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Anode-free lithium metal batteries (AFLBs) have attracted considerable attention due to their high theoretical specific capacity and absence of Li. However, the heterogeneous Li deposition and stripping on the lithiophobic Cu collector hamper AFLBs in practice. To achieve a uniform and reversible Li deposition, a carbon-based layer on the Cu collector has attracted intense interest due to its high conductivity. However, the 2D single-component carbon-based interface is inadequate lithiophilic for obtaining the homogeneous Li deposition and preventing the lithium dendrite from piercing the separator. Herein, we present a 3D embedded lithiophilic SiO2 nanoparticles-graphene nanosheet matrix (SiO2@G-M) on the Cu collector by organic nano carbon source. In this structure, the lithiophilic SiO2 nanoparticles as active points promote the homogeneous lithium nucleation and the 3D graphene nanosheet matrix offers homogenous electron distribution and voids to prevent the piercing. Finally, SiO2@G-M/Li cell shows a high coulombic efficiency of 98.62 % after 100 cycles at a high current density of 2 mA cm-2 with an areal capacity of 1 mAh cm-2.
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Metal-halide perovskite nanocrystals (NCs) are one of the most promising emitters for the application of display and nanolight sources. The full width at half-maximum (FWHM) of photoluminescence (PL) emission is essential for color purity, which however remains a difficulty to further reduce the FWHM of the perovskite NCs at room temperature. Here, we show the quasi-sphere perovskite NCs with narrow PL emission at a deep-blue wavelength of â¼430 nm; its PL FWHM reaches â¼11 nm at room temperature, owing to the monodispersion in size distribution as well as the symmetric quasi-sphere morphology of NCs releasing the fine structure splitting-induced inhomogeneous broadening. Through regulating A cations with respect to the ratio of FA (or MA)-to-Cs and Cs-to-Pb, the PL emission of the NCs could be tuned from â¼505 to â¼430 nm combined with varied morphologies from large cube to small quasi-sphere. Such spectroscopic and morphological discrepancies are supposed to be attributed to the different crystalline kinetics that is strongly dependent on the synthetic condition. To be specific, in the case of increasing FA (or MA)-to-Cs, the growth rate of CsPbBr3 and FAPbBr3 (or MAPbBr3) perovskites is determined by the reactivity of transient species, while in the case of decreasing the Cs-to-Pb ratio, the growth rate of perovskites is slowed down by the serious reduction of Cs+ in the precursor. This study provides an effective strategy to adjust the emission across from green to deep-blue color and promotes the perovskite NCs with a narrow FWHM, and tunable PL emission facilitates in application of optoelectronic devices.
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The development of high-performance artificial synaptic neuromorphic devices poses a significant challenge in the creation of biomimetic sensing neural systems that seamlessly integrate both sensory and computational functionalities. In pursuit of this objective, promising bionic opto-olfactory co-sensory artificial synapse devices are constructed utilizing the BP-C/CNT (2D/1D) hybrid filter membrane as the resistive layer. Experimental results demonstrated that the devices seamlessly integrated the light modulation, gas detection, and biological synaptic functions into a single device while addressing the challenge with separating artificial synaptic devices from sensors. These devices offered the following advantages: 1) Simulating visual synapses, they can effectively replicate fundamental synaptic functions under both electrical and optical stimulation. 2) By emulating olfactory synapse responses to specific gases, they can achieve ultra-low detection limits and rapid identification of ethanol and acetone gases. 3) They enable photo-olfactory co-sensing simulations that mimic synaptic function under light-modulated pulse conditions in distinct gas environments, facilitating the study of synaptic learning rules and Pavlovian responses. This work provides a pioneering approach for exploring highly stable 2D BP-based optoelectronics and advancing the development of biomimetic neural systems.
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Biónica , Sinapsis , Sinapsis/fisiología , Biónica/métodos , Biomimética/métodos , Nanotubos de Carbono/química , Olfato/fisiologíaRESUMEN
The design and construction of highly efficient electrocatalysts for overall water splitting and urea electrolysis are significantly important for promoting energy conversion and realizing green hydrogen production. In this work, we constructed a multi-phase heterojunction through a simple hydrothermal and phosphorization process. The P-doped NiFe2O4 (P-NiFe2O4) nanoparticles were uniformly anchored on the bamboo-like N-doped carbon nanotubes (NCNTs) grown via a NiFe-alloy autocatalysis. The electronic structure and coordination environment of active species were optimized by the synergistic action of P doping, well-dispersed ultrafine NiFe2O4, and NCNTs matrix with good conductivity, enhancing their quantity and activity for electrocatalysis. Consequently, the P-NiFe2O4/NCNTs/NiFe exhibits excellent HER and OER activities with an overpotential of 111 and 266â mV at 10â mA cm-2 in 1â M KOH, respectively. The symmetrical overall water-splitting cell using P-NiFe2O4/NCNTs/NiFe as both anode and cathode delivers 10â mA cm-2 at a voltage of 1.604â V in 1â M KOH. Notably, the two-electrode cell requires a low voltage of 1.467â V to achieve a current density of 10â mA cm-2 in 1â M KOH solution with 0.6â M urea. This designed catalysts display outstanding reaction kinetics and catalytic stability. This work provides useful guidance for applying transition metal-based catalysts for hydrogen production.
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Modification of oxygen evolution co-catalyst (OEC) on the surface of bismuth vanadate (BiVO4) can effectively improve the kinetics of water oxidation, but it is still limited by the small hole extraction driving force at the BiVO4/OEC interface. Modulating the BiVO4/OEC interface with a hole transfer layer (HTL) is expected to facilitate hole transport from BiVO4 to the OEC surface. Herein, a copper(I) thiocyanate (CuSCN) HTL is inserted between BiVO4 and NiFeOx OEC to create BiVO4/CuSCN/NiFeOx photoanode, resulting in a significant enhancement of photoelectrochemical (PEC) water splitting performance. From electrochemical analyses and density functional theory (DFT) simulations, the markedly enhanced PEC performance is attributed to the insertion of CuSCN as an HTL, which promotes the extraction of holes from BiVO4 surface and boosts the water oxidation kinetics. The optimal photoanode achieves a photocurrent density of 5.6 mA cm-2 at 1.23 V versus the reversible hydrogen electrode (vs. RHE) and an impressive charge separation efficiency of 96.2 %. This work offers valuable insights into the development of advanced photoanodes for solar energy conversion and emphasizes the importance of selecting an appropriate HTL to mitigate recombination at the BiVO4/OEC interface.
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1D nanowire networks, sharing similarities of structure, information transfer, and computation with biological neural networks, have emerged as a promising platform for neuromorphic systems. Based on brain-like structures of 1D nanowire networks, neuromorphic synaptic devices can overcome the von Neumann bottleneck, achieving intelligent high-efficient sensing and computing function with high information processing rates and low power consumption. Here, high-temperature neuromorphic synaptic devices based on SiC@NiO core-shell nanowire networks optoelectronic memristors (NNOMs) are developed. Experimental results demonstrate that NNOMs attain synaptic short/long-term plasticity and modulation plasticity under both electrical and optical stimulation, and exhibit advanced functions such as short/long-term memory and "learning-forgetting-relearning" under optical stimulation at both room temperature and 200 °C. Based on the advanced functions under light stimulus, the constructed 5 × 3 optoelectronic synaptic array devices exhibit a stable visual memory function up to 200 °C, which can be utilized to develop artificial visual systems. Additionally, when exposed to multiple electronic or optical stimuli, the NNOMs effectively replicate the principles of Pavlovian classical conditioning, achieving visual heterologous synaptic functionality and refining neural networks. Overall, with abundant synaptic characteristics and high-temperature thermal stability, these neuromorphic synaptic devices offer a promising route for advancing neuromorphic computing and visual systems.
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The injection and leakage of charge carriers have a significant impact on the optoelectronic performance of GaN-based lasers. In order to improve the limitation of the laser on charge carriers, a slope-shape hole-barrier layer (HBL) and electron-barrier layer (EBL) structure are proposed for near-UV (NUV) GaN-based lasers. We used Crosslight LASTIP for the simulation and theoretical analysis of the energy bands of HBL and EBL. Our simulations suggest that the energy bands of slope-shape HBL and EBL structures are modulated, which could effectively suppress carrier leakage, improve carrier injection efficiency, increase stimulated radiation recombination rate in quantum wells, reduce the threshold current, improve optical field distribution, and, ultimately, improve laser output power. Therefore, using slope-shape HBL and EBL structures can achieve the superior electrical and optical performance of lasers.
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Over the past few decades, the critical role played by cellular contractility associated mechanotransduction in the regulation of cell functions has been revealed. In this case, numerous biomaterials have been chemically or structurally designed to manipulate cell behaviors through the regulation of cellular contractility. In particular, adhesive proteins including fibronectin, poly-L-lysine and collagen type I have been widely applied in various biomaterials to improve cell adhesion. Therefore, clarifying the effects of adhesive proteins on cellular contractility has been valuable for the development of biomaterial design. In this study, reference-free traction force microscopy with a well-organized microdot array was designed and prepared to investigate the relationship between adhesive proteins, cellular contractility, and mechanotransduction. The results showed that fibronectin and collagen type I were able to promote the assembly of focal adhesions and further enhance cellular contraction and YAP activity. In contrast, although poly-L-lysine supported cell spreading and elongation, it was inefficient at inducing cell contractility and activating YAP. Additionally, compared with cellular morphogenesis, cellular contraction was essential for YAP activation.
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Fibronectinas , Mecanotransducción Celular , Fibronectinas/metabolismo , Mecanotransducción Celular/fisiología , Microscopía de Fuerza Atómica , Colágeno Tipo I , Polilisina , Tracción , Adhesión Celular , Materiales BiocompatiblesRESUMEN
The design and synthesis of efficient, inexpensive, and long-term stable heterostructured electrocatalysts with high-density dislocations for hydrogen evolution reaction in alkaline media and seawater are still a great challenge. An amorphous/crystalline/amorphous sandwiched structure with abundant dislocations were synthesized through thermal phosphidation strategies. The dislocations play an important role in the hydrogen evolution reactions. Copious dislocation defects, combined with cracks, and the synergistic interfacial effect between crystalline phase and amorphous phase regulate the electronic structure of electrocatalyst, provide more active sites, and thus endow the electrocatalysts with excellent catalytic activity under alkaline water and seawater. The overpotentials of P-NiMoO4 at 10 mA/cm2 in 1 M KOH aqueous solution and seawater are 45 and 75 mV, respectively. Additionally, the P-NiMoO4 electrocatalyst exhibits long-term stability over 100 h. This study provides a simple approach for synthesizing amorphous/crystalline/amorphous sandwiched non-noble-metal electrocatalysts with abundant dislocations for hydrogen evolution reaction.
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Memristor-based artificial synapses are regarded as the most promising candidate to develop brain-like neuromorphic network computers and overcome the bottleneck of Von-Neumann architecture. Violet phosphorus (VP) as a new allotrope of available phosphorus with outstanding electro-optical properties and stability has attracted more and more attention in the past several years. In this study, large-scale, high-yield VP microfiber vertical arrays have been successfully developed on a Sn-coated graphite paper and are used as the memristor functional layers to build reliable, low-power artificial synaptic devices. The VP devices can well mimic the major synaptic functions such as short-term memory (STM), long-term memory (LTM), paired-pulse facilitation (PPF), spike timing-dependent plasticity (STDP), and spike rate-dependent plasticity (SRDP) under both electrical and light stimulation conditions, even the dendritic synapse functions and simple logical operations. By virtue of the excellent performance, the VP artificial synapse devices can be conductive to building high-performance optic-neural synaptic devices simulating the human-like optic nerve system. On this basis, Pavlov's associative memory can be successfully implemented optically. This study provides a promising approach for the design and manufacture of VP-based artificial synaptic devices and outlines a direction with multifunctional neural devices.
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Lithium-sulfur (Li-S) batteries have ultrahigh theoretical specific capacity and energy density, which are considered to be very promising energy storage devices. However, the slow redox kinetics of polysulfides are the main reason for the rapid capacity decay of Li-S batteries. A reasonable electrocatalyst for the Li-S battery should reduce the reaction barrier and accelerate the reaction kinetics of the bidirectional catalytic conversion of lithium polysulfides (LiPSs), thereby reducing the cumulative concentration of LiPSs in the electrolyte. In this report, porous N-doped carbon nanofibers decorated with independent dual metal sites as catalysts for Li-S batteries were fabricated in one step using a fusion-foaming method. Experimental and theoretical analyses demonstrate that the synergistic effect of independent dual metal sites provides strong LiPS affinity, improved electronic conductivity, and enhanced redox kinetics of polysulfides. Therefore, the assembled Li-S battery exhibits high rate performance (discharge specific capacity of 771 mA h g-1 at 2C) and excellent cycle stability (capacity decay rate of 0.51% after 1000 cycles at 1C).
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Quantum-well intermixing (QWI) technology is commonly considered as an effective methodology to tune the post-growth bandgap energy of semiconductor composites for electronic applications in diode lasers and photonic integrated devices. However, the specific influencing mechanism of the interfacial strain introduced by the dielectric-layer-modulated multiple quantum well (MQW) structures on the photoluminescence (PL) property and interfacial quality still remains unclear. Therefore, in the present study, different thicknesses of SiO2-layer samples were coated and then annealed under high temperature to introduce interfacial strain and enhance atomic interdiffusion at the barrier-well interfaces. Based on the optical and microstructural experimental test results, it was found that the SiO2 capping thickness played a positive role in driving the blueshift of the PL peak, leading to a widely tunable PL emission for post-growth MQWs. After annealing, the blueshift in the InGaAs/AlGaAs MQW structures was found to increase with increased thickness of the SiO2 layer, and the largest blueshift of 30 eV was obtained in the sample covered with a 600 nm thick SiO2 layer that was annealed at 850 °C for 180 s. Additionally, significant well-width fluctuations were observed at the MQW interface after intermixing, due to the interfacial strain introduced by the thermal mismatch between SiO2 and GaAs, which enhanced the inhomogeneous diffusion rate of interfacial atoms. Thus, it can be demonstrated that the introduction of appropriate interfacial strain in the QWI process is of great significance for the regulation of MQW band structure as well as the control of interfacial quality.
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Single-atomic transition metal-nitrogen-carbon (M-N-C) structures are promising alternatives toward noble-metal-based catalysts for oxygen reduction reaction (ORR) catalysis involved in sustainable energy devices. The symmetrical electronic density distribution of the MâN4 moieties, however, leads to unfavorable intermediate adsorption and sluggish kinetics. Herein, a Fe-N-C catalyst with electronic asymmetry induced by one nearest carbon vacancy adjacent to FeâN4 is conceptually produced, which induces an optimized d-band center, lowered free energy barrier, and thus superior ORR activity with a half-wave potential (E1/2 ) of 0.934 V in a challenging acidic solution and 0.901 V in an alkaline solution. When assembled as the cathode of a Zinc-air battery (ZAB), a peak power density of 218 mW cm-2 and long-term durability up to 200 h are recorded, 1.5 times higher than the noble metal-based Pt/C+RuO2 catalyst. This work provides a new strategy on developing efficient M-N-C catalysts and offers an opportunity for the real-world application of fuel cells and metal-air batteries.
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Black phosphorus (BP), as a burgeoning two-dimensional material, has shown good electrocatalytic activity due to its unique electronic structure and abundant active sites.However, the presence of lone pair electrons in black phosphorus leads to its poor stability and rapid degradation in an oxygen/water environment, which greatly limits its practical application. Herein, BP-Co heterojunctions were synthesized on carbon nanotube@nitrogen-doped carbon (BP-Co/CNT@NC) by the pyrolysis of ZnCo-zeolitic imidazolate frameworks and subsequent solvothermal treatment. The BP-Co Schottky junction improved the electrocatalytic stability of BP, modulated its electronic structure, improved its conductivity and electron transfer during the electrocatalytic reaction. Density functional theory calculation was used to confirm the electron transfer and redistribution at the interface between BP and Co, which constructed an oppositely charged region and formed a strong built-in field. Energy band configuration analysis revealed a narrowed band gap because of the formation of BP-Co Schottky junction. Consequently, the optimized BP-Co/CNT@NC exhibited a superior oxygen evolution reaction (OER) performance, a low overpotential of 370 mV@100 mA/cm2, with a small Tafel slope of 40 mV/dec and good long-term stability. Particularly, the catalyst has an excellent OER performance at the high current density of 100-400 mA/cm2. This strategy improves the stability of BP electrocatalysts and strengthens their utilization in electrocatalytic applications.
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Pursuing high power density lithium metal battery with high safety is essential for developing next-generation energy-storage devices, but uncontrollable electrolyte degradation and the consequence formed unstable solid-electrolyte interface (SEI) make the task really challenging. Herein, an ionic liquid (IL) confined MOF/Polymer 3D-porous membrane was constructed for boosting in situ electrochemical transformations of Janus-heterarchical LiF/Li3 N-rich SEI films on the nanofibers. Such a 3D-Janus SEI-incorporated into the separator offers fast Li+ transport routes, showing superior room-temperature ionic conductivity of 8.17×10-4 â S cm-1 and Li+ transfer number of 0.82. The cryo-TEM was employed to visually monitor the in situ formed LiF and Li3 N nanocrystals in SEI and the deposition of Li dendrites, which is greatly benefit to the theoretical simulation and kinetic analysis of the structural evolution during the battery charge and discharge process. In particular, this membrane with high thermal stability and mechanical strength used in solid-state Li||LiFePO4 and Li||NCM-811 full cells and even in pouch cells showed enhanced rate-performance and ultra-long life spans.
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To understand the underlying mechanism of the interfacial charge transfer and local chemical state variation in the nonprecious-based hydrogen evolution reaction (HER) electrocatalysts, a model system of the NiO/CeO2 heterostructure was chosen for investigation using a combination of the advanced electron microscopic characterization and first-principles calculations. The results directly proved that interfacial charge transfer occurs from Ni to Ce, leading to reduction in the valence state of Ce and increased formation of VO. This would optimize ΔGH* and facilitate the hydrogen evolution process, resulting in outstanding HER performance in 1 M KOH with a low overpotential of 99 mV at the current density of 10 mAâ¢cm-2 and a modest Tafel slope of 78.4 mVâ¢dec-1 for the NiO/CeO2 heterostructure sample. Therefore, the improved HER performance could be attributed to the synergistic coupling interactions and electron redistribution at the interface of NiO and CeO2. These results concretely demonstrate the direct determination of the interfacial structure of the heterostructure and provide atomistic insights to unravel the underlying mechanism of interfacial charge transfer induced HER performance improvement.
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White-light-emitting carbon dots (WCDs) show innate advantages as phosphors in white light-emitting diodes (WLEDs). For WLEDs, the color rendering index (CRI) is the most important metric to evaluate its performance. Herein, WCDs are prepared by a facile one-step solvothermal reaction of trimellitic acid and o-phenylenediamine. It consists of four CDs identified by column chromatography as blue, green, yellow, red, and thus white light is a superposition of these four types of light. The mixture of the four CDs undergoes Förster resonance energy transfer to induce the generation of white light. The photoluminescence of WCDs originates from the synergistic effect of carbon core and surface states. Thereinto, the carbon core states dominate in RCDs, and the increase of amide contents and degree of conjugation promote the redshift of the emission spectra, which is further confirmed by theoretical calculations. In addition, a high CRI of 97 is achieved when the WCDs are used as phosphors to fabricate WLEDs, which is almost the highest value up to now. The multicolor LEDs can also be fabricated by using the four multicolor CDs as phosphors, respectively. This work provides a novel approach to explore the rapid preparation of low-cost, high-performance WCDs and CDs-based WLEDs.
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In order to solve the problem of poor compatibility between modified-ZIF-8 nanoparticles and mask matrix polypropylene (PP) and melt-blown materials, in this work, PP based modified-ZIF-8 antibacterial masterbatch was prepared employing surface modification and torque blending method. IR, SEM, XRD, XPS, DSC results confirm that the antibacterial masterbatch maintains the chemical and crystal structure of modified-ZIF-8 and the thermal stability of PP. Photocatalytic performance indicates that the antibacterial masterbatch basically maintains the photoresponse range of modified-ZIF-8, has narrower band gap and the superior photocatalytic performance than that of modified-ZIF-8. The photocatalytic antibacterial mechanism of ·O2- and h+ as antibacterial active species is revealed according to the energy band structure and free radical capture experiment. The photocatalytic antibacterial activity of the antibacterial masterbatch against Staphylococcus aureus and Escherichia coli under different dosage holds that the relationship between antibacterial rate and antibacterial agent concentration conforms to Beta distribution, demonstrating second-order kinetic behavior. The antibacterial properties reach the maximum when the loading of modified-ZIF-8 is 2% of the total weight of PP and melt-blown materials. S. aureus and E. coli could be completely killed when the simulated sunlight is irradiated for 30 min. These results indicate that PP based modified-ZIF-8 antibacterial masterbatch has potential application in photocatalytic antibacterial masks.
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The anti-counterfeiting technology of banknotes, bills and negotiable securities is constantly copied, and it is urgent to upgrade its anti-counterfeiting technology. In view of the defect of easy replication of single-wavelength anti-counterfeiting technology, the bonded copolymer PMEuTb was synthesized, employing the technique of first coordination and then polymerization. The molecular structure of copolymer PMEuTb was confirmed by infrared spectrum and UV-vis absorption spectrum. The internal mechanism of negative correlation between initiator concentration and number-average molecular weight Mn of the copolymer was revealed, and the positive correlation between Mn and luminescent behavior of the copolymer was analyzed. The luminescent properties of copolymer PMEuTb with initiator amount of 0.1% were investigated, the copolymer PMEuTb exhibits dual-wavelength emission of green light and red light under the excitation of ultraviolet light at 254 nm and 365 nm. The copolymer has the lifetime of 1.083 ms at 5D4-7F5 transition and 0.665 ms at 5D0-7F2 transition, which belongs to phosphorescent emitting materials. The copolymer remains stable at 240 °C, and variable temperature photoluminescent spectra demonstrate the luminescent intensity remains 85% at 333 K, meeting the requirements of room temperature phosphorescent anti-counterfeiting materials. The luminescent patterns made by standard screen printing display the green and cuticolor logo at 254 nm and 365 nm, respectively, indicating that the bonded phosphors PMEuTb has potential application in phosphorescent anti-counterfeiting.
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Due to the upstream pressure of lithium resources, low-cost sodium-ion batteries (SIBs) have become the most potential candidates for energy storage systems in the new era. However, anode materials of SIBs have always been a major problem in their development. To address this, V2 C/Fe7 S8 @C composites with hierarchical structures prepared via an in situ synthesis method are proposed here. The 2D V2 C-MXene as the growth substrate for Fe7 S8 greatly improves the rate capability of SIBs, and the carbon layer on the surface provides a guarantee for charge-discharge stability. Unexpectedly, the V2 C/Fe7 S8 @C anode achieves satisfactory sodium storage capacity and exceptional rate performance (389.7 mAh g-1 at 5 A g-1 ). The sodium storage mechanism and origin of composites are thoroughly studied via ex situ characterization techniques and first-principles calculations. Furthermore, the constructed sodium-ion capacitor assembled with N-doped porous carbon delivers excellent energy density (135 Wh kg-1 ) and power density (11 kW kg-1 ), showing certain practical value. This work provides an advanced system of sodium storage anode materials and broadens the possibility of MXene-based materials in the energy storage.