Efficient adsorption of chloroquine phosphate by a novel sodium alginate/tannic acid double-network hydrogel in a wide pH range

Abstract

In this work, a novel double-network composite hydrogel (SA/TA), composed of sodium alginate (SA) and tannic acid (TA), was designed and fabricated by a successive cross-linking method using Ti(IV) and Ca(II) as crosslinkers. SA/TA exhibited reinforced mechanical strength and anti-swelling properties because of the double-network structure. SA/TA was used as an adsorbent for removal of a popular antiviral drug, chloroquine phosphate (CQ), in water. The adsorption performance of SA/TA was systematically investigated, to study various effects including those of TA mass content, solution pH, adsorption time, and initial CQ concentration. Adsorption was also examined in presence of inorganic and organic coexisting substances commonly found in wastewater, and under different actual water samples. Batch experimental results indicated that SA/TA could maintain higher and more stable CQ uptakes within a wide solution pH range from 3.0 to 10.0, compared to its precursor, SA hydrogel, owing to the addition of TA-Ti(IV) coordination network. The maximum experimental CQ uptake exhibited by the 1:1 (by wt) SA/TA (SA/TA2) was as high as 0.699 mmol/g at the initial pH of 9.0. A high concentration of coexisting NaCl evidently reduced the CQ uptakes of SA/TA2 due to the electrostatic shielding effect, moreover, divalent cations including Ca(II) and Mg(II) also inhibited the adsorption of CQ due to competitive adsorption. However, humic acid had little effect on this adsorption. Considering the apparent adsorption performance, the aforementioned effects of various factors and the spectroscopic characterizations, multi-interactions are suggested for adsorption including chelation, electrostatic interactions, π-π electron donor-acceptor interaction and hydrogen bonding. SA/TA showed a slight loss in adsorption capacity toward CQ and sustained physicochemical structural stability, even after six adsorption–desorption cycles. In addition to CQ, SA/TA could be efficiently used for adsorption of two other antivirus drugs, namely, hydroxychloroquine sulfate and oseltamivir phosphate. This work provides an effective strategy for the design and fabrication of novel adsorbents that can effectively adsorb antiviral drugs over a wide pH range.