond the 270th cycle, and also maintains a high capacity of 170 mAh g^?1 at extremely high speeds of 100 C. The full‐cell exhibits a higher energy density up to 121 Wh kg^?1 and maintains high energy density of 60.1 Wh kg^?1 at 18.0 kW kg^?1. This system could thus be a practical energy storage system to fill the gap between batteries and supercapacitors.