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activation of sulfite by metal-organic framework-derived cobalt nanoparticles for organic pollutants removal

Journal of Environmental Sciences 2023年第2期124卷 350-359页

作者： Xianjie Feng Deming Wu Xueyi Shen Yu Guo Yangyang Lv Aihua Xu Xiaoxia Li Hubei Key Laboratory of Biomass Fibers and Eco-dyeing and Finishing Wuhan Textile UniversityWuhan 430200China School of Chemistry and Chemical Engineering Wuhan Textile UniversityWuhan 430200China School of Environmental Engineering Wuhan Textile UniversityWuhan 430200China

sulfite(SO_(3)^(2−))activation is one of the most potential sulfate-radical-based advanced oxidation processes,and the catalysts with high efficiency and low-cost are greatly *** this study,the cobalt nanoparticles embedded in nitrogen-doped graphite layers(Co@NC),were used to activate SO32−for removal of Methyl Orange in aqueous *** Co@NC catalysts were synthesized via pyrolysis of Co^(2+)-based metal-organic framework(Co-MOF),where CoO was firstly formed at 400℃ and then partially reduced to Co nanoparticles embedded in carbon layers at 800℃.The Co@NC catalysts were more active than other cobaltbased catalysts such as Co^(2+),Co_(3)O_(4) and CoFe_(2)O_(4),due to the synergistic effect of metallic Co and CoxOy.A series of chain reaction between Co species and dissolved oxygen was established,with the production and transformation of SO_(3)•−,SO_(5)^(2−),and subsequent active radicals SO_(4)•−and HO•.In addition,HCO_(3)−was found to play a key role in the reaction by complexing with Co species on the surface of the *** results provide a new promising strategy by using the Co@NC catalyst for SO3_(2)−oxidation to promote organic pollutants degradation.

关键词： sulfite activation Co-MOF(Co^(2+)-based metal organic frameworks) Nitrogen-doped carbon Bicarbonate Sulfate radical

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Efficient activation of sulfite for reductive-oxidative degradation of chloramphenicol by carbon-supported cobalt ferrite catalysts

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Chinese Chemical Letters 2023年第10期34卷 106-110页

作者： Yongjie Li Mingjie Huang Wen-Da Oh Xiaohui Wu Tao Zhou School of Environmental Science and Engineering Huazhong University of Science and TechnologyWuhan 430074China School of Chemical Sciences Universiti Sains MalaysiaPenang 11800Malaysia

activation of(bi)sulfite(S(IV))by metal oxides is strongly limited by low electrons *** this study,two carbon-supported cobalt ferrites spinels(CoFe^(2)O_(4) QDs-GO and CoFe^(2)O_(4) MOFs-CNTs)have been successfully synthesized by one-step solvothermal *** was found that both catalysts could efficiently activate S(IV),with rapid reductive dechlorination and then oxidative degradation of a recalcitrant antibiotic chloramphenicol(CAP).Characterizations revealed that CoFe^(2)O_(4) spinels were tightly coated on the carbon bases(GO and CNTs),with effectiveness of the internal transfer of electrons.O_(2)˙−was identified for the reductive dechlorination of CAP,with simultaneously detection of both•OH and SO_(4)^(˙−)responsible for further oxidative *** sulfur oxygen radical conversion reactions and molecular oxygen activation would occur together upon the carbon-based ***-separated interfacial reductive-oxidation of CAP would occur with dechlorination of CAP by O_(2)^(˙−)on the carbon bases,and oxidative degradation of intermediates by SO_(4)^(˙−/•)OH upon the CoFe^(2)O_(4) catalysts.

关键词： Cobalt ferrite spinel sulfite activation Reductive dechlorination Carbon supports Sulfur oxygen radical reactions

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Efficient degradation of atrazine through in-situ anchoring NiCo_(2)O_(4) nanosheets on biochar to activate sulfite under neutral condition

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Journal of Environmental Sciences 2023年第4期126卷 81-94页

作者： Lizhen Feng Yijin Yuan Xianqin He Mengsi Wu Lizhi Zhang Jingming Gong Key Laboratory of Pesticide&Chemical Biology of Ministry of Education Institute of Environmental&Applied ChemistryInternational Joint Research Center for Intelligent Biosensing Technology and HealthCollege of ChemistryCentral China Normal UniversityWuhan 430079China

sulfite (S(IV)) is a promising substitute for sulfate radical-based advanced oxidation ***,a composite of in-situ anchoring Ni Co_(2)O_(4)nanosheets on biochar (BC) was firstly employed as a heterogeneous activator for sulfite (Ni Co_(2)O_(4)@BC-sulfite) to degrade atrazine (ATZ) in the neutral *** synergistic coupling of BC and Ni Co_(2)O_(4)endows the resulting composite excellent catalytic activity.82% of the degradation ratio of ATZ (1 mg/L) could be achieved within 10 min at initial concentrations of 0.6 g/L Ni Co_(2)O_(4)@BC,3.0 mmol/L sulfite in neutral *** further supplementing sulfite into the system at 20 min (considering the depletion of sulfite),outstanding degradation efficiency (100%) were achieved in the next 10 min without any other energy input by the Ni Co_(2)O_(4)@BC-sulfite *** features of the prepared catalysts and the effects of some key parameters on ATZ degradation were systematically examined.A strong inner-sphere complexation (≡Co_(2)+/Ni^(2+)-SO_(3)^(2-)) was explored between sulfite and the metal sites on the Ni Co_(2)O_(4)@BC *** redox cycle of the surface metal efficiently mediated sulfite activation and triggered the series radical chain *** generated radicals,in particular the surface-bound radicals were involved in ATZ *** performance liquid chromatography-tandem mass spectrometry (LC-MS) technique was used to detect the degradation *** functional theory (DFT) calculations were performed to illustrate the possible degradation pathways of ***,an underlying mechanism for ATZ removal was *** present study offered a low-cost and sustainable catalyst for sulfite activation to remove ATZ in an environmentally friendly manner from wastewater.

关键词： NiCo_(2)O_(4) Biochar sulfite activation Atrazine Surface radicals Neutral condition

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Understanding the role of transition metal single-atom electronic structure in oxysulfur radical-mediated oxidative degradation

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Environmental Science and Ecotechnology 2024年第4期20卷 247-258页

作者： Guanshu Zhao Jing Ding Jiayi Ren Qingliang Zhao Chengliang Mao Kun Wang Jessica Ye Xueqi Chen Xianjie Wang Mingce Long State Key Laboratory of Urban Water Resources and Environment School of EnvironmentHarbin Institute of TechnologyHarbin150090China Solar Fuels Group Department of ChemistryUniversity of Toronto80 St.George StreetTorontoOntarioM5S 3H6Canada School of Physics Harbin Institute of TechnologyHarbin150001China School of Environmental Science and Engineering Key Laboratory of Thin Film and Microfabrication Technology(Ministry of Education)Shanghai Jiao Tong University800 Dongchuan RoadShanghai200240China

The ubiquity of refractory organic matter in aquatic environments necessitates innovative removal *** radical-based advanced oxidation has emerged as an attractive solution,offering high selectivity,enduring efficacy,and anti-interference *** many technologies,sulfite activation,leveraging its cost-effectiveness and lower toxicity compared to conventional persulfates,stands ***,the activation process often relies on transition metals,suffering from low atom *** we introduce a series of single-atom catalysts(SACs)employing transition metals on g-C_(3)N_(4)substrates,effectively activating sulfite for acetaminophen *** highlight the superior performance of Fe/CN,which demonstrates a degradation rate constant significantly surpassing those of Ni/CN and Cu/*** investigation into the electronic and spin polarization characteristics of these catalysts reveals their critical role in catalytic efficiency,with oxysulfur radical-mediated reactions ***,under visible light,the catalytic activity is enhanced,attributed to an increased generation of oxysulfur radicals and a strengthened electron donation-back donation *** proximity of Fe/CN's d-band center to the Fermi level,alongside its high spin polarization,is shown to improve sulfite adsorption and reduce the HOMO-LUMO gap,thereby accelerating photo-assisted sulfite *** work advances the understanding of SACs in environmental applications and lays the groundwork for future water treatment technologies.

关键词： Single-atom catalysts(SACs) Oxysulfur radical sulfite activation Spin polarization Electronic structure

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