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One-Step Synthesis of Hierarchical, Bimodal Nanoporous Carbons via Co-templating with Bottlebrush and Linear Block Copolymers

We
report the preparation of hierarchically ordered porous carbon
films with ∼5 nm mesopores distributed within a continuous
carbon framework surrounding ∼100 nm macropores. The hierarchical
carbons are prepared using bottlebrush block copolymers (BBCP) of
large molecular weight (Mw = 1800 kg mol–1), low-molecular-weight linear block copolymers (LBCPs),
and phenol-formaldehyde resin, which cooperatively assemble to yield
“planet–satellite” morphologies following carbonization.
The combination of BBCPs and LBCPs as co-templates enables a generalized
strategy to design functional materials in which the pore sizes of
both the mesopores and macropores are tuned within a continuous matrix
and the mesopores uniformly surround macropores. The template is an
ideal route for fabrication of tailored devices. The hierarchical
carbon films exhibit exceptional performance as supercapacitor electrodes,
with capacitance reaching up to C = 1420 mF cm–2 at 16 mA cm–2 (corresponding to
177 F g–1 at 2 A g–1 with mass
loading 8 mg cm–2) resulting from a combination
of high surface area and controlled pore structures. In such an application,
the hierarchical carbons outperform devices that contain exclusively
mesopores templated by the LBCP or only the macropores templated by
the BBCP.