<p>Supercapacitors deliver high power but are limited in compact applications by low volumetric energy and power densities. Two-dimensional materials like graphene, despite their high packing density, are hindered by poor ion transport kinetics. A rapid thermal annealing step generates unusually curved turbostratic graphene crystallites, integrated and interwoven within disordered domains in micron-size particles to yield multiscale graphene. Ion insertion into the interlayers enables precise pore-ion matching and partial charge transfer, enabling a high Brunauer-Emmett-Teller surface area-normalized capacitance of 85 µF/cm<sup>2</sup>. Here, we show that multiscale graphene exhibits rapid ion transport dynamics within the curved crystallites and disordered domains. When the thin electrodes are assembled into symmetric pouch cell devices, they deliver a stack-level volumetric energy density of 99.5 Wh/L in ionic liquid electrolytes and 49.2 Wh/L in organic electrolyte with a high power density of 69.2 kW/L at 9.6 Wh/L.</p>

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Operando interlayer expansion of multiscale curved graphene for volumetrically-efficient supercapacitors

  • Petar Jovanović,
  • Meysam Sharifzadeh Mirshekarloo,
  • Phillip Aitchison,
  • Mahdokht Shaibani,
  • Mainak Majumder

摘要

Supercapacitors deliver high power but are limited in compact applications by low volumetric energy and power densities. Two-dimensional materials like graphene, despite their high packing density, are hindered by poor ion transport kinetics. A rapid thermal annealing step generates unusually curved turbostratic graphene crystallites, integrated and interwoven within disordered domains in micron-size particles to yield multiscale graphene. Ion insertion into the interlayers enables precise pore-ion matching and partial charge transfer, enabling a high Brunauer-Emmett-Teller surface area-normalized capacitance of 85 µF/cm2. Here, we show that multiscale graphene exhibits rapid ion transport dynamics within the curved crystallites and disordered domains. When the thin electrodes are assembled into symmetric pouch cell devices, they deliver a stack-level volumetric energy density of 99.5 Wh/L in ionic liquid electrolytes and 49.2 Wh/L in organic electrolyte with a high power density of 69.2 kW/L at 9.6 Wh/L.