Comparative study on removal of platinum cytostatic drugs at trace level by cysteine, diethylenetriamino functionalized Si-gels and polyethyleneimine functionalized sponge : Adsorption performance and mechanisms
Han, Dong (Universitat Autònoma de Barcelona. Departament de Química)
López-Mesas, Montserrat (Universitat Autònoma de Barcelona. Departament de Química)
Luaces, Markel (University of Havana)
Enamorado, Yusleydi (University of Havana)
Sanadar, Martina (Università di Udine)
Melchior, Andrea (Università di Udine)
Valiente Malmagro, Manuel (Universitat Autònoma de Barcelona. Departament de Química)

Fecha:	2023
Resumen:	To efficiently remove trace Pt-based cytostatic drugs (Pt-CDs) from aqueous environments, a comparative investigation was conducted on the adsorption behavior of three commercial adsorbents including cysteine-functionalized silica gel (Si-Cys), 3-(diethylenetriamino) propyl-functionalized silica gel (Si-DETA) and open-celled cellulose MetalZorb® sponge (Sponge). The research on the adsorption of cisplatin and carboplatin encompasses investigations of pH dependence, adsorption kinetics, adsorption isotherms, and adsorption thermodynamics. The obtained results were compared with those of PtCl42− to better understand the adsorption mechanisms. The adsorption of cisplatin and carboplatin by Si-Cys was significantly better than Si-DETA and Sponge, which suggested that in chelation-dominated chemisorption, thiol groups provided high-affinity sites for Pt(II) complexation. Adsorption of the anion PtCl42− was more pH dependent and generally superior to that of cisplatin and carboplatin, benefiting from the contribution of ion association with protonated surfaces. The removal process of aqueous Pt(II) compounds occurred by the hydrolysis of complexes in solution and subsequent adsorption, and the specific adsorption process was explained by the synergistic action of ion association and chelation mechanisms. The rapid adsorption processes involving diffusion and chemisorption were well described by pseudo-second-order kinetic model. The isotherm studies suggested monolayer adsorption, consistent with the Langmuir model. Indicated from the adsorption enthalpy results, the chelation of cisplatin and carboplatin with thiol groups was an endothermic reaction, while the adsorption of PtCl42− was exothermic. At 343 K, Si-Cys achieved 98. 5 ± 0. 1 % (cisplatin) and 94. 1 ± 0. 1 % (carboplatin) removal. To validate the obtained findings, the described process was applied to urine samples doped with Pt-CDs as analog of hospital wastewaters and the removal was very efficient, ranging from 72 ± 1 % to 95 ± 1 %, when using Si-Cys as adsorbent, although limited matrix effects were observed.
Ayudas:	European Commission 778266
Nota:	Altres ajuts: acords transformatius de la UAB
Derechos:	Aquest document està subjecte a una llicència d'ús Creative Commons. Es permet la reproducció total o parcial, la distribució, la comunicació pública de l'obra i la creació d'obres derivades, sempre que no sigui amb finalitats comercials, i sempre que es reconegui l'autoria de l'obra original.
Lengua:	Anglès
Documento:	Article ; recerca ; Versió publicada
Materia:	Platinum cytostatics ; Adsorption ; Cisplatin ; Carboplatin ; Functionalized adsorbents
Publicado en:	Science of the total environment, Vol. 891 (September 2023) , art. 164385, ISSN 1879-1026

DOI: 10.1016/j.scitotenv.2023.164385
PMID: 37244605

11 p, 2.0 MB

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