Electrochemical Performance of Nitrogen-Doped Carbons: From Fundamental Studies to Practical Pouch Device

Berta Pérez-Román , M. Alejandra Mazo , Laura Pascual , József Sándor Pap , Csaba Balázsi , Sara Ruiz-Martínez-Alcocer , Alejandra García-Gómez , Jesús López-Sánchez , Fernando Rubio-Marcos

Battery Energy ›› 2026, Vol. 5 ›› Issue (1) : e70057

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Battery Energy ›› 2026, Vol. 5 ›› Issue (1) :e70057 DOI: 10.1002/bte2.20250057
RESEARCH ARTICLE
Electrochemical Performance of Nitrogen-Doped Carbons: From Fundamental Studies to Practical Pouch Device
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Abstract

Nitrogen-doped carbide-derived carbons (N-CDCs) are promising materials for energy storage due to their tunable structure and chemistry. Here, we design a molecular architecture strategy to promote nitrogen incorporation and microstructural control during the synthesis of N-CDCs. By varying polymerization and pyrolysis conditions, we obtain materials with hierarchical porosity and high specific surface area (SBET >2000 m2 g−1) and nitrogen content between 1.8 and 6.4 wt.%. Electrochemical evaluation in aqueous 6 M KOH using both three- and two-electrode configurations, identifies nitrogen doping, defect density, and hierarchical porosity as key contributors to performance. The optimized N-CDC delivers a specific capacitance of 210 F g−1 at 1 A g−1, with high retention at elevated current densities. A proof-of-concept pouch cell shows 100 F g−1 at 0.5 A g−1 and stable cycling over 5000 cycles, resulting in superior coulombic efficiency. The practical applicability is demonstrated with two pouch cells connected in series to power an electronic watch (1.5 V). These findings demonstrate the effectiveness of molecular-level control in the design of high-performance carbon-based supercapacitor electrodes.

Keywords

aqueous electrolyte / carbide-derived carbon / electrochemistry / hierarchical porosity / nitrogen doping / pouch cell / supercapacitor

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Berta Pérez-Román, M. Alejandra Mazo, Laura Pascual, József Sándor Pap, Csaba Balázsi, Sara Ruiz-Martínez-Alcocer, Alejandra García-Gómez, Jesús López-Sánchez, Fernando Rubio-Marcos. Electrochemical Performance of Nitrogen-Doped Carbons: From Fundamental Studies to Practical Pouch Device. Battery Energy, 2026, 5(1): e70057 DOI:10.1002/bte2.20250057

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References

[1]

D. R. Lobato-Peralta, P. U. Okoye, and C. Alegre, “A Review on Carbon Materials for Electrochemical Energy Storage Applications: State of the Art, Implementation, and Synergy With Metallic Compounds for Supercapacitor and Battery Electrodes,” Journal of Power Sources617 (2024): 235140.

[2]

O. O. Yolcan, “World Energy Outlook and State of Renewable Energy: 10-Year Evaluation,” Innovation and Green Development2 (2023): 100070.

[3]

Z. Zhai, L. Zhang, T. Du, et al., “A Review of Carbon Materials for Supercapacitors,” Materials & Design221 (2022): 111017.

[4]

S. Mishra, R. Srivastava, and A. Muhammad, et al., “The Impact of Physicochemical Features of Carbon Electrodes on the Capacitive Performance of Supercapacitors: A Machine Learning Approach,” Scientific Reports13 (2023): 6494.

[5]

P. Staiti and F. Lufrano, “A Study of the Electrochemical Behaviour of Electrodes in Operating Solid-State Supercapacitors,” Electrochimica Acta53 (2007): 710-719.

[6]

H. Park, J. Chung, B. Lim, and C. Jung, “Design of Highly Capacitive and Durable Supercapacitors Using Activated Carbons With Different Pore Structures: Petroleum Coke and Oil Palm,” Journal of Industrial and Engineering Chemistry80 (2019): 301-310.

[7]

J. Phiri, J. Dou, T. Vuorinen, P. A. C. Gane, and T. C. Maloney, “Highly Porous Willow Wood-Derived Activated Carbon for High-Performance Supercapacitor Electrodes,” ACS Omega4 (2019): 18108-18117.

[8]

S. P. Gupta, B. A. Kakade, B. R. Sathe, Q. Qiao, D. J. Late, and P. S. Walke, “Thermally Driven High-Rate Intercalated Pseudocapacitance of Flower-Like Architecture of Ultrathin Few Layered δ-MnO2 Nanosheets on Carbon Nano-Onions,” ACS Applied Energy Materials3 (2020): 11398-11409.

[9]

D. Mohapatra, G. Dhakal, M. S. Sayed, B. Subramanya, J. J. Shim, and S. Parida, “Sulfur Doping: Unique Strategy to Improve the Supercapacitive Performance of Carbon Nano-Onions,” ACS Applied Materials & Interfaces11 (2019): 8040-8050.

[10]

L. Vivas and D. P. Singh, “A Highly Efficient Graphene Gold Based Green Supercapacitor Coin Cell Device for Energy Storage,” Frontiers in Energy Research9 (2022): 1.

[11]

T. Cetinkaya and R. A. W. Dryfe, “Electrical Double Layer Supercapacitors Based on Graphene Nanoplatelets Electrodes in Organic and Aqueous Electrolytes: Effect of Binders and Scalable Performance,” Journal of Power Sources408 (2018): 91-104.

[12]

G. Feng, S. Li, J. S. Atchison, V. Presser, and P. T. Cummings, “Molecular Insights Into Carbon Nanotube Supercapacitors: Capacitance Independent of Voltage and Temperature,” Journal of Physical Chemistry C117 (2013): 9178-9186.

[13]

C. Masarapu, H. F. Zeng, K. H. Hung, and B. Wei, “Effect of Temperature on the Capacitance of Carbon Nanotube Supercapacitors,” ACS Nano3 (2009): 2199-2206.

[14]

B. Dyatkin, O. Gogotsi, B. Malinovskiy, Y. Zozulya, P. Simon, and Y. Gogotsi, “High Capacitance of Coarse-Grained Carbide Derived Carbon Electrodes,” Journal of Power Sources306 (2016): 32-41.

[15]

Y. Zhao, W. Wang, D. B. Xiong, et al., “Titanium Carbide Derived Nanoporous Carbon for Supercapacitor Applications,” International Journal of Hydrogen Energy37 (2012): 19395-19400.

[16]

M. A. Mazo, M. T. Colomer, A. Tamayo, and J. Rubio, “Microstructure-Electrochemical Behavior Relationships of Hierarchically Micro-Mesoporous Silicon Oxycarbide Derived Materials Obtained by the Pyrolysis of Trietoxysilane/Dimethyldiphenylsiloxane Hybrids,” Journal of Alloys and Compounds870 (2021): 159427.

[17]

M. Rose, Y. Korenblit, E. Kockrick, et al., “Hierarchical Micro- and Mesoporous Carbide-Derived Carbon as a High-Performance Electrode Material in Supercapacitors,” Small7 (2011): 1108-1117.

[18]

J. Yang, H. Wu, M. Zhu, et al., “Optimized Mesopores Enabling Enhanced Rate Performance in Novel Ultrahigh Surface Area Meso-/Microporous Carbon for Supercapacitors,” Nano Energy33 (2017): 453-461.

[19]

W. Zhu and D. Shen, “Synthesis of Bi2O3/Hierarchical Porous Carbon Composites for Supercapacitor Application,” Journal of Energy Storage79 (2024): 110118.

[20]

N. P. D. Ngidi, A. F. Koekemoer, and S. S. Ndlela, “Application of Metal Oxide/Porous Carbon Nanocomposites in Eelectrochemical Capacitors: A Review,” Physics and Chemistry of the Earth135 (2024): 103698.

[21]

Y. Zhou, J. Ren, L. Xia, et al., “Nitrogen-Doped Hierarchical Porous Carbon Framework Derived From Waste Pig Nails for High-Performance Supercapacitors,” ChemElectroChem4 (2017): 3181-3187.

[22]

F. Su, C. K. Poh, J. S. Chen, et al., “Nitrogen-Containing Microporous Carbon Nanospheres With Improved Capacitive Properties,” Energy & Environmental Science4 (2011): 717-724.

[23]

K. Xia, Y. Cheng, H. Zhang, F. Han, L. Duan, and X. Liu, “Highly Microporous Nitrogen-Doped Carbon Derived From Silicon Oxycarbide Ceramics for Supercapacitor Application,” Journal of Inorganic and Organometallic Polymers and Materials2023, 33: 2023.

[24]

Z. Gao, J. Pan, Y. Wang, et al., “N, S Co-Doped Silicon Oxycarbide-Derived Carbon@NiO/NiCo2O4 With 3D/1D Assembled Model for Asymmetric Supercapacitors With Enhanced Rate Performance,” Colloids and Surfaces A: Physicochemical and Engineering Aspects713 (2025): 136468.

[25]

M. A. Mazo, M. Colomer, A. Tamayo, and J. Rubio, “Hierarchical Porous Fluorine-Doped Silicon Oxycarbide Derived Materials: Physicochemical Characterization and Electrochemical Behaviour,” Microporous and Mesoporous Materials330 (2022): 111604.

[26]

L. Ding, L. Wang, J. Zhang, et al., “Nanozymes Regulated by Nitrogen Element: Mechanism, Design, and Application,” Advanced Powder Materials3 (2024): 100191.

[27]

C. Xiong, C. Zheng, Z. Zhang, et al., “Polyaniline@Cellulose Nanofibers Multifunctional Composite Material for Supercapacitors, Electromagnetic Interference Shielding and Sensing,” Journal of Materials2025, 11: 100841.

[28]

C. Xiong, B. Wang, Y. Yin, et al., “Preparation and Electrochemical Dynamics Simulation of Cellulose-Based Composite Films With Different Hierarchical Structures Applied in Supercapacitors,” Cellulose32 (2025): 1821-1833.

[29]

Q. Xiong, C. Xiong, M. Zhang, et al., “Personal Health Assistant HES-CHAT e-Skins: Integrated Mechanosensitivity, Electromagnetic Shielding, and Electrochemical Energy Storage,” Journal of Materials Chemistry A13 (2025): 12084-12096.

[30]

S. L. Candelaria, B. B. Garcia, D. Liu, and G. Cao, “Nitrogen Modification of Highly Porous Carbon for Improved Supercapacitor Performance,” Journal of Materials Chemistry2012, 22: 9884.

[31]

C. Li, Z. Song, M. Liu, et al., “Template-Induced Graphitic Nanodomains in Nitrogen- Doped Carbons Enable High-Performance Sodium-Ion Capacitors,” Energy & Environmental Materials2024, 7: 1.

[32]

J. Merida, M. T. Colomer, F. Rubio, and M. A. Mazo, “Highly Porous Carbon Materials Derived From Silicon Oxycarbides and Effect of the Pyrolysis Temperature on Their Electrochemical Response,” International Journal of Molecular Sciences24 (2023): 13868.

[33]

S. Zhang, S. Tsuzuki, K. Ueno, K. Dokko, and M. Watanabe, “Upper Limit of Nitrogen Content in Carbon Materials,” Angewandte Chemie International Edition54 (2015): 1302-1306.

[34]

G. N. Yushin, E. N. Hoffman, A. Nikitin, H. Ye, M. W. Barsoum, and Y. Gogotsi, “Synthesis of Nanoporous Carbide-Derived Carbon by Chlorination of Titanium Silicon Carbide,” Carbon43 (2005): 2075-2082.

[35]

Z. Lei, M. Zhao, L. Dang, et al., “Structural Evolution and Electrocatalytic Application of Nitrogen-Doped Carbon Shells Synthesized by Pyrolysis of Near-Monodisperse Polyaniline Nanospheres,” Journal of Materials Chemistry19 (2009): 5985.

[36]

Z. Lei, D. Bai, and X. S. Zhao, “Improving the Electrocapacitive Properties of Mesoporous CMK-5 Carbon With Carbon Nanotubes and Nitrogen Doping,” Microporous and Mesoporous Materials147 (2012): 86-93.

[37]

Y. Jiang, S. Chowdhury, and R. Balasubramanian, “New Insights Into the Role of Nitrogen-Bonding Configurations in Enhancing the Photocatalytic Activity of Nitrogen-Doped Graphene Aerogels,” Journal of Colloid and Interface Science534 (2019): 574-585.

[38]

J. Li, W. Y. Zan, H. Kang, et al., “Graphitic-N Highly Doped Graphene-Like Carbon: A Superior Metal-Free Catalyst for Efficient Reduction of Co2,” Applied Catalysis B: Environmental298 (2021): 120510.

[39]

K. Ramachandran, G. Subburam, X. H. Liu, et al., “Nitrogen-Doped Porous Carbon Nanofoams With Enhanced Electrochemical Kinetics for Superior Sodium-Ion Capacitor,” Rare Metals41 (2022): 2481-2490.

[40]

J. R. Pels, F. Kapteijn, J. A. Moulijn, Q. Zhu, and K. M. Thomas, “Evolution of Nitrogen Functionalities in Carbonaceous Materials During Pyrolysis,” Carbon33 (1995): 1641-1653.

[41]

C. Zhang, W. Shen, K. Guo, M. Xiong, J. Zhang, and X. Lu, “A Pentagonal Defect-Rich Metal-Free Carbon Electrocatalyst for Boosting Acidic O2 Reduction to H2O2 production,” Journal of the American Chemical Society145 (2023): 11589-11598.

[42]

M. Thommes, K. Kaneko, A. V. Neimark, et al., “Physisorption of Gases, With Special Reference to the Evaluation of Surface Area and Pore Size Distribution (IUPAC Technical Report),” Pure and Applied Chemistry87 (2015): 1051-1069.

[43]

Y. Gogotsi, A. Nikitin, H. Ye, et al., “Nanoporous Carbide-Derived Carbon With Tunable Pore Size,” Nature Materials2 (2003): 591-594.

[44]

L. Zhu, Y. Li, J. Zhang, et al., “Regulating the Interconnected Microporous Structure of Porous Carbon by Alkali Metal Ions for Improved Surface and Space Utilization for Organic Supercapacitors,” Applied Surface Science638 (2023): 158051.

[45]

C. Vakifahmetoglu, V. Presser, S. H. Yeon, P. Colombo, and Y. Gogotsi, “Enhanced Hydrogen and Methane Gas Storage of Silicon Oxycarbide Derived Carbon,” Microporous and Mesoporous Materials144 (2011): 105-112.

[46]

S. H. Yeon, P. Reddington, Y. Gogotsi, J. E. Fischer, C. Vakifahmetoglu, and P. Colombo, “Carbide-Derived-Carbons With Hierarchical Porosity From a Preceramic Polymer,” Carbon48 (2010): 201-210.

[47]

G. Yushin, A. Nikitin, and Y. Gogotsi, 8 Carbide-Derived Carbon, 2006.

[48]

B. Pérez-Román, A. Merchán del Real, J. Rubio, M. A. Mazo, and F. Rubio-Marcos, “Innovative Strategies for Nitrogen-Incorporating Silicon Oxycarbide-Based Preceramic Polymer Synthesis,” Materials Advances2024, 5: 2040.

[49]

M. Ayiania, E. Weiss-Hortala, M. Smith, J. S. McEwen, and M. Garcia-Perez, “Microstructural Analysis of Nitrogen-Doped Char by Raman Spectroscopy: Raman Shift Analysis From First Principles,” Carbon. 2020, 167: 559.

[50]

C. Hu, S. Sedghi, A. Silvestre-Albero, et al., “Raman Spectroscopy Study of the Transformation of the Carbonaceous Skeleton of a Polymer-Based Nanoporous Carbon Along the Thermal Annealing Pathway,” Carbon85 (2015): 147-158.

[51]

A. Sadezky, H. Muckenhuber, H. Grothe, R. Niessner, and U. Pöschl, “Raman Microspectroscopy of Soot and Related Carbonaceous Materials: Spectral Analysis and Structural Information,” Carbon43 (2005): 1731-1742.

[52]

Á. Peña, J. López-Sánchez, L. Sacco, et al., “Beyond Conventional Characterization: Defect Engineering Role for Sensitivity and Selectivity of Room-Temperature UV-Assisted Graphene-Based NO2 Sensors,” Talanta286 (2025): 127507.

[53]

A. Y. Lee, K. Yang, N. D. Anh, et al., “Raman Study of D* Band in Graphene Oxide and Its Correlation With Reduction,” Applied Surface Science536 (2021): 147990.

[54]

M. Seredych, D. Hulicova-Jurcakova, G. Q. Lu, and T. J. Bandosz, “Surface Functional Groups of Carbons and the Effects of Their Chemical Character, Density and Accessibility to Ions on Electrochemical Performance,” Carbon46 (2008): 1475-1488.

[55]

B. Xu, S. Hou, G. Cao, F. Wu, and Y. Yang, “Sustainable Nitrogen-Doped Porous Carbon With High Surface Areas Prepared From Gelatin for Supercapacitors,” Journal of Materials Chemistry22 (2012): 19088.

[56]

D. Wang, Z. Xu, Y. Lian, C. Ban, and H. Zhang, “Nitrogen Self-Doped Porous Carbon With Layered Structure Derived From Porcine Bladders for High-Performance Supercapacitors,” Journal of Colloid and Interface Science542 (2019): 400-409.

[57]

D. Hulicova-Jurcakova, M. Seredych, G. Q. Lu, and T. J. Bandosz, “Combined Effect of Nitrogen- and Oxygen-Containing Functional Groups of Microporous Activated Carbon on Its Electrochemical Performance in Supercapacitors,” Advanced Functional Materials2009, 19: 438.

[58]

Y. D. Ma, J. F. Gao, X. W. Chen, and L. B. Kong, “Regulation of the Mesopore Proportion of Porous Carbon for Optimizing the Performance of Electric Double Layer Capacitors,” Journal of Energy Storage2021, 35: 102299.

[59]

D. W. Wang, F. Li, M. Liu, G. Q. Lu, and H. M. Cheng, “3D Aperiodic Hierarchical Porous Graphitic Carbon Material for High-Rate Electrochemical Capacitive Energy Storage,” Angewandte Chemie International Edition47 (2008): 373-376.

[60]

V. Augustyn, P. Simon, and B. Dunn, “Pseudocapacitive Oxide Materials for High-Rate Electrochemical Energy Storage,” Energy & Environmental Science7 (2014): 1597.

[61]

U. B. Nasini, V. G. Bairi, S. K. Ramasahayam, S. E. Bourdo, T. Viswanathan, and A. U. Shaikh, “Phosphorous and Nitrogen Dual Heteroatom Doped Mesoporous Carbon Synthesized via Microwave Method for Supercapacitor Application,” Journal of Power Sources250 (2014): 257-265.

[62]

D. Xie, S. Liu, W. Wei, et al., “Nitrogen-Doped Porous Carbon Fiber as a Self-Supporting Electrode for Boosting Zinc-Ion Hybrid Supercapacitors,” Industrial & Engineering Chemistry Research63 (2024): 21146-21153.

[63]

B. Perez-Roman, R. Layek, M. Rodriguez, F. Rubio, J. Rubio, and A. Tamayo, “Insights Into the Structural and Surface Characteristics of Microporous Carbide Derived Carbons Obtained Through Single and Double Halogen Etching,” Microporous and Mesoporous Materials310 (2021): 110675.

[64]

N. Venkatesan, T. Kesavan, M. Raja, K. Ramanujam, and N. N. Fathima, “Efficient Electrochemical Performance of Nitrogen-Doped Porous Activated Carbon for High Energy Symmetric Pouch Cell Supercapacitors,” Journal of Energy Storage55 (2022): 105698.

[65]

C. Poochai, C. Sriprachuabwong, N. Srisamrarn, et al., Applied Organometallic Chemistry2019, 489, 989.

[66]

B. K. Chakrabarti and C. T. J. Low, “Scaling to Practical Pouch Cell Supercapacitor: Electrodes by Electrophoretic Deposition,” Next Energy4 (2024): 100137.

[67]

B. K. Chakrabarti, K. B. Dönmez, Z. Çobandede, and C. T. J. Low, “Practical Pouch Cell Supercapacitor Electrodes by Electrophoretic Deposition of Activated Carbon on Nickel Foam,” ChemElectroChem11 (2024): 1.

[68]

Y. Anil Kumar, S. Vignesh, T. Ramachandran, et al., “Advancements in Novel Electrolyte Materials: Pioneering the Future of Supercapacitive Energy Storage,” Journal of Industrial and Engineering Chemistry145 (2025): 191-215.

[69]

W. Meng, H. Li, Z. Luo, et al., “High-Voltage Aqueous Supercapacitors Enabled by Polysiloxane Passivation Coating-Modified Carbon Cloth Electrode,” Carbon230 (2024): 119679.

[70]

S. Brunauer, P. H. Emmett, and E. Teller, “Adsorption of Gases in Multimolecular Layers,” Journal of the American Chemical Society60 (1938): 309-319.

[71]

E. P. Barrett, L. G. Joyner, and P. P. Halenda, “The Determination of Pore Volume and Area Distributions in Porous Substances. I. Computations From Nitrogen Isotherms,” Journal of the American Chemical Society73 (1951): 373-380.

[72]

J. López-Sánchez, Á. Peña, A. Serrano, et al., “Generation of Defective Few-Layered Graphene Mesostructures by High-Energy Ball Milling and Their Combination With FeSiCuNbB Microwires for Reinforcing Microwave Absorbing Properties,” ACS Applied Materials & Interfaces15 (2023): 3507-3521.

[73]

M. D. Stoller and R. S. Ruoff, “Best Practice Methods for Determining an Electrode Material's Performance for Ultracapacitors,” Energy & Environmental Science3 (2010): 1294.

[74]

A. Laheäär, P. Przygocki, Q. Abbas, and F. Béguin, “Appropriate Methods for Evaluating the Efficiency and Capacitive Behavior of Different Types of Supercapacitors,” Electrochemistry Communications60 (2015): 21-25.

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