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. 2023 Dec 9;8(50):48181-48190.
doi: 10.1021/acsomega.3c07119. eCollection 2023 Dec 19.

Insights on the Synthesis of Al-MCM-41 with Optimized Si/Al Ratio for High-Performance Antibiotic Adsorption

Vinicius M S Macedo  1 , Eliezer L Gomes  2 , Juan C Moreno-Piraján  3 , Liliana Giraldo  4 , Laura P Tovar  2 , Sarah I P M N Alves  5 , Luís A M Ruotolo  6 , Romilda Fernandez-Felisbino  2
Affiliations

Insights on the Synthesis of Al-MCM-41 with Optimized Si/Al Ratio for High-Performance Antibiotic Adsorption

Vinicius M S Macedo et al. ACS Omega. .

Abstract

Studies indicate that approximately two-thirds of the rivers of the world are contaminated by pharmaceutical compounds, especially antibiotics and hormones. Data reported by the World Health Organization (WHO, 2015) revealed an increase of 65% in antibiotic consumption between 2000 and 2015, with a worldwide increase of 200% expected up to 2030. Environmental contamination by antibiotics and their metabolites can cause the alteration of bacterial genes, leading to the generation of superbacteria. In this work, adsorption was explored as a strategy to mitigate antibiotic contamination, proposing the use of the Al-MCM-41 mesoporous material as an efficient and high-capacity adsorbent. Evaluation of the influence of the synthesis parameters enabled understanding of the main variables affecting the adsorption capacity of Al-MCM-41 for the removal of a typical antibiotic, amoxicillin (AMX). It was found that the adsorbent composition and specific surface area were the main factors that should be optimized in order to obtain the highest AMX removal capacity. Using statistical tools, the best Si/Al ratio in Al-MCM-41 was found to be 10.5, providing an excellent AMX uptake of 132.2 mg per gram of adsorbent. The Si/Al ratio was the most significant factor affecting the adsorption. The cation-π interactions increased with an increase of the Al content, while the interactions involving silanols (Yoshida H-bonding and dipole-dipole hydrogen bridges) decreased.

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Conflict of interest statement

The authors declare no competing financial interest.

Figures

Figure 1
Figure 1
Diffractograms of the calcined Al-MCM-41 samples obtained using Si/Al ratios of (a) 16.1 and (b) 5.0 and 10.5 (S-CP).
Figure 2
Figure 2
(a) N2 adsorption–desorption isotherms for samples S-1, S-2, S-3, and S-8. Liquid N2 (at 77 K), in the relative pressure range from 0.06 to 0.97; (b) FTIR absorption spectra for samples S-2, S-9, S-8-AMX, and S-2-AMX.
Figure 3
Figure 3
TG (a) and DTG (b) curves for the synthesized samples.
Figure 4
Figure 4
(a) AMX uptake on sample S-8 (Si/Al = 16.1), as a function of contact time (C0 = 200 mg AMX L–1); (b) adsorption isotherm for the S-CP sample. Adsorption conditions: pH 5.0 and 25 °C.
Figure 5
Figure 5
Pareto charts of the standardized effects (p = 0.05) for (a) %R and (b) qe.
Figure 6
Figure 6
AMX adsorption capacities at equilibrium (C0 = 200 mg L–1, pH 5.0, and 25 °C).
Figure 7
Figure 7
Schematic illustration of the Al-MCM-41 aluminosilicate framework. (Adapted with permission from Naik et al., 2010. Copyright 2023 Elsevier).
Figure 8
Figure 8
3D dimensions of the AMX molecule (a), speciation (b), and interactions with the Al-MCM-41 surface (c).
See this image and copyright information in PMC

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