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      Tuning the Multifunctional Surface Chemistry of Reduced Graphene Oxide via Combined Elemental Doping and Chemical Modifications

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          Abstract

          The synthesis of graphene materials with multiple surface chemistries and functionalities is critical for further improving their properties and broadening their emerging applications. We present a simple chemical approach to obtain bulk quantities of multifunctionalized reduced graphene oxide (rGO) that combines chemical doping and functionalization using the thiol-ene click reaction. Controllable modulation of chemical multifunctionality was achieved by simultaneous nitrogen doping and gradual chemical reduction of graphene oxide (GO) using ammonia and hydrazine, followed by covalent attachment of amino-terminated thiol molecules using the thiol-ene click reaction. A series of N-doped rGO (N-rGO) precursors with different levels of oxygen groups were synthesized by adjusting the amount of reducing agent (hydrazine), followed by subsequent covalent attachment of cysteamine via the thermal thiol-ene click reaction to yield different ratios of mixed functional groups including N (pyrrolic N, graphitic N, and aminic N), S (thioether S, thiophene S, and S oxides), and O (hydroxyl O, carbonyl O, and carboxyl O) on the reduced GO surface. Detailed XPS analysis confirmed the disappearance of unstable pyridinic N in cys-N-rGO and the reduction degree threshold of N-rGO for effective cysteamine modification to take place. Our study establishes a strong correlation between different reduction degrees of N-rGO with several existing oxygen functional groups and addition of new tunable functionalities including covalently attached nitrogen (amino) and sulfur (C–S–C, C=S, and S–O). This simple and versatile approach provides a valuable contribution for practical designing and synthesis of a broad range of functionalized graphene materials with tailorable functionalities, doping levels, and interfacial properties for potential applications such as polymer composites, supercapacitors, electrocatalysis, adsorption, and sensors.

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          The reduction of graphene oxide

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            Combined Effect of Nitrogen- and Oxygen-Containing Functional Groups of Microporous Activated Carbon on its Electrochemical Performance in Supercapacitors

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              Thiol–ene “click” reactions and recent applications in polymer and materials synthesis: a first update

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                Author and article information

                Journal
                ACS Omega
                ACS Omega
                ao
                acsodf
                ACS Omega
                American Chemical Society
                2470-1343
                11 November 2019
                26 November 2019
                : 4
                : 22
                : 19787-19798
                Affiliations
                School of Chemical Engineering and Advanced Materials and ARC Hub for Graphene Enabled Industry Transformation, The University of Adelaide , Adelaide, SA 5005, Australia
                [§ ]School of Agriculture, Food and Wine, The University of Adelaide , PMB 1, Waite Campus, Glen Osmond, SA 5064, Australia
                []Research & Business Partnerships, Research Services, The University of Adelaide , Adelaide, SA 5000, Australia
                Author notes
                Article
                10.1021/acsomega.9b02642
                6882126
                Copyright © 2019 American Chemical Society

                This is an open access article published under an ACS AuthorChoice License, which permits copying and redistribution of the article or any adaptations for non-commercial purposes.

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