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Peer-reviewedCC BY 4.0ACS Omega

Sequential Electrochemical Construction of Hierarchical LIG/PPy/MnO2 Microsupercapacitors with High Areal Capacitance and Device-Level Stability

  • Tianqi Lu1
  • Yinting Li1
  • Haoran Mo1
  • Jiadi Mao1
  • Saddam Weheabby1
  • Aseel Alnaimi1
  • Ze Chen1
  • Ammar Al-Hamry1
  • Marcio Vidotti2
  • Ahmed S. G. Khalil3,4,5
  • Olfa Kanoun1
5 affiliations
  1. 1Chemnitz University of Technology , , ,
  2. 2Universidade Federal do Paraná (UFPR) , , CxP 19032, , ,
  3. 3Fayoum University , , ,
  4. 4EvoSmarTec GmbH , Alfredstr. 81 , ,
  5. 5Egypt-Japan University of Science and Technology , , ,
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Abstract

Achieving high areal energy storage in flexible microsupercapacitors while maintaining compatibility with direct planar patterning remains challenging, particularly when multiple pseudocapacitive components must be sequentially integrated without compromising electrode accessibility or device level performance. In this paper, we develop a sequential electrochemical construction strategy to integrate polypyrrole (PPy) and manganese dioxide (MnO2) directly onto interdigitated laser-induced graphene (LIG) electrodes without preformed composite powders, slurry casting, or polymer binders. Porous LIG serves as the conductive framework and current collector, followed by in situ PPy electropolymerization and subsequent MnO2 electrodeposition. Systematic control of LIG processing, PPy growth, MnO2 deposition, and gel electrolyte composition establishes a fabrication window that balances electrical conductivity, pseudocapacitive material loading, and structural accessibility while preserving the underlying porous LIG architecture. Stepwise LIG, LIG/PPy, and LIG/PPy/MnO2 controls exhibit the same performance hierarchy at both the individual electrode and complete device levels, demonstrating that the electrochemical gains introduced during sequential functionalization are retained after complete microsupercapacitor (MSC) assembly. The resulting LIG/PPy/MnO2 device delivers an areal capacitance of 621.2 mF cm–2 at 0.37 mA cm–2 and a maximum areal energy density of 55.22 μWh cm–2 at 0.1494 mW cm–2. Extended rate measurements further demonstrate continued electrochemical operation up to 5 mA cm–2 under substantially increased current demand. The device retains 97.04% of its flat state capacitance at 180° static bending, exhibits a device-to-device RSD of 2.29%, retains 94.5% capacitance after 60 days of ambient storage, and maintains 85.1% after 5000 GCD cycles. Series integration further extends the operating voltage from 0.8 to 2.4 V with predictable electrical scaling and enables three MSCs to power a red LED for approximately 183 s. These results establish a directly patterned and independently controlled approach for translating hierarchical pseudocapacitive construction into high areal energy storage, reproducible device performance, and scalable voltage output.

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Cite

BibTeXRIS
BibTeX
@article{lu2026sequential,
  title = {{Sequential Electrochemical Construction of Hierarchical LIG/PPy/MnO2 Microsupercapacitors with High Areal Capacitance and Device-Level Stability}},
  author = {Tianqi Lu and Yinting Li and Haoran Mo and Jiadi Mao and Saddam Weheabby and Aseel Alnaimi and Ze Chen and Ammar Al-Hamry and Marcio Vidotti and Ahmed S. G. Khalil and Olfa Kanoun},
  journal = {ACS Omega},
  year = {2026},
  month = nov,
  doi = {10.1021/acsomega.6c10408},
  url = {https://pubs.acs.org/acsodf/article/doi/10.1021/acsomega.6c10408/5463435/Sequential-Electrochemical-Construction-of},
  note = {CC BY 4.0},
}
RIS
TY  - JOUR
TI  - Sequential Electrochemical Construction of Hierarchical LIG/PPy/MnO2 Microsupercapacitors with High Areal Capacitance and Device-Level Stability
AU  - Tianqi Lu
AU  - Yinting Li
AU  - Haoran Mo
AU  - Jiadi Mao
AU  - Saddam Weheabby
AU  - Aseel Alnaimi
AU  - Ze Chen
AU  - Ammar Al-Hamry
AU  - Marcio Vidotti
AU  - Ahmed S. G. Khalil
AU  - Olfa Kanoun
PY  - 2026
DA  - 2026/11/04
JO  - ACS Omega
DO  - 10.1021/acsomega.6c10408
UR  - https://pubs.acs.org/acsodf/article/doi/10.1021/acsomega.6c10408/5463435/Sequential-Electrochemical-Construction-of
AB  - Achieving high areal energy storage in flexible microsupercapacitors while maintaining compatibility with direct planar patterning remains challenging, particularly when multiple pseudocapacitive components must be sequentially integrated without compromising electrode accessibility or device level performance. In this paper, we develop a sequential electrochemical construction strategy to integrate polypyrrole (PPy) and manganese dioxide (MnO2) directly onto interdigitated laser-induced graphene (LIG) electrodes without preformed composite powders, slurry casting, or polymer binders. Porous LIG serves as the conductive framework and current collector, followed by in situ PPy electropolymerization and subsequent MnO2 electrodeposition. Systematic control of LIG processing, PPy growth, MnO2 deposition, and gel electrolyte composition establishes a fabrication window that balances electrical conductivity, pseudocapacitive material loading, and structural accessibility while preserving the underlying porous LIG architecture. Stepwise LIG, LIG/PPy, and LIG/PPy/MnO2 controls exhibit the same performance hierarchy at both the individual electrode and complete device levels, demonstrating that the electrochemical gains introduced during sequential functionalization are retained after complete microsupercapacitor (MSC) assembly. The resulting LIG/PPy/MnO2 device delivers an areal capacitance of 621.2 mF cm–2 at 0.37 mA cm–2 and a maximum areal energy density of 55.22 μWh cm–2 at 0.1494 mW cm–2. Extended rate measurements further demonstrate continued electrochemical operation up to 5 mA cm–2 under substantially increased current demand. The device retains 97.04% of its flat state capacitance at 180° static bending, exhibits a device-to-device RSD of 2.29%, retains 94.5% capacitance after 60 days of ambient storage, and maintains 85.1% after 5000 GCD cycles. Series integration further extends the operating voltage from 0.8 to 2.4 V with predictable electrical scaling and enables three MSCs to power a red LED for approximately 183 s. These results establish a directly patterned and independently controlled approach for translating hierarchical pseudocapacitive construction into high areal energy storage, reproducible device performance, and scalable voltage output.
SN  - 2470-1343
ER  -