Synthesis of 3-D Graphene via Combustion Synthesis of Magnesium and Calcium/Magnesium Oxalates

Abstract

We demonstrate a novel and simple protocol for the fast and autothermal synthesis of layered graphene-related nanomaterial via the self-sustaining combustion synthesis. Various initial composition of starting reactants (Mg/CaC 2 O 4 and Mg/MgC 2 O 4 ) were tested and the effects of the operational parameters were systemically investigated in terms of the efficiency of product formation and its characteristics. The obtained products were analyzed using X-ray diffraction, electron microscopy, Raman spectroscopy and thermogravimetric analysis. The as-produced 3D graphene-related material has interesting properties and can be used in supercapacitors and as adsorbent for the removal of organic compounds. Graphene, a unique two-dimensional (2D) array of monolayer carbon atoms packed into a dense honeycomb crystal, has attracted much attention because of its diverse and extraordinary properties, i.e. electronic, magnetic, thermal, lubricant, chemical, optical, and mechanical.1 Graphene-related materials are also postulated to be used in energy conversion and storage.2 Thus, graphene and graphene-related materials have shown many applications in nanoelectronics, 3 sensors, 4 composite materials, 5 and in an environmental engineering.6 Carbon and graphitic materials have also been for decades a workhorse material in electrochemistry.7 Graphene was first produced by Novoselov et al. by mechanical exfoliation of graphite in 2004. 8 Since then many techniques have been proposed to obtain graphene with a main approach via energy-and timeconsuming wet chemistry route of graphite exfoliation. Jankovsky et al. 9 presented recently in details the thermal exfoliation/reduction of graphite oxide.The focus of this work is to obtain hierarchical layered carbons. Such few-layered graphene is also called 3D graphene 10 which, in fact, has many potential applications including energy storage (capacitors, electrodes), gas sensing, catalysis, biomedicine (biocompatible scaffolds), adsorption, hydrogels, and composites. As for example, Zhang et al. reported recently the synthesis of porous 3D graphene-based material with excellent properties for such applications. 11Herein we apply a self-propagating high-temperature synthesis (SHS), also called combustion synthesis (thermolysis) which has been widely used for years for fabrication of many compounds with large negative heat of formation.12,13 Such fast process usually progresses in a self-sustaining and energy self-efficient regime.7 In fact, we have shown elsewhere that SiC nanowires can be efficiently synthesized from simple starting reactants (Si/Teflon).14,15 Zhao et al. presented recently 16 an approach for synthesizing graphene through a magnesiothermic reduction of calcium carbonate, while Poh et al. 17 synthesized graphenes for electrochemical applications via reduction of CO 2 by lithium.The aim of this work was to test such a synthetic strategy for converting carbon-containing Ca/Mg oxalates into 3D graphene-related materials. The electrochemical measurements were performed to e...

Plasma enhanced synthesis of N doped vertically aligned carbon nanofibers on 3D graphene

“…Our group in the past used Ni powder to synthesize 3DG pellets and graphene paper . Another interesting way of making a 3DG structure was reported by Huczko et al by combustion of magnesium/calcium oxalates. A bottom‐up approach like self‐assembly has also been employed for synthesis of 3DG .…”

Continuous and catalyst free synthesis of graphene sheets in thermal plasma jet

“…Graphene materials can be also synthesized via reduction of graphene oxides using (i) chemical reducers [18][19][20], (ii) electrochemical processes [21][22][23][24] and (iii) thermal routes [6,25]. Finally, graphene materials were also obtained via combustion synthesis [26][27][28].…”

Graphene‐Like Carbon Nanostructures From Combustion Synthesis

“…We showed earlier that SiC nanowires can be easily and autothermally formed in the Si/PTFE system . Carbon nanomaterials, including graphene‐related ones, were obtained via Mg and Si reduction of appropriate oxidants: CO x , C x N y H z , GO and CF x , C 2 H 2 O 4 , MgC 2 O 4 , and CaC 2 O 4 . Natural carbon‐bearing minerals (dolomite, limestone, siderite) can also be CS processed .…”

“…We showed elsewhere that such nanomaterial possesses interesting properties regarding the removal of organic compounds. [15] The reaction chamber is equipped with a polycarbonate observation port. From LSR (light signal registration) data one may calculate the combustion wave speed, reaction oscillations, and its kinetics via changes of normalize signal intensity.…”

“…The highly porous morphology of the purified raw nanoproduct (resulting from the acid etching of Mg/MgO/CaO components) is clearly seen with “punctured” (after leaching) petal‐like layered carbon nanostructures, clearly dominating the final product (E,F), along with the soot particles. We showed elsewhere that such nanomaterial possesses interesting properties regarding the removal of organic compounds …”