Ultrahigh-throughput exfoliation of graphite into pristine ‘single-layer’ graphene using microwaves and molecularly engineered ionic liquids

Matsumoto, Michio; Saito, Yûsuke; Park, Chiyoung; Fukushima, Takanori; Aida, Takuzo

doi:10.1038/nchem.2315

Cited by 296 publications

(220 citation statements)

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“…The graphene sheets showed negligible deterioration and were redispersible (up to 100 mg/mL) in the ILs. 27 The favorable properties exhibited by ether functionalized ILs over their alkyl counterparts, leading to such a wide range of applications, has prompted the exploration of their nanoscale structure in order to understand the origins of their desirable properties and how they can be further enhanced.Molecular dynamics (MD) simulations suggest that there is reduced electrostatic interaction between cations and anions in ether functionalized ILs, due to the polar ether group, when compared to ) unless CC License in place (see abstract). ecsdl.org/site/terms_use address.…”

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Connecting Structural and Transport Properties of Ionic Liquids with Cationic Oligoether Chains

Lall-Ramnarine

Zhao

Rodriguez

et al. 2017

J. Electrochem. Soc.

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X-ray diffraction and molecular dynamics simulations were used to probe the structures of two families of ionic liquids containing oligoether tails on the cations. Imidazolium and pyrrolidinium bis(trifluoromethylsulfonyl)amide ILs with side chains ranging from 4 to 10 atoms in length, including both linear alkyl and oligo-ethylene oxide tails, were prepared. Their physical properties, such as viscosity, conductivity and thermal profile, were measured and compared for systematic trends. Consistent with earlier literature, a single ether substituent substantially decreases the viscosity of pyrrolidinium and imidazolium ILs compared to their alkyl congeners. Remarkably, as the number of ether units in the pyrrolidinium ILs increases there is hardly any increase in the viscosity, in contrast to alkylpyrrolidinium ILs where the viscosity increases steadily with chain length. Viscosities of imidazolium ether ILs increase with chain length but always remain well below their alkyl congeners. To complement the experimentally determined properties, molecular dynamics simulations were run on the two ILs with the longest ether chains. The results point to specific aspects that could be useful for researchers designing ILs for specific applications. The focus of the ionic liquid (IL) community is shifting beyond the mere measurement of physical properties and identification of trends arising from particular structural moieties. Researchers are delving deeper into the nanostructural interactions between the ions to determine the topographical landscape of the ions within the liquids that influence IL properties.1-3 Such information is valuable when tuning the properties of ILs for particular applications. The ability to tune the properties of ionic liquids for specific applications is a major factor in their allure as remarkable solvents that make it possible to do extreme chemistry without extreme conditions. It has been acknowledged that although ionic liquids have a combination of physical properties that make them attractive alternatives to traditional solvents, they have relatively high viscosities that hamper their practical application in large-scale processes. For example, in the area of electrochemical energy storage devices there is still an urgent need for improved electrolytes exhibiting properties of combustion resistance, high conductivity, and wide electrochemical windows. ILs with improved transport properties (viscosity, conductivity and diffusivity) would be perfect candidates to address this need. Structural modification of the IL cation and anion is a proven tool to dramatically alter IL properties. In particular, substituting ether functionalities for alkyl functionalities on IL cations has been shown to reduce the viscosity of ionic liquids significantly.2,4-6 In this work we examine the effect of incorporating oligoether side chains of varying lengths (1-3 repeating ethoxy units, Figure 1) on the physical properties and structural characteristics of imidazolium and pyrrolidinium NTf 2 ionic liquids in ...

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Connecting Structural and Transport Properties of Ionic Liquids with Cationic Oligoether Chains

Lall-Ramnarine

Zhao

Rodriguez

et al. 2017

J. Electrochem. Soc.

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Section: Properties and Preparationmentioning

confidence: 99%

“…It is reported that graphite and graphene,44 as well as ionic liquids,45 are thought to efficiently absorb microwaves. As shown in Figure 4b, Aida et al reported that with the assistance of microwave irradiation, graphite suspended in molecularly engineered oligomeric ionic liquids allows for ultrahigh‐efficiency exfoliation (93% yield) with a high selectivity (95%) towards “single‐layer” graphene (thicknesses <1 nm) in 30 minutes 46…”

Section: Properties and Preparationmentioning

confidence: 99%

Human‐Like Sensing and Reflexes of Graphene‐Based Films

et al. 2016

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Humans have numerous senses, wherein vision, hearing, smell, taste, and touch are considered as the five conventionally acknowledged senses. Triggered by light, sound, or other physical stimulations, the sensory organs of human body are excited, leading to the transformation of the afferent energy into neural activity. Also converting other signals into electronical signals, graphene‐based film shows its inherent advantages in responding to the tiny stimulations. In this review, the human‐like senses and reflexes of graphene‐based films are presented. The review starts with the brief discussions about the preparation and optimization of graphene‐based film, as where as its new progress in synthesis method, transfer operation, film‐formation technologies and optimization techniques. Various human‐like senses of graphene‐based film and their recent advancements are then summarized, including light‐sensitive devices, acoustic devices, gas sensors, biomolecules and wearable devices. Similar to the reflex action of humans, graphene‐based film also exhibits reflex when under thermal radiation and light actuation. Finally, the current challenges associated with human‐like applications are discussed to help guide the future research on graphene films. At last, the future opportunities lie in the new applicable human‐like senses and the integration of multiple senses that can raise a revolution in bionic devices.

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“…Ever since chemically exfoliated graphene (e.g., graphene oxide, acidified graphene, and reduced graphene oxide) was shown to have a number of structural defects89, recent studies have focused on a physical process, especially on pristine graphene produced by the liquid-phase exfoliation of graphite. Various types of dispersants (surfactants, polymers, ionic liquids, proteins, and nanotubes) have been proposed for the direct production of pristine graphene from graphite10111213141516. Many of these dispersants, however, decrease the electrical conductivity of graphene because they disrupt the extended aromatic conjugated systems and cover the graphene with nonconductive molecules1617.…”

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Rational and practical exfoliation of graphite using well-defined poly(3-hexylthiophene) for the preparation of conductive polymer/graphene composite

Iguchi

Higashi

Funasaki

et al. 2017

Sci Rep

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Processing and manipulation of highly conductive pristine graphene in large quantities are still major challenges in the practical application of graphene for electric device. In the present study, we report the liquid-phase exfoliation of graphite in toluene using well-defined poly(3-hexylthiophene) (P3HT) to produce a P3HT/graphene composite. We synthesize and use regioregular P3HT with controlled molecular weights as conductive dispersants for graphene. Simple ultrasonication of graphite flakes with the P3HT successfully produces single-layer and few-layer graphene sheets dispersed in toluene. The produced P3HT/graphene composite can be used as conductive graphene ink, indicating that the P3HT/graphene composite has high electrical conductivity owing to the high conductivity of P3HT and graphene. The P3HT/graphene composite also works as an oxidation-resistant and conductive film for a copper substrate, which is due to the high gas-barrier property of graphene.

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Ultrahigh-throughput exfoliation of graphite into pristine ‘single-layer’ graphene using microwaves and molecularly engineered ionic liquids

Cited by 296 publications

References 50 publications

Connecting Structural and Transport Properties of Ionic Liquids with Cationic Oligoether Chains

Connecting Structural and Transport Properties of Ionic Liquids with Cationic Oligoether Chains

Human‐Like Sensing and Reflexes of Graphene‐Based Films

Rational and practical exfoliation of graphite using well-defined poly(3-hexylthiophene) for the preparation of conductive polymer/graphene composite

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