title: Superior Charge Storage and Power Density of a Conducting Polymer-Modified Covalent Organic Framework.
abstract: The low conductivity of two-dimensional covalent organic frameworks (2D COFs), and most related coordination polymers, limits their applicability in optoelectronic and electrical energy storage (EES) devices. Although some networks exhibit promising conductivity, these examples generally lack structural versatility, one of the most attractive features of framework materials design. Here we enhance the electrical conductivity of a redox-active 2D COF film by electropolymerizing 3,4-ethylenedioxythiophene (EDOT) within its pores. The resulting poly(3,4-ethylenedioxythiophene) (PEDOT)-infiltrated COF films exhibit dramatically improved electrochemical responses, including quantitative access to their redox-active groups, even for 1 μm-thick COF films that otherwise provide poor electrochemical performance. PEDOT-modified COF films can accommodate high charging rates (10-1600 C) without compromising performance and exhibit both a 10-fold higher current response relative to unmodified films and stable capacitances for at least 10 000 cycles. This work represents the first time that electroactive COFs or crystalline framework materials have shown volumetric energy and power densities comparable with other porous carbon-based electrodes, thereby demonstrating the promise of redox-active COFs for EES devices.
authors.affiliation: Department of Chemistry and Chemical Biology, Baker Laboratory, Cornell University , Ithaca, New York 14853-1301, United States.
authors.forename: Catherine R
authors.initials: CR
authors.lastname: Mulzer
authors.affiliation: Department of Chemistry and Chemical Biology, Baker Laboratory, Cornell University , Ithaca, New York 14853-1301, United States.
authors.forename: Luxi
authors.initials: L
authors.lastname: Shen
authors.affiliation: Department of Chemistry and Chemical Biology, Baker Laboratory, Cornell University, Ithaca, New York 14853-1301, United States; Department of Chemistry, Northwestern University, Evanston, Illinois 60208, United States.
authors.forename: Ryan P
authors.initials: RP
authors.lastname: Bisbey
authors.affiliation: Department of Chemistry and Chemical Biology, Baker Laboratory, Cornell University , Ithaca, New York 14853-1301, United States.
authors.forename: James R
authors.initials: JR
authors.lastname: McKone
authors.affiliation: Department of Chemistry and Chemical Biology, Baker Laboratory, Cornell University , Ithaca, New York 14853-1301, United States.
authors.forename: Na
authors.initials: N
authors.lastname: Zhang
authors.affiliation: Department of Chemistry and Chemical Biology, Baker Laboratory, Cornell University , Ithaca, New York 14853-1301, United States.
authors.forename: Héctor D
authors.initials: HD
authors.lastname: Abruña
authors.affiliation: Department of Chemistry and Chemical Biology, Baker Laboratory, Cornell University, Ithaca, New York 14853-1301, United States; Department of Chemistry, Northwestern University, Evanston, Illinois 60208, United States.
authors.forename: William R
authors.initials: WR
authors.lastname: Dichtel