Catalytic activation of peroxymonosulfate by Mn/N co-doped porous carbon for effective phenol degradation: crucial role of non-radical pathways

被引:8
作者
Guo, Qi [1 ]
Xu, Jihong [1 ]
Tang, Rui [1 ,2 ]
Min, Yulin [1 ,2 ]
Hu, Zhenhu [3 ]
Shi, Penghui [1 ,2 ]
机构
[1] Shanghai Univ Elect Power, Shanghai Key Lab Mat Protect & Adv Mat Elect Power, Shanghai 200090, Peoples R China
[2] Shanghai Inst Pollut Control & Ecol Secur, Shanghai 200090, Peoples R China
[3] Hefei Univ Technol, Sch Civil Engn, Anhui Engn Lab Rural Water Environm & Resource, Hefei 230009, Peoples R China
关键词
ADVANCED OXIDATION; PERSULFATE; GRAPHENE; OXYGEN; PMS; PEROXYDISULFATE; EVOLUTION; RADICALS;
D O I
10.1039/d3nj00340j
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
In the degradation process of organic pollutants, compared with the free radical pathway, the non-radical pathway shows the advantages of mild oxidation ability, strong anti-interference, and adaptation to different pH values. In this study, a manganese-nitrogen co-doped porous carbon (Mn-N@C-1) with high nitrogen content was prepared to improve the contribution rate of non-radical pathways to the degradation process of organic pollutants. The high performance of Mn-N@C-1 is attributed to the formation of Mn-N-x sites between Pyridine N and Mn, which can effectively oxidize organic pollutants in water (phenol, bisphenol A, 2,4-dichlorophenol). In addition, the catalyst exhibits high catalytic activity over a wide pH range (pH = 3-9) and has good immunity to inorganic anions. Moreover, the Mn-N-x site and graphitic-N are considered to be the generation sites of singlet oxygen, and the role of metastable Mn-N@C-1/PMS* complexes in the electron transfer process is explored. Overall, this study explores the crucial role of non-radical pathways in the degradation of organic pollutants by carbon-based materials.
引用
收藏
页码:5420 / 5430
页数:11
相关论文
共 57 条
  • [1] Identification of hydroxyl and sulfate free radicals involved in the reaction of 1,4-dioxane with peroxone activated persulfate oxidant
    Cashman, Michaela A.
    Kirschenbaum, Louis
    Holowachuk, Justin
    Boving, Thomas B.
    [J]. JOURNAL OF HAZARDOUS MATERIALS, 2019, 380
  • [2] Non-photochemical production of singlet oxygen via activation of persulfate by carbon nanotubes
    Cheng, Xin
    Guo, Hongguang
    Zhang, Yongli
    Wu, Xiao
    Liu, Yang
    [J]. WATER RESEARCH, 2017, 113 : 80 - 88
  • [3] Cobalt Single Atoms on Tetrapyridomacrocyclic Support for Efficient Peroxymonosulfate Activation
    Chu, Chiheng
    Yang, Ji
    Zhou, Xuechen
    Huang, Dahong
    Qi, Haifeng
    Weon, Seunghyun
    Li, Jianfeng
    Elimelech, Menachem
    Wang, Aiqin
    Kim, Jae-Hong
    [J]. ENVIRONMENTAL SCIENCE & TECHNOLOGY, 2021, 55 (02) : 1242 - 1250
  • [4] Co/N co-doped carbonaceous polyhedron as efficient peroxymonosulfate activator for degradation of organic pollutants: Role of cobalt
    Dai, Huiwang
    Zhou, Wenjun
    Wang, Wei
    [J]. CHEMICAL ENGINEERING JOURNAL, 2021, 417
  • [5] Biochar co-doped with nitrogen and boron switching the free radical based peroxydisulfate activation into the electron-transfer dominated nonradical process
    Dou, Jibo
    Cheng, Jie
    Lu, Zhijiang
    Tian, Ziqi
    Xu, Jianming
    He, Yan
    [J]. APPLIED CATALYSIS B-ENVIRONMENTAL, 2022, 301
  • [6] Peroxydisulfate activation by atomically-dispersed Fe-Nx on N-doped carbon: Mechanism of singlet oxygen evolution for nonradical degradation of aqueous contaminants
    Du, Ningjie
    Liu, Ying
    Li, Qiuju
    Miao, Wei
    Wang, Dandan
    Mao, Shun
    [J]. CHEMICAL ENGINEERING JOURNAL, 2021, 413
  • [7] Sulfate saturated biosorbent-derived Co-S@NC nanoarchitecture as an efficient catalyst for peroxymonosulfate activation
    Du, Weiyan
    Zhang, Qingzhu
    Shang, Yanan
    Wang, Wei
    Li, Qian
    Yue, Qinyan
    Gao, Baoyu
    Xu, Xing
    [J]. APPLIED CATALYSIS B-ENVIRONMENTAL, 2020, 262
  • [8] Insights into perovskite-catalyzed peroxymonosulfate activation: Maneuverable cobalt sites for promoted evolution of sulfate radicals
    Duan, Xiaoguang
    Su, Chao
    Miao, Jie
    Zhong, Yijun
    Shao, Zongping
    Wang, Shaobin
    Sun, Hongqi
    [J]. APPLIED CATALYSIS B-ENVIRONMENTAL, 2018, 220 : 626 - 634
  • [9] Nitrogen-Doped Graphene for Generation and Evolution of Reactive Radicals by Metal-Free Catalysis
    Duan, Xiaoguang
    Ao, Zhimin
    Sun, Hongqi
    Indrawirawan, Stacey
    Wang, Yuxian
    Kang, Jian
    Liang, Fengli
    Zhu, Z. H.
    Wang, Shaobin
    [J]. ACS APPLIED MATERIALS & INTERFACES, 2015, 7 (07) : 4169 - 4178
  • [10] Mn-doped g-C3N4 composite to activate peroxymonosulfate for acetaminophen degradation: The role of superoxide anion and singlet oxygen
    Fan, Jinhong
    Qin, Hehe
    Jiang, Simin
    [J]. CHEMICAL ENGINEERING JOURNAL, 2019, 359 : 723 - 732