Electrode Materials For Energy Storage Research Articles

CoNiSe2/Fe-CoNiSe2 yolk–shell nanoboxes from metal-organic frameworks for high-performance supercapacitor

Due to excellent activity, electronic conductivity, and stability, transition metal selenide shows incredible potential for energy storage and conversion. In this work, trimetallic CoNiSe2/Fe-CoNiSe2 yolk-shell nanoboxes (YSBs) are developed via ZIF-67/NiCoFe Prussian blue analogue (PBA) precursors as efficient electrode materials for high-performance supercapacitors (SCs). Structural engineering of the PBA framework with Co-Fe oxide increases the topological complexity of the nanostructure. The energy storage activity is effectively improved because of the open structure and larger surface area. The presence of trimetallic selenides in CoNiSe2/Fe-NiCoSe2 YSBs improves the electronic structures and thus electrochemical performances and enhanced conductivity of the nanostructure compared with oxide counterparts. As a result, it enables attractive electrochemical performance when used as an electrode for battery-type supercapacitors. CoNiSe2/Fe-CoNiSe2 yolk-shell nanoboxes show high specific capacity of 1091.2 C/g at 1.0 A/g, good acceleration performance (55% at 20 A/g), and excellent cycle stability (85% recovery after 5000 charge/discharge cycles). Furthermore, the NiCoSe2/Fe-NiCoSe2 YSBs//AC hybrid SC demonstrates an energy density above 76.5 Wh/Kg at a power density of 2378.7 W/Kg. These results suggest that the current strategy may provide a way for designing efficient electrode materials for energy storage by preparing trimetallic chalcogenides with yolk-shell structures.

2D and Layered Ti-based Materials for Supercapacitors and Rechargeable Batteries: Synthesis, Properties, and Applications

: Titanium-based two-dimensional (2D) and layered compounds with open and stable crystal structures have attracted increasing attention for energy storage and conversion purposes, e.g., rechargeable alkali-ion batteries and hybrid capacitors, due to their superior rate capability derived from the intercalation-type or pseudocapacitive kinetics. Various strategies, including structure design, conductivity enhancement, surface modification, and electrode engineering, have been implemented to effectively overcome the intrinsic drawbacks while simultaneously maintaining their advantages as promising and competitive electrode materials for advanced energy storage and conversion. Here, we provide a comprehensive overview of the recent progress on Ti-based compound materials for highrate and low-cost electrochemical energy storage applications (mainly on rechargeable batteries and supercapacitors). The energy storage mechanisms, structure-performance relations, and performanceoptimizing strategies in these typical energy storage devices are discussed. Moreover, major challenges and perspectives for future research and industrial application are also illustrated.

Wet‐Chemistry: A Useful Tool for Deriving Metal–Organic Frameworks toward Supercapacitors and Secondary Batteries

AbstractMetal–organic frameworks (MOFs) possess the advantages of tailorable porosity, adjustable composition, and tunable topologies and are considered promising precursors and self‐templates for the synthesis of complex nanostructures as advanced electrode materials for energy storage. Among various strategies, wet‐chemical method endows better control over topological evolution and compositional transformation of MOF crystals. Herein, the authors comprehensively review the recent achievements on wet‐chemical derivation of MOF via etching, ion‐exchange, hydrolysis, and chemical transformation, underscore the corresponding mechanisms, and highlight their important applications in supercapacitors and secondary batteries.

Universal Strategy for Preparing Highly Stable PBA/Ti3C2Tx MXene toward Lithium-Ion Batteries via Chemical Transformation.

Prussian blue analogues (PBAs) are believed to be intriguing anode materials for Li+ storage because of their tunable composition, designable topologies, and tailorable porous structures, yet they suffer from severe capacity decay and inferior cycling stability due to the volume variation upon lithiation and high electrical resistance. Herein, we develop a universal strategy for synthesizing small PBA nanoparticles hosted on two-dimensional (2D) MXene or rGO (PBA/MX or PBA/rGO) via an in situ transformation from ultrathin layered double hydroxides (LDH) nanosheets. 2D conductive nanosheets allow for fast electron transport and guarantee the full utilization of PBA even at high rates; at the meantime, PBA nanoparticles effectively prevent 2D materials from restacking and facilitate rapid ion diffusion. The optimized Ni0.8Mn0.2-PBA/MX as an anode for lithium-ion batteries (LIBs) delivers a capacity of 442 mAh g-1 at 0.1 A g-1 and an excellent cycling robustness in comparison with bare PBA bulk crystals. We believe that this study offers an alternative choice for rationally designing PBA-based electrode materials for energy storage.

Hierarchical NiCo-LDH core/shell homostructural electrodes with MOF-derived shell for electrochemical energy storage

Constructing hierarchical structure is an effective strategy to boost the electrochemical performance of layered double hydroxide (LDH) materials, but the rational design of such delicate architectures is still challenging. Herein, a unique hierarchical core/shell homostructure with NiCo-LDH nanorods (NCNRs) as core and NiCo-LDH nanosheets (NCNSs) as shell is constructed via in-situ ZIF shell growth and subsequent ion exchange-coprecipitation process. Such novel hierarchical structure provides a large accessible surface area and more exposed electrochemical active sites. The in-situ growth and conversion process contribute to the formation of robust adhesion between the core and the shell, which could facilitate the effective charge and ion diffusion, as well as improve the mechanical stability. Benefiting from the unique structure, the NCNRs@NCNSs electrode exhibits a high capacitance of 2640.2 F g−1, along with the good rate performance and cyclic stability. Furthermore, the as-assembled asymmetric supercapacitor of NCNRs@NCNSs//AC device displays a high energy density of 22.81 Wh kg−1 at the power density of 374.95 W kg−1. This work demonstrates a new strategy for designing hierarchical LDH with core/shell structure as electrode materials for superior electrochemical energy storage.

MOF‐derived Multi‐Shelled NiP2 Microspheres as High‐Performance Anode Materials for Sodium‐/Potassium‐Ion Batteries

Development of high capacity, high‐rate performance, long cycling life, and low‐cost electrode materials is highly desirable for sodium‐ion batteries (SIBs) and potassium‐ion batteries (PIBs) to pave the way for their rapid commercialization. Herein, NiP2 nanoparticles loaded in multi‐shelled hollow N‐doped carbon microspheres (NiP2@MHNC) are successfully prepared. The built‐in heterogeneous interfaces between NiP2 and N‐doped carbon promote Na+/K+ diffusion; the robust C–N, N–Ni bonds stabilize the structure of electrodes and accelerate the electrons transfer; and the multi‐shelled hollow structure with large specific surface area effectively buffers the volume expansion to ensure cycling stability. Endowed with the aforementioned synergistic effect, the NiP2@MHNC exhibits remarkable enhancement in electrochemical performance with 346.6 mA h g−1 after 300 cycles for SIB and 142 mA h g−1 after 200 cycles for PIBs at 0.1 A g−1. Moreover, the synergistic effect on electrochemical reaction kinetics is systematically analyzed. Further, the mechanism of sodium storage for NiP2@MHNC is also investigated. The research experience and conclusions in this study based on synergistic effect of heterogeneous interfaces, N‐doped carbon, and multi‐shelled hollow structure open up a meaningful route to design other similar advanced composite electrode materials in energy storage and conversion field.

Nanostructure and Advanced Energy Storage: Elaborate Material Designs Lead to High-Rate Pseudocapacitive Ion Storage.

The drastic need for development of power and electronic equipment has long been calling for energy storage materials that possess favorable energy and power densities simultaneously, yet neither capacitive nor battery-type materials can meet the aforementioned demand. By contrast, pseudocapacitive materials store ions through redox reactions with charge/discharge rates comparable to those of capacitors, holding the promise of serving as electrode materials in advanced electrochemical energy storage (EES) devices. Therefore, it is of vital importance to enhance pseudocapacitive responses of energy storage materials to obtain excellent energy and power densities at the same time. In this Review, we first present basic concepts and characteristics about pseudocapacitive behaviors for better guidance on material design researches. Second, we discuss several important and effective material design measures for boosting pseudocapacitive responses of materials to improve rate capabilities, which mainly include downsizing, heterostructure engineering, adding atom and vacancy dopants, expanding interlayer distance, exposing active facets, and designing nanosheets. Finally, we outline possible developing trends in the rational design of pseudocapacitive materials and EES devices toward high-performance energy storage.

Three‐Dimensional Porous Carbon Materials from Coix lacryma‐jobi L. Shells for High‐Performance Supercapacitor

AbstractThree‐dimensional (3D) porous carbon materials are widely concerned because of their excellent electrochemical performance in supercapacitors. Herein, a new porous Coix lacryma‐jobi L. shells‐based carbon (CSC) is prepared by carbonization and activation for super‐capacitors. The obtained CSC‐3 (CSC‐x, x: KOH/CSC mass ratio) possesses abundant porous structures, some functional groups with nitrogen and oxygen atoms, and good electrochemical performance. When the mass ratio of KOH to CSC is 3 : 1, the obtained CSC‐3 has the largest specific surface area (SSA, 1191.7 m2 g−1). Besides the material exhibits good electrochemical capability in the three‐electrode system with 6 m KOH aqueous electrolyte, such as desirable specific capacitance (at 0.5 A g−1, the specific capacitance is 413.5 F g−1), ideal rate performance (from 0.5 A g−1 to 10 A g−1, the specific capacitance retention rate is 70.86 %) and long cycle life (the specific capacitance only reduced by 2.47 % after 5000 cycles at 0.5 A g−1). Assembled symmetric supercapacitor (CSC‐3//CSC‐3) shows gratifying energy density (11.58 Wh Kg−1 at the power density of 324.93 W Kg−1 in 6 m KOH aqueous electrolyte and 14.67 Wh Kg−1 at 474.93 W Kg−1 in 1 m Na2SO4 aqueous electrolyte). This work provides possibility of utilizing waste Coix lacryma‐jobi L. shells to produce low‐cost and high‐performance super‐capacitor electrode materials for sustainable electrochemical energy storage.

Insight into the composition effect of nickel cobalt layered double hydroxide nanoarrays with the enhanced synergistic effect for supercapacitor electrode

Rational post-treatment of Ni/Co-based electrode with high mass-loading in term of the increase of surface active sites and the enhancement of the synergistic effect is facile to achieve desirable electrochemical performances for energy storage. In this work, the composition effects on the structure and capacitive performance of NiCo layered double hydroxide (NiCo LDH) nanostructured is discussed, and subsequently the structural diversity of NiCo LDH is regulated via an alkali conversion. The result suggests that bimetallic synergistic effect can be enhanced via the charge exchange during alkali conversion, resulting in gradual increase surface content of Ni3+ and Co3+ cations. Such evolution endows Ni0.60Co0.40 LDH nanoarrays with outstanding performance as a battery-type Faradaic electrode material for supercapacitor, with areal capacity of 5.15 C cm−2 at 5 mA cm−2, excellent rate capability and high cyclic stability. The presented work not only provides a promising electrode material for supercapacitor, but also offers a new route toward understand the composition effect, bimetallic synergistic effect and the activation of Ni/Co-based electrode materials for energy storage and conversion.

Facile synthesis of Veitchia merilli coir-based porous carbon using combined chemical and physical activation routes as electrode material for energy storage

This study aimed to prepare Veitchia merilli coir (VMC) through pre-carbonisation process, followed by chemical activation using potassium hydroxide as an activating agent. The experiment was conducted under different pyrolytic physical activation temperatures of 650, 700, and 750 °C with the code VMS-650, VMS-700, and VMS-750 for each sample. Physical activation methods develop or modify the pore structure, specific surface area, and microstructure of activated carbon. Furthermore, the prepared VMCs were characterised using X-ray diffraction, Fourier transform infrared, scanning electron microscope, energy dispersive X-ray, and cyclic voltammetry with a symmetrical two-electrode system in 1 M H2SO4 solution. The microstructure analysis showed that the VMC carbon electrode has an amorphous structure with two broad peaks at 2θ angles around 26° and 44° corresponding to the (002) and (100) planes, with the L c VMS-700 having a value of 16.007 nm. The VMC electrode has a C≡C carbon bond as a functional group, which extends in bands from 2311.79 to 2373.51 cm−1. Meanwhile, the VMS-700 electrode shows a combined surface morphology of nanofibers as well as mesopores, and the energy dispersive X-ray results showed carbon content of 92.83%. The electrochemical properties of supercapacitor cells indicated this electrode had the highest specific capacitance value of 264.2 F g−1. From the obtained results, the respective physical and electrochemical properties of the carbon electrodes and supercapacitor cells showed that the activated VMC-700 at 700 °C is the optimum temperature to produce the best performance compared to 650 and 750 °C.

CoP/Cu3P heterostructured nanoplates for high-rate supercapacitor electrodes

CoP is considered as a promising electrode material for supercapacitors owing to the concomitant covalent and metallic bonds which lead to high electrical conductivity and high theoretical capacitance. However, the practical low specific capacitance and poor rate capability limit its further applications. Here, a novel CoP/Cu3P heterostructured nanoplate is fabricated via a facile phosphorization process. Due to the synergistic effects of heterostructure, the ionic and electronic diffusion kinetics in the CoP/Cu3P are significantly improved. The CoP/Cu3P electrode manifests an excellent electrochemical performance of 734.2 F g−1 at 1.0 A g−1, a state-of-the-art rate capability of 53.2% capacitance retention even when the current density increases to 50.0 A g−1, and an excellent cycling performance. A hybrid asymmetric device constructed with CoP/Cu3P as positive electrode delivers a high energy density of 28.6 Wh kg−1 at the power density of 775.0 W kg−1, and an ultra-high power density of 38.8 kW kg−1 at 9.7 Wh kg−1. Theoretical calculations further confirm that the heterostructure can effectively tune the electronic structure of CoP and Cu3P, and improve the charge transport. This study provides insight into the rational design of high-rate performance electrode materials in energy storage.

CH3NH3][M(HCOO)3]-based 2D porous NiCo2S4 nanosheets for high-performance supercapacitors with high power densities

Cost-effective and high-performance electrode materials for energy storage and conversion are essential for commercial applications. In this work, the influence of solvent on the morphologies of [CH3NH3][M(HCOO)3] precursors was studied to design and synthesize two-dimensional (2D) porous NiCo2S4 nanosheets with different structures. As an electrode material for supercapacitors, Microflower-NiCo2S4 exhibits excellent capacitance (1,141 F g−1 at 1 A g−1) and stability (88.2% of initial capacitance maintained after 5,000 cycles at 5 A g−1). Moreover, an asymmetric capacitor was constructed using Microflower-NiCo2S4 and porous carbon (PC) and demonstrated an energy density of 51.25 Wh kg−1 at a power density of 397.5 W kg−1. When two Microflower-NiCo2S4//PC asymmetric supercapacitors were assembled in series, the device supplied power for an alarm clock with dimensions of 6.1 × 6.1 cm2 for more than 32 min. Therefore, the preparation of metal sulfides and metal oxides with hollow structures using a [CH3NH3][M(HCOO)3]-template has potential applications in energy storage and conversion.

Mesoporous Carbon Materials for Electrochemical Energy Storage and Conversion

AbstractTo meet the high‐speed commercialization demands of electrochemical energy storage and conversion devices, the development of high‐performance and low‐cost electrode materials is urgently necessary. Mesoporous carbon, which shows excellent intrinsic characteristics and flexible structure, has raised a surge of interest recently since it offers opportunities for improving the energy or power density and durability as well as reducing the cost of electrodes. In this paper, we first review primary methods for preparing mesoporous carbons. Next, the obstacles in lithium batteries, supercapacitors, proton exchange membrane fuel cells and water electrolyzers are analyzed and the recent progresses of mesoporous carbon based electrode designs in solving these obstacles are systematically introduced. Finally, we outline current challenges and future directions of developing mesoporous carbon based electrode materials in electrochemical energy storage and conversion devices. In creating this review, we hope to give a succinct introduction to the mesoporous carbon and provide meaningful references for its future research.

Hollow FeS2 nanospheres encapsulated in N/S co-doped carbon nanofibers as electrode material for electrochemical energy storage

Pyrite iron sulfide (FeS2) is a fascinating electrode material for energy reserve devices because of its high theoretical capacity, non-polluting nature and abundant resources. However, the practical application has been extremely inhibited owing to its poor rate capacity and short cyclability caused by volume change during charge/discharge processes. In this article, a novel nanocomposite that is hollow FeS2 nanospheres encapsulated in N/S co-doped carbon nanofibers (FeS2CNFs) was synthesized through electrostatic spinning. The FeS2CNFs nanocomposite demonstrates a terrific specific capacity of 511 F g−1 at 1 A g−1 for all-solid-state supercapacitors. The FeS2CNFs as electrode material for sodium-ion batteries (SIB) displays a specific capacity of 827.7 mAh g−1 and possesses a capacity of 490.6 mAh g−1 at 0.05 A g−1 after 200 cycles. The results indicate that this encapsulated structure can guarantee the integrity of electrode materials. And the abundant defects in carbon nanofibers caused by N/S co-doping may increase electrochemical reaction sites to facilitate charge transfer. The N/S co-doped FeS2CNFs nanocomposite exhibits a great potential for applying in SIB and supercapacitors.

Pseudocapacitive Co‐Free Trimetallic Ni‐Zn‐Mn Perovskite Fluorides Enable Fast‐Rechargeable Zn‐Based Aqueous Batteries

AbstractThe Zn‐ion batteries (ZIBs) have been largely confined by the sluggish diffusion kinetics of the cathode, and to develop the Co‐free electrode materials for Zn‐based aqueous batteries (ZABs) is of great importance for practical applications. Herein, a novel fast‐rechargeable ZAB constructed using a new type of pseudocapacitive Co‐free trimetallic Ni‐Zn‐Mn perovskite fluorides (ABF3, KNZMF) cathode is demonstrated. A deep study on the charge storage mechanisms of the KNZMF electrode materials has been conducted by various ex situ techniques, showing a typical conversion mechanism in the alkaline media along with the redox‐active or inert property for Ni/Mn or Zn species and the largely bulk phase transitions of ABF3 perovskite nanocrystals into amorphous metal oxides/(oxy)hydroxides nanosheets. Interestingly, the Co‐free KNZMF and Zn//KNZMF ZAB exhibit superior performance to the Co‐rich trimetallic Ni‐Co‐Mn ABF3 (KNCMF) and Zn//KNCMF ZAB, which is largely owing to the superior redox potential, OH− adsorption, deprotonation process, and surface electroactive sites of redox‐active Ni/Mn species confirmed by ex situ characterizations and density functional theory. The findings shed lights on developing advanced electrode materials for high performance electrochemical energy storage.

Ultrafast flashlight sintered mesoporous NiO nanosheets for stable asymmetric supercapacitors

Ultrafast flashlight sintering (FLS) has become an important green manufacturing technology for the structural reformation of various nanomaterials. Nickel oxide (NiO) has been extensively studied as a promising electrode material for electrochemical energy storage owing to its high theoretical specific capacitance, low cost, and appropriate chemical compatibility. This study reports the fabrication of mesoporous ultrathin NiO nanosheets on carbon cloth (CC) as green electrodes for flexible supercapacitors (SCs) through an exceptional ultrafast millisecond FLS process at room temperature. The optimized FLS-NiO@i12J electrode exhibited a remarkable specific capacity of 202.3 mA h g−1 (1215 F g−1) at a current density of 2 A g−1. Strikingly, the as-fabricated FLS-NiO electrodes outperformed the time and energy-consuming conventional thermally annealed (CTA) NiO electrodes. Furthermore, the flexible FLS-NiO@i12J//rGO asymmetric SCs deliver a remarkable energy density of 47.18 Wh kg−1 at a power density of 758.37 W Kg−1 and extraordinary cycling stability performance after 15,000 cycles. In addition, the FLS-NiO@i12J electrodes offer unique mesoporous structures, high surface areas, and numerous open-pore channels of ultrathin NiO nanosheets that facilitate fast transport of ions and rapid redox reactions. Thus, the present approach is promising for designing advanced electrode materials for flexible energy storage applications.

Improved energy conversion and storage performance enabled by hierarchical zigzag-like P-doped CuCo2O4 nanosheets based 3D electrode materials

Developing a bi-functional material which can meet both electrochemical water splitting and supercapacitors (SCs) is a hot spot in current research. In this study, hierarchical zigzag-like phosphorus doped CuCo 2 O 4 nanosheets based 3D electrode materials were successfully synthesized via a hydrothermal method and followed by thermal treatment. Since the unique morphology of 2D nanosheets with zigzag-like edges could provide more reactive sites, which is not only conducive to the hydrogen evolution reaction (HER), but also conducive to the electrochemical energy storage. Meanwhile, the doping of phosphorus was adopted to improve the conductivity, which would further enhance the electrochemical properties of CuCo 2 O 4 . Thereafter, its performance for HER and SCs in 1 M KOH were systematically investigated. As an electrode for HER, it only required a low overpotential of 152 mV to reach 10 mA cm −2 with a Tafel slope of 115.7 mV dec −1 . Furthermore, I-t test result showed an excellent stability. As an electrode for SCs, it exhibited a high specific capacity of 896.9C g −1 at 1 A g −1 in three-electrode system. All in all, the obtained hierarchical zigzag-like phosphorus doped CuCo 2 O 4 nanosheets provided a feasible route for the design of bi-functional electrode materials both for energy conversion and storage. • The hierarchical zigzag-like P-doped CuCo 2 O 4 nanosheets based 3D electrode materials were successfully prepared. • P-doped CuCo 2 O 4 nanosheets based electrode exhibited improved electrocatalytic activity for HER and excellent stability. • P-doped CuCo 2 O 4 electrode materials can attain great specific capacitances of 1993 F g −1 and excellent endurance performance. • The synthesized zigzag-like P-doped CuCo 2 O 4 nanosheets can be sustainable bifunctional materials for HER and supercapacitors.

Construction of metal-organic framework derived Co-Mo-S nanosheets arrays as high-performance electrode for battery-supercapacitor hybrid devices

Bimetallic metal-organic framework (MOF) has attracted great interest as an electrode for supercapacitors. Most metal sources are limited to valences of + 2 and + 3. We select metal sources of Co (II) and Mo (VI) and demonstrated a crystalline bimetallic MOF precursor prepared by using a facile chemical synthesis. The one-step solvothermal strategy is assisted by thioacetamide (TAA) for the self-assembly Co-Mo-S nanosheet arrays (Co-Mo-S NSAs). TAA-induced etching is essential to regulate the assembly of amorphous structures. Otherwise, only a single-structure crystalline Co-Mo-S could be obtained. The Co-Mo-S NSAs show a large specific capacitance of 1805.28 F g−1 at a current density of 0.5 A g−1. A Co-Mo-S NSAs//AC battery−supercapacitor hybrid (BSH) make with activated carbon as the negative electrode and Co-Mo-S NSAs as the positive electrode. At a current density of 0.5 A g−1, the BSH shows a high energy density of 169.73 Wh kg−1 and a power density of 371.44 W kg−1. After 50,000 cycles, the capacitance retention rate is as high as 94.44%, showing good reversibility and cycle life. This work provides an effective strategy for manufacturing bimetallic MOF-based metal sulfide heterostructure electrode materials for practical energy storage and conversion.

Nitrogen-doped carbon nanofibers derived from phenolic-resin-based analogues for high-performance lithium-ion batteries

The preparation of one-dimensional (1-D) carbon nanofibers (CNFs) for lithium-ion battery (LIB) anode materials plays a crucial role in electrochemical energy storage, but it still remains a great challenge due to the limited synthesis methods. Herein, we use a facile strategy to prepare the nitrogen-doped porous CNFs with high aspect ratio by direct pyrolysis of their phenolic-resin-based precursors in ammonium atmosphere. The polymer precursors are synthesized via a hydrothermal approach and have very high carbon yield over 50% in mass. Benefited from the unique 1-D porous structure, high nitrogen content and good conductivity, the ammonium-treated N-doped porous CNFs demonstrate an outstanding electrochemical lithium storage performance. The as-prepared N-doped porous CNFs demonstrates a high irreversible capacity of 325.2 mA h g−1 at 1000 mA g−1 together with an excellent long cycling performance (485.1 mA h g−1 at 500 mA g−1) after 500 cycles. This work offers a facile preparation strategy of the N-doped porous CNFs for high-efficiency energy storage electrode materials.

Untying the Bundles of Solution‐Synthesized Graphene Nanoribbons for Highly Capacitive Micro‐Supercapacitors

AbstractThe precise bottom‐up synthesis of graphene nanoribbons (GNRs) with controlled width and edge structures may compensate for graphene's limitations, such as the absence of an electronic bandgap. At the same time, GNRs maintain graphene's unique lattice structure in one dimension and provide more open‐edge structures compared to graphene, thus allowing faster ion diffusion, which makes GNRs highly promising for energy storage systems. However, the current solution‐synthesized GNRs suffer from severe aggregation due to the strong π–π interactions, which limits their potential applications. Thus, it is indispensable to develop a facile and scalable approach to exfoliate the GNRs from the postsynthetic aggregates, yielding individual nanoribbons. Here, a high‐shear‐mixing approach is demonstrated to untie the GNR bundles into practically individual GNRs, by introducing suitable molecular interactions. The micro‐supercapacitor (MSC) electrode based on solution‐processed GNR film exhibits an excellent volumetric capacitance of 355 F cm−3 and a high power density of 550 W cm−3, reaching the state‐of‐the‐art performance of graphene and related carbon materials, and thus demonstrating the great potential of GNRs as electrode materials for future energy storage.