Fabrication of tunable mesoporous crosslinked functional surfaces directed by dual triblock copolymers and ion...

A dual-surfactant-regulated (Synperonic@F-108 and Pluronic@P-123) self-assembled microemulsion templating methodology was devised to construct PBAs@Dopamine-F108/P123 (PD-FP) core-shell composites with mesoporous cross-linked surfaces and precisely engineered pore architectures, from which the target product resulting from selenium doping (PD-Se) was subsequently obtained via calcination. The mechanistic foundations underlying composite formation and the quantitative contributions of pivotal synthetic variables were systematically examined, enabling precise and efficient modulation of the chemical environment at the porous functional interface as well as deliberate regulation of pore size distribution. This dual optimization substantially enhanced the accessibility of internal active sites under solution-phase conditions while preserving the mechanical integrity of the overall framework. Complementarily, molecular dynamics (MD) simulations were employed to compute critical parameters, including the characteristic ion adsorption capacity, hydrogen bond count, and interfacial tension at the two-phase interface of PD-Se-1 which was obtained after calcination and doping of PD-F_0.1P_2.9 within the electrolyte, thereby furnishing atomic-level structural corroboration for both the physicochemical characterization results and the electrochemical performance of the electrode material. In a three-electrode configuration, PD-Se-1 delivered an exceptional specific capacitance of 2246 F g^-1. Systematic comparative evaluations were subsequently conducted by assembling PD-Se-1 into asymmetric supercapacitors (ASCs) in conjunction with selenium-doped dopamine hollow porous networks (DPN-Se) and activated carbon (AC), which further substantiated the pronounced structure-property advantages conferred by homogeneous electrode architectures over their heterogeneous counterparts. Collectively, this study established a universal strategy for constructing high-performance porous functional interfaces with stable performance characteristics, offering mechanistic insights and translational guidance for the advancement of next-generation energy storage systems.