Catalytic oxidation of clofibric acid by peroxydisulfate activated with wood-based biochar: Effect of biochar pyrolysis temperature, performance and mechanism

Zhu, Kangmeng; Wang, Xisong; Geng, Mengzi; Chen, Dong; Lin, Huang; Zhang, Hui

doi:10.1016/j.cej.2019.06.006

Cited by 166 publications

(23 citation statements)

References 85 publications

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“…Prior to this study, other ringopening reaction intermediates were found during the ozonation of clofibric acid (Rosal et al, 2009). According to our data and to other previous works (Doll and Frimmel, 2004;Kosjek et al, 2009;Zhu et al, 2019) A possible explanation is that these reaction intermediates are present in the collected samples at concentration levels, which are below the instrumental quantification limit of the used chromatographic system or because of their chemical instability during the cultivation conditions.…”

Section: Products Of the Transformation Of Clofibric Acid By Streptomyces Miug 489supporting

confidence: 73%

Enhancing the biodegradation efficiency of a emergent refractory water pollutant by a bacterial isolate through a statistical process optimization approach

Favier

Ungureanu

Simion

et al. 2021

Process Safety and Environmental Protection

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Clofibric acid, the main pharmacologically-active metabolite of pharmaceutical products used as antilipaemic agent has received, in last years, an increased interest because of its wellknown recalcitrance to biodegradation and its high persistence in the aquatic environment. This molecule passes unchanged or poorly transformed in wastewater treatment plants. An indigenous strain of Streptomyces, named MIUG 4.89 was previously selected, exhibited the ability to favor clofibric acid biodegradation within submerged cultivation in controlled biotechnological conditions. Thus, in order to enhance the biodegradation of this refractory molecule, mathematical modeling and statistical optimization designs associated to Plackett-Burman Design and Response Surface Methodology were used to evaluate and optimize the effects of different major culture conditions of this bacterial isolate. According to the results, under optimized culture conditions (5 g L -1 glucose, inoculation level 4.7%, 27.5°C and 20 days of incubation) the strain Streptomyces MIUG 4.89 exhibited a successful removal of clofibric acid with a biodegradation yield of 54%, which is in agreement with model J o u r n a l P r e -p r o o f 3 prediction. Thus, under optimized conditions, the removal yield was enhanced, which is very promising accounting for the refractory character of this water pollutant.

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Section: Products Of the Transformation Of Clofibric Acid By Streptomyces Miug 489supporting

confidence: 73%

Enhancing the biodegradation efficiency of a emergent refractory water pollutant by a bacterial isolate through a statistical process optimization approach

Favier

Ungureanu

Simion

et al. 2021

Process Safety and Environmental Protection

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“…% after a heat treatment . Therefore, the carbonaceous materials were gradually inactivated in persulfate activation after the introduction of a large number of oxygen groups, , whereas their activities could be restored by thermal decomposition of the oxygen moieties. ,, Figure b shows that the carbonyl and carboxyl groups present good linearity with ln k obs (eqs S2 and S3), that is, the more oxygen groups, the lower reaction rate. The relatively low R 2 for hydroxyl correlation (0.762) was due to the insignificant effect of the hydroxyl group and strong influences of the other groups.…”

Section: Resultsmentioning

confidence: 96%

“…However, the origin of nonradical oxidation by carbocatalysis is still debatable because of the physicochemical and structural complexity of pristine carbon atoms, ,, such as heteroatom doping and functionality, ,,, structural defects, − graphitic degrees, ,− porosity, and dimensional structures. , Nitrogen-doping in CNTs was consolidated to initiate nonradical oxidation via electron transfer by formation of PMS/CNT complexes (CNT/PMS*) because of the strong coupling of positively charged carbon atoms with the negatively charged peroxide O–O bond . Yun et al proposed that CNTs could act as a conductor to accelerate electron transfer from the adsorbed organics to the activated persulfate , because of the outer-sphere interactions of persulfate with the highly conjugated π system of CNTs. − The ketonic/carbonyl groups (CO) on nanodiamonds or CNTs were identified to be the primary active sites for 1 O 2 production in persulfate activation.…”

Section: Introductionmentioning

confidence: 99%

Insights into the Electron-Transfer Regime of Peroxydisulfate Activation on Carbon Nanotubes: The Role of Oxygen Functional Groups

Ren

Xiong

Nie

et al. 2019

Environ. Sci. Technol.

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557

183

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Carbon-driven advanced oxidation processes are appealing in wastewater purification because of the metal-free feature of the carbocatalysts. However, the regime of the emerging nonradical pathway is ambiguous because of the intricate carbon structure. To this end, this study was dedicated to unveil the intrinsic structure-performance relationship of peroxydisulfate (PDS) activation by carbon nanotubes (CNTs) toward nonradical oxidation of organics such as phenol (PE) via electron transfer. Eighteen analogical CNTs were synthesized and functionalized with different categories and contents of oxygen species. The quenching tests and chronopotentiometry suggest that an improved reactivity of surface-regulated CNTs was attributed to the reinforced electron-transfer regime without generation of free radicals and singlet oxygen. The quantitative structure–activity relationships were established and correlated to the Tafel equation, which unveils the nature of the nonradical oxidation by CNT-activated PDS complexes (CNT-PDS*). First, a decline in the concentration of oxygen groups in CNTs will make the zeta potential of the CNT become less negative in neutral solutions, which facilitated the adsorption of PDS because of weaker electrostatic repulsion. Then, the metastable CNT-PDS* was formed, which elevated the oxidation capacity of the CNT. Finally, PE would be oxidized over CNT-PDS* via electron transfer to fulfill the redox cycle. Moreover, the nonradical oxidation rate was uncovered to be exponentially related with the potential of the complexes, suggesting that the nonradical oxidation by the CNT-PDS* undergoes a mechanism analogous to anodic oxidation.

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“…Advanced oxidation processes (AOPs) based on metal-free carbonaceous materials with persulfates are promising for green remediation of aqueous organic pollutants. − The primary reactive oxygen species (ROS) in persulfate-based AOPs (PS-AOPs) typically involve hydroxyl radical (•OH), , sulfate radical (SO 4 •– ), − singlet oxygen ( 1 O 2 ), − and carbon-activated persulfate complexes, − which can attack and oxidize organic contaminants via either radical or nonradical reactions.…”

Section: Introductionmentioning

confidence: 99%

The Intrinsic Nature of Persulfate Activation and N-Doping in Carbocatalysis

Ren

Nie

Zhou

et al. 2020

Environ. Sci. Technol.

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675

195

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Persulfates activation by carbon nanotubes (CNT) has been evidenced as nonradical systems for oxidation of organic pollutants. Peroxymonosulfate (PMS) and peroxydisulfate (PDS) possess discrepant atomic structures and redox potentials, while the nature of their distinct behaviors in carbocatalytic activation has not been investigated. Herein, we illustrated that the roles of nitrogen species in CNT-based persulfate systems are intrinsically different. In PMS activation mediated by nitrogen-doped CNT (N-CNT), surface chemical modification (N-doping) can profoundly promote the adsorption quantity of PMS, consequently elevate potential of derived nonradical N-CNT–PMS* complexes, and boost organic oxidation efficiency via an electron-transfer regime. In contrast, PDS adsorption was not enhanced upon incorporating N into CNT due to the limited equilibrium adsorption quantity of PDS, leading to a relatively lower oxidative potential of PDS/N-CNT system and a mediocre degradation rate. However, with equivalent persulfate adsorption on N-CNT at a low quantity, PDS/N-CNT exhibited a stronger oxidizing capacity than PMS/N-CNT because of the intrinsic higher redox potential of PDS than PMS. The oxidation rates of the two systems were in great linearity with the potentials of carbon–persulfate* complexes, suggesting N-CNT activation of PMS and PDS shared the similar electron-transfer oxidation mechanism. Therefore, this study provides new insights into the intrinsic roles of heteroatom doping in nanocarbons for persulfates activation and unveils the principles for a rational design of reaction-oriented carbocatalysts for persulfate-based advanced oxidation processes.

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Catalytic oxidation of clofibric acid by peroxydisulfate activated with wood-based biochar: Effect of biochar pyrolysis temperature, performance and mechanism

Cited by 166 publications

References 85 publications

Enhancing the biodegradation efficiency of a emergent refractory water pollutant by a bacterial isolate through a statistical process optimization approach

Enhancing the biodegradation efficiency of a emergent refractory water pollutant by a bacterial isolate through a statistical process optimization approach

Insights into the Electron-Transfer Regime of Peroxydisulfate Activation on Carbon Nanotubes: The Role of Oxygen Functional Groups

The Intrinsic Nature of Persulfate Activation and N-Doping in Carbocatalysis

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