Design Of Nanoarchitectures Research Articles

High-Entropy Engineering in Hollow Layered Hydroxide Arrays to Boost 5-Hydroxymethylfurfural Electrooxidation by Suppressing Oxygen Evolution.

The electricity-driven 5-hydroxymethylfurfural (HMF) oxidation reaction has exhibited increasing potential to produce high-value-added 2,5-furandicarboxylic acid (FDCA). Unfortunately, the competitive oxygen evolution reaction (OER) can decrease the yield and Faradaic efficiency (FE) of FDCA under high potentials. Here, we report a general MOF-templated strategy to construct a new class of hollow high-entropy layered hydroxide array (HE-LHA) electrocatalysts including quinary, senary, and septenary phases composed of CoNiMnCuZn with Cd and Mg on carbon cloth (CC) for boosting the HMF oxidation reaction (HMFOR) by suppressing the OER. Impressively, the septenary CC@CoNiMnCuZnCdMg-LHA exhibits a low potential of 1.42 VRHE for the HMFOR but a high potential of 1.68 VRHE for the OER to achieve 100 mA cm-2, ranking it among one of the best electrocatalysts for the HMFOR. Finite element simulations show its hollow array morphology can induce a strong local electric field over all of the shell, thus favoring the electrocatalytic process. In situ electrochemical impedance spectroscopy and theoretical calculations further reveal that the Co, Ni, Cu, Zn, Mn, Cd, and Mg metals in high-entropy LHAs can accelerate the HMFOR but suppress the OER by optimizing the adsorption energy of the HMF* and OH*. This work sheds light on the rational design and construction of high-entropy nanoarchitectures for advanced electrocatalysis.

Topology Selectivity of a Conformationally Flexible Precursor by Selenium Doping

Conformational arrangements within nanostructures play a crucial role in shaping the overall configuration and determining the properties, for example in covalent/metal organic framework (COF/MOF) synthesis. In on-surface synthesis, conformational diversity often leads to uncontrollable or disordered structures. Therefore, exploration on controlling and directing the conformational arrangements is significant in achieving desired nanoarchitectures. In this study, a conformationally flexible precursor 2,4,6-tris(3-bromophenyl)-1,3,5-triazine (mTBPT) was employed, and a random phase consisting of C3h and Cs conformers was first obtained after deposition of mTBPT on Cu(111) from room temperature (RT) to ~365 K as expected. By low coverage (0.01 ML) selenium (Se) doping, we achieved the selectivity of the C3h conformer greatly and improved the nanopore structural homogeneity. The ordered 2D metal organic nanostructure from mTBPT could be fulfilled by Se doping from RT to ~365 K, and the deposition sequence of mTBPT and Se did not make any difference. Through the combination of high-resolution scanning tunneling microscopy and non-contact atomic force microscopy, we explored the regulation of the conformationally flexible mTBPT on Cu(111) and achieved the high topology selectivity by low coverage Se doping. Density functional theory calculations revealed the energy regulation of organometallics before and after Se doping at atomic level. These results could enrich the on-surface synthesis toolbox of conformationally flexible precursors, for the design of complex nanoarchitectures, and for future development of engineered nanomaterials and nanodevices. Figure 1

Order-in-disordered ultrathin carbon nanostructure with nitrogen-rich defects bridged by pseudographitic domains for high-performance ion capture

Carbon materials with defect-rich structure are highly demanded for various electrochemical scenes, but encountering a conflict with the deteriorative intrinsic conductivity. Herein, we build a highway-mediated nanoarchitecture that consists of the ordered pseudographitic nanodomains among disordered highly nitrogen-doped segments through a supramolecular self-assembly strategy. The “order-in-disorder” nanosheet-like carbon obtained at 800 °C (O/D NSLC-800) achieves a tradeoff with high defect degree (21.9 at% of doped nitrogen) and compensated electrical conductivity simultaneously. As expected, symmetrical O/D NSLC-800 electrodes exhibit superior capacitive deionization (CDI) performance, including brackish water desalination (≈82 mgNaCl g−1 at a cell voltage of 1.6 V in a 1000 mg L−1 NaCl solution) and reusage of actual refining circulating cooling water, outperforming most of the reported state-of-the-art CDI electrodes. The implanted pseudographitic nanodomains lower the resistance and activation energy of charge transfer, which motivates the synergy of hosting sites of multiple nitrogen configurations. Our findings shed light on electrically conductive nanoarchitecture design of defect-rich materials for advanced electrochemical applications based on molecular-level modulation.

Hollow Co3O4 nanoparticles on CNF with polydopamine assistance for enhanced supercapacitor electrodes

Transition metal oxides (TMOs) are increasingly recognized as viable cathode materials for pseudocapacitors, due to their substantial theoretical capacity, widespread availability, and environmental benignity. However, their practical application is hindered by significant volumetric expansion during reactions and their inherently limited electrical conductivity. The design of hollow nanoarchitectures, coupled with carbonaceous material integration, has emerged as a potent approach to surmount these limitations. Herein, we reported a stepwise synthesis method where Cobalt oxide (Co3O4) nanoparticles, anchored onto carbon nanofibers (CNF) pre-modified with Polydopamine (PDA) known for its superior adhesion, were transformed into HCo3O4@C@CNF composite materials via a high-temperature annealing process. The mass ratio of Co3O4 to CNF was optimized, with a 3:1 ratio being identified as ideal. This optimized HCo3O4@C@CNF electrode exhibited outstanding electrochemical performance, attaining a significant specific capacitance of 2992 F g-1 at 3 A g-1 and maintaining a 91% capacitance retention rate following 8000 charge-discharge cycles. The CNF acted as an efficient conductive network, substantially enhancing the electrical conductance. Furthermore, the incorporation of PDA facilitated a more uniform dispersion and substantial loading of Co3O4, while the carbon shell, formed upon carbonization, effectively prevented the agglomeration of HCo3O4 nanoparticles, enhancing the overall stability and performance of the electrode. Therefore, the synthesized HCo3O4@C@CNF electrodes exhibit a viable approach for the preparation of electrode materials with high-performance.

Accessing versatile tensile ductility of amorphous materials by fractal nanoarchitecture design

Amorphous materials have been known to be intrinsically brittle under tensile stress. This is especially true in silicon-based and metallic-based glasses. In particular, for the latter, they quite often show promising mechanical properties superior to their crystalline counterparts. However, lacking tensile ductility strongly prohibits them from servicing the societies. Although with decades of immense research efforts, we are still waiting for a sophisticated solution. To march in this direction, in this work, we are dedicated to finding a practical method by smart fractal nano-architecture design through advanced computational modeling. This mainly aims to circumvent the intrinsic strain localization at the nano-scale to avoid catastrophic failure. By distributing the external strain to numerous self-confined nano-branches, we successfully achieve astonishing and tunable tensile ductility. This strategy proves to be very effective for different classes of amorphous materials. We found that the tensile properties of the nano-architectured glasses depend on both the constituent elements and the nanostructure. This demonstrates our flexible capability to design desired mechanical properties for a specific material at any spatial length scale. The current findings will inspire experimental realization by cutting-edge 3D-printing techniques and call for optimal design by top-notch graph neural network deep learning algorithms. This work also proposes a new ’structure’-property relationship to efficiently bridge experimental fabrication and computational design.

Eco-friendly aqueous spinning of robust and porous carbon nanotube/graphene hybrid microelectrodes: The graphene oxide size effect

An eco-friendly, cost-effective, and scalable aqueous spinning of robust and porous hybrid fibers consisting of carbon nanotubes (CNTs) and graphene has been developed. We focus on the design of nanoarchitecture within CNT fibers involving the precise control of CNT bundle size and alignment, porosity, and the interaction between CNTs and Graphene. The effect of graphene oxides (GO) sizes on the quality of CNT/GO aqueous dispersions and the structures/properties of the as-spun fibers was investigated, and nano-sized GO was found to be most effective in reducing CNT bundle size, improving CNT alignment, and strengthening the fibers. After high-temperature treatment, the specific strength and specific conductivity of these CNT/graphene hybrid fibers reached to 1.02 N/tex and 1202.01 S m2/g, which were 7.39 and 1.21 times higher than those of pure CNT fibers. Meanwhile, the CNT/graphene hybrid fibers also have a high specific capacity of 168 F g−1. The combination of high mechanical, electrical, and electrochemical performances makes the CNT/graphene hybrid fibers promising materials for wearable electronics.

Topology selectivity of a conformationally flexible precursor through selenium doping

Conformational arrangements within nanostructures play a crucial role in shaping the overall configuration and determining the properties, for example in covalent/metal organic frameworks. In on-surface synthesis, conformational diversity often leads to uncontrollable or disordered structures. Therefore, the exploration of controlling and directing the conformational arrangements is significant in achieving desired nanoarchitectures. Herein, a conformationally flexible precursor 2,4,6-tris(3-bromophenyl)−1,3,5-triazine is employed, and a random phase consisting of C3h and Cs conformers is firstly obtained after deposition of the precursor on Cu(111) at room temperature to 365 K. At low coverage (0.01 ML) selenium doping, we achieve the selectivity of the C3h conformer and improve the nanopore structural homogeneity. The ordered two-dimensional metal organic nanostructure can be fulfilled by selenium doping from room temperature to 365 K. The formation of the conformationally flexible precursor on Cu(111) is explored through the combination of high-resolution scanning tunneling microscopy and non-contact atomic force microscopy. The regulation of energy diagrams in the absence or presence of the Se atom is revealed by density functional theory calculations. These results can enrich the on-surface synthesis toolbox of conformationally flexible precursors, for the design of complex nanoarchitectures, and for future development of engineered nanomaterials.

Chiroplasmonic DNA Scaffolded "Fusilli" Structures.

DNA is an ideal template for the design of nanoarchitectures with molecular-like features. Here, we present an optimized assembly strategy for the concatenation of DNA quasi-rings into long scaffolds. Ionic strength, which played a major role during self-assembly, produced the expected high quality only at 15 mM MgCl2. Atomic force microscopy (AFM) characterization showed several micrometer long tubular structures that were used as templates for the positioning of plasmonic nanoparticles (NPs) along a three-dimensional helical path using DNA tethers. As imaged by high-resolution scanning transmission electron microscopy (HR-STEM) and modeled by theoretical calculations, the NPs distributed into a "fusilli" fashion (i.e., a helical pasta shape), displaying chiroptical activity as revealed by a bisignated CD absorption, centered at the plasmon resonance wavelength. The present structures contribute to enrich the ever-developing arena of chiroplasmonic DNA-based nanomaterials and demonstrate that large assemblies are attainable for their future application to develop metamaterials.

Rapid one-step aqueous synthesis of porous PtAg wavy nanochains for methanol electrooxidation with a high CO-tolerance

Tailored morphology of porous binary Pt-based nanostructures is a powerful way to improve their catalytic properties. Herein, we develop a facile aqueous solution approach for the rational one-step synthesis of PtAg nanochains via direct nucleation followed by the oriented attachment growth mechanism under sonication at room temperature. This allows the green and simple fabrication of PtAg wavy nanochains (200 nm length and 20 nm width) with spatially interconnected pores (10 nm) and a high surface area (55.02 m2/g). These merits endowed the methanol oxidation reaction (MOR) performance of PtAg nanochains with a mass activity of (1.12 mA/µgPt) that was about 1.83, 2.8, and 3.11 times higher than those of PtAg nanodendrites, Pt nanodendrites, and commercial Pt/C, respectively, owing to porous nanochain morphology and alloying effect. Intriguingly, visible-light irradiation enhances the MOR performance of PtAg nanochain by nearly 1.5 times, owing to its great photoelectric response properties. The MOR activity of PtAg nanochains is among the highest reported Pt-based electrocatalysts. The presented method may open new edges on the rational design of porous Pt-based nanoarchitecture for various catalytic applications.

2D petal-like PdAg nanosheets promote efficient electrocatalytic oxidation of ethanol and methanol.

The development of efficient alcohol electrooxidation catalysts is of vital importance for the commercialization of direct liquid fuel cells. As emerging advanced catalysts, two-dimensional (2D) noble metal nanomaterials have attracted much research attention due to their intrinsic structural advantages. Herein, we report the synthesis of petal-like PdAg nanosheets (NSs) with an ultrathin 2D structure and jagged edges via a facile wet-chemical approach, combining doping engineering and morphology tuning. Notably, the highly active sites and Pd-Ag composition endowed PdAg NSs with improved toxicity tolerance and substantially improved the durability toward the ethanol/methanol oxidation reaction (EOR/MOR). Moreover, the electronic effect and synergistic effect significantly enhanced the EOR and MOR activities in comparison with Pd NSs and commercial Pd/C. This work provides efficient catalysts for fuel electrooxidations and deep insight into the rational design and fabrication of novel 2D nanoarchitecture.

3D binder-free nanoarchitecture design of porous silicon/graphene fibers for ultrastable lithium storage

Enhancing the stability and fast-charging capability of battery electrodes is of paramount importance in the field of battery technology. Silicon (Si), renowned for its high specific capacity, has emerged as a promising candidate for anodes. However, the limited structural stability and electron/ion conductivity of silicon-based anodes have raised significant concerns, including fractures and the continuous formation of unstable solid-electrolyte interphase (SEI) layers, leading to rapid capacity decay. In this study, we introduce a comprehensive approach to fabricating a binder-free and free-standing anode electrode paper using a combination technique of employing electrospinning, magnetron sputtering, and chemical vapor deposition (CVD) techniques. This developed paper electrode incorporates a 3D interconnected network of nitrogen-doped vertical graphene nanosheets (VGs) that connect porous carbon fibers (PCFs) with uniformly distributed Si nanoparticles (VGs@Si@PCFs). The as-fabricated VGs@Si@PCFs paper effectively addresses the mechanical and chemical stability issues commonly associated with Si anodes. The VGs@Si@PCFs anode demonstrates a remarkable reversible capacity of 2205 mAh g-1 at 0.1 A g-1 and exhibits exceptional cycling performance with 83.5% capacity retention at 1.0 A g-1 after 3000 cycles. This design leverages the nanoporous carbon fibers and nitrogen-doped vertical graphene nanosheets as flexible and conductive supports, enhancing the robustness and flexibility of the electrode. Additionally, mechanical modeling reveals that the overall Mises strain in the porous VGs@Si@PCFs structure is significantly lower compared to nonporous cases, potentially minimizing low-cycle fatigue. Our free-standing Si/C composite anode introduces a new class of low-strain Si-based materials, showcasing significantly improved stabilities and fast-charging capabilities.

Heterostructured Ni2P/NiMo-layered double hydroxide nanoarrays with enriched redox active sites for supercapacitors

The electroactivity and cyclic stability of transition metal phosphides (TMPs) for supercapacitors are restricted by inadequate redox active sites and huge volume changes during the charging/discharging process. Herein, a three-dimensional (3D) porous Ni2P/NiMo-layered double hydroxide (NiMo-LDH) heterostructure with large specific surface and abundant pore channels is explored as a self-supporting supercapacitor electrode. The well-defined hierarchical pore structure can offer numerous electroactive sites and short ion/electron pathways. The generation of heterointerfaces between multi-dimensional Ni2P and two-dimensional (2D) NiMo-LDH nanosheets endows the hybrid composite with improved electrical conductivity and structural robustness. Consequently, the special nanoarchitecture design achieves a specific capacity of 198.6 mAh g−1 (2.28 mAh cm−2) at 1 A g−1 and an impressive rate performance of 78.3% at 20 A g−1. More importantly, the assembled Ni2P/NiMo-LDH//orange peel-derived porous carbon (OPC) asymmetric supercapacitor (ASC) device delivers a remarkable specific energy of 63.7 Wh kg−1 at a specific power of 1138.3 W kg−1 and long-term cycling stability (91.7% over 10,000 cycles). The research highlights that the hybridization of TMPs and other nanostructured battery-type materials may produce a synergistic effect and boost the capacitive properties.

Catalysis Sans Catalyst Loss: The Origins of Prolonged Stability of Graphene-Metal-Graphene Sandwich Architecture for Oxygen Reduction Reactions.

Over the past decades, the design of active catalysts has been the subject of intense research efforts. However, there has been significantly less deliberate emphasis on rationally designing a catalyst system with a prolonged stability. A major obstacle comes from the ambiguity behind how catalyst degrades. Several degradation mechanisms are proposed in literature, but with a lack of systematic studies, the causal relations between degradation and those proposed mechanisms remain ambiguous. Here, a systematic study of a catalyst system comprising of small particles and single atoms of Pt sandwiched between graphene layers, GR/Pt/GR, is studied to unravel the degradation mechanism of the studied electrocatalyst for oxygen reduction reaction(ORR). Catalyst suffers from atomic dissolution under ORR harsh acidic and oxidizing operation voltages. Single atoms trapped in point defects within the top graphene layer on their way hopping through toward the surface of GR/Pt/GR architecture. Trapping mechanism renders individual Pt atoms as single atom catalyst sites catalyzing ORR for thousands of cycles before washed away in the electrolyte. The GR/Pt/GR catalysts also compare favorably to state-of-the-art commercial Pt/C catalysts and demonstrates a rational design of a hybrid nanoarchitecture with a prolonged stability for thousands of operation cycles.

A flower‐like VO2(B)/V2CTx heterojunction as high kinetic rechargeable anode for sodium‐ion batteries

AbstractVO2(B) is considered as a promising anode material for the next‐generation sodium‐ion batteries (SIBs) due to its accessible raw materials and considerable theoretical capacity. However, the VO2(B) electrode has inherent defects such as low conductivity and serious volume expansion, which hinder their practical application. Herein, a flower‐like VO2(B)/V2CTx (VO@VC) heterojunction was prepared by a simple hydrothermal synthesis method with in situ growth. The flower‐like structure composed of thin nanosheets alleviates the volume expansion, as well as the rapid Na+ transport pathways are built by the heterojunction structure, resulting in long‐term cycling stability and superior rate performance. At a current density of 100 mA g−1, VO@VC anode can maintain a specific capacity of 276 mAh g−1 with an average coulombic efficiency of 98.7% after 100 cycles. Additionally, even at a current density of 2 A g−1, the VO@VC anode still exhibited a capacity of 132.9 mAh g−1 for 1000 cycles. The enhanced reaction kinetics can be attributed to the fast Na+ adsorption and storage at interfaces, which has been confirmed by the experimental and theoretical methods. These results demonstrate that the tailored nanoarchitecture design and additional surface engineering are effective strategies for optimizing vanadium‐based anode.

CuO/TiO2 heterostructure-based sensors for conductometric NO2 and N2O gas detection at room temperature

Nitrous oxide (N2O) is hazardous gas extensively used in surgeries as an anesthetic and released into the atmosphere without any treatment. Despite low concentrations in the atmosphere, it has for 300 times larger warming coefficient to the greenhouse effect than CO2. There are only a few studies dedicated to the development of N2O gas sensors, but not for room temperature (RT) and ultra-low concentrations. In this study, we developed an ultrasensitive gas-sensing device operating at RT based on CuO/TiO2 heterojunctioned nanointerfaces prepared by scalable reactive magnetron sputtering technique with glancing angle deposition. The CuO/TiO2 heterojunctioned nanointerfaces demonstrated N2O gas sensitivity for ∼2 times higher than TiO2 mono-layer, and the device exhibits an outstanding detection limit of 50 ppb at RT, quick response and recovery times (∼36 s and ∼50 s). The ultrasensitivity of gas sensor is achieved by providing control over nanoarchitecture and comparable size of the nanorods-like structure to the doubled Debye lengths (∼70–80 nm). The applied nanoarchitecture design opens a flexible platform for different gas sensing devices where the array of p-n heterojunction nanorods was utilized efficiently and with technological simplicity. The statistical analysis of variances shows that obtained data is more confident and reproducible.

Fully sprayed MXene-based high-performance flexible piezoresistive sensor for image recognition

High-performance flexible pressure sensors provide comprehensive tactile perception and are applied in human activity monitoring, soft robotics, medical treatment, and human-computer interface. However, these flexible pressure sensors require extensive nano-architectural design and complicated manufacturing and are time-consuming. Herein, a highly sensitive, flexible piezoresistive tactile sensor is designed and fabricated, consisting of three main parts: the randomly distributed microstructure on T-ZnOw/PDMS film as a top substrate, multilayer Ti3C2-MXene film as an intermediate conductive filler, and the few-layer Ti3C2-MXene nanosheet-based interdigital electrodes as the bottom substrate. The MXene-based piezoresistive sensor with randomly distributed microstructure exhibits a high sensitivity over a broad pressure range (less than 10 ​kPa for 175 ​kPa−1) and possesses an out-standing permanence of up to 5000 cycles. Moreover, a 16-pixel sensor array is designed, and its potential applications in visualizing pressure distribution and an example of tactile feedback are demonstrated. This fully sprayed MXene-based pressure sensor, with high sensitivity and excellent durability, can be widely used in, electronic skin, intelligent robots, and many other emerging technologies.

Mass Loading-Independent Lithium Storage of Transitional Metal Compounds Achieved by Multi-Dimensional Synergistic Nanoarchitecture.

Nanostructured transitional metal compounds (TMCs) have demonstrated extraordinary promise for high-efficient and rapid lithium storage. However, good performance is usually limited to electrodes with low mass loading (≤1.0 mg cm-2 ) and is difficult to realize at higher mass loading due to increased electrons/ions transport limitations in the thicker electrode. Herein, the multi-dimensional synergistic nanoarchitecture design of graphene-wrapped MnO@carbon microcapsules (capsule-like MnO@C-G) is reported, which demonstrates impressive mass loading-independent lithium storage properties. Highly porous MnO nanoclusters assembled by 0D nanocrystals facilitate sufficient electrolyte infiltration and shorten the solid-state ions transport path. 1D carbon shell, 2D graphene, and 3D continuous network with tight interconnection accelerate electrons transport inside the thick electrode. The capsule-like MnO@C-G delivers ultrahigh gravimetric capacity retention of 91.0% as the mass loading increases 4.3 times, while the areal capacities increase linearly with the mass loading at various current densities. Specifically, the capsule-like MnO@C electrode delivers a remarkable areal capacity of 2.0 mAh cm-2 at a mass loading of 3.0 mg cm-2 . Moreover, the capsule-like MnO@C also demonstrates excellent performance in full battery applications. This study demonstrates the effectiveness of multi-dimensional synergistic nanoarchitecture in achieving mass loading-independent performance, which can be extended to other TMCs for electrochemical energy storage.

Design of nanoarchitecture for synergistic interactions to realize nanoflower-like Ni3S4 supported on graphene sheets as high-performance supercapacitor electrodes

Design of nanoarchitecture for synergistic interactions to realize nanoflower-like Ni3S4 supported on graphene sheets as high-performance supercapacitor electrodes

High-Energy and High-Power Primary Li-CFx Batteries Enabled by the Combined Effects of the Binder and the Electrolyte

Several effective methods have been developed recently to demonstrate simultaneous high energy and high power density in Lithium - carbon fluoride (Li-CFx) batteries. These methods can achieve as high as a 1000 Wh/kg energy density at a 60–70 kW/kg power density (40–50 C rate) in coin cells and a 750 Wh/kg energy density at a 12.5 kW/kg power density (20 C rate) in pouch cells. This performance is made possible by an ingenious nano-architecture design, controlled porosity, boron doping, and electrolyte additives. In the present study, we show that a similarly great performance, a 931 Wh/kg energy density at a 59 kW/kg power density, can be achieved by using a polyacrylonitrile binder and a LiBF4 electrolyte in Li-graphite fluoride coin cells. We also demonstrate that the observed effect is the result of the right combination of the binder and the electrolyte. We propose that the mechanistic origin of the observed phenomena is an electro-catalytic effect of the polyacrylonitrile binder. While our proposed method has a competitive performance, it also offers a simple implementation and a scalable production of high-energy and high-power primary Li-CFx cells.

High‐rate sodium‐ion storage of vanadium nitride via surface‐redox pseudocapacitance

AbstractVanadium nitride (VN) electrode displays high‐rate, pseudocapacitive responses in aqueous electrolytes, however, it remains largely unclear in nonaqueous, Na+‐based electrolytes. The traditional view supposes a conversion‐type mechanism for Na+ storage in VN anodes but does not explain the phenomena of their size‐dependent specific capacities and underlying causes of pseudocapacitive charge storage behaviors. Herein, we insightfully reveal the VN anode exhibits a surface‐redox pseudocapacitive mechanism in nonaqueous, Na+‐based electrolytes, as demonstrated by kinetics analysis, experimental observations, and first‐principles calculations. Through ex situ X‐ray photoelectron spectroscopy and semiquantitative analyses, the Na+ storage is characterized by redox reactions occurring with the V5+/V4+ to V3+ at the surface of VN particles, which is different from the well‐known conversion reaction mechanism. The pseudocapacitive performance is enhanced through nanoarchitecture design via oxidized vanadium states at the surface. The optimized VN‐10 nm anode delivers a sodium‐ion storage capability of 106 mAh g−1 at the high specific current of 20 A g−1, and excellent cycling performance of 5000 cycles with negligible capacity losses. This work demonstrates the emerging opportunities of utilizing pseudocapacitive charge storage for realizing high‐rate sodium‐ion storage applications.