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Understanding solvothermal reductive reactions of graphene oxide in boron and ammonia solutions

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Abstract

Graphene has several favourable characteristics for both current and prospective applications. However, there are some economic issues emanating from the current methods of graphene synthesis and the need for high dispersibility in most potential applications. Reduced graphene oxide (RGO) is a suitable alternative that addresses these shortfalls. The synthesis of RGO via graphene oxide (GO) is leading to a quest for effective and ‘greener’ reduction protocols that simultaneously tune physicochemical properties for specific applications. Herein the study and comparison of the effects of electrophilic (empty orbitals on boron in boric anhydride) and nucleophilic (lone pairs on nitrogen in ammonia) solutions in solvothermal reduction of GO are presented. The study provides a better interpretation of the defect intensity, from Raman spectroscopy analysis, in relation to the conductivity of RGO. The highest increase in the C/O ratio from 2.48 (GO) to 11.36 (NRGO) suggests that ammonia displays the most reductive effect. Nucleophilic attack of carbon atoms within the oxygen functionalities of GO possibly enhanced reduction. Hydrothermal, and solvothermal reduction in electrophilic and nucleophilic solutions improved conductivity by two, three and five orders of magnitude relative to pristine GO, respectively. The sheet resistance, carrier concentration, and mobility of the superior NRGO were 93 Ω cm, 3.51 × 1018 cm−3 and 0.02 cm2 V−1 s−1, respectively. The solvent properties are dynamic in both the solvothermal reduction of GO and electronic property tailoring of RGO. The current work paves the way for future, cost-effective, facile reduction and doping protocols that tailor the physicochemical properties of graphene derivatives from the solvent nature. This is a practical economic approach that solves conductivity issues of GO whilst avoiding the use of toxic chemicals and high temperatures toward effective electronic devices.

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Acknowledgements

The author wishes to thank the University of KwaZulu-Natal (UKZN) and the University of Zimbabwe for providing the necessary support to this work. The author is also grateful to Annegret Stark, Bice S. Martincigh and Vincent O. Nyamori for postdoctoral mentorship, Matthew L. Davies for funding acquisition and mentorship, and James Mcgettrick for assistance in X-ray photoelectron spectroscopy analysis.

Funding

This work is based on research supported wholly by funding through the EPSRC GCRF SUNRISE project (Grant Number: EP/P032591/1) and in part, by the National Research Foundation (NRF) of South Africa (Grant Number: 116631).

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  1. School of Chemistry and Physics, University of KwaZulu-Natal, Westville Campus, Private Bag X54001, Durban, 4000, South Africa

    Edwin T. Mombeshora

  2. Department of Chemistry and Earth Sciences, University of Zimbabwe, Mount Pleasant, Post Office Box MP167, Harare, Zimbabwe

    Edwin T. Mombeshora

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ETM solely contributed to the conceptualization, methodology, experimental analysis, formal analysis, validation, writing, and editing of the manuscript.

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Mombeshora, E.T. Understanding solvothermal reductive reactions of graphene oxide in boron and ammonia solutions. J Mater Sci: Mater Electron 34, 521 (2023). https://doi.org/10.1007/s10854-023-09955-x

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