The true promise of MXene as a practical supercapacitor electrode hinges on the simultaneous advancement of its three-dimensional (3D) assembly and the engineering of its nanoscopic architecture, two critical factors for facilitating mass transport and enhancing an electrode's charge-storage performance. Herein, we present a straightforward strategy to engineer robust 3D freestanding MXene (TiCT) hydrogels with hierarchically porous structures. The tetraamminezinc(II) complex cation ([Zn(NH)]) is selected to electrostatically assemble colloidal MXene nanosheets into a 3D interconnected hydrogel framework, followed by a mild oxidative acid-etching process to create nanoholes on the MXene surface. These hierarchically porous, conductive holey-MXene frameworks facilitate 3D transport of both electrons and electrolyte ions to deliver an excellent specific capacitance of 359.2 F g at 10 mV s and superb capacitance retention of 79% at 5000 mV s, representing a 42.2% and 15.3% improvement over pristine MXene hydrogel, respectively. Even at a commercial-standard mass loading of 10.1 mg cm, it maintains an impressive capacitance retention of 52% at 1000 mV s. This rational design of an electrode by engineering nanoholes on MXene nanosheets within a 3D porous framework dictates a significant step forward toward the practical use of MXene and other 2D materials in electrochemical energy storage systems.

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http://www.ncbi.nlm.nih.gov/pmc/articles/PMC10832346PMC
http://dx.doi.org/10.1021/acsnano.3c11551DOI Listing

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