journal article·2025-01-01Open access

Highly selective generation of singlet oxygen via peroxymonosulfate activation by Mn–N supported biochar

Huan Wu, Fangfang Ji, Bin Zhou, Shikun Gao, Zhe Zhang

AIP Advances· Volume 15· Issue 1

Abstract

In this study, manganese–nitrogen sites were incorporated into biochar (BC) to activate peroxymonosulfate (PMS) for the degradation of sulfamethoxazole (SMX). Characterization techniques, including scanning electron microscopy and others, confirmed the successful doping of Manganese–Nitrogen (Mn–N) sites into the BC (referred to as MnN@BC). The study revealed that the integration of Mn–N active sites in BC modified the electronic polarization and facilitated electron transfer. It is worth noting that a remarkable synergistic effect (SI = 6.92) was witnessed in the MnN@BC/PMS system. Under optimal conditions, SMX was nearly completely eliminated within 40 minutes. Radical scavenging experiments indicated that Hydroxyl Radical (•OH), Sulfate Radicals (SO4•−), superoxide radicals (O2•−), and singlet oxygen (1O2) all played significant roles in the degradation of SMX. Density functional theory calculations were employed to further investigate the mechanism of enhanced electron transfer of PMS facilitated by the loading of BC on the Mn–N site. Cyclic experiments and characterizations conducted before and after recycling demonstrated that MnN@BC exhibited remarkable stability and reusability. This study probed into the mechanism of PMS activation by transition metal and non-metal dual active sites and offered strategies for more effective and sustainable degradation of pollutants.
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Research context

OpenAlex topics: Advanced oxidation water treatment · Advanced Photocatalysis Techniques · Water Quality Monitoring and Analysis

SciVX discovery tags are terminology-based. OpenAlex topics are source-provided classifications.

Affiliations

Intelligent Construction Technology Application Service Center, School of Architecture and Engineering, Chongqing City Vocational College 1 , Chongqing 402160,

T. Y. Lin International 2 , Chongqing 400074,

School of River and Ocean Engineering, Chongqing Jiaotong University 3 , Chongqing 400074,

Environmental Engineering and Science Program, Department of Chemical and Environmental Engineering (ChEE), University of Cincinnati 4 , Cincinnati, Ohio 45221-0071,

Funding

2023 Science and Technology project of Chongqing City Vocational College · Research and Innovation Program for Graduate Students in Chongqing Jiaotong University

References (42)

Show source-provided references
1. Heavy metal water pollution: A fresh look about hazards, novel and conventional remediation methods10.1016/j.eti.2021.101504 ↗
2. A comprehensive update on antibiotics as an emerging water pollutant and their removal using nano-structured photocatalysts10.1016/j.jece.2020.104796 ↗
3. A review on the ecotoxicological effect of sulphonamides on aquatic organisms10.1016/j.toxrep.2022.03.034 ↗
4. Transformation products of sulfonamides in aquatic systems: Lessons learned from available environmental fate and behaviour data10.1016/j.scitotenv.2022.154744 ↗
5. Occurrence and adsorptive removal of sulfonamides and β-blockers in African and Asian water matrices: A comprehensive review10.1016/j.envadv.2023.100435 ↗
6. Construction of a myoglobin scaffold-based biocatalyst for the biodegradation of sulfadiazine and sulfathiazole10.1016/j.jhazmat.2023.133147 ↗
7. Environmental impact and biological removal processes of pharmaceutically active compounds: The particular case of sulfonamides, anticonvulsants and steroid estrogens10.1080/10643389.2019.1642831 ↗
8. Critical review on hazardous pollutants in water environment: Occurrence, monitoring, fate, removal technologies and risk assessment10.1016/j.scitotenv.2021.149134 ↗
9. Sulfate radicals-based advanced oxidation technology in various environmental remediation: A state-of-the-art review10.1016/j.cej.2020.126232 ↗
10. Nonradical oxidation processes in PMS-based heterogeneous catalytic system: Generation, identification, oxidation characteristics, challenges response and application prospects10.1016/j.cej.2020.128312 ↗
11. Strategies for enhancing peroxymonosulfate activation by heterogenous metal-based catalysis: A review10.1016/j.cjche.2022.07.032 ↗
12. Metal-based catalysts for persulfate and peroxymonosulfate activation in heterogeneous ways: A review10.1016/j.cej.2021.132323 ↗
13. Applications of vacancy defect engineering in persulfate activation: Performance and internal mechanism10.1016/j.jhazmat.2023.130971 ↗
14. Unveiling the versatile performance of transition metal sulfides in peroxymonosulfate activation10.1016/j.cej.2024.154682 ↗
15. Heterogeneous activation of persulfate by metal and non-metal catalyst for the degradation of sulfamethoxazole: A review10.1016/j.cej.2022.135277 ↗
16. Ordered mesoporous materials for water pollution treatment: Adsorption and catalysis10.1016/j.gee.2023.11.001 ↗
17. The application of transition metal-modified biochar in sulfate radical based advanced oxidation processes10.1016/j.envres.2022.113340 ↗
18. Recent advancements and challenges in emerging applications of biochar-based catalysts10.1016/j.biotechadv.2023.108181 ↗
19. Potential role of biochar in advanced oxidation processes: A sustainable approach10.1016/j.cej.2020.126582 ↗
20. Radical induced degradation of acetaminophen with Fe3O4 magnetic nanoparticles as heterogeneous activator of peroxymonosulfate10.1016/j.jhazmat.2014.05.068 ↗
21. Enhanced peroxymonosulfate activation via complexed Mn(II): A novel non-radical oxidation mechanism involving manganese intermediates10.1016/j.watres.2021.116856 ↗
22. Transition metal single-atom embedded on N-doped carbon as a catalyst for peroxymonosulfate activation: A DFT study10.1016/j.cej.2022.135428 ↗
23. Dual redox cycles of Mn(Ⅱ)/Mn(III) and Mn(III)/Mn(IV) on porous Mn/N co-doped biochar surfaces for promoting peroxymonosulfate activation and ciprofloxacin degradation10.1016/j.jcis.2022.12.008 ↗
24. Regulating Fe-spin state by atomically dispersed Mn–N in Fe–N–C catalysts with high oxygen reduction activity10.1360/tb-2021-0145 ↗
25. Iron-nitrogen co-doped biochar (FeN@BC) as particle electrode for three-dimensional (3D) electro-peroxydisulfate process for tetracycline degradation10.1063/5.0197850 ↗
26. Degradation of organic pollutants by peroxymonosulfate activated by MnO2 with different crystalline structures: Catalytic performances and mechanisms10.1016/j.cej.2019.05.170 ↗
27. Manganese-nitrogen co-doped biochar (MnN@BC) as particle electrode for three-dimensional (3D) electro-activation of peroxydisulfate: Active sites enhanced radical/non-radical oxidation10.1016/j.jhazmat.2023.132089 ↗
28. Shake up satellites and fluorescence property of carbon nitride and hydrogenated carbon nitride: Annealing effect10.1016/j.susc.2012.11.003 ↗
29. Mn-modification effects on Nb2O5 structural, optical and vibrational properties10.1088/1742-6596/935/1/012047 ↗
30. Effect of g-C3N4 amount on green synthesized GdFeO3/g-C3N4 nanocomposites as promising compounds for solid-state hydrogen storage10.1016/j.ijhydene.2022.02.202 ↗
31. MoS2 nanosheets: A designed structure with high active site density for the hydrogen evolution reaction10.1021/cs400384h ↗
32. Nonradical degradation of microorganic pollutants by magnetic N-doped graphitic carbon: A complement to the unactivated peroxymonosulfate10.1016/j.cej.2019.123724 ↗
33. Roles of structure defect, oxygen groups and heteroatom doping on carbon in nonradical oxidation of water contaminants10.1016/j.watres.2020.116244 ↗
34. The generation and transformation mechanisms of reactive oxygen species in the environment and their implications for pollution control processes: A review10.1016/j.envres.2024.119592 ↗
35. MOFs-derived defect carbon encapsulated magnetic metallic Co nanoparticles capable of efficiently activating PMS to rapidly degrade dyes10.1016/j.seppur.2022.120812 ↗
36. Influences and mechanisms of phosphate ions onto persulfate activation and organic degradation in water treatment: A review10.1016/j.watres.2022.118896 ↗
37. N-doped graphite encapsulated metal nanoparticles catalyst for removal of bisphenol A via activation of peroxymonosulfate: A singlet oxygen-dominated oxidation process10.1016/j.cej.2021.128890 ↗
38. Review of characteristics, generation pathways and detection methods of singlet oxygen generated in advanced oxidation processes (AOPs)10.1016/j.cej.2023.143778 ↗
39. Natural magnetite as an efficient green catalyst boosting peroxydisulfate activation for pollutants degradation10.1016/j.cej.2024.151076 ↗
40. Mn-doped g-C3N4 composite to activate peroxymonosulfate for acetaminophen degradation: The role of superoxide anion and singlet oxygen10.1016/j.cej.2018.11.165 ↗
41. A new generation pathway of singlet oxygen in heterogeneous single–atom Mn catalyst/peroxymonosulfate system10.1016/j.cej.2024.148629 ↗
42. A comparative study of multicomponent adsorption of phenolic compounds on GAC and ACFs10.1016/j.jhazmat.2008.12.086 ↗