Hydrogen-bonded micelle assembly directed conjugated microporous polymers for nanospherical carbon frameworks towards dual-ion capacitors

Well-orchestrated carbon nanostructure with superb stable framework and high surface accessibility is crucial for zinc-ion hybrid capacitors (ZIHCs). Herein, a hydrogen-bonded micelle self-assembly strategy is proposed for morphology-controllable synthesis of conjugated microporous polymers (CMPs) derived carbon to boost zinc ion storage capability. In the strategy, F127 micellar assembly through intermolecular hydrogen bonds serves as structure-directed agents, directing CMPs’ oligomers grow into nanospherical assembly. The nanospherical carbon frameworks derived from CMPs (CNS-2) have shown maximized surface accessibility due to their plentiful tunable porosity and hierarchical porous structure with abundant mesoporous interconnected channels, and superb stability originating from CMPs’ robust framework, thus the CNS-2-based ZIHCs exhibit ultrahigh energy density of 163 Wh kg⁻¹ and ultralong lifespan with 93 % capacity retention after 200, 000 cycles at 20 A g⁻¹. Charged ion storage efficiency also lies in dual-ion alternate uptake of Zn²⁺ and CF₃SO₃⁻ as well as chemical redox of Zn²⁺ with carbonyl/pyridine motifs forming O–Zn–N bonds. Maximized surface accessibility and dual-ion storage mechanism ensure excellent electrochemical performance. Thus, the hydrogen-bond-guide micelle self-assembly strategy has provided a facile way to design nanoarchitectures of CMPs derived carbon for advanced cathodes of ZIHCs.