Graphite Oxide Story – From the Beginning Till the Graphene Hype

Lerf, A.

doi:10.1002/9781119069447.ch1

Cited by 5 publications

(3 citation statements)

References 109 publications

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“…The much less abundant and much more oxidized soluble fragments -oxidative debris (OD)strongly adhere to these flat bwGO entities and are composed of polyaromatic molecules of widely varying sizes and with a large number of oxygen functionalities anchored to the edges. In fact, the early literature, before the seminal work of Hummers and Offeman [21], already indicated that aqueous KMnO 4 treatments of coals and cokes produced aromatic polycarboxylic acids [22,23]; the same acids (including mellitic acid) were obtained when graphite oxide is produced using chlorate-based oxidation methods [24], as corroborated recently by Lerf [25]. Consequently, OD acts as a surfactant able to disperse clean bwGO sheets.…”

Section: Introductionmentioning

confidence: 76%

New insights into oxygen surface coverage and the resulting two-component structure of graphene oxide

Martı́n-Gullón

Pérez

Domene

et al. 2020

Carbon

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Section: Introductionmentioning

confidence: 76%

New insights into oxygen surface coverage and the resulting two-component structure of graphene oxide

Martı́n-Gullón

Pérez

Domene

et al. 2020

Carbon

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“…Furthermore, the berthollide (nonstoichiometric) nature and strong hydrophilicity of GO cause a great difficulty in defining its structure . A number of efforts have been made to elucidate the structure of GO in the early years from 1930 to 1990 based on reaction observations and XRD signals, but they were not widely recognized for the lack of unambiguous evidence . With the assistance of NMR, the models proposed by Klinowski and co-workers received much attention. − The Lerf-Klinowski model (Figure a), though with an uncertainty in the edge groups, was later supported and complemented by Zettl and co-workers via ultrahigh-resolution TEM (Figure b) and Pacilé et al as well by TEM and NEXAFS .…”

Section: Basic Chemistries For 3d Graphene Materials Synthesismentioning

confidence: 99%

3D Graphene Materials: From Understanding to Design and Synthesis Control

2020

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Carbon materials, with their diverse allotropes, have played significant roles in our daily life and the development of material science. Following 0D C60 and 1D carbon nanotube, 2D graphene materials, with their distinctively fascinating properties, have been receiving tremendous attention since 2004. To fulfill the efficient utilization of 2D graphene sheets in applications such as energy storage and conversion, electrochemical catalysis, and environmental remediation, 3D structures constructed by graphene sheets have been attempted over the past decade, giving birth to a new generation of graphene materials called 3D graphene materials. This review starts with the definition, classifications, brief history, and basic synthesis chemistries of 3D graphene materials. Then a critical discussion on the design considerations of 3D graphene materials for diverse applications is provided. Subsequently, after emphasizing the importance of normalized property characterization for the 3D structures, approaches for 3D graphene material synthesis from three major types of carbon sources (GO, hydrocarbons and inorganic carbon compounds) based on GO chemistry, hydrocarbon chemistry, and new alkali-metal chemistry, respectively, are comprehensively reviewed with a focus on their synthesis mechanisms, controllable aspects, and scalability. At last, current challenges and future perspectives for the development of 3D graphene materials are addressed.

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“…Several structural models, both varied and overlapping, were proposed throughout its long past. ,− The discovery of graphene refueled extensive studies on GO using modern techniques, and there are distinct methods of graphene oxidation leading to varying compositions and morphologies . In spite of all these efforts, the dominant opinion of the pregraphene era prevails: the largely intact hexagonal backbone with occasional holes, epoxides, and alcohols (tertiary) as primary functional groups, >CO and −COOH groups in the holes as well as in the periphery with some leftover unsaturated regions.…”

Section: Introductionmentioning

confidence: 99%

Nature of Interactions between Epoxides in Graphene Oxide

2019

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Graphene oxide exhibits extensive disorder with a multitude of functional groups and holes making its structure an abstract concept. Multiple structural models make it a dark horse and hamper its utility despite its synthetic ease, maneuverability, and promising applications. Here we probe the impact of the epoxidation process, which is arguably the first kinetic step in graphene oxidation, to identify the induced vulnerabilities of its backbone and to cognize possible pathways for further oxidation. Probing the topological and geometrical variations in the distribution of epoxide on the graphene lattice, we find that the conformational entropy, driven by the combinatorial growth of isomers, aids and abets disorder. Graph theoretical enumeration gives 16 distinct epoxide environments within symmetrically equivalent epoxides. Their stability is primarily influenced by the steric repulsion between the oxygen lone pairs and overlap compatibility of the interepoxy C–C bond. Avoiding steric repulsion either by topology or by equatorial splaying of oxygens leads to stability, without which the network is weakened either by elongation of C–C bonds or by axial splaying of oxygens leading to uneven C–O bonds. The proposed unzipping of the underlying epoxy C–C bond through the cooperativity of strain from three-membered rings and conjugative stabilization from residual sp2 character are found to be incongruous. With an improved bonding model of epoxide, we account for the observed variations in C–C bond lengths and energetics of epoxides in different environments that facilitate strategic mechanistic control for further oxidation.

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Graphite Oxide Story – From the Beginning Till the Graphene Hype

Cited by 5 publications

References 109 publications

New insights into oxygen surface coverage and the resulting two-component structure of graphene oxide

New insights into oxygen surface coverage and the resulting two-component structure of graphene oxide

3D Graphene Materials: From Understanding to Design and Synthesis Control

Nature of Interactions between Epoxides in Graphene Oxide

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