TY - JOUR
T1 - Trace cisplatin and carboplatin removal by 3-mercaptopropionic acid and L-cysteine functionalized sponges
T2 - Adsorption behaviour and mechanism
AU - Han, Dong
AU - López-Mesas, Montserrat
AU - Boada, Roberto
AU - Farías, Tania
AU - Lazo Fraga, Ana R.
AU - Valiente, Manuel
N1 - Publisher Copyright:
© 2023 The Author(s)
PY - 2023/9/15
Y1 - 2023/9/15
N2 - This study presents functionalized open-celled cellulose Metalzorb® sponge (Sponge) with 3-mercaptopropionic acid (MPA) and L-Cysteine (Cys), and the resulting MPA@Sponge and Cys@Sponge showed significantly improved removal efficiency towards trace cisplatin and carboplatin against Sponge. MPA@Sponge achieved maximum removal of 88.9 ± 0.5% for cisplatin and 85.2 ± 0.4% for carboplatin, while Cys@Sponge achieved maximum removal of 75 ± 2% and 59 ± 1%. In contrast, Sponge only achieved removal of 29 ± 4% and 4 ± 1%, respectively. It suggests that thiol groups serve as favourable binding sites for Pt complexation. Carboplatin exhibits lower adsorption compared to cisplatin due to its limited hydration. However, the presence of Cl− in stock and high temperature facilitate the hydration and the formation of active derivatives of carboplatin, thereby enhancing its adsorption. The rapid adsorption processes of cisplatin and carboplatin are well described by the pseudo-second-order kinetic model involving diffusion and chemisorption. The results from adsorption isotherms revealed a monolayer adsorption that aligns with the principles proposed by the Langmuir model. High temperature significantly enhances the adsorption, and the positive enthalpies indicate that the binding of Pt with thiol groups is endothermic process. X-ray absorption spectroscopy measurements at the Pt L3-edge revealed a similar coordination environment of the adsorbed Pt on both functionalized adsorbents, which can be attributed to the formation of four Pt-S bonds during the adsorption. To assess the validity of the adsorption results under realistic medium conditions, an adsorption study was carried out by using diluted urine spiked with trace platinum cytostatic drugs to simulate hospital wastewater. 90.2 ± 0.3% of cisplatin and 77.0 ± 0.2% of carboplatin was effectively removed by MPA@Sponge from diluted urine.
AB - This study presents functionalized open-celled cellulose Metalzorb® sponge (Sponge) with 3-mercaptopropionic acid (MPA) and L-Cysteine (Cys), and the resulting MPA@Sponge and Cys@Sponge showed significantly improved removal efficiency towards trace cisplatin and carboplatin against Sponge. MPA@Sponge achieved maximum removal of 88.9 ± 0.5% for cisplatin and 85.2 ± 0.4% for carboplatin, while Cys@Sponge achieved maximum removal of 75 ± 2% and 59 ± 1%. In contrast, Sponge only achieved removal of 29 ± 4% and 4 ± 1%, respectively. It suggests that thiol groups serve as favourable binding sites for Pt complexation. Carboplatin exhibits lower adsorption compared to cisplatin due to its limited hydration. However, the presence of Cl− in stock and high temperature facilitate the hydration and the formation of active derivatives of carboplatin, thereby enhancing its adsorption. The rapid adsorption processes of cisplatin and carboplatin are well described by the pseudo-second-order kinetic model involving diffusion and chemisorption. The results from adsorption isotherms revealed a monolayer adsorption that aligns with the principles proposed by the Langmuir model. High temperature significantly enhances the adsorption, and the positive enthalpies indicate that the binding of Pt with thiol groups is endothermic process. X-ray absorption spectroscopy measurements at the Pt L3-edge revealed a similar coordination environment of the adsorbed Pt on both functionalized adsorbents, which can be attributed to the formation of four Pt-S bonds during the adsorption. To assess the validity of the adsorption results under realistic medium conditions, an adsorption study was carried out by using diluted urine spiked with trace platinum cytostatic drugs to simulate hospital wastewater. 90.2 ± 0.3% of cisplatin and 77.0 ± 0.2% of carboplatin was effectively removed by MPA@Sponge from diluted urine.
KW - Adsorption
KW - Carboplatin
KW - Cisplatin
KW - Pt-based cytostatics
KW - Thiol-functionalization
KW - XAS
UR - http://www.scopus.com/inward/record.url?scp=85165428130&partnerID=8YFLogxK
UR - https://www.mendeley.com/catalogue/f5d6e8de-59c1-325c-81f0-21a59d2e8389/
U2 - 10.1016/j.cej.2023.144894
DO - 10.1016/j.cej.2023.144894
M3 - Article
AN - SCOPUS:85165428130
SN - 1385-8947
VL - 472
JO - Chemical Engineering Journal
JF - Chemical Engineering Journal
M1 - 144894
ER -