GTS-UAB Research Group, Department of Chemistry, Faculty of Science, Universitat Autònoma de Barcelona, Bellaterra, (Cerdanyola del Vallès), 08193 Barcelona, Spain.
Faculty of Chemistry, University of Havana, 10400 Havana, Cuba.
Sci Total Environ. 2023 Sep 15;891:164385. doi: 10.1016/j.scitotenv.2023.164385. Epub 2023 May 25.
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 PtCl 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 PtCl 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 PtCl 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.
为了有效去除水中痕量铂类细胞毒性药物（Pt-CDs），本研究对比考察了三种商业吸附剂（巯基化硅胶（Si-Cys）、二乙烯三胺基丙基化硅胶（Si-DETA）和开孔纤维素 MetalZorb®海绵（Sponge））对顺铂和卡铂的吸附行为。研究内容涵盖了 pH 依赖性、吸附动力学、吸附等温线和吸附热力学等方面。此外，还通过与 PtCl 的对比研究，深入了解了吸附机制。研究结果表明，Si-Cys 对顺铂和卡铂的吸附效果明显优于 Si-DETA 和 Sponge，这表明在螯合主导的化学吸附中，巯基为 Pt(II) 配合物提供了高亲和性的结合位点。阴离子 PtCl 的吸附对 pH 的依赖性更强，通常优于顺铂和卡铂，这得益于与质子化表面的离子缔合贡献。水溶液中 Pt(II) 化合物的去除过程是通过溶液中配合物的水解和随后的吸附来实现的，而特定的吸附过程可以通过离子缔合和螯合机制的协同作用来解释。快速的吸附过程涉及扩散和化学吸附，这一过程可以很好地用伪二阶动力学模型来描述。等温线研究表明，单层吸附符合 Langmuir 模型。从吸附焓的结果可以看出，顺铂和卡铂与巯基的螯合是一个吸热反应，而 PtCl 的吸附是放热的。在 343 K 下，Si-Cys 对顺铂和卡铂的去除率分别达到 98.5±0.1%和 94.1±0.1%。为了验证所获得的结果，该方法被应用于含有 Pt-CDs 的尿液样品（作为医院废水的模拟物）的处理中，结果表明，当使用 Si-Cys 作为吸附剂时，去除效率非常高，范围在 72±1%到 95±1%之间，尽管观察到有限的基质效应。
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