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<p>Liquid-phase exfoliation (LPE) is a process frequently used to overcome the interactions between layers in layered materials
to produce small sheets of material, with remarkable properties and high value applications. Materials are prepared via
direct or indirect sonication in a solvent that must be able to effectively disperse and stabilize the sheets produced.
Unfortunately, the preferred solvents for exfoliation processes are often toxic and possess several health risks. In this work,
we show that LPE in greener solvents can be used to access nanostructures of biochar and further improve the applications
of this renewable and bio-based material. Herein, pristine and oxidized biochars prepared from hardwood and softwood
biomass waste (e.g. sludge, bark, and sawdust) are exfoliated in a range of solvents to allow the identification of benign
alternatives that could afford highly concentrated dispersions. The majority of biochar nanostructures produced after
exfoliation are stacked nanosheets containing between 2-8 layers (average 15 nm thickness). Correlations between
effective LPE of biochar in solvents and different solvent parameters, including Kamlet-Taft, were established and allowed
greener solvents to be used. Surface modification of biochars (e.g. via oxidation) has potential to increase their dispersibility
in more benign solvents. LPE of oxidized biochars is more efficient in hydrogen-bond accepting solvents due to the
increased concentration of carboxylic acid and alcohol functional groups on the surface of particles, when compared to non-
functionalized biochars. Dispersions containing 0.20-0.75 mg/mL exfoliated oxidized biochar were obtained in solvents such
as polyethylene glycols, glycerol formal and e-caprolactone. Moreover, LPE of pristine biochars in dimethyl carbonate, ethyl
acetate, and solketal gave similar yields to more commonly used solvent for this process, N-methyl-2-pyrrolidone (NMP) a
known reprotoxic molecule.
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