In situ generation and efficient activation of H2O2 for pollutant degradation over CoMoS2 nanosphere-embedded rGO nanosheets and its interfacial reaction mechanism

Han, Muen; Lyu, Lai; Huang, Yin‐Mei; Liang, Junrong; Xue, Meimei; Wu, Tao; Li, Jiayi; Chen, Mei‐Ping; Hu, Chun

doi:10.1016/j.jcis.2019.02.062

Cited by 50 publications

(18 citation statements)

References 52 publications

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“…In this situation, about 90% H 2 O 2 is utilized and a high degree of organic pollutants are oxidized. With an increase in the cation-π interaction, the consumption of H 2 O 2 was greatly decreased in CoMoS 2 nanosphere-embedded rGO nanosheets ( Han et al., 2019 ) owing to the reduction of O 2 to H 2 O 2 using energy of the pollutants. Therefore, the strong cation-π interaction provides a feasibility of utilizing the energy of the organic pollutants.…”

Section: Introductionmentioning

confidence: 99%

Cation-π induced surface cleavage of organic pollutants with ⋅OH formation from H2O for water treatment

et al. 2021

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Summary High energy consumption is impedimental for eliminating refractory organic pollutants in water by applying advanced oxidation processes (AOPs). Herein, we develop a novel process for destructing these organics in chemical conjuncted Fe 0 -Fe y C z /Fe x , graphited ZIF-8, and rGO air-saturated aqueous suspension without additional energy. In this process, a strong Fe-π interaction occurs on the composite surface, causing the surface potential energy ∼310.97 to 663.96 kJ/mol. The electrons for the adsorbed group of pollutants are found to delocalize to around the iron species and could be trapped by O 2 in aqueous suspension , producing ⋅ OH, H, and adsorbed organic cation radicals, which are hydrolyzed or hydrogenated to intermediate. The target pollutants undergo surface cleavage and convert H 2 O to ⋅ OH, consuming chemical adsorption energy (∼2.852–9.793 kJ/mol), much lower than that of AOPs. Our findings provide a novel technology for water purification and bring new insights into pollutant oxidation chemistry.

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Section: Introductionmentioning

confidence: 99%

Cation-π induced surface cleavage of organic pollutants with ⋅OH formation from H2O for water treatment

et al. 2021

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“…Fenton technology, one of the most powerful advanced oxidation processes (AOPs), is widely used to remove refractory organic pollutants from wastewater due to the generation of the highly aggressive hydroxyl radicals ( • OH, E 0 = 2.80 V/NHE) through the reduction of hydrogen peroxide (H 2 O 2 ) by Fe 2+ or other reducing transition metals. − Compared with homogeneous reactions, heterogeneous Fenton/Fenton-like processes overcome the defects of iron-sludge accumulation, a narrow working pH range and difficulty in recycling , and have become promising AOPs for water treatment. However, the developed heterogeneous Fenton/Fenton-like processes still do not deviate from the basic principle of the classical Fenton reaction.…”

Section: Introductionmentioning

confidence: 99%

Efficient Fenton-like Process for Pollutant Removal in Electron-Rich/Poor Reaction Sites Induced by Surface Oxygen Vacancy over Cobalt–Zinc Oxides

Zhan

Zhang

et al. 2020

Environ. Sci. Technol.

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To achieve high efficiency and low consumption for water treatment in the Fenton reaction, we use the surface oxygen vacancies (OVs) as the electron temporary residences to construct a dual-reaction-center (RDC) Fenton-like catalyst with abundant surface electron-rich/poor areas consisting of OV-rich Co-ZnO microparticles (OV-CoZnO MPs). The lattice-doping of Co into ZnO wurtzite results in the formation of OVs with unpaired electrons (electron-rich OVs) and electron-deficient Co3+ sites according to the structural and electronic characterizations. Both experimental and theoretical calculations prove that the electron-rich OVs are responsible for the capture and reduction of H2O2 to generate hydroxyl radicals, which quickly degrades pollutants, while a large amount of pollutants are adsorbed at the electron-deficient Co3+ sites and act as electron donors for the system, accompanied by their own oxidative degradation. The electrons obtained from the pollutants in the electron-deficient sites are transferred to the OVs through the internal bond bridge to achieve the balance of electron gain/loss. Through this process, pollutants are efficiently converted and degraded by multiple pathways in a wide range of pH (4.5–9.5). The reaction rate of the OV-CoZnO MPs/H2O2 system is increased by ∼17 times compared with the non-DRC system. This discovery provides a sustainable strategy for pollutant utilization, which shows new implications for solving the troublesome issues of the Fenton reaction and for developing novel environmental remediation technologies.

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“…A double-compartment reactor equipped with a bipolar membrane was employed to realize SO 2 removal and H 2 O 2 generation synchronously, in which the α-Fe 2 O 3 photoanode and GDE cathode were placed in the anodic and cathodic chambers, respectively. Solar light and electricity are necessary for not only stimulation of the photoanode but also trigger of H 2 O 2 generation . After inletting SO 2 into the anolyte, SO 3 2– was formed and oxidized to SO 4 2– by the photogenerated holes ( h + ) on the α-Fe 2 O 3 electrode, while the separated electrons ( e – ) were transferred to the GDE cathode to complete the HPR process.…”

Section: Resultsmentioning

confidence: 99%

“…Solar light and electricity are necessary for not only stimulation of the photoanode but also trigger of H 2 O 2 generation. 66 After inletting SO 2 into the anolyte, SO 3 2− was formed and oxidized to SO 4 2− by the photogenerated existence of SO 3 2− . The experiments were repeated in various catholytes with pH of 2, 3, and 4 to evaluate the influence of pH (Figure 3b).…”

Section: ■ Materials and Methodsmentioning

confidence: 99%

Efficient SO₂ Removal and Highly Synergistic H₂O₂ Production Based on a Novel Dual-Function Photoelectrocatalytic System

Mei

Bai

Chen

et al. 2020

Environ. Sci. Technol.

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The direct conversion of SO2 to SO3 is rather difficult for flue gas desulfurization due to its inert dynamic with high reaction activation energy, and the absorption by wet limestone-gypsum also needs the forced oxidation of O2 to oxidize sulfite to sulfate, which is necessary for additional aeration. Here, we propose a method to remove SO2 with highly synergistic H2O2 production based on a novel dual-function photoelectrocatalytic (PEC) system in which the jointed spontaneous reaction of desulfurization and H2O2 production was integrated instead of nonspontaneous reaction of O2 to H2O2. SO2 was absorbed by alkali liquor then oxidized quickly into SO4 2– by a nanorod α-Fe2O3 photoanode, which possessed high alkali corrosion resistance and electron transport properties. H2O2 was produced simultaneously in the cathode chamber on a gas diffusion electrode and was remarkably boosted by the conversion reaction of SO3 2– to SO4 2– in the anode chamber in which the released chemical energy was effectively used to increase H2O2. The photocurrent density increased by 40% up to 1.2 mA·cm–2, and the H2O2 evolution rate achieved 58.8 μmol·L–1·h–1·cm–2 with the synergistic treatment of SO2, which is about five times than that without SO2. This proposed PEC cell system offers a cost-effective and environmental-benign approach for dual purpose of flue gas desulfurization and simultaneous high-valued H2O2 production.

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In situ generation and efficient activation of H2O2 for pollutant degradation over CoMoS2 nanosphere-embedded rGO nanosheets and its interfacial reaction mechanism

Cited by 50 publications

References 52 publications

Cation-π induced surface cleavage of organic pollutants with ⋅OH formation from H2O for water treatment

Cation-π induced surface cleavage of organic pollutants with ⋅OH formation from H2O for water treatment

Efficient Fenton-like Process for Pollutant Removal in Electron-Rich/Poor Reaction Sites Induced by Surface Oxygen Vacancy over Cobalt–Zinc Oxides

Efficient SO₂ Removal and Highly Synergistic H₂O₂ Production Based on a Novel Dual-Function Photoelectrocatalytic System

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In situ generation and efficient activation of H2O2 for pollutant degradation over CoMoS2 nanosphere-embedded rGO nanosheets and its interfacial reaction mechanism

Cited by 50 publications

References 52 publications

Cation-π induced surface cleavage of organic pollutants with ⋅OH formation from H2O for water treatment

Cation-π induced surface cleavage of organic pollutants with ⋅OH formation from H2O for water treatment

Efficient Fenton-like Process for Pollutant Removal in Electron-Rich/Poor Reaction Sites Induced by Surface Oxygen Vacancy over Cobalt–Zinc Oxides

Efficient SO2 Removal and Highly Synergistic H2O2 Production Based on a Novel Dual-Function Photoelectrocatalytic System

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Efficient SO₂ Removal and Highly Synergistic H₂O₂ Production Based on a Novel Dual-Function Photoelectrocatalytic System