Interaction between graphene oxide and acetaminophen in water under simulated sunlight: Implications for environmental photochemistry of PPCPs

Abstract

In recent years, graphene oxide (GO) as a new carbon material has been widely investigated as adsorbent and catalyst. However, effects of GO on the micro-pollutants such as pharmaceuticals and personal care products (PPCPs) under sunlight remains unclear. In this study, the degradation of PPCPs in a simulated sunlight-GO photocatalytic system was systematically investigated. Specifically, GO rapidly degrade 95% of acetaminophen (APAP) within 10 min under simulated sunlight irradiation (λ ≥ 350 nm). The influencing factors such as APAP concentration, pH, GO dosage, water matrixes (Cl−, NO3−, HCO3−, SO42−, Ca2+, Fe3+and fulvic acid) were investigated. At a GO dosage of 100 mg L−1 and an initial pH of 7, the APAP (5 μM) photodegradation kinetic constant kobs was calculated to be 0.4547 min−1. In practical applications, the GO photocatalysis system still degrade over 90% APAP within 60 min in real surface water. The electron spin resonance and radical scavenging experiments revealed that the dominated active species for degrading APAP was photogenerated holes (h+), while other mechanisms (1O2 and O2•−/HO2•) played a minor role. Furthermore, the photochemical transformation of some other typical PPCPs were comparatively studied to reveal the relationship between degradation kinetics and molecular structure. Based on descriptive variables including molar refractive index parameter, octanol-water partition coefficient, dissociation constant and dipole moment, a quantitative structural-activity relationship (QSAR) model for predicting pseudo-first-order rate constants was established with a high significance (R2 = 0.996, p < 0.05). This study helps to understand the interaction between GO and PPCPs and its effects on the photochemical transformation of PPCPs in water.