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Fabrication and application of composite adsorbents made by one-pot electrochemical exfoliation of graphite in surfactant ionic liquid/nanocellulose mixtures

Jamaluddin NA, Mohamed A, Bakar SA, Ardyani T, Sagisaka M, Saito H, et al.

Phys Chem Chem Phys, 2021 Sep 15;23(35):19313-19328.
PMID: 34524298 DOI: 10.1039/d1cp02206g

Previously, surfactant-assisted exfoliated graphene oxide (sEGO) formed with the triple-chain surfactant TC14 (sodium 1,4-bis(neopentyloxy)-3-(neopentylcarbonyl)-1,4-dioxobutane-2-sulfonate) was applied in wastewater treatment. The extent of dye-removal and the adsorption capacity of the sEGO formed with this triple-chain surfactant outperformed those of two other systems, namely, the di-chain version of TC14 (AOT14; sodium 1,2-bis-(2,2-dimethyl-propoxycarbonyl)-ethanesulfonate) and the single-chain surfactant sodium n-dodecylsulfate. In the present study, to further optimise the surfactant chemical structure, the sodium ion of TC14 was substituted with 1-butyl-3-methyl-imidazolium (BMIM) generating surfactant ionic liquids (SAILs; 1-butyl-3-imidazolium 1,4-bis(neopentyloxy)-3-(neopentyloxycarbonyl)-1,4-dioxobutane-2-sulfonate), hereafter denoted as BMIM-TC14. This SAIL, together with nanofibrillated kenaf cellulose (NFC), was used to electrochemically exfoliate graphite, yielding BMIM-TC14 sEGO/NFC composites. These highly hydrophobic polymer composites were then used for the removal of methylene blue (MB) from aqueous solution. 1H NMR spectroscopy was used to elucidate the structure of the synthesised SAILs. The morphologies of the resulting nanocomposites were investigated using Raman spectroscopy, field-emission scanning electron microscopy, and high-resolution transmission electron microscopy. Analysis using small-angle neutron scattering was performed to examine the aggregation behaviour of sEGO and custom-made SAILs. Zeta potential, surface tension, and dynamic light-scattering measurements were used to study the aqueous properties and colloidal stability of the suspension. Amongst the surfactants tested, BMIM-TC14 sEGO/NFC exhibited the highest MB adsorption ability, achieving 99% dye removal under optimum conditions. These results highlight the importance of modifying the hydrophilic moieties of amphiphilic compounds to improve the performance of sEGO/NFC composites as effective adsorbents for wastewater treatment.
Preparation of conductive cellulose paper through electrochemical exfoliation of graphite: The role of anionic surfactant ionic liquids as exfoliating and stabilizing agents

Mohamed A, Ardyani T, Bakar SA, Sagisaka M, Umetsu Y, Hussin MRM, et al.

Carbohydr Polym, 2018 Dec 01;201:48-59.
PMID: 30241844 DOI: 10.1016/j.carbpol.2018.08.040

A facile electrochemical exfoliation method was established to efficiently prepare conductive paper containing reduced graphene oxide (RGO) with the help of single chain anionic surfactant ionic liquids (SAILs). The surfactant ionic liquids are synthesized from conventional organic surfactant anions and a 1-butyl-3-methyl-imidazolium cation. For the first time the combination of SAILs and cellulose was used to directly exfoliate graphite. The ionic liquid 1-butyl-3-methyl-imidazolium dodecylbenzenesulfonate (BMIM-DBS) was shown to have notable affinity for graphene, demonstrating improved electrical properties of the conductive cellulose paper. The presence of BMIM-DBS in the system promotes five orders of magnitude enhancement of the paper electrical conductivity (2.71 × 10-5 S cm-1) compared to the native cellulose (1.97 × 10-10 S cm-1). A thorough investigation using electron microscopy and Raman spectroscopy highlights the presence of uniform graphene incorporated inside the matrices. Studies into aqueous aggregation behavior using small-angle neutron scattering (SANS) point to the ability of this compound to act as a bridge between graphene and cellulose, and is responsible for the enhanced exfoliation level and stabilization of the resulting dispersion. The simple and feasible process for producing conductive paper described here is attractive for the possibility of scaling-up this technique for mass production of conductive composites containing graphene or other layered materials.
Surfactants with aromatic headgroups for optimizing properties of graphene/natural rubber latex composites (NRL): Surfactants with aromatic amine polar heads

Ardyani T, Mohamed A, Bakar SA, Sagisaka M, Umetsu Y, Mamat MH, et al.

J Colloid Interface Sci, 2019 Jun 01;545:184-194.
PMID: 30878784 DOI: 10.1016/j.jcis.2019.03.012

HYPOTHESIS: The compatibility of surfactants and graphene surfaces can be improved by increasing the number of aromatic groups in the surfactants. Including aniline in the structure may improve the compatibility between surfactant and graphene further still. Surfactants can be modified by incorporating aromatic groups in the hydrophobic chains or hydrophilic headgroups. Therefore, it is of interest to investigate the effects of employing anilinium based surfactants to disperse graphene nanoplatelets (GNPs) in natural rubber latex (NRL) for the fabrication of electrically conductive nanocomposites.
EXPERIMENTS: New graphene-philic surfactants carrying aromatic moieties in the hydrophilic headgroups and hydrophobic tails were synthesized by swapping the traditional sodium counterion with anilinium. 1H NMR spectroscopy was used to characterize the surfactants. These custom-made surfactants were used to assist the dispersion of GNPs in natural rubber latex matrices for the preparation of conductive nanocomposites. The properties of nanocomposites with the new anilinium surfactants were compared with commercial sodium surfactant sodium dodecylsulfate (SDS), sodium dodecylbenzenesulfonate (SDBS), and the previously synthesized aromatic tri-chain sodium surfactant TC3Ph3 (sodium 1,5-dioxo-1,5-bis(3-phenylpropoxy)-3-((3phenylpropoxy)carbonyl) pentane-2-sulfonate). Structural properties of the nanocomposites were studied using Raman spectroscopy, field emission scanning electron microscopy (FESEM), and high-resolution transmission electron microscopy (HRTEM). Electrical conductivity measurements and Zeta potential measurements were used to assess the relationships between total number of aromatic groups in the surfactant molecular structure and nanocomposite properties. The self-assembly structure of surfactants in aqueous systems and GNP dispersions was assessed using small-angle neutron scattering (SANS).
FINDINGS: Among these different surfactants, the anilinium version of TC3Ph3 namely TC3Ph3-AN (anilinium 1,5-dioxo-1,5-bis(3-phenylpropoxy)-3-((3phenylpropoxy)carbonyl) pentane-2-sulfonate) was shown to be highly efficient for dispersing GNPs in the NRL matrices, increasing electrical conductivity eleven orders of magnitude higher than the neat rubber latex. Comparisons between the sodium and anilinium surfactants show significant differences in the final properties of the nanocomposites. In general, the strategy of increasing the number of surfactant-borne aromatic groups by incorporating anilinium ions in surfactant headgroups appears to be effective.
Field data on pre-season rice straw degradation using a microbial substrate and the effects on methane emissions during rice cultivation

Jumat F, Rahman MHA, Bakar SA, Shakri NA, Kamaruzaman R, Bakar NAA, et al.

Data Brief, 2023 Aug;49:109383.
PMID: 37600135 DOI: 10.1016/j.dib.2023.109383

Rice straw is one of the most abundant biomass wastes derived from rice cultivation activities. The current rice straw management practice during the wet (rainy) season in Malaysia involves the integration of straw into the soil. This practice offers both advantages and disadvantages to rice farmers and the environment. Straw integration may improve nutrient availability while concurrently causing high greenhouse gas (GHG) emissions due to the increase in soil carbon activity. In this work, the use of microbial substrate to enhance the degradation of straw was compared to an existing technique that used no additional inputs during soil integration. The data collected consisted of overall microbial enzyme production, soil organic carbon, soil nitrogen content, seasonal greenhouse gas emissions, plant characteristics, and crop yield. In brief, these data can be used as means of demonstrating the effects of improved straw degradation during the pre-season on the overall GHG emissions during the planting season.