Abstract
A series of carbon nanotubes doped with Fe and/or Cu, Fe100−xCux/CNT (x = 0, 25, 50, 75 and 100) has been prepared by an easy method of wetness impregnation of commercial multiwalled carbon nanotubes previously oxidized with nitric acid. The wide characterization of the solids by different techniques demonstrates that the incorporation of Fe and Cu to the CNTs has been successfully produced. Fe100−xCux/CNT samples were tested as catalysts in the removal of paracetamol from aqueous solution by a combined process of adsorption and Fenton-like oxidation. Under mild conditions, 25 °C and natural pH of solution, i.e., nearly neutral, values of oxidation of paracetamol between 90.2% and 98.3% were achieved after 5 h of reaction in most of cases. Furthermore, with the samples containing higher amounts of copper, i.e., Cu100/CNT and Fe25Cu75/CNT, only 2 h were necessary to produce depletion values of 73.2% and 87.8%, respectively. The influence of pH and dosage of H2O2 on the performance has also been studied. A synergic effect between both Cu+/Cu2+ and Fe2+/Fe3+ in Fenton-like reaction was observed. These results demonstrate that Fe100−xCux/CNT are powerful Fenton-like catalyst for degradation of paracetamol from aqueous solution and they could be extended to the removal of other organic pollutants.
Highlights
Advanced oxidation processes (AOPs) are based on the formation of highly reactive radicals capable to degrade recalcitrant organic wastewater contaminants with high efficiency [1,2,3,4]
Recyclability of Catalysts SomeTheuxsp, ethriempeanratcsetfaomrolstduedcoyminpgostithioen rwecays creladbuicleitdybeotfwtehene ac2a1ta%ly(fsotsr Fwe2e5Creu75c/CarNriTe)danodu5t2, %more concrS(efotoemrlyFee,e7w5xCpiuteh2r5/itCmhNreenTet)s.oTffhoterhesextuccaedptyatilnoyngstwtsh,aeFs erthe10ce0y/cCcalNtaablTyi,lsitCtycuoon10ft0a/tCihneNincTgaotaannllydysittrshoewn,mei.reoe.s,cFtaear1cr00it/eiCvdNeoTou,ntf,eom,r Fwoerh2e5iCcchuo, n7t5hc/eCreNteTly., Twhitehrtefhisnruaelletsodofefpthrleeetuicosanatbaoillyfitsytpsaa,rrFaeece1s0tha0om/CwoNnl Tiw,nCaFsuig1a0ul0mr/CeoNs9t.Tthaendsathmeemforst baocthiveHo2One2, Fdeo2s5aCgeus7,5/aCltNhoTu.gThhethresults of reudseacboimlitpyosairteiosnhoocwcunrriendFfiagsuterrew9.hen the higher amount of oxidant was used. For this catalyst two stages seemed to exist in the heterogeneous Fenton reaction: the induction period and rapid degradation stage, the degradation rates were accelerated after about 90 min after the adding of H2O2, 1.0as clearly seen by the values of the ap12snptdccayycrclelee nt constant rate calculated for both stages (Ta12bsntdlcceyyccle4le)
We reported for the first time the preparation of Fe-Cu doped carbon nanotubes by an easy method and their application as efficient catalysts for the degradation of paracetamol (90–98% in 5 h) by a combined process of adsorption and Fenton-like oxidation under mild reaction conditions, 25 ◦C and pH nearly neutral
Summary
Advanced oxidation processes (AOPs) are based on the formation of highly reactive radicals capable to degrade recalcitrant organic wastewater contaminants with high efficiency [1,2,3,4]. Heterogeneous processes based on the production of hydroxyl radicals from the decomposition of H2O2 by the action of catalysts containing the Fe3+/Fe2+ couple [5,6,7,8,9] or other elements with multiple redox state [10] have been broadly used They are known as heterogeneous Fenton-like processes and overcome the drawbacks of homogenous counterparts of the limited narrow working pH (3–4) and the necessity of recovering the leached iron from the wastewater. Due to the hydrophobic character of their surface, CNTs exhibit more active sites to interact with organic pollutants In this regard, different articles have reported the use of iron oxides supported over CNTs as heterogeneous Fenton catalysts for the degradation of phenolic compounds [28,29,30,31], herbicides [32], antibiotics [33] and dyes [34]. The stability and recyclability of the catalysts, as well as the leaching and mineralization degree have been studied
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