Interfacial Hydrogen Bond Engineering: Enabling Rapid 3D Assembly of MXene Thick Electrodes with High Mass Loading and Fast Charge Transport

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Abstract Micro‐supercapacitors (MSCs) hold great promise for powering next‐generation microelectronics. However, their practical deployment remains severely hindered by low areal energy densities (≤100 µWh cm − 2 ) under constrained footprints (<1 cm 2 )—primarily due to the challenges in constructing 3D thick electrodes with high mass loading and efficient charge transport. Herein, a scalable and cost‐effective strategy is presented for fabricating MXene‐based 3D thick electrodes (>2400 µm) by intensifying interfacial hydrogen‐bond interactions between oxygen plasma‐activated carbon felt and Ti 3 C 2 T x MXene nanosheets. This interfacial engineering approach drives the rapid and robust self‐assembly of MXene flakes into a hierarchically porous, low‐tortuosity architecture while transforming the carbon felt into a multifunctional 3D conductive framework—simultaneously enhancing structural integrity, charge carrier mobility, and post‐fabrication processability. The resulting ultra‐thick electrodes abandon inactive binder/additives and fully exploit the vertical space, maximizing active material utilization. When paired with MnO 2 nanowires/carbon nanotube hybrid cathodes, MSCs with the demonstrated MXene‐based thick anodes achieve a 2.3 V output and a high areal energy density of 818 µWh cm − 2 . This work overcomes the long‐standing trade‐off between electrode thickness and charge transport kinetics in thick electrodes and establishes a versatile framework for architecting high‐energy‐density MSCs, advancing the development of integrated microelectronics for the future.

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