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초록

Structurally modulated donor-acceptor (D-A) moieties are key constituents in designing redox-active conjugated polymers (RACPs), which serve as promising pseudocapacitive electrode materials due to their broad potential windows, superior redox behavior, and tunable electronic properties. Herein, we introduce silylethynyl-functionalized benzodithiophene (Si-BDT), a planar donor moiety developed by lateral side-chain engineering, copolymerized with rylene diimide acceptors, naphthalene diimide (NDI) and perylene diimide (PDI), synthesized by the Stille cross-coupling polymerization reaction. The supercapacitor performance of these polymers was assessed in two organic-salt electrolytes, tetrabutylammonium hexafluorophosphate (TBAPF6) and tetraethylammonium tetrafluoroborate (TEABF4). The computational analysis explored non-covalent interaction (NCI) between the electrode and electrolyte and confirmed that both electrodes exhibited a stronger interaction with TBAPF6, thereby facilitating improved charge transfer and electrochemical performance. Both electrodes were operated within a wide potential window of -1.7 to 0.7 V. Si-BDT-PDI outperformed Si-BDT-NDI, achieving a higher specific capacity of 267 C g-1 at 1 A g-1 due to electrode-electrolyte interactions enhanced by several topographic pores. Furthermore, a hybrid supercapacitor integrating a Si-BDT-PDI anode and a porous activated carbon cathode achieved an outstanding energy density of 55 W h kg-1 and a power density of 13 380 W kg-1 across a 2.7 V potential window.

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