Paracetamol adsorption in acidic, neutral and basic media on three activated carbons with different chemistry surfaces was studied. A granular activated carbon (GAC) was prepared from coconut shell; starting from this sample, an oxidized activated carbon (GACo) was obtained by treating the GAC with a boiling solution of 6 M nitric acid, so to generate a greater number of oxygenated surface groups. In addition, a reduced activated carbon (GACr) was obtained by heating the GAC at 1173 K, to remove the oxygenated surface groups. Paracetamol adsorption was higher for GACr due to the lower presence of oxygenated surface functional groups. Moreover, adsorption was highest at neutral pH. The magnitude of the interactions between paracetamol molecules and activated carbons was studied by measuring the immersion enthalpies of activated carbons in solution of paracetamol at different concentrations and pH values and by calculating the interaction enthalpy. The highest value was obtained for GACr in a paracetamol solution of 1000 mg L−1 at pH 7, confirming that paracetamol adsorption is favoured on basic activated carbons at pH values near to neutrality. Finally, the Gibbs energy changes confirmed the latter result, allowing explaining the different magnitudes of the interactions between paracetamol and activated carbons, as a function of solution pH.
The adsorption of salicylic acid, acetaminophen, and methylparaben (pharmaceutical products derived from phenol) on carbons activated with different surface chemistries was carried out. We evaluated the effect of the physicochemical properties of the adsorbent and adsorbates on the adsorption capacity. A study of the adsorbate–adsorbent interactions via immersion calorimetry in the analytes solutions at different concentrations was included, in addition to the equilibrium data analysis. The results show that the pharmaceutical compounds (2.28–0.71 mmol g−1) have lower adsorption capacities in the activated carbon with the highest content of oxygenated groups (acids), while the activated carbons with amphoteric characteristics increase the capacities of adsorption (2.60–1.38 mmol g−1). This behavior may be associated with the increased affinity between the adsorbent and solvent due to the presence of polar groups, which was corroborated by the high immersion enthalpy value in water (ΔHimmH2O = −66.6 J g−1). The equilibrium data, adjusted to the Freundlich adsorption model, indicated that the heterogeneous adsorption processes involve immersion enthalpy values between −9.42 and −24.3 J g−1.
In this study, the mechanisms of methylparaben adsorption onto activated carbon (AC) are elucidated starting from equilibrium and thermodynamic data. Adsorption tests are carried out on three ACs with different surface chemistry, in different pH and ionic strength aqueous solutions. Experimental results show that the methylparaben adsorption capacity is slightly affected by pH changes, while it is significantly reduced in the presence of high ionic strength. In particular, methylparaben adsorption is directly dependent on the micropore volume of the ACs and the π- stacking interactions, the latter representing the main interaction mechanism of methylparaben adsorption from liquid phase. The equilibrium adsorption data are complemented with novel calorimetric data that allow calculation of the enthalpy change associated with the interactions between solvent-adsorbent, adsorbent-adsorbate and the contribution of the ester functional group (in the methylparaben structure) to the adsorbate–adsorbent interactions, in different pH and ionic strength conditions. It was determined that the interaction enthalpy of methylparaben-AC in water increases (absolute value) slightly with the basicity of the activated carbons, due to the formation of interactions with π- electrons and basic functional groups of ACs. The contribution of the ester group to the adsorbate-adsorbent interactions occurs only in the presence of phenol groups on AC by the formation of Brønsted–Lowry acid–base interactions.
Drugs are considered emerging pollutants from water sources and are
therefore considered to be of high toxicological risk to aquatic fauna.
Activated carbon adsorption is one of the methods approved by the
Word Health Organization to remove pharmaceutical compounds from water
in treatment plants due to its cost and easy implementation. This
study presents the modification of a commercial activated carbon by
heat treatment at 1073, 1173, and 1273 K. The impact of the physicochemical
changes of the adsorbent on the adsorption capacity of salicylic acid
and methylparaben, compounds derived from phenol, was studied. Finally,
the adsorbate–adsorbent interactions are evaluated through
immersion calorimetry. It is observed that at 1173 K, activated carbon
increases its surface area by 29%. At higher temperatures, the surface
area drops to 21%. In the activated carbon subjected to heat treatment
at 1173 K, it increases the adsorption capacity of salicylic acid
and methylparaben by 24 and 34%, respectively, compared to activated
carbons subjected to higher temperatures. The interaction enthalpies
(adsorbate–adsorbent interaction) have values between −12
and 5 J g–1.
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