TY - JOUR

T1 - Interaction between graphene oxide and acetaminophen in water under simulated sunlight: Implications for environmental photochemistry of PPCPs

AU - Zou, Yongrong

AU - Wang, Wenyu

AU - Wang, Hao

AU - Pan, Cong

AU - Xu, Jing

AU - Pozdnyakov, Ivan P.

AU - Wu, Feng

AU - Li, Jinjun

N1 - Funding Information: This work was supported financially by National Natural Science Foundation of China (No. 22061132001 , 42077350 , 21876137 ), and Russian Science Foundation (Grant RSF-NSFC No. 21-43-00004 ). The author appreciates helpful comments from the editors and reviewers. Publisher Copyright: © 2022 Elsevier Ltd

PY - 2023/1/1

Y1 - 2023/1/1

N2 - 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.

AB - 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.

KW - Graphene oxide

KW - Photochemical transformation

KW - Photooxidation of PPCPs

KW - QSAR

KW - Simulated sunlight

UR - http://www.scopus.com/inward/record.url?scp=85142141920&partnerID=8YFLogxK

UR - https://www.mendeley.com/catalogue/acd3fe40-2aff-316f-8ac8-5acf3341ccfd/

U2 - 10.1016/j.watres.2022.119364

DO - 10.1016/j.watres.2022.119364

M3 - Article

C2 - 36413833

AN - SCOPUS:85142141920

VL - 228

JO - Water Research

JF - Water Research

SN - 0043-1354

IS - Pt A

M1 - 119364

ER -