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1.
ACS Appl Mater Interfaces ; 13(35): 41537-41544, 2021 Sep 08.
Artigo em Inglês | MEDLINE | ID: mdl-34428366

RESUMO

The energy density formula illuminated that widening the voltage window and maximizing capacitance are effective strategies to boost the energy density of supercapacitors. However, aqueous electrolyte-based devices generally afford a voltage window less than 1.2 V in view of water electrolysis, and chemically converted graphene yields mediocre capacitance. Herein, multi-electron redox-reversible, structurally stable indanthrone (IDT) π-backbones were rationally coupled with the reduced graphene oxide (rGO) framework to form IDT@rGO molecular heterojunctions. Such conductive agent- and binder-free film electrodes delivered a maximized capacitance of up to 345 F g-1 in a potential range of -0.2 to 1.0 V. The partner film electrode-Ti3C2Tx MXene which worked in the negative potential range of -0.1 to -0.6 V-afforded a capacitance as large as 769 F g-1. Thanks to the perfect complementary potentials of the IDT@rGO heterojunction positive electrode and Ti3C2Tx MXene negative partner, the polyvinyl alcohol/H2SO4 hydrogel electrolyte-based flexible asymmetric supercapacitor delivered an enlarged voltage window of 1.6 V and an impressive energy density of 17 W h kg-1 at a high power density of 8 kW kg-1, plus remarkable rate capability and cycling life (capacitance retention of ∼90% after 10000 cycles) as well as exceptional flexibility and bendability.

2.
ACS Appl Mater Interfaces ; 10(29): 24679-24688, 2018 Jul 25.
Artigo em Inglês | MEDLINE | ID: mdl-29968469

RESUMO

In this contribution, we describe a novel, facile, and scalable methodology for high degree functionalization toward graphene by the reaction between bulk graphite fluoride and in situ generated amine anion. Using this, the rationally designed sulfanilic acid pending on a graphene scaffold (G-SO3H), a two-dimensional (2D) π-conjugated counterpart of poly(styrenesulfonate), is available. Combined reliable characterizations demonstrate that a very large quantity of sulfanilic blocks are linked to graphene through the foreseen substitution of carbon-fluorine units and an unexpected reductive defluorination simultaneously proceeds during the one-step reaction, endowing the resultant G-SO3H with splendid dispersity in various solvents and film-forming property via the former, and with recovered 2D π-conjugation via the latter. Besides, the work function of G-SO3H lies at -4.8 eV, well matched with the P3HT donor. Awarded with these fantastic merits, G-SO3H behaves capable in hole collection and transport, indicated by the enhanced device efficiency and stability of polymer solar cells (PSCs) based on intensively studied P3HT:PCBM blends as an active layer. In particular, comparison with conventional poly(3,4-ethylenedioxythiophene) doped with poly(styrenesulfonate) and recently rising and shining graphene oxide, G-SO3H outperforms above 17 and 24%, respectively, in efficiency. More impressively, when these three unencapsulated devices are placed in a N2-filled glovebox at around 25 °C for 7 weeks, or subject to thermal treatment at 150 °C for 6 h also in N2 atmosphere, or even rudely exposed to indoor air, G-SO3H-based PSCs exhibit the best stability. These findings enable G-SO3H to be a strongly competitive alternative of the existing hole extraction materials for PSC real-life applications.

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