Collaborative modification strategy to improve the formation of biochar-derived persistent free radicals for aniline removal via peroxymonosulfate activation
Abstract This study explores a novel approach to biochar modification aimed at increasing persistent free radical (PFR) formation on biochar surfaces, thereby enhancing aniline removal via peroxymonosulfate (PMS) activation. By adjusting pyrolysis temperatures and doping ratios, optimal conditions w...
Saved in:
| Main Authors: | , , , , , , , , , |
|---|---|
| Format: | Article |
| Language: | English |
| Published: |
Springer
2025-01-01
|
| Series: | Biochar |
| Subjects: | |
| Online Access: | https://doi.org/10.1007/s42773-024-00416-0 |
| Tags: |
Add Tag
No Tags, Be the first to tag this record!
|
| _version_ | 1832571469225263104 |
|---|---|
| author | Zilong Zhao Shuting Zhu Shuyu Qi Ting Zhou Yang Yang Feng Wang Qi Han Wenyi Dong Hongjie Wang Feiyun Sun |
| author_facet | Zilong Zhao Shuting Zhu Shuyu Qi Ting Zhou Yang Yang Feng Wang Qi Han Wenyi Dong Hongjie Wang Feiyun Sun |
| author_sort | Zilong Zhao |
| collection | DOAJ |
| description | Abstract This study explores a novel approach to biochar modification aimed at increasing persistent free radical (PFR) formation on biochar surfaces, thereby enhancing aniline removal via peroxymonosulfate (PMS) activation. By adjusting pyrolysis temperatures and doping ratios, optimal conditions were established. Spearman's analysis highlighted the importance of C=C bonds, the ID/IG ratio, and pyridinic N in generating PFRs. The modified biochar derived at 500 ℃ (MB500), in conjunction with the PMS system demonstrated impressive efficiency, achieving 92% aniline removal within 30 min. Detailed adsorption tests and active species detection indicated that aniline degradation occurred through both direct oxidation by PFRs and indirect oxidation by reactive species, particularly superoxide radicals (O₂⋅⁻). Furthermore, the synergistic effects of heteroatom nitrogen and Na2CO3 modifications significantly impacted PFR formation and stability. These findings provide valuable insights into the mechanisms of PFR-mediated catalytic oxidation, highlighting the key roles of pyridinic rings, with or without oxygenated groups, in enhancing catalytic performance of biochar. This research advances the understanding of biochar surface chemistry and presents an effective strategy for developing high-performance biochar-based catalysts for environmental remediation, addressing the limitations of unmodified biochar through targeted surface modifications. Graphical Abstract |
| format | Article |
| id | doaj-art-acc2006425924026b270f783ab7dfa4b |
| institution | Kabale University |
| issn | 2524-7867 |
| language | English |
| publishDate | 2025-01-01 |
| publisher | Springer |
| record_format | Article |
| series | Biochar |
| spelling | doaj-art-acc2006425924026b270f783ab7dfa4b2025-02-02T12:35:44ZengSpringerBiochar2524-78672025-01-017111910.1007/s42773-024-00416-0Collaborative modification strategy to improve the formation of biochar-derived persistent free radicals for aniline removal via peroxymonosulfate activationZilong Zhao0Shuting Zhu1Shuyu Qi2Ting Zhou3Yang Yang4Feng Wang5Qi Han6Wenyi Dong7Hongjie Wang8Feiyun Sun9School of Civil and Environmental Engineering, Harbin Institute of Technology ShenzhenSchool of Civil and Environmental Engineering, Harbin Institute of Technology ShenzhenSchool of Civil and Environmental Engineering, Harbin Institute of Technology ShenzhenSchool of Civil and Environmental Engineering, Harbin Institute of Technology ShenzhenSchool of Civil and Environmental Engineering, Harbin Institute of Technology ShenzhenSchool of Civil and Environmental Engineering, Harbin Institute of Technology ShenzhenSchool of Civil and Environmental Engineering, Harbin Institute of Technology ShenzhenSchool of Civil and Environmental Engineering, Harbin Institute of Technology ShenzhenSchool of Civil and Environmental Engineering, Harbin Institute of Technology ShenzhenSchool of Civil and Environmental Engineering, Harbin Institute of Technology ShenzhenAbstract This study explores a novel approach to biochar modification aimed at increasing persistent free radical (PFR) formation on biochar surfaces, thereby enhancing aniline removal via peroxymonosulfate (PMS) activation. By adjusting pyrolysis temperatures and doping ratios, optimal conditions were established. Spearman's analysis highlighted the importance of C=C bonds, the ID/IG ratio, and pyridinic N in generating PFRs. The modified biochar derived at 500 ℃ (MB500), in conjunction with the PMS system demonstrated impressive efficiency, achieving 92% aniline removal within 30 min. Detailed adsorption tests and active species detection indicated that aniline degradation occurred through both direct oxidation by PFRs and indirect oxidation by reactive species, particularly superoxide radicals (O₂⋅⁻). Furthermore, the synergistic effects of heteroatom nitrogen and Na2CO3 modifications significantly impacted PFR formation and stability. These findings provide valuable insights into the mechanisms of PFR-mediated catalytic oxidation, highlighting the key roles of pyridinic rings, with or without oxygenated groups, in enhancing catalytic performance of biochar. This research advances the understanding of biochar surface chemistry and presents an effective strategy for developing high-performance biochar-based catalysts for environmental remediation, addressing the limitations of unmodified biochar through targeted surface modifications. Graphical Abstracthttps://doi.org/10.1007/s42773-024-00416-0Persistent free radicalsBiocharSynergistic modificationPeroxymonosulfateAniline degradation |
| spellingShingle | Zilong Zhao Shuting Zhu Shuyu Qi Ting Zhou Yang Yang Feng Wang Qi Han Wenyi Dong Hongjie Wang Feiyun Sun Collaborative modification strategy to improve the formation of biochar-derived persistent free radicals for aniline removal via peroxymonosulfate activation Biochar Persistent free radicals Biochar Synergistic modification Peroxymonosulfate Aniline degradation |
| title | Collaborative modification strategy to improve the formation of biochar-derived persistent free radicals for aniline removal via peroxymonosulfate activation |
| title_full | Collaborative modification strategy to improve the formation of biochar-derived persistent free radicals for aniline removal via peroxymonosulfate activation |
| title_fullStr | Collaborative modification strategy to improve the formation of biochar-derived persistent free radicals for aniline removal via peroxymonosulfate activation |
| title_full_unstemmed | Collaborative modification strategy to improve the formation of biochar-derived persistent free radicals for aniline removal via peroxymonosulfate activation |
| title_short | Collaborative modification strategy to improve the formation of biochar-derived persistent free radicals for aniline removal via peroxymonosulfate activation |
| title_sort | collaborative modification strategy to improve the formation of biochar derived persistent free radicals for aniline removal via peroxymonosulfate activation |
| topic | Persistent free radicals Biochar Synergistic modification Peroxymonosulfate Aniline degradation |
| url | https://doi.org/10.1007/s42773-024-00416-0 |
| work_keys_str_mv | AT zilongzhao collaborativemodificationstrategytoimprovetheformationofbiocharderivedpersistentfreeradicalsforanilineremovalviaperoxymonosulfateactivation AT shutingzhu collaborativemodificationstrategytoimprovetheformationofbiocharderivedpersistentfreeradicalsforanilineremovalviaperoxymonosulfateactivation AT shuyuqi collaborativemodificationstrategytoimprovetheformationofbiocharderivedpersistentfreeradicalsforanilineremovalviaperoxymonosulfateactivation AT tingzhou collaborativemodificationstrategytoimprovetheformationofbiocharderivedpersistentfreeradicalsforanilineremovalviaperoxymonosulfateactivation AT yangyang collaborativemodificationstrategytoimprovetheformationofbiocharderivedpersistentfreeradicalsforanilineremovalviaperoxymonosulfateactivation AT fengwang collaborativemodificationstrategytoimprovetheformationofbiocharderivedpersistentfreeradicalsforanilineremovalviaperoxymonosulfateactivation AT qihan collaborativemodificationstrategytoimprovetheformationofbiocharderivedpersistentfreeradicalsforanilineremovalviaperoxymonosulfateactivation AT wenyidong collaborativemodificationstrategytoimprovetheformationofbiocharderivedpersistentfreeradicalsforanilineremovalviaperoxymonosulfateactivation AT hongjiewang collaborativemodificationstrategytoimprovetheformationofbiocharderivedpersistentfreeradicalsforanilineremovalviaperoxymonosulfateactivation AT feiyunsun collaborativemodificationstrategytoimprovetheformationofbiocharderivedpersistentfreeradicalsforanilineremovalviaperoxymonosulfateactivation |