期刊
JOURNAL OF HAZARDOUS MATERIALS
卷 422, 期 -, 页码 -出版社
ELSEVIER
DOI: 10.1016/j.jhazmat.2021.126867
关键词
Polyoxometalates; Graphene; Phthalate acid ester; Removal; Oxidation
资金
- National Natural Science Foundation of China [51578119, 51908241, 51908109, 52000002]
- Jilin Provincial Science and Technology Department [20180414069GH, YDZJ202101ZYTS037]
- Fundamental Research Funds for the Central Universities [2412020FZ012]
- Jilin Provincial Development and Reform Commission 2021 provincial budget capital construction fund innovation capacity construction project [2021C0405]
- Brook Byers Institute for Sustainable Systems at the Georgia Institute of Technology
- Hightower Chair at the Georgia Institute of Technology
- Georgia Research Alliance at the Georgia Institute of Technology
- Environmental Protection Scientific Research Project [2020-14, JiHuanKeZi 418]
The study demonstrates the effective degradation of PAEs using POMs/graphene hybrids, with POM molecules embedded onto graphene to form a catalyst for high-efficiency oxidation reactions. The designed HPMoV@Surf(n)/GO(20 wt%) is found to degrade various PAEs, remove over 70% of TOC and COD, and show good removal performance in a wastewater treatment plant.
Phthalate acid esters (PAEs) have been adsorbed and oxidatively degraded into small molecules including lactic acid (LA), formic acid (FA), H2O and CO2 using polyoxometalates (POMs)/graphene hybrids. We demonstrated that super-lower concentrations of PAEs could be oxidized, which was due to their unique structure. POM molecules have been embedded onto graphene to form H5PMo10V2O40@surfactant(n)/Graphene(L wt%) (abbreviated as HPMoV@Surf(n)/GO(L wt%)) using surfactants with the carbon chain length n = 2, 4, 6 and 8 for the loading of HPMoV. The coexistence of the graphene and surfactant layer (on HPMoV@Surf(n)/GO(20 wt %)) adsorbed PAE molecules and transported them rapidly to HPMoV active sites. And n values determined the electron transfer ability between graphene and POMs that promoted PAEs oxidation. The loading of POMs on the surface of graphene permitted HPMoV@Surf(n)/GO(L wt%) act as interfacial catalyst which degraded various PAEs (i.e., diethyl phthalate (DEP), diallyl phthalate (DAP) and di (2-ethylhexyl) phthalate (DEHP)) while removed more than 70% of TOC and COD. The degradation of DEP achieved 93.0% with HPMoV@Surf(n)/GO (20 wt%) and H2O2, which followed first-order kinetics and the reaction activation energy (Ea) of 23.1 kJ/mol. Further, HPMoV@Surf(n)/GO(20 wt%) showed potential for the removal of PAEs in Wastewater Treatment Plant (WWTP), and the degradation efficiency for PAE (DEP) in secondary effluent achieved 55.0%. In addition, the loading method for POMs on graphene eliminated the leaching of POMs from graphene, and the degradation efficiency could still reach 88.1% after ten recycles.
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