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Efficient H2O2 electrogeneration at graphite felt modified via electrode polarity reversal: Utilization for organic pollutants degradation.

ABSTRACT: Electrochemical synthesis of H2O2 offers a great potential for water treatment. However, a significant challenge is the development of efficient cathode materials for the process. Herein, we implement a practical electrochemical cathode modification to support efficient H2O2 electrogeneration via the reduction of dissolved anodic O2. Graphite felt (GF) is in situ anodically modified by electrode polarity reversal technique in an acid-free, low-conductivity electrolyte. The modified GF exhibits a significantly higher activity towards O2 reduction. Up to 183.3% higher H2O2 yield is obtained by the anodized GF due to the increased concentrations of oxygen-containing groups and the hydrophilicity of the surface, which facilitates electron and mass transfer between GF and the electrolyte. Another significant finding is the ability to produce H2O2 at a high yield under neutral pH and low current intensity by the modified GF (35% of the charge need to produce the same amount by unmodified GF). Long-term stability testing of the modified GF showed a decay in the electrode's activity for H2O2 production after 30 consecutive applications. However, the electrode regained its optimal activity for H2O2 production after a secondary modification by electrode polarity reversal. Finally, in situ electrochemically modified GF is more effective for removal of reactive blue 19 (RB19, 20 mg/L) and ibuprofen (IBP, 10 mg/L) by the electro-Fenton process. The modified GF removed 62.7% of RB19 compared to only 28.1% by the unmodified GF in batch reactors after 50 min. Similarly, 75.3% IBP is removed by the modified GF compared to 57.6% by the unmodified GF in a flow-through reactor after 100 min.

SUBMITTER: Zhou W

PROVIDER: S-EPMC7314056 | biostudies-literature | 2019 May

REPOSITORIES: biostudies-literature

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Efficient H2O2 electrogeneration at graphite felt modified via electrode polarity reversal: Utilization for organic pollutants degradation.

Zhou Wei W Rajic Ljiljana L Meng Xiaoxiao X Nazari Roya R Zhao Yuwei Y Wang Yan Y Gao Jihui J Qin Yukun Y Alshawabkeh Akram N AN

Chemical engineering journal (Lausanne, Switzerland : 1996) 20190130

Electrochemical synthesis of H2O2 offers a great potential for water treatment. However, a significant challenge is the development of efficient cathode materials for the process. Herein, we implement a practical electrochemical cathode modification to support efficient H2O2 electrogeneration via the reduction of dissolved anodic O2. Graphite felt (GF) is in situ anodically modified by electrode polarity reversal technique in an acid- ...[more]

PMID: 32581640

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Project description:The structure-electroactivity relationship of graphene has been studied using coronene (Cor), polyaromatic hydrocarbon (PAH), and a subunit of graphene as a model system by chemically modified electrode approach. In general, graphene and PAH do not show any redox activity in their native form. Herein, we report a simple electrochemical approach for the conversion of electro-inactive coronene to a highly redox-active molecule (Cor-Redox; E°' = 0.235 ± 0.005 V vs Ag/AgCl) after being adsorbed on graphitic carbon nanomaterial and preconditioned at an applied potential, 1.2 V vs Ag/AgCl, wherein, the water molecule oxidizes to dioxygen via hydroxyl radical (•OH) intermediate, in acidic solution (pH 2 KCl-HCl). When the same coronene electrochemical experiment was carried out on an unmodified glassy carbon electrode, there was no sign of faradic signal, revealing the unique electrochemical behavior of the coronene molecule on graphitic nanomaterial. The Cor-Redox peak is found to be highly symmetrical (peak-to-peak potential separation of ?0 V tested by cyclic voltammetry (CV)) and surface-confined (?Cor-Redox = 10.1 × 10-9 mol cm-2) and has proton-coupled electron-transfer (?E°'/?pH = -56 mV pH-1) character. Initially, it was speculated that Cor is converted to a hydroxy group-functionalized Cor molecule (dihydroxy benzene derivative) on the graphitic surface and showed the electrochemical redox activity. However, physicochemical characterization studies including Raman, IR, transmission electron microscopy (TEM), X-ray photoelectron spectroscopy (XPS), redox-site selective oxidation probe, cysteine (for dihydroxy benzene), radical scavenger ((2,2,6,6-tetramethylpiperidin-1-yl)oxyl, TEMPO), and scanning electrochemical microscopy (SECM) using ferricyanide redox couple have revealed that coronene cationic radical species like electroactive molecule is formed on graphitic material upon the electrochemical oxidation reaction at a high anodic potential. It has been proposed that •OH generated as an intermediate species from the water oxidation reaction is involved in the coronene cationic radical species. Studies on coronene electrochemical reaction at various carbon nanomaterials like multiwalled carbon, single-walled carbon, graphite, graphene oxide, and carbon nanofiber revealed that graphitic structure (without any oxygen functional groups) and its ?-? bonding are key factors for the success of the electrochemical reaction. The coronene molecular redox peak showed an unusual electrocatalytic reduction of hydrogen peroxide similar to the peroxidase enzyme-biocatalyzed reduction reaction in physiological solution.

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Efficient H2O2 electrogeneration at graphite felt modified via electrode polarity reversal: Utilization for organic pollutants degradation.

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Efficient H<sub>2</sub>O<sub>2</sub> electrogeneration at graphite felt modified via electrode polarity reversal: Utilization for organic pollutants degradation.

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