Crucial role of nitrogen vacancies in carbon activated persulfate toward nonradical abatement of micropollutants from secondary effluent

被引:15
作者
Li, Fangzhou [1 ]
Sun, Lu [2 ]
Wang, Haojie [1 ]
Dong, Heng [1 ]
Li, Fei [1 ]
Wu, Xiaoyan [3 ]
Zhan, Sihui [1 ,4 ]
机构
[1] Nankai Univ, Coll Environm Sci & Engn, MOE Key Lab Pollut Proc & Environm Criteria, Tianjin 300350, Peoples R China
[2] Nankai Univ, Inst Modern Opt, Tianjin Key Lab Microscale Opt Informat Sci & Tech, Tianjin 300350, Peoples R China
[3] Tianjin Recyclable Resources Inst, All China Federat Supply & Mkt Cooperat, Tianjin 300191, Peoples R China
[4] Tianjin Univ, Sch Environm Sci & Engn, Tianjin 300350, Peoples R China
来源
APPLIED CATALYSIS B-ENVIRONMENT AND ENERGY | 2025年 / 361卷
基金
中国国家自然科学基金;
关键词
Micropollutants; Persulfate activation; Nonradical oxidation; N vacancy; Microelectric field; Secondary effluent; DOPED GRAPHENE; SINGLET OXYGEN; REDUCTION; OXIDATION; REMOVAL; DEFECT;
D O I
10.1016/j.apcatb.2024.124584
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
Biomass-derived carbonaceous materials exhibit fascinating potentials in nonradical oxidation of micropollutants (MPs) by activating persulfate and their performances mainly rest on graphitic N. However, the simultaneously derived N vacancy received little attention. Herein, a graphene-like material rich in N vacancy was synthesized from coffee residues. It showed excellent removal efficiency (95 %) and degradation kinetics (0.21 min(-1)) in abating tetracycline antibiotics from secondary effluent and significant biotoxicity was diminished. Solid nonradical oxidation consisting of electron transfer (89 %) and singlet oxygen (O-1(2)) oxidation (11 %) was determined. By tracking O-1(2) source and electron flow, ketone group appeared at N vacancy was found as the critical site to grab electrons from peroxydisulfate (PDS) with production of O-1(2). Then the electrons were transferred to graphitic N driven by the microelectric field between them. This work notices the function of vacancies in biomass resources for high-efficient removal of MPs from real water matrix.
引用
收藏
页数:11
相关论文
共 61 条
[31]   An insight into metal organic framework derived N-doped graphene for the oxidative degradation of persistent contaminants: formation mechanism and generation of singlet oxygen from peroxymonosulfate [J].
Liang, Ping ;
Zhang, Chi ;
Duan, Xiaoguang ;
Sun, Hongqi ;
Liu, Shaomin ;
Tade, Moses O. ;
Wang, Shaobin .
ENVIRONMENTAL SCIENCE-NANO, 2017, 4 (02) :315-324
[32]   Rapid and selective oxidation of refractory sulfur-containing micropollutants in water using Fe-TAML/H2O2 [J].
Liu, Qingquan ;
Fu, Zhiqiang ;
Wang, Zhongyu ;
Chen, Jingwen ;
Cai, Xiyun .
APPLIED CATALYSIS B-ENVIRONMENTAL, 2022, 315
[33]   Peroxydisulfate activation by sulfur-doped ordered mesoporous carbon: Insight into the intrinsic relationship between defects and 1O2 generation [J].
Liu, Shiyu ;
Lai, Cui ;
Zhou, Xuerong ;
Zhang, Chen ;
Chen, Liang ;
Yan, Huchuan ;
Qin, Lei ;
Huang, Danlian ;
Ye, Haoyang ;
Chen, Wenfang ;
Li, Ling ;
Zhang, Mingming ;
Tang, Lin ;
Xu, Fuhang ;
Dengsheng .
WATER RESEARCH, 2022, 221
[34]   Electrochemical activation of periodate with graphite electrodes for water decontamination: Excellent applicability and selective oxidation mechanism [J].
Luo, Mengfan ;
Zhang, Heng ;
Shi, Yang ;
Zhao, Jia ;
Feng, Can ;
Yin, Jialong ;
Liu, Yang ;
Zhou, Peng ;
Xiong, Zhaokun ;
Lai, Bo .
WATER RESEARCH, 2023, 240
[35]   Micropollutants removal and health risk reduction in a water reclamation and ecological reuse system [J].
Ma, Xiaoyan Y. ;
Li, Qiyuan ;
Wang, Xiaochang C. ;
Wang, Yongkun ;
Wang, Donghong ;
Huu Hao Ngo .
WATER RESEARCH, 2018, 138 :272-281
[36]   2D N-Doped Porous Carbon Derived from Polydopamine-Coated Graphitic Carbon Nitride for Efficient Nonradical Activation of Peroxymonosulfate [J].
Miao, Jie ;
Geng, Wei ;
Alvarez, Pedro J. J. ;
Long, Mingce .
ENVIRONMENTAL SCIENCE & TECHNOLOGY, 2020, 54 (13) :8473-8481
[37]   Ball milling-assisted preparation of N-doped biochar loaded with ferrous sulfide as persulfate activator for phenol degradation: Multiple active sites-triggered radical/non-radical mechanism [J].
Qu, Jianhua ;
Xu, Yuan ;
Zhang, Xiubo ;
Sun, Mingze ;
Tao, Yue ;
Zhang, Xinmiao ;
Zhang, Guangshan ;
Ge, Chengjun ;
Zhang, Ying .
APPLIED CATALYSIS B-ENVIRONMENT AND ENERGY, 2022, 316
[38]   Origins of Electron-Transfer Regime in Persulfate-Based Nonradical Oxidation Processes [J].
Ren, Wei ;
Cheng, Cheng ;
Shao, Penghui ;
Luo, Xubiao ;
Zhang, Hui ;
Wang, Shaobin ;
Duan, Xiaoguang .
ENVIRONMENTAL SCIENCE & TECHNOLOGY, 2022, 56 (01) :78-97
[39]   The Intrinsic Nature of Persulfate Activation and N-Doping in Carbocatalysis [J].
Ren, Wei ;
Nie, Gang ;
Zhou, Peng ;
Zhang, Hui ;
Duan, Xiaoguang ;
Wang, Shaobin .
ENVIRONMENTAL SCIENCE & TECHNOLOGY, 2020, 54 (10) :6438-6447
[40]   Insights into the Electron-Transfer Regime of Peroxydisulfate Activation on Carbon Nanotubes: The Role of Oxygen Functional Groups [J].
Ren, Wei ;
Xiong, Liangliang ;
Nie, Gang ;
Zhang, Hui ;
Duan, Xiaoguang ;
Wang, Shaobin .
ENVIRONMENTAL SCIENCE & TECHNOLOGY, 2020, 54 (02) :1267-1275