Dataset Information

Elucidating Charge Transport Mechanisms in Cellulose-Stabilized Graphene Inks.

ABSTRACT: Solution-processed graphene inks that use ethyl cellulose as a polymer stabilizer are blade-coated into large-area thin films. Following blade-coating, the graphene thin films are cured to pyrolyze the cellulosic polymer, leaving behind an sp2-rich amorphous carbon residue that serves as a binder in addition to facilitating charge transport between graphene flakes. Systematic charge transport measurements, including temperature-dependent Hall effect and non-contact microwave resonant cavity characterization, reveal that the resulting electrically percolating graphene thin films possess high mobility (≈ 160 cm2 V-1 s-1), low energy gap, and thermally activated charge transport, which develop weak localization behavior at cryogenic temperatures.

SUBMITTER: de Moraes ACM

PROVIDER: S-EPMC8201474 | biostudies-literature | 2020

REPOSITORIES: biostudies-literature

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Elucidating Charge Transport Mechanisms in Cellulose-Stabilized Graphene Inks.

de Moraes Ana C M ACM Obrzut Jan J Sangwan Vinod K VK Downing Julia R JR Chaney Lindsay E LE Patel Dinesh D Elmquist Randolph E RE Hersam Mark C MC

Journal of materials chemistry. C 20200101

Solution-processed graphene inks that use ethyl cellulose as a polymer stabilizer are blade-coated into large-area thin films. Following blade-coating, the graphene thin films are cured to pyrolyze the cellulosic polymer, leaving behind an sp<sup>2</sup>-rich amorphous carbon residue that serves as a binder in addition to facilitating charge transport between graphene flakes. Systematic charge transport measurements, including temperature-dependent Hall effect and non-contact microwave resonant ...[more]

PMID: 34131488

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Project description:This study investigates the solid-state charge transport properties of the oxidized forms of dioxythiophene-based alternating copolymers consisting of an oligoether-functionalized 3,4-propylenedioxythiophene (ProDOT) copolymerized with different aryl groups, dimethyl ProDOT (DMP), 3,4-ethylenedioxythiophene (EDOT), and 3,4-phenylenedioxythiophene (PheDOT), respectively, to yield copolymers P(OE3)-D, P(OE3)-E, and P(OE3)-Ph. At a dopant concentration of 5 mM FeTos3, the electrical conductivities of these copolymers vary significantly (ranging between 9 and 195 S cm-1) with the EDOT copolymer, P(OE3)-E, achieving the highest electrical conductivity. UV-vis-NIR and X-ray spectroscopies show differences in both susceptibility to oxidative doping and extent of oxidation for the P(OE3) series, with P(OE3)-E being the most doped. Wide-angle X-ray scattering measurements indicate that P(OE3)-E generally demonstrates the lowest paracrystallinity values in the series, as well as relatively small π-π stacking distances. The significant (i.e., order of magnitude) increase in electrical conductivity of doped P(OE3)-E films versus doped P(OE3)-D or P(OE3)-Ph films can therefore be attributed to P(OE3)-E exhibiting both the highest carrier ratios in the P(OE3) series, along with good π-π overlap and local ordering (low paracrystallinity values). Furthermore, these trends in the extent of doping and paracrystallinity are consistent with the reduced Fermi energy level and transport function prefactor parameters calculated using the semilocalized transport (SLoT) model. Observed differences in carrier ratios at the transport edge (ct) and reduced Fermi energies [η(c)] suggest a broader electronic band (better overlap and more delocalization) for the EDOT-incorporating P(OE3)-E polymer relative to P(OE3)-D and P(OE3)-Ph. Ultimately, we rationalize improvements in electrical conductivity due to microstructural and doping enhancements caused by EDOT incorporation, a structure-property relationship worth considering in the future design of highly electrically conductive systems.

Dataset Information

Elucidating Charge Transport Mechanisms in Cellulose-Stabilized Graphene Inks.

Publications

Elucidating Charge Transport Mechanisms in Cellulose-Stabilized Graphene Inks.

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