In Situ Mineralization of Biomass-Derived Hydrogels Boosts Capacitive Electrochemical Energy Storage in Free-Standing 3D Carbon Aerogels

Anjali Achazhiyath Edathil; Babak Rezaei; Kristoffer Almdal; Stephan Sylvest Keller

doi:10.1002/eem2.12591

Energy & Environmental Materials ›› 2024, Vol. 7 ›› Issue (2) :12591 DOI: 10.1002/eem2.12591

RESEARCH ARTICLE

In Situ Mineralization of Biomass-Derived Hydrogels Boosts Capacitive Electrochemical Energy Storage in Free-Standing 3D Carbon Aerogels

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Abstract

Here, a novel fabrication method for making free-standing 3D hierarchical porous carbon aerogels from molecularly engineered biomass-derived hydrogels is presented. In situ formed flower-like CaCO₃ molecularly embedded within the hydrogel network regulated the pore structure during in situ mineralization assisted one-step activation graphitization (iMAG), while the intrinsic structural integrity of the carbon aerogels was maintained. The homogenously distributed minerals simultaneously acted as a hard template, activating agent, and graphitization catalyst. The decomposition of the homogenously distributed CaCO₃ during iMAG followed by the etching of residual CaO through a mild acid washing endowed a robust carbon aerogel with high porosity and excellent electrochemical performance. At 0.5 mA cm^-2, the gravimetric capacitance increased from 0.01 F g^-1 without mineralization to 322 F g^-1 with iMAG, which exceeds values reported for any other free-standing or powder-based biomass-derived carbon electrodes. An outstanding cycling stability of ~104% after 1000 cycles in 1 M HClO₄ was demonstrated. The assembled symmetric supercapacitor device delivered a high specific capacitance of 376 F g^-1 and a high energy density of 26 W h kg^-1 at a power density of 4000 W kg^-1, with excellent cycling performance (98.5% retention after 2000 cycles). In combination with the proposed 3D printed mold-assisted solution casting (3DMASC), iMAG allows for the generation of free-standing carbon aerogel architectures with arbitrary shapes. Furthermore, the novel method introduces flexibility in constructing free-standing carbon aerogels from any ionically cross-linkable biopolymer while maintaining the ability to tailor the design, dimensions, and pore size distribution for specific energy storage applications.

Keywords

biomass / carbon aerogel / sustainable energy materials / free-standing / supercapacitors

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Anjali Achazhiyath Edathil, Babak Rezaei, Kristoffer Almdal, Stephan Sylvest Keller. In Situ Mineralization of Biomass-Derived Hydrogels Boosts Capacitive Electrochemical Energy Storage in Free-Standing 3D Carbon Aerogels. Energy & Environmental Materials, 2024, 7(2): 12591 DOI:10.1002/eem2.12591

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