Synthesis of Graphene-Based Nanocomposites for Environmental Remediation Applications: History
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Rohit Goyat
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Yajvinder Saharan
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Joginder Singh
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Ahmad Umar
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Sheikh Akbar

The term graphene was coined using the prefix “graph” taken from graphite and the suffix “-ene” for the C=C bond, by Boehm et al. in 1986. The synthesis of graphene can be done using various methods. The synthesized graphene was further oxidized to graphene oxide (GO) using different methods, to enhance its multitude of applications. Graphene oxide (GO) is the oxidized analogy of graphene, familiar as the only intermediate or precursor for obtaining the latter at a large scale. Graphene oxide has recently obtained enormous popularity in the energy, environment, sensor, and biomedical fields and has been handsomely exploited for water purification membranes. GO is a unique class of mechanically robust, ultrathin, high flux, high-selectivity, and fouling-resistant separation membranes that provide opportunities to advance water desalination technologies. The facile synthesis of GO membranes opens the doors for ideal next-generation membranes as cost-effective and sustainable alternative to long existing thin-film composite membranes for water purification applications. 

  • graphene
  • synthesis process
  • polymeric membranes
  • environmental remediation
  • composites

1. Introduction

Graphene is a purified form of graphite that recently gained enormous popularity in the energy [1][2][3], environment [4][5][6][7][8], membranes [1][7], sensor [9][10][11][12], and biomedical fields [13][14][15][16][17][18][19][20][21][22][23][24][25][26]. It is a sp2 hybridized, hexagonally arranged, chain of polycyclic aromatic hydrocarbon with a honeycomb crystal lattice [27]. It is the most recent element of carbon allotropes and is actually the basic building block of other important carbon allotropes, including 3D graphite, 1D carbon nanotubes (CNTs), and 0D fullerene (C60), as shown in Figure 1.
Molecules 27 06433 g001 550
Figure 1. Structural representation of 2D graphene with different dimensions. [Reprinted with permission from ref. [28], Wan, X., Huang, Y., & Chen, Y. (2012). Focusing on energy and optoelectronic applications: a journey for graphene and graphene oxide at large scale. Accounts of chemical research, 45(4), 598–607. Copyright © American Chemical Society].
The name graphene was coined by Boehm in 1986 [1], taking the prefix “graph” from graphite and the suffix “-ene” for sp2 hybridized carbon, and was finally accepted by the International Union for Pure and Applied Chemistry in 1997 [29][30][31][32][33]. Furthermore, it became famous worldwide in 2004 when Geim and Novoselov obtained a single sheet of graphene on solid support, for which they were honored with the Nobel Prize in Physics in 2010 [34]. The main achievements of graphene in a timeline of history from 1840 to 2018 are shown in Figure 2.
Molecules 27 06433 g002 550
Figure 2. Schematic representation of a graphene timeline.

2. General Methods of Graphene Synthesis

Generally, graphene can be synthesized using two different routes, viz, bottom-up and top-down [33][35][36], as depicted in Figure 3.
Molecules 27 06433 g003 550
Figure 3. Schematic representation of the general methods for graphene synthesis.

3. Graphene Oxide (GO)

In comparison to graphene, graphene oxide is considered a more versatile and advanced material. GO has a broad range of oxygen containing functional groups such as carboxyl, hydroxyl, epoxy, carbonyl, and keto groups on its surface.
GO has shown great potential in a variety of fields by virtue of its high surface area [37], unique mechanical strength [38], and excellent optical and magnetic properties [39]. In comparison to other carbon-based nanomaterials, GO is considered a green oxidant, as it is enriched with oxygen-containing functional groups [40][41]. Further, GO has an aromatic scaffold, which acts as a template to anchor active species behaving as an organo-catalyst [42][43]. 

3.1. Synthesis of GO

In 1840, German scientist Schafhacutl was given the first report on the synthesis of graphene oxide and graphite intercalated compounds [44]. For the very first time, he attempted to exfoliate graphite and tried to purify impure graphite “kish” from iron smelters [27]. To date, several methods, as shown in Table 1, have been proposed.
Table 1. List of different methods used to synthesize graphene oxide.
Methods Year Starting Material Different Oxidants Used Reaction Time for GO Synthesis Temperature °C Features References
Brodie 1859 Graphite KclO3, HNO3 3–4 days 60 First attempt to synthesize GO [45]
Staudenmaier 1898 Graphite KclO3, H2SO4, HNO3 96 h Room temperature Improved efficiency [46]
Hummers 1958 Graphite KmnO4, H2SO4, NaNO3 <2 h <20–35–98 Water-free, less than 2 h of reaction time [47]
Fu 2005 Graphite KmnO4, H2SO4, NaNO3 <2 h 35 Validation of NaNO3 [48]
Shen 2009 Graphite Benzoyl peroxide 10 min 110 Fast and non-acidic [49]
Su 2009 Graphite KmnO4, H2SO4 4 h Room temperature Large-size GO sheets formed [50]
Marcano and Tour 2010 & 2018 Graphite KmnO4, H3PO4, H2SO4 12 h 50 Eco-friendly resulting in a high yield [51]
Sun 2013 Graphite KmnO4, H2SO4 1.5 h Room temperature-90 High-yield and safe method [52]
Eigler 2013 Graphite KmnO4, NaNO3, H2SO4 16 h 10 High-quality GO produced [53]
Chen 2015 Graphite KmnO4, H2SO4 <1 h 40–95 High-yield product [54]
Panwar 2015 Graphite H2SO4, H3PO4, KmnO4, HNO3 3 h 50 Three component acids and high-yield product [55]
Peng 2015 Graphite K2FeO4, H2SO4 1 h Room temperature Results in a high-yield and eco-friendly method [56]
Rosillo-Lopez 2016 Graphite HNO3 20 h Room temperature Nano-sized GO obtained [57]
Yu 2016 Graphite K2FeO4, KmnO4 H2SO4, H3BO3 (NH4)2S2O8 5 h <5–35–95 Low manganite impurities and high yield obtained [58]
Dimiev 2016 Graphite 98% H2SO4, fuming H2SO4 3–4 h Room temperature 25 nm thick and ~100%conversion rate [59]
Pei 2018 Graphite foil H2SO4 <5 min Room temperature High efficiency [60]
Ranjan 2018 Graphite H2SO4, H3PO4, KmnO4 <24 h <RT-35–95 Cooled exothermal reaction to make the process
safe		 [61]
The most preferred methods are Brodie [45], Staudenmaier [46], and Hummers [47], as shown in Figure 4. From these familiar methods, a number of variations have been derived to improve the overall yield and quality of the GO. In 1859, Brodie used graphite as the starting material for the synthesis of graphene oxide (GO). In his experimental work, he used KclO4 (strong oxidizing agent) along with nitric acid and heated the content at 60 °C for 3–4 days [45]. The GO obtained was soluble in pure or basic water. The chemical composition showed mainly carbon, oxygen, and hydrogen with the general formula C11H4O5. After nearly four decades, in 1898, Staudenmaier and Hoffmann modified Brodie’s method and trimmed down the reaction time of graphene oxide synthesis from 4 days to 2 days [46]. The nitric acid used in Brodie method was also replaced with sulfuric acid, which further reduced the liberation of toxic gases such as NO2 or N2O4.
Molecules 27 06433 g011 550
Figure 4. Schematic representation of the synthesis of graphene oxide with different methods.
In 1958, Hummer reduced the reaction time from 2 days to 12 h by using KmnO4 as the oxidizing agent instead of KclO4, followed by the addition of sodium nitrate, but the problem of toxic gases still remains a challenge [47]. Further, in 2010, at Rice University, Tour’s group [51] replaced sodium nitrate with phosphoric acid and increased the amount of KmnO4. This improvement made the process eco-friendly, as it completely stops the release of toxic gases such as NO2, N2O4 or ClO2, along with easy temperature control and better yield [51]. In addition to this, the GO suspension obtained was treated with hydrogen peroxide (H2O2) to eliminate all impurities due to permanganate and manganese dioxide.
Furthermore, the final color of the product GO varies from army green to light yellow, depending on the carbon-to-oxygen ratios [62], as depicted in Table 2.
Table 2. Effect of acid concentration, reaction temperature, reaction time, and the quantity of the oxidizing agent on the oxidation of graphene [62].
S. No. Source of Carbon H2SO4
(in mL)		 Other Ingredients Temp.
(in °C)		 Time
(in h)		 C:O Colour of GO Obtained
1 Graphite 15.0 1.0 g Na2Cr2O7 30 72 16:1 Black
2 Graphite 15.0 4.0 g Na2Cr2O7 30 72 3.4:1 Black
3 Graphite 15.0 15.0 mL 70% HNO3
3.0 g KmnO4,		 30 24 -- Black
4 Graphite 20.0 11.0 g KclO3,
10.0 mL 70% HNO3		 0–60 33 3.1:1 Midnight green
5 Graphite 30.0 3.0 g KmnO4,1.0 g
NaNO3		 30 2 3.0:1 Bluish green
6 Graphite 30.0 3.0 g KmnO4,1.0 g
NaNO3		 45 1 -- Green
7 Graphite 22.5 3.0 g KmnO4,1.0 g
NaNO3		 45 1 -- Brittle yellow
8 Graphite 22.5 3.0 g KmnO4,0.5 g
NaNO3		 45 1 -- Yellow
9 Graphite 22.5 3.0 g KmnO4,0.5 g
NaNO3		 45 0.5 2.3:1 Yellow
10 Graphite 22.5 3.0 g KmnO4,0.5 g
NaNO3		 35 0.5 2.05:1 Bright yellow
11 Graphite 22.5 3.0 g KmnO4, 1.0 g
fuming HNO3		 35 1 -- Bright yellow
12 Graphite 22.5 3.0 g KmnO4, 1.0 g
BaNO3		 45 2 -- Light green

3.2. Structural Aspects of GO

Various structural models of GO, as shown in Figure 5, have been proposed and were refined over the years by the advancement of characterization techniques and technologies. The structural history of GO started in 1936, when Hofmann and Rudolf [63] proposed the first structure of GO in which epoxy groups were unsystematically spotted over the graphene sheets, and then in 1946, Ruess [64] restructured the Hofmann model by introducing hydroxyl moieties and the alternation of the basal plane structure from an sp2 to an sp3 hybridized carbon system.
Molecules 27 06433 g012 550
Figure 5. Schematic representation of the year-wise progress in proposed structures of graphene oxide [63][64][65][66][67][68][69][70].
Scholz and Boehm in 1969 [65] proposed a GO structure that was less ordered, having C=C and periodically cleaved C-C bonds within the channeled carbon layers labeled with carbonyl and hydroxyl groups. Further, in 1994, Nakajima and Matsuo [66] presented a graphite intercalation compound (GIC) to look like a lattice framework. Adding to the history, in 1998, Lerf and Klinowski et al. (L–K model) [67][68] proposed a uniform carbon lattice framework GO structure with randomly distributed benzene rings having attached epoxides, carboxyl, and hydroxyl groups. Thereafter, in 2006, Szabó and coworkers [69] put forward a carboxylic-acid-free model comprising two distinct domains: a trans-linked cyclohexyl species interspersed with tertiary alcohols, 1,3-ethers, and a keto/quinoidal species corrugated network. Even closer to the present time, in 2018, Liu et al. [70] experimentally noticed oxygen bonding and evidenced the C=O bonds on the edge and plane of GO, confirming parts of earlier proposed models, especially the L–K model.
Among the above-discussed models from 1936 to 2018, the L–K model has been accepted the most, due to good interpretability over the majority of experimental observations and the ease of further adaption and modification.

3.3. Characterization of GO

In order to authenticate the synthesis of GO and to analyze its chemical configuration, a range of characterization techniques have been employed by numerous research groups. For example, in order to achieve the information of size and surface morphology of graphene oxide, SEM, TEM, and AFM were used abroad [71][72][73][74][75]. With respect to the elemental analysis of graphene oxide, quantitative XPS, EDX, and inductively coupled plasma mass spectrometry (ICP-MS) were utilized generally [76][77][78][79][80][81][82][83][84]. Additionally, Raman spectra, XRD, and FTIR spectra are widely used to point out the graphene oxide chemical structure [84][85][86][87][88]. 

This entry is adapted from the peer-reviewed paper 10.3390/molecules27196433

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