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All issues Volume 5 / No 2 (2026) Natl Sci Open, 5 2 (2026) 20260005 Full HTML
Open Access
Issue
Natl Sci Open
Volume 5, Number 2, 2026
Article Number 20260005
Number of page(s) 12
Section Materials Science
DOI https://doi.org/10.1360/nso/20260005
Published online 01 February 2026

© The Author(s) 2026. Published by Science Press and EDP Sciences.

Licence Creative CommonsThis is an Open Access article distributed under the terms of the Creative Commons Attribution License (https://creativecommons.org/licenses/by/4.0), which permits unrestricted use, distribution, and reproduction in any medium, provided the original work is properly cited.

INTRODUCTION

In recent years, with the sustained growth of global energy demand and growing environmental issues, functional mesoporous materials with high-performance in energy storage and conversion have become a hot topic in the interdisciplinary fields [1–14]. This is because the mesoporous carbon materials not only possess mesoporous structural characteristics (rich pore channels) but also have the inherent advantages, such as good electrical conductivity [15–19]. Especially, the one-dimensional (1D) hierarchical porous carbon-based materials with their unique structural advantages have shown significant application potential in supercapacitors, catalysts, aerospace, automobiles, sports equipment, etc. [20–28]. Such hierarchical 1D mesoporous carbon nanoparticles with multi-level pore channels are potentially able to overcome the performance bottlenecks of traditional carbon materials and possess good capabilities in the regulation of properties [29–31].

In the past decade, some typical methods, involving emulsion-directed or hard templates, have been developed to synthesize the desirable one-dimensional hierarchical porous carbon-based materials, and some porous architectures have achieved [32–35]. For the emulsion-guided method, the obtained carbon materials lack pores and have an uneven pore structure. And for the conventional hard method, the pore structure is monotonous, and it is difficult to precisely control the pore channel structure (pore configuration) and construct multi-level pores. To date, for the synthesis of one-dimensional hierarchical porous carbon-based materials, traditional template methods have been continuously optimized while various new preparation approaches have emerged. Regarding performance modification, heteroatom doping and metal-based composite strategies have become the core modification approaches [36–39]; in terms of the application, they also performed good specific capacitance and rate performance in supercapacitors [40–42], demonstrating the application potential. However, traditional one-dimensional carbon materials are limited by their microporous structure and often suffer from high mass transfer resistance and uneven distribution of active sites, which restricts the improvement of their performance.

To address these issues, in this work, we propose a single-micelle-based dual-templates assembly strategy, combining the advantages of soft template (polystyrene-block-poly (4-vinylpyridine)-block-poly (ethylene oxide) (PS-PVP-PEO) micelles) and hard template (one-dimensional SiO2), to achieve the controllable preparation of one-dimensional hierarchical porous nitrogen-doped carbon materials. 1D N-mC is a hollow rod-shaped material with a length of ~350 nm. Its surface is decorated with spherical nanoparticles, exhibiting high roughness, and the inner surface contains micropores with a pore size of 1.0–2.5 nm. It features a three-level hierarchical interconnected structure of micropores, mesopores and macropores, with a specific surface area of 496 m2 g−1 and a pore volume of 0.62 cm3 g−1. The mesopore diameter is adjustable within 10–35 nm. Composed of C, O and N, it is rich in hydroxyl and other functional groups, exhibiting strong hydrophilicity. At a current density of 1 A g−1, its specific capacitance reaches 320 F g−1, retaining 270 F g−1 at 10 A g−1, with only 11% capacity decay after 5000 cycles.

RESULTS

Synthesis and characterization

One-dimensional hierarchical porous pore nitrogen-doped carbon materials were synthesized by the single-micelle-based dual-templates assembly strategy. The single micelle synthesized from PEO-PVP-PS was used as the template agent, and hydrochloric dopamine was used as the carbon source. Tetraethyl orthosilicate (TEOS) and cetyltrimethylammonium bromide (CTAB) were introduced (Figure 1a). First, one-dimensional SiO2 rods were prepared using CTAB as the structure-directing agent and TEOS as the silicon source. Then, the PS-PVP-PEO unimicellar ethanol solution was added dropwise to the SiO2 rod dispersion, and the micelles were assembled on the SiO2 surface at room temperature with stirring. Subsequently, the pH was adjusted, and dopamine hydrochloride was added. Afterwards, the mixture was stirred to enable dopamine nucleation and polymerization on the composite template. Next, the programmed calcination was performed in a nitrogen atmosphere to remove the micelles and carbonize the dopamine. Finally, SiO2 was etched with hydrofluoric acid to obtain the target one-dimensional hierarchical porous nitrogen-doped carbon nanorods (1D N-mC).

Thumbnail: Figure 1 Refer to the following caption and surrounding text. Figure 1

(a) Schematic illustration of the synthesis of one-dimensional hierarchical porous nitrogen-doped carbon materials; (b) SEM, (c, d) TEM, and (e) HAADF-STEM images, and (f–h) energy dispersive X-ray spectroscopy (EDX) elemental mapping images of the 1D N-mC material.

Scanning electron microscopy (SEM) images show that it has a uniform rod-like structure with a length of approximately 350 nm, and a large number of spherical nanoparticles are distributed on the surface, with a relatively high surface roughness (Figure 1b); transmission electron microscopy (TEM) images further reveal that the material has a hollow nanorod structure, with a single-layer spherical mesopore on the surface without impurities, demonstrating excellent structural uniformity (Figure 1c). High-resolution TEM (HRTEM) shows that the diameter of the spherical mesopores is approximately 10 nm, with a wall thickness of 30 nm, and the mesopores are uniformly distributed over a wide range (Figure 1d); the medium-high angle annular dark-field (HAADF-STEM) images confirm that there are ultra-small pores of 1.0–2.5 nm on the inner surface of the material (Figure 1e), indicating that the ultra-small pores, large pores, and surface spherical mesopores are interconnected, forming a three-level system of “micro-pore-mesopore-large-pore” pore channels. The element mapping images show that the C, O, and N elements are uniformly distributed (Figure 1f, g, h), verifying the successful construction of a uniform nitrogen-doped carbon structure.

The nitrogen adsorption-desorption test indicates that the isotherm of 1D N-mC is a typical IV-type curve (Figure 2a). The adsorption amount sharply increases in the low-pressure region (P/P0 < 0.1), confirming the existence of micropores; the narrow-range hysteresis loop in the medium-pressure region (P/P0 ≈ 0.4–0.8) indicates uniform mesopore diameters, and the mesopore diameters calculated by the Barrett-Joyner-Halenda (BJH) model are concentrated at 12.3 nm (Figure 2b); the sudden increase in adsorption amount at the high-pressure region (P/P0 > 0.9) suggests the presence of macropores. The BET specific surface area of the porous material is high to 494 m2 g−1, and the total pore volume is 0.62 cm3 g−1, providing sufficient space for ion transport and exposure of active sites. The X-ray diffraction (XRD) spectrum shows a broadened (002) crystal plane diffraction peak at 25° (d ≈ 0.34 nm), indicating that the carbon material has many defects (Figure 2c); the Fourier transform infrared spectroscopy (FTIR) analysis shows that the broad peak at 3400 cm−1 corresponds to the N–H stretching vibration, the 1600 cm−1 peak belongs to the C=C skeleton vibration of the aromatic ring, and the multiple peaks in the 1000–1300 cm−1 range originate from the C–O–C/C–OH bond vibrations, confirming that the material surface is rich in hydroxyl, epoxy, and other oxygen-containing functional groups, and has strong hydrophilicity (Figure 2d).

Thumbnail: Figure 2 Refer to the following caption and surrounding text. Figure 2

Characterization of mesoporous carbon materials. (a) N2 adsorption-desorption isotherm; (b) pore size distribution plot; (c) XRD pattern; (d) FTIR spectrum; (e–h) XPS spectra; (i) Raman spectrum.

The X-ray photoelectron spectroscopy (XPS) full-spectrum scan confirms that 1D N-mC contains only three elements: C, O, and N, with high purity and no impurities (Figure 2e). Oxygen atom doping can alter the electron cloud distribution of carbon materials, enhance the electrical conductivity of the materials, and introduce active sites that are conducive to charge transfer (Figure 2f). The high-resolution C1s spectrum identifies characteristic peaks at 284.4 eV (C=C, sp2 carbon framework), 284.9 eV (C–N, nitrogen-doped carbon structure), and 290.7 eV (O–C=O, carboxylic acid group), indicating the presence of graphite-like carbon network, nitrogen-doped sites, and oxygen-containing functional groups in the material (Figure 2g); the N1s spectrum (Figure 2h) further distinguishes the forms of nitrogen, with coexistence of 398.1 eV (pyridine nitrogen), 400.2 eV (pyrrole nitrogen), 401.3 eV (graphite nitrogen), and 403.2 eV (oxidized nitrogen), providing abundant active sites and a controllable electronic structure for the material. The intensity ratio of the D band (1379 cm−1, disordered carbon/defect vibration) to the G band (1555 cm−1, sp2 carbon face internal stretching vibration) in the Raman spectrum is ID/IG = 1.06 (Figure 2i), confirming the presence of high-density defects and nanocrystalline boundaries in the carbon framework of the material, which is consistent with the XRD results.

The formation mechanism of 1D N-mC consists of three steps (Figure 3). The first step involves using micelles to form rod-shaped silica. CTAB acts as the cationic surfactant and self-assembles in a water solution to form rod-shaped micelles. TEOS hydrolyzes in an alkaline environment to generate silicic acid, which subsequently condenses to form SiO2 rods. After removing the CTAB micelles, mesoporous silica nanorods are obtained. The concentration of CTAB can control the morphology of SiO2. High concentration leads to an increase in diameter, while low concentration may result in the formation of spherical particles. The second step is the assembly of the single micelle on SiO2 interfaces. The single micelle of PS-PVP-PEO self-assembles into a core-shell-corona structure in ethanol (PS is the core, PVP is the shell, and PEO is the corona). The PVP segments of the PS-PVP-PEO micelles are positively charged and attract the negatively charged SiO2 surface through electrostatic attraction. The spatial steric hindrance effect of the PEO segments of micelles inhibits micelle aggregation, ensuring high monodispersity. The third step is dopamine coating and carbonization. The dopamine precursor polymerizes on the surface of the single micelle and SiO2 through electrostatic attraction due to spatial limitations. When the micelle and silica come into contact, dopamine cannot polymerize, forming pores. After carbonization and removal of the template, mesoporous structures were formed on the carbon shell, resulting in the one-dimensional mesoporous carbon nanorods.

Thumbnail: Figure 3 Refer to the following caption and surrounding text. Figure 3

Formation mechanism of one-dimensional hierarchically porous carbon nanomaterials.

Supercapacitor performance

To evaluate the influence of the aforementioned multi-level pore structure and nitrogen doping characteristics on the energy storage performance, a systematic electrochemical performance test of 1D N-mC was conducted for supercapacitors. Nano-carbon rods (N-CNR) and hollow nano-carbon rods (1D N-C) were employed as reference samples. Through a three-electrode system, cyclic voltammetry (CV) tests reveal that all samples exhibit typical double-layer capacitance characteristics, with CV curves approaching ideal rectangles (Figure 4a). Among them, the integral area of the CV curve of 1D N-mC is significantly larger than that of the reference samples, indicating the highest specific capacitance. When the scan rate is increased from 10 to 200 mV s−1, the CV curve of 1D N-mC is only slightly inclined without significant deformation (Figure 4b), demonstrating excellent rate performance [43,44]. In galvanostatic charge-discharge (GCD) tests, at a high current density of 10 A g−1, the charge-discharge curve of 1D N-mC remains symmetrical and isosceles triangles (Figure 4c), without significant voltage drop, further confirming its excellent charge storage capacity.

Thumbnail: Figure 4 Refer to the following caption and surrounding text. Figure 4

Electrochemical performance of 1D N-mC in a three-electrode system. (a) Comparative CV curves of three materials at 10 mV s−1; (b) CV curves of 1D N-mC; (c) comparative GCD profiles of three materials at 2 A g−1; (d) GCD profiles of 1D N-mC; (e) amplified fit of impedance and equivalent circuit diagram; (f) specific capacitance comparison of three materials; (g) logarithmic current vs. logarithmic scan rate obtained in the cathodic direction; (h) typical charge storage contributions from capacitive and diffusion processes in 1D N-mC at 10 mV s−1 from cyclic voltammetry; (i) comparative histogram of percentage contributions from capacitive and diffusion-controlled charge storage in 1D N-mC at scan rates from 10 to 200 mV s−1.

The electrochemical impedance spectroscopy (EIS) analysis reveals that the EIS Nyquist curve exhibits a small-diameter semicircle in the high-frequency region, corresponding to the small value of the low charge transfer resistance (Rct), indicating that 1D N-mC has excellent conductivity for rapid electron transfer throughout the electrode. The curve in the low-frequency region presents a steep and nearly vertical straight line, suggesting that the hierarchical pore structure of 1D N-mC can provide short and unobstructed diffusion channels for electrolyte ions. Additionally, the internal series resistance (Rs) within the 1D N-mC electrode is relatively low, which could also be demonstrated by the intercept at the real axis (Z′) of the middle EIS Nyquist curve (Figure 4e).

The specific capacitance (Figure 4f) was calculated based on the GCD curve. For 1D N-mC at current densities of 1, 2, 3, 4, and 5 A/g, the specific capacitance is 320, 310, 292.5, 280, and 272.5 F g−1 respectively, which is apparently higher than that of N-CNR and 1D N-C under the same conditions. Even at a high current density of 10 A/g, 1D N-mC still maintains a specific capacitance of 270 F g−1, with a capacity retention rate of 84.4%, while the capacity retention rates of 1D N-C and N-CNR are only 76.8% and 71.3%, respectively.

To further explore the charge storage mechanism, the reaction kinetics was analyzed through CV curves: According to the formula i = avb, the b value of 1D N-mC is 0.76–0.83 (Figure 4g), indicating that charge storage is mainly controlled by the capacitance process; further quantitative analysis through i = k1v + k2v1/2 shows that at a scan rate of 10 mV s−1, the contribution of diffusion control accounts for 76% of the total capacitance (Figure 4h), and with the scan rate increasing to 200 mV s−1, the contribution of surface capacitance increases to 59% (Figure 4i), confirming that the hierarchical pore structure can achieve efficient charge storage at different rates.

To further investigate the capacitive behavior of 1D N-mC, electrochemical tests were performed in a two-electrode configuration with 1 M Na2SO4 electrolyte, over a potential window of 0–1.3 V. When the voltage window increases from 0.5 to 1.2 V, the current density response shows a stepwise enhancement, but all CV curves display a rectangular shape with no significant changes. However, a slight peak is observed at 1.2–1.3 V, indicating that an oxygen reduction reaction occurred on the electrode. Therefore, the optimal voltage window for the symmetrical capacitor is determined to be 1.2 V (Figure 5a). Even at a high scan rate of 100 mV s−1, the CV curve still maintains a rectangular morphology (Figure 5b); the GCD test shows (Figure 5c) that the specific capacitance at 1 A g−1 was 205.8 F g−1, and it remains at 125 F g−1 at 10 A g−1, with a capacity retention rate of 60%. In the cycle stability test (Figure 5d), after cycling 5000 times at a current density of 10 A g−1, the initial capacitance is maintained at 89%, and the Coulomb efficiency was close to 100%.

Thumbnail: Figure 5 Refer to the following caption and surrounding text. Figure 5

Electrochemical performance of 1D N-mC in symmetric supercapacitors. (a) CV curves at different voltage windows; (b) CV curves at various scan rates; (c) GCD profiles at different current densities; (d) cycling stability at 10 A g−1; (e) Ragone plot comparing this material with previously reported carbon-based supercapacitors in 1 M NaSO4 electrolyte.

In the Ragone plot, the relationship between the energy density and power density of 1D N-mC symmetric capacitors is estimated [45–54]. It shows an energy density ranging from 41.2 to 25 Wh kg−1, and the weight power density increases from 600.5 to 6000 W kg−1, which is superior to most porous carbon-based symmetric supercapacitors previously reported (Figure 5e).

DISCUSSION

This study prepared one-dimensional hierarchical porous nitrogen-doped carbon materials (1D N-mC) through a single-micelle-based dual-templates assembly strategy. The correlation between the material structure and its properties was systematically explored, which was further addressed from the following two aspects.

(1) In terms of synthesis strategy, traditional hard/soft template methods for mesoporous carbon suffer from poor structural controllability and complex processes. This study innovatively combines the advantages of PS-PVP-PEO single micelle (soft template) and 1D SiO2 (hard template) via single-micelle-based dual-templates assembly strategy, precisely controlling mesopore size (10–40 nm) and balancing pore uniformity with structural stability. Uniform monolayered spherical mesopores are enabled by single micelles, and the 1D SiO2 hard template guides the fabrication of rod-like structures. Moreover, the subsequent etching process creates hollow channels to enhance mass transfer performance. Dopamine serves as a carbon/nitrogen source, realizing that the carbon skeleton construction and the nitrogen doping simultaneously provide abundant active sites. Controllable adjustment of mesopore size and SiO2 morphology is realized through the regulation of block copolymer molecular weight and CTAB concentration, furnishing a facile approach to the design of 1D hierarchical porous carbon.

For supercapacitor performance, 1D N-mC’s “micropore-mesopore-macropore” hierarchical structure exerts remarkable synergistic effects. For instance, micropores (494 m2 g−1 high specific surface area) provide abundant active sites; 12.3 nm mesopores can shorten the ion diffusion paths and reduce the mass transfer resistance; macropores and hollow structures facilitate electrolyte penetration and alleviate charge-discharge volume expansion. Additionally, nitrogen doping optimizes the performance: graphitic N enhances conductivity, pyridinic/pyrrolic N adds pseudocapacitance, and oxygen-containing groups boost hydrophilicity. Electrochemical tests show 84.4% capacity retention rate at 10 A g−1 and only 11% decay after 5000 cycles, outperforming N-CNR and 1D N-C.

CONCLUSIONS

This study focuses on the controllable preparation of one-dimensional hierarchical porous carbon materials for supercapacitors. A single-micelle-based dual-templates assembly strategy was proposed to address the structural defects and performance bottlenecks of traditional materials, successfully synthesizing one-dimensional hierarchical porous nitrogen-doped carbon materials (1D N-mC). The material has a high specific surface area of 494 m2 g−1. It possesses uniform mesopores (12.3 nm) and a three-level pore structure (micropore-mesopore-macropore). The mesopore size is tunable (10–35 nm) by adjusting the copolymer molecular weight. Nitrogen is uniformly distributed in the material in the forms of pyridinic nitrogen and graphitic nitrogen. As a supercapacitor electrode, 1D N-mC exhibits excellent performance: 320 F g−1 specific capacitance at 1 A g−1, 84.4% capacity retention at 10 A g−1, and only 11% decay after 5000 cycles. The symmetric supercapacitor based on this new porous architecture achieves high energy density (25–41.2 Wh kg−1) and power density (600.5–6000 W kg−1), outperforming most traditional carbon-based counterparts, which benefits from the synergistic effect of hierarchical pore-enhanced mass transfer and nitrogen doping-regulated electronics. This strategy provides a new approach for the structural design and performance optimization of carbon-based materials for energy storage.

Data availability

The original data are available from corresponding authors upon reasonable request.

Funding

This work was supported by the National Key Research and Development Program of China (2024YFE0101100) under its Singapore-China Joint Flagship Project (Clean Energy), the National Natural Science Foundation of China (22305132, 22475112 and 22365021), the Inner Mongolia Natural Science Foundation (2025LHMS02016), and the Open Research Fund of CNMGE Platform & NSCC-TJ (CNMGE2025001).

Author contributions

R.G. and B.L. conceived and designed the experiments and wrote the manuscript. X.F., D.L. and S.L. analyzed the data. X.C. and G.J. provided the electrochemical-test protocols and reviewed the manuscript. Y.D., P.Z., J.L., S.J.L. and S.S.L. participated in the experiments and in writing the manuscript. Y.Z. initiated and designed the project. Z.Z., Y.Z. and D.L. provided funding and reviewed the manuscript.

Conflict of interest

The authors declare no conflict of interest.

Supplementary information

Supplementary file provided by the authors. Access Supplementary Material

The supporting information is available online at https://doi.org/10.1360/nso/20260005. The supporting materials are published as submitted, without typesetting or editing. The responsibility for scientific accuracy and content remains entirely with the authors.

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All Figures

Thumbnail: Figure 1 Refer to the following caption and surrounding text. Figure 1

(a) Schematic illustration of the synthesis of one-dimensional hierarchical porous nitrogen-doped carbon materials; (b) SEM, (c, d) TEM, and (e) HAADF-STEM images, and (f–h) energy dispersive X-ray spectroscopy (EDX) elemental mapping images of the 1D N-mC material.
In the text
Thumbnail: Figure 2 Refer to the following caption and surrounding text. Figure 2

Characterization of mesoporous carbon materials. (a) N2 adsorption-desorption isotherm; (b) pore size distribution plot; (c) XRD pattern; (d) FTIR spectrum; (e–h) XPS spectra; (i) Raman spectrum.
In the text
Thumbnail: Figure 3 Refer to the following caption and surrounding text. Figure 3

Formation mechanism of one-dimensional hierarchically porous carbon nanomaterials.
In the text
Thumbnail: Figure 4 Refer to the following caption and surrounding text. Figure 4

Electrochemical performance of 1D N-mC in a three-electrode system. (a) Comparative CV curves of three materials at 10 mV s−1; (b) CV curves of 1D N-mC; (c) comparative GCD profiles of three materials at 2 A g−1; (d) GCD profiles of 1D N-mC; (e) amplified fit of impedance and equivalent circuit diagram; (f) specific capacitance comparison of three materials; (g) logarithmic current vs. logarithmic scan rate obtained in the cathodic direction; (h) typical charge storage contributions from capacitive and diffusion processes in 1D N-mC at 10 mV s−1 from cyclic voltammetry; (i) comparative histogram of percentage contributions from capacitive and diffusion-controlled charge storage in 1D N-mC at scan rates from 10 to 200 mV s−1.
In the text
Thumbnail: Figure 5 Refer to the following caption and surrounding text. Figure 5

Electrochemical performance of 1D N-mC in symmetric supercapacitors. (a) CV curves at different voltage windows; (b) CV curves at various scan rates; (c) GCD profiles at different current densities; (d) cycling stability at 10 A g−1; (e) Ragone plot comparing this material with previously reported carbon-based supercapacitors in 1 M NaSO4 electrolyte.
In the text

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