Simultaneous degradation of trace antibiotics in water by adsorption and catalytic oxidation induced by N-doped reduced graphene oxide (N-rGO): synergistic mechanism

Aimed at current difficulties in the treatment of trace antibiotics in water, an adsorption-catalytic oxidation system was established by combining persulfate and graphene, which have the dual functions of adsorption and catalysis, for simultaneous enrichment and degradation of trace antibiotics in...

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Main Authors: Nan Wu, Xuemin Zhang, Xue Zhang, Kai Yang, Yanjuan Li
Format: Article
Language:English
Published: IOP Publishing 2022-01-01
Series:Materials Research Express
Subjects:
Online Access:https://doi.org/10.1088/2053-1591/ac7284
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author Nan Wu
Xuemin Zhang
Xue Zhang
Kai Yang
Yanjuan Li
author_facet Nan Wu
Xuemin Zhang
Xue Zhang
Kai Yang
Yanjuan Li
author_sort Nan Wu
collection DOAJ
description Aimed at current difficulties in the treatment of trace antibiotics in water, an adsorption-catalytic oxidation system was established by combining persulfate and graphene, which have the dual functions of adsorption and catalysis, for simultaneous enrichment and degradation of trace antibiotics in water. The experimental results showed that over 90% sulfamethoxazole could be degraded by the proposed system. The activation energy of the proposed system was 7.9 kJ mol ^−1 , which was significantly lower than those of typical Co catalysts and some carbon-based catalysts. Synergistic effect analysis revealed that catalytic oxidation was the key degradation kinetic of the proposed system, while adsorption showed a significant enhancement effect. Specifically, a compound with large adsorption capacity tended to be degraded preferably and rapidly. Characterization results indicated that N atoms were doped into the graphene framework, resulting in significant impacts on the activation process of potassium bisulfate by activating the sp ^2 C system. Quenching and free radical trapping experiments revealed that degradation catalyzed by the proposed system was a non-free radical oxidation reaction dominated by singlet oxygen. In summary, the proposed design was rational, N-rGO surface provided good adsorption and catalysis sites, the synergistic effect of adsorption and catalytic oxidation led to rapid and effective enrichment and in situ degradation of trace antibiotics in water.
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spelling doaj.art-581cbd58d5db49e7baf234f4f78d625a2023-08-09T16:13:51ZengIOP PublishingMaterials Research Express2053-15912022-01-019606560110.1088/2053-1591/ac7284Simultaneous degradation of trace antibiotics in water by adsorption and catalytic oxidation induced by N-doped reduced graphene oxide (N-rGO): synergistic mechanismNan Wu0https://orcid.org/0000-0001-9544-7638Xuemin Zhang1Xue Zhang2Kai Yang3Yanjuan Li4Key Laboratory of Yellow River Water Environment in Gansu Province, Lanzhou Jiaotong University , Lanzhou 730070, People’s Republic of China; School of Environment and Municipal Engineering, Lanzhou Jiaotong University , Lanzhou 730070, People’s Republic of ChinaKey Laboratory of Yellow River Water Environment in Gansu Province, Lanzhou Jiaotong University , Lanzhou 730070, People’s Republic of China; School of Environment and Municipal Engineering, Lanzhou Jiaotong University , Lanzhou 730070, People’s Republic of China; Engineering Research Center for Cold and Arid Regions Water Resource Comprehensive Utilization, Min-istry of Education, Lanzhou 730070, People’s Republic of ChinaSchool of Petrochemical Engineering, Lanzhou Petrochemical University of Vocational Technology , Lanzhou 730060, People’s Republic of ChinaKey Laboratory of Yellow River Water Environment in Gansu Province, Lanzhou Jiaotong University , Lanzhou 730070, People’s Republic of China; School of Environment and Municipal Engineering, Lanzhou Jiaotong University , Lanzhou 730070, People’s Republic of ChinaSchool of Civil Engineering, Lanzhou University of Technology , Lanzhou 730000, People’s Republic of ChinaAimed at current difficulties in the treatment of trace antibiotics in water, an adsorption-catalytic oxidation system was established by combining persulfate and graphene, which have the dual functions of adsorption and catalysis, for simultaneous enrichment and degradation of trace antibiotics in water. The experimental results showed that over 90% sulfamethoxazole could be degraded by the proposed system. The activation energy of the proposed system was 7.9 kJ mol ^−1 , which was significantly lower than those of typical Co catalysts and some carbon-based catalysts. Synergistic effect analysis revealed that catalytic oxidation was the key degradation kinetic of the proposed system, while adsorption showed a significant enhancement effect. Specifically, a compound with large adsorption capacity tended to be degraded preferably and rapidly. Characterization results indicated that N atoms were doped into the graphene framework, resulting in significant impacts on the activation process of potassium bisulfate by activating the sp ^2 C system. Quenching and free radical trapping experiments revealed that degradation catalyzed by the proposed system was a non-free radical oxidation reaction dominated by singlet oxygen. In summary, the proposed design was rational, N-rGO surface provided good adsorption and catalysis sites, the synergistic effect of adsorption and catalytic oxidation led to rapid and effective enrichment and in situ degradation of trace antibiotics in water.https://doi.org/10.1088/2053-1591/ac7284trace antibioticsN-doped grapheneadsorptioncatalytic oxidationsynergistic mechanism
spellingShingle Nan Wu
Xuemin Zhang
Xue Zhang
Kai Yang
Yanjuan Li
Simultaneous degradation of trace antibiotics in water by adsorption and catalytic oxidation induced by N-doped reduced graphene oxide (N-rGO): synergistic mechanism
Materials Research Express
trace antibiotics
N-doped graphene
adsorption
catalytic oxidation
synergistic mechanism
title Simultaneous degradation of trace antibiotics in water by adsorption and catalytic oxidation induced by N-doped reduced graphene oxide (N-rGO): synergistic mechanism
title_full Simultaneous degradation of trace antibiotics in water by adsorption and catalytic oxidation induced by N-doped reduced graphene oxide (N-rGO): synergistic mechanism
title_fullStr Simultaneous degradation of trace antibiotics in water by adsorption and catalytic oxidation induced by N-doped reduced graphene oxide (N-rGO): synergistic mechanism
title_full_unstemmed Simultaneous degradation of trace antibiotics in water by adsorption and catalytic oxidation induced by N-doped reduced graphene oxide (N-rGO): synergistic mechanism
title_short Simultaneous degradation of trace antibiotics in water by adsorption and catalytic oxidation induced by N-doped reduced graphene oxide (N-rGO): synergistic mechanism
title_sort simultaneous degradation of trace antibiotics in water by adsorption and catalytic oxidation induced by n doped reduced graphene oxide n rgo synergistic mechanism
topic trace antibiotics
N-doped graphene
adsorption
catalytic oxidation
synergistic mechanism
url https://doi.org/10.1088/2053-1591/ac7284
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AT xueminzhang simultaneousdegradationoftraceantibioticsinwaterbyadsorptionandcatalyticoxidationinducedbyndopedreducedgrapheneoxidenrgosynergisticmechanism
AT xuezhang simultaneousdegradationoftraceantibioticsinwaterbyadsorptionandcatalyticoxidationinducedbyndopedreducedgrapheneoxidenrgosynergisticmechanism
AT kaiyang simultaneousdegradationoftraceantibioticsinwaterbyadsorptionandcatalyticoxidationinducedbyndopedreducedgrapheneoxidenrgosynergisticmechanism
AT yanjuanli simultaneousdegradationoftraceantibioticsinwaterbyadsorptionandcatalyticoxidationinducedbyndopedreducedgrapheneoxidenrgosynergisticmechanism