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Tuning the morphology of block copolymer self-assembly-directed ultra-large porous carbons for electrochemical energy storage applications
Author(s)
Date Issued
January 9, 2026
Type
Article
Abstract
Developing carbon materials with well-defined macroporous structures is important for improving ion transport in high-rate electrochemical energy storage (EES) systems. While block copolymer (BCP) self-assembly directed carbons have shown promise, most reports remain limited to the mesoporous regime. In this work, we demonstrate a co-assembly strategy using ultra-large molar mass poly(styrene-block-2-dimethylaminoethyl methacrylate) (PS-b-PDMAEMA, or simply SA) diblock copolymers and phenolic resols to access tunable macroporous morphologies. By adjusting the tetrahydrofuran/ethyl acetate (THF/EA) solvent ratio and introducing small molar mass homo-polystyrene (hPS) as a domain-swelling agent, we achieve co-continuous carbon structures with pore sizes ranging from 50 nm to nearly 1 μm. This represents a substantial extension beyond what is typically achieved with BCP-derived morphologies. The ideal THF/EA ratio chosen in this work was 8:2, based on the reproducibility of resultant co-continuous structures and suppression of non-desirable micelle formation or macrophase segregated occlusions of carbon. The resulting carbons exhibit a highly interconnected pore network, moderate conductivity (∼2.47 S/cm), and specific surface areas of ∼700 m2 g−1. Raman spectroscopy suggests partially graphitized domains, with crystallite size estimated at 2.8 nm. Electrochemical measurements using a three-electrode setup confirm efficient charge storage behavior, with a specific capacitance of 6.6 F/g at 10 mV/s and 66 % retention at 100 mV/s. These findings highlight the potential of this system as a monolithic 3D carbon electrode platform for future high-performance EES devices.
Citation
Polymer, 343, 2026