Abstract
We investigated the influence mechanism of N-doping for dissolved black carbon (DBC) photodegradation of organic pollutants. The degradation performance of N-doped dissolved black carbon (NDBC) for tetracycline (TC) (71%) is better than that for methylene blue (MB) (28%) under irradiation. These levels are both better than DBC degradation performances for TC (68%) and MB (18%) under irradiation. Reactive species quenching experiments suggest that h+ and \(\cdot{\rm{O}}_2^ - \) are the main reactive species for NDBC photodegraded TC, while ·OH and h+ are the main reactive species for NDBC photodegraded MB. ·OH is not observed during DBC photodegradation of MB. This is likely because N-doping increases valence-band (VB) energy from 1.55 eV in DBC to 2.04 eV in NDBC; the latter is strong enough to oxidize water to form ·OH. Additionally, N-doping increases the DBC band gap of 2.29 to 2.62 eV in NDBC, resulting in a higher separation efficiency of photo-generated electrons-holes in NDBC than in DBC. All these factors give NDBC stronger photodegradation performance for TC and MB than DBC. High-performance liquid chromatography-mass spectrometry (HPLC-MS) characterization and toxicity evaluation with the quantitative structure-activity relationship (QSAR) method suggest that TC photodegradation intermediates produced by NDBC have less aromatic structure and are less toxic than those produced by DBC. We adopted a theoretical approach to clarify the relationship between the surface groups of NDBC and the photoactive species produced. Our results add to the understanding of the photochemical behavior of NDBC.
摘要
目 的
1. 将传统解释可溶性黑炭(DBC)结构的理论与能带结构理论相结合, 定量研究DBC的光活性物种与能带结构的关系. 2. 阐明氮元素掺杂对DBC结构光降解污染物的影响机制.
创新点
通过能带结构理论阐明氮元素掺杂使DBC对有机污染物具有更高的光降解性能的机制.
方 法
1. 通过实验分析, 证明氮元素成功掺入DBC; 2. 通过光降解实验数据, 证明氮掺杂的DBC提高对有机污染物的光降解效率; 3. 通过活性物种捕获和分子探针实验确定主要的贡献物种, 进一步结合能带结构理论阐明两种可溶性的黑碳在光降解过程中产生的贡献物种的不同的原因.
结 论
氮掺杂促进了生物炭衍生的DBC对四环素 (TC) 和亚甲基蓝 (MB) 的光降解性能. 这可能是由于以下原因: (1)氮掺杂使DBC的价带能量从1.55 eV增加到氮掺杂的可溶性黑炭 (NDBC) 的2.04 eV, 这足以使NDBC的水氧化形成·OH. 换句话说, NDBC可以产生–OH和 \(\cdot{\rm{O}}_2^ - \), 而DBC只能产生 \({\rm{O}}_2^ - \). (2) 氮掺杂使DBC的带隙从2.29 eV增加到2.62 eV, 从而导致光生电子孔的分离效率提高, 最终促进光降解效率. (3) 氮掺杂降低DBC在光照下的稳定性, 使DBC对可见光的反应更加灵敏.
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This work is supported by the Project of the State Key Laboratory of Pollution Control and Resource Reuse Foundation, Nanjing University (No. PCRRF21012), and the Project Funded by the Priority Academic Program Development of Jiangsu Higher Education Institutions, China. The authors thank the High-Performance Computing Center of Nanjing University for its support in theoretical calculation.
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Ying GUO and Yong GUO conceived and designed the study. Guowei XU produced and characterized the dissolved black carbon. Zixuan XU and Keophoungeun KANMANY performed the analysis of the photodegradation mechanisms. Ying GUO performed the possible photodegradation pathways and toxicity analysis. Ting CHEN and Yong GUO performed the computation section. Ying GUO, Mengxia CHEN, Soukthakhane SINSONESACK, and Yong GUO wrote the paper and revised and edited the final version with contributions obtained from all authors.
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N-doping offering higher photodegradation performance of dissolved black carbon for organic pollutants: experimental and theoretical studies
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Guo, Y., Chen, M., Chen, T. et al. N-doping offering higher photodegradation performance of dissolved black carbon for organic pollutants: experimental and theoretical studies. J. Zhejiang Univ. Sci. A 25, 340–356 (2024). https://doi.org/10.1631/jzus.A2300081
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DOI: https://doi.org/10.1631/jzus.A2300081