In-situ formation of surface reactive oxygen species on defective sites over N-doped biochar in catalytic ozonation

Cheng, Yizhen; Wang, Binyuan; Shen, Jiayi; Kang, Jing; Zhao, Shengxin; Zhu, Xinwei; Shen, Linlu; Wang, Shuyu; Shen, Yang; Chen, Zhonglin

doi:10.1016/j.cej.2022.140232

Cited by 40 publications

(9 citation statements)

References 88 publications

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“…When using methanol as the solvent, the characteristic and strong peak of DMPO-O 2 •– ( a N = 14.2 G, a H β = 11.4 G, a H γ1 = 1.2 G) appeared at the beginning of the reaction in the O 3 /ZNC400 system, but the intensity decreased as the reaction proceeded (Figure S8b). Thus, O 2 •– serves as a crucial intermediate in the chain reaction of HCO, which would swiftly convert into • OH via eqs – to initiate the attack on ATZ in the O 3 /ZNC400 system . Further exploration was conducted to determine the relative contributions of multiple ROS to the ATZ degradation.…”

Section: Resultsmentioning

confidence: 99%

“…To reveal the potential synergistic catalytic effect between ZnO and the carbon substrate, the in situ Raman spectrum of the O 3 /ZNC400 was investigated (Figure f). Two minor characteristic peaks assigned to *O at 1020 cm –1 and surface peroxide species (*O 2 ) at 884 cm –1 appeared, assigned to the in situ O 3 decomposition . Intriguingly, no adsorbed O 3 adsorption peak at 1080 cm –1 was observed in the O 3 /ZNC400 system, while a phenomenal signal was observed in the O 3 /NC system.…”

Section: Resultsmentioning

confidence: 99%

“…Two minor characteristic peaks assigned to *O at 1020 cm −1 and surface peroxide species (*O 2 ) at 884 cm −1 appeared, assigned to the in situ O 3 decomposition. 50 Intriguingly, no adsorbed O 3 adsorption peak at 1080 cm −1 was observed in the O 3 / ZNC400 system, while a phenomenal signal was observed in the O 3 /NC system. This observation implies a potential preference for O 3 to selectively adsorb onto carbon substrates, subsequently undergoing swift decomposition by ZnO within ZNC400 to • OH, giving rise to the silent peak for the O 3 / ZNC400.…”

Section: Revelation Of Synergistic Catalytic Mechanismmentioning

confidence: 93%

“…•− serves as a crucial intermediate in the chain reaction of HCO, which would swiftly convert into • OH via eqs 6−8 to initiate the attack on ATZ in the O 3 /ZNC400 system. 50 Further exploration was conducted to determine the relative contributions of multiple ROS to the ATZ degradation. Figure 3c shows that the contribution of • OH in the O 3 alone system was 83.0% because of the rapid reaction of ATZ with…”

Section: Ros Exploration and Omentioning

confidence: 99%

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Synergistic Catalytic Ozonation Mediated by Dual Active Sites of Oxygen Vacancies and Defects in Biomass-Derived Composites for Long-Lasting Water Decontamination

Cheng,

Chen,

Yan

et al. 2024

ACS Catal.

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Environmental decontamination relies on low-cost, sustainable materials to drive diverse catalytic redox reactions. In this work, we used low-cost biomass to develop nanocomposites of N-doped carbon-supported zinc oxide (ZNC400) at a low temperature (400 °C), which exhibited ultrahigh activity in heterogeneous catalytic ozonation (HCO) for organic water decontamination. Our experimental and computational studies revealed the collaborative functions of dual active centers of defective carbons and oxygen vacancies (OVs)-containing zinc oxide (ZnO) at the composite interface for successive ozone (O 3 ) adsorption and catalytic decomposition, respectively. Inspiringly, OVs on ZnO will spontaneously dissociate water molecules (H 2 O) to form surface hydroxyl groups (−OH) as key intermediates to accelerate O 3 decomposition. This synergistic interplay results in the continuous generation of hydroxyl radicals ( • OH) and maintains over 90.2% atrazine (ATZ) removal over five successive cycles, endowing ZNC400 with substantial reusability. Furthermore, four ATZ degradation pathways were proposed, and the corresponding toxicity was evaluated by the embryonic development of zebrafish in the treated water. Overall, the engineered dual-function catalyst effectively addresses the long-standing issue of poor stability of carbon materials in HCO and offers high-performance, cheap, and green catalysts for advanced water purification.

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Section: Resultsmentioning

confidence: 99%

Section: Resultsmentioning

confidence: 99%

Section: Revelation Of Synergistic Catalytic Mechanismmentioning

confidence: 93%

Section: Ros Exploration and Omentioning

confidence: 99%

See 2 more Smart Citations

Synergistic Catalytic Ozonation Mediated by Dual Active Sites of Oxygen Vacancies and Defects in Biomass-Derived Composites for Long-Lasting Water Decontamination

Cheng,

Chen,

Yan

et al. 2024

ACS Catal.

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“…However, when suitable catalytic conditions are established, ozone can be decomposed on the catalyst surface via a two-step reaction, this is shown in Eqs. 4 , 5 , where O* and O2* are ROS on the catalyst surface ( Aziz et al, 2018 ; Hajer et al, 2022 ; Cheng et al, 2023 ). The reaction forms ROS with strong oxidation capacity, and ROS has a significant effect on microbial eradication as well as on the treatment of pollutants ( Yuan et al, 2018 ).…”

Section: Introductionmentioning

confidence: 99%

Synergistic graphene-MnOx/honeycomb activated carbon (G-MnOx/HAC) and plasma technology for eradication of pathogenic microorganisms

Zhang

Jia

et al. 2023

Front. Chem.

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This paper addresses the risk for environmental transmission of pathogenic microorganisms in confined spaces and the serious health hazards for personnel, and research on efficient eradication methods for the pathogenic microorganisms was carried out to provide technical support for ensuring the health of personnel in confined spaces. A series of graphene-MnO2 (G-MnO2) catalytic materials was prepared by hydrothermal and precipitation methods, and processing parameters such as the graphene doping method, the raw material ratio and the plasma action time were optimized. It was shown that G-MnOX-P/HAC prepared by a one-step precipitation method and with a graphene doping ratio of 10% had the best bactericidal effect in a dielectric barrier discharge (DBD) reactor after 4 min of reaction. The eradication rates for Escherichia coli (E. coli), Staphylococcus aureus (S. aureus), coronavirus and Aspergillus niger were all greater than 99.9%. The characterization techniques TEM, SEM, XRD, XPS, BET and FT-IR showed that the G-MnOX-P samples prepared by the one-step precipitation method had larger specific surface areas with more oxygen vacancies and functional groups on the surfaces, which was conducive to decomposition of the ozone generated by the dissociated plasma and formation of reactive oxygen species (ROS) for the microbial eradication process. Finally, by comparing the ozone-decomposition activity with the plasma co-catalytic performance, it was verified that efficient decomposition of the ozone facilitated the eradication of microorganisms. Based on this, an analysis of the mechanism for efficient eradication was carried out.

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3D Carbon Microspheres with a Maze‐Like Structure and Large Mesopore Tunnels Built From Rapid Aerosol‐Confined Coherent Salt/Surfactant Templating

Li,

Hu,

Jiang

et al. 2023

Small

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Hierarchically porous carbons with tailor‐made properties are essential for applications wherein rich active sites and fast mass transfer are required. Herein, a rapid aerosol‐confined salt/surfactant templating approach is proposed for synthesizing hierarchically porous carbon microspheres (HPCMs) with a maze‐like structure and large mesopore tunnels for high‐performance tri‐phase catalytic ozonation. The confined assembly in drying microdroplets is crucial for coherent salt (NaCl) and surfactant (F127) dual templating without macroscopic phase separation. The HPCMs possess tunable sizes, a maze‐like structure with highly open macropores (0.3–30 µm) templated from NaCl crystal arrays, large intrawall mesopore tunnels (10–45 nm) templated from F127, and rich micropores (surface area >1000 m2 g−1) and oxygen heteroatoms originated from NaCl‐confined carbonization of phenolic resin. The structure formation mechanism of the HPCMs and several influencing factors on properties are elaborated. The HPCMs exhibit superior performance in gas–liquid–solid tri‐phase catalytic ozonation for oxalate degradation, owing to their hierarchical pore structure for fast mass transfer and rich defects and oxygen‐containing groups (especially carbonyl) for efficient O3 activation. The reactive oxygen species responsible for oxalate degradation and the influences of several structure parameters on performance are discussed. This work may provide a platform for producing hierarchically porous materials for various applications.

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In-situ formation of surface reactive oxygen species on defective sites over N-doped biochar in catalytic ozonation

Cited by 40 publications

References 88 publications

Synergistic Catalytic Ozonation Mediated by Dual Active Sites of Oxygen Vacancies and Defects in Biomass-Derived Composites for Long-Lasting Water Decontamination

Synergistic Catalytic Ozonation Mediated by Dual Active Sites of Oxygen Vacancies and Defects in Biomass-Derived Composites for Long-Lasting Water Decontamination

Synergistic graphene-MnOx/honeycomb activated carbon (G-MnOx/HAC) and plasma technology for eradication of pathogenic microorganisms

3D Carbon Microspheres with a Maze‐Like Structure and Large Mesopore Tunnels Built From Rapid Aerosol‐Confined Coherent Salt/Surfactant Templating

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