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Environmentally Benign Metal-Free Reduction of GO Using Molecular Hydrogen: A Mechanistic Insight.

ABSTRACT: A simple yet effective methodology to obtain high-quality reduced graphene oxide (RGO) using a tetrahydrofuran suspension of GO under hydrogen at moderate pressure has been demonstrated. The extent of reduction as a function of the pressure of hydrogen gas, temperature, and time was studied, where the abstraction of oxygen is achievable with least mutilation of C-sp² bonds, hence upholding the integrity of the graphene sheet. Herein, the formation of a short-lived species is proposed, which is possibly responsible for such reduction. A detailed theoretical calculation along with in situ UV-visible experiments reveals the existence of a transient solvated electron species in the reaction medium. The hydrogen RGO (HRGO) achieved a C/O atomic ratio of 11.3. The conductivity measurements show that HRGO reached as high as 934 S/m, which indicates a high quality of RGO. The process is hassle-free, environmentally benign, and can be scaled up effortlessly without compromising the quality of the material.

SUBMITTER: Rai R

PROVIDER: S-EPMC6643654 | biostudies-literature | 2018 Nov

REPOSITORIES: biostudies-literature

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Environmentally Benign Metal-Free Reduction of GO Using Molecular Hydrogen: A Mechanistic Insight.

Rai Ritu R Ahmed Zubair Z Kumar Rajinder R Kumawat Rameshwar L RL Chordiya Kalyani K Maruyama Takahiro T Ali Md Ehesan ME Bagchi Vivek V

ACS omega 20181108 11

A simple yet effective methodology to obtain high-quality reduced graphene oxide (RGO) using a tetrahydrofuran suspension of GO under hydrogen at moderate pressure has been demonstrated. The extent of reduction as a function of the pressure of hydrogen gas, temperature, and time was studied, where the abstraction of oxygen is achievable with least mutilation of C-sp<sup>2</sup> bonds, hence upholding the integrity of the graphene sheet. Herein, the formation of a short-lived species is proposed, ...[more]

PMID: 31458176

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Project description:Flexible metal-organic frameworks offer a route towards high useable hydrogen storage capacities with minimal swings in pressure and temperature via step-shaped adsorption and desorption profiles. Yet, the understanding of hydrogen-induced flexibility in candidate storage materials remains incomplete. Here, we investigate the hydrogen storage properties of a quintessential flexible metal-organic framework, ZIF-7. We use high-pressure isothermal hydrogen adsorption measurements to identify the pressure-temperature conditions of the hydrogen-induced structural transition in ZIF-7. The material displays narrow hysteresis and has a shallow adsorption slope between 100 K and 125 K. To gain mechanistic insight into the cause of the phase transition correlating with stepped adsorption and desorption, we conduct powder neutron diffraction measurements of the D2 gas-dosed structures at conditions across the phase change. Rietveld refinements of the powder neutron diffraction patterns yield the structures of activated ZIF-7 and of the gas-dosed material in the dense and open phases. The structure of the activated phase of ZIF-7 is corroborated by the structure of the activated phase of the Cd congener, CdIF-13, which we report here for the first time based on single crystal X-ray diffraction measurements. Subsequent Rietveld refinements of the powder patterns for the gas-dosed structure reveal that the primary D2 adsorption sites in the dense phase form D2-arene interactions between adjacent ligands in a sandwich-like adsorption motif. These sites are prevalent in both the dense and the open structure for ZIF-7, and we hypothesize that they play an important role in templating the structure of the open phase. We discuss the implications of our findings for future approaches to rationally tune step-shaped adsorption in ZIF-7, its congeners, and flexible porous adsorbents in general. Lastly, important to the application of flexible frameworks, we show that pelletization of ZIF-7 produces minimal variation in performance.

Dataset Information

Environmentally Benign Metal-Free Reduction of GO Using Molecular Hydrogen: A Mechanistic Insight.

Publications

Environmentally Benign Metal-Free Reduction of GO Using Molecular Hydrogen: A Mechanistic Insight.

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