Enhancing the catalytic activity of g-C3N4 through Me doping (Me = Cu, Co and Fe) for selective sulfathiazole degradation via redox-based advanced oxidation process

被引:251
|
作者
Oh, Wen-Da [1 ]
Chang, Victor W. C. [1 ]
Hu, Zhong-Ting [2 ]
Goei, Ronn [1 ]
Lim, Teik-Thye [1 ,2 ]
机构
[1] Nanyang Technol Univ, Nanyang Environm & Water Res Inst, 1 Cleantech Loop,CleanTech One, Singapore 637141, Singapore
[2] Nanyang Technol Univ, Div Environm & Water Resources Engn, Sch Civil & Environm Engn, 50 Nanyang Ave, Singapore 639798, Singapore
关键词
Sulfate radical; Graphitic carbon nitride; Metal-doped; Peroxymonosulfate; Sulfathiazole; Secondary wastewater effluent; CARBON NITRIDE NANOSHEET; NATURAL ORGANIC-MATTER; HETEROGENEOUS CATALYSTS; RATE CONSTANTS; PEROXYMONOSULFATE; REMOVAL; WATER; PERSULFATE; MECHANISM; RADICALS;
D O I
10.1016/j.cej.2017.04.107
中图分类号
X [环境科学、安全科学];
学科分类号
08 ; 0830 ;
摘要
In this study, Me-doped g-C3N4 (Me = Cu, Co and Fe) catalysts with various % w/w of Me dopant are prepared by a versatile calcination protocol for catalytic redox-based advanced oxidation process. The characterization study using FESEM, EDX, TEM, XRD, TGA, XPS, FTIR and BET indicates that all the Me-doped g-C3N4 consist of irregular morphology with at least 1.4-1.9 times higher surface area than that of pristine g-C3N4. The catalysts were used to generate SO4 center dot- from peroxymonosulfate (PMS) for selective sulfathiazole (STZ) degradation. The results show that the catalytic activities of the Me -doped g-C3N4 are in the following order: Co-doped g-C3N4 (0.59% wow Co, Co-g-4) > Fe -doped g-C3N4 >> Cu-doped g-C3N4 similar to pristine g-C3N4. The excessive Me doping have a negative effect on catalytic performance due to the undesired SO4 center dot- scavenging by surface defects (-C N) and excess Me. The STZ degradation were highly influenced by the pH, catalyst loading and Oxone (R) dosage. The predominant reactive radical is identified to be SO4 which contributes to >82% of total STZ degradation. The LC/MS/MS system was used to confirm the selectivity of SO4 center dot- for STZ degradation. The main STZ degradation pathway is also proposed. The performance of Co-g-4/PMS system for STZ removal in the treated drinking water (TW) and secondary wastewater effluent (SE) was investigated. It is found that, despite having poorer performance compared with the DI water due to the presence of various water matrix species particularly the dissolved organic matter, the selectivity of SO4 center dot- for STZ in SE and TW is evidenced. Overall, the Co-g-4/PMS system shows promising performance and excellent stability for selective catalytic degradation of sulfonamide antibiotics in water. (C) 2017 Elsevier B.V. All rights reserved.
引用
收藏
页码:260 / 269
页数:10
相关论文
共 48 条
  • [41] Z-scheme g-C3N4/Bi6Fe1.5Co0.5Ti3O18 heterojunctions with enhanced visible-light photocatalytic activity towards organics degradation
    Ge, Wen
    Liu, Kong
    Deng, Shukang
    Shen, Lanxian
    Yang, Peizhi
    APPLIED SURFACE SCIENCE, 2022, 572
  • [42] High performance of reduced graphene oxide and g-C3N4 co-doped CuFe2O4 for peroxymonosulfate activation under visible light: Degradation process of sulfamethazine via a singlet oxygen dominated pathway
    Zhou, Jianzhuo
    Sun, Qiunan
    Wang, Xuejiang
    Liu, Yiyang
    Xia, Siqing
    Zhao, Jianfu
    CHEMICAL ENGINEERING JOURNAL, 2024, 485
  • [43] Associative Role of g-C3N4 to BiVO4 via Favorable Crystallinity and Rapid Charge-Carrier Transport for an Improved Photoelectrochemical Water Oxidation Process: An In Situ Composite Explored through Different Carbon Nitride Precursors
    Ghosh, Sangeeta
    Hajra, Paramita
    Kundu, Sukumar
    Baduri, Swarnendu
    Ray, Debasish
    Bhattacharya, Chinmoy
    ACS APPLIED ENGINEERING MATERIALS, 2023, 1 (11): : 2892 - 2902
  • [44] A novel S-scheme photocatalyst Fe2O3/Bi2O3/g-C3N4 with enhanced visible-light photocatalytic performance for antibiotic degradation and CO2 reduction: RSM-based optimization
    Amari, Abdelfattah
    Aljibori, Hakim S. Sultan
    Algarni, Zaina
    Elboughdiri, Noureddine
    Diab, M. A.
    Baek, Kwang-Hyun
    Mahariq, Ibrahim
    JOURNAL OF INDUSTRIAL AND ENGINEERING CHEMISTRY, 2024, 140 : 599 - 616
  • [45] An innovative dual-mode catalytic strategy for Boosting the Mineralization of organic pollutants through Dark-Light Cycle-Mediated Alternative Transformation pathways with NC/C3N4 in persulfate-based advanced oxidation process
    Cheng, Junjie
    Tu, Xinman
    Lv, Xinding
    Zhang, Li
    Zhou, Rentao
    Luo, Shaohua
    Zeng, Honghu
    Li, Tingting
    Zou, Jianping
    CHEMICAL ENGINEERING JOURNAL, 2025, 506
  • [46] Theoretical insights of catalytic oxidation of Hg0 on g-C3N4-supported Fe/Co/Ni-based bi-metallic catalysts using O2 in coal-fired flue gas as the oxidant
    Liu, Shuai
    Xu, Mengxia
    Pang, Chengheng
    Lester, Edward
    Wu, Tao
    FUEL, 2021, 306
  • [47] Theoretical insights of catalytic oxidation of Hg0 on g-C3N4-supported Fe/Co/Ni-based bi-metallic catalysts using O2 in coal-fired flue gas as the oxidant
    Liu, Shuai
    Xu, Mengxia
    Pang, Chengheng
    Lester, Edward
    Wu, Tao
    Fuel, 2021, 306
  • [48] Preparation of Ag-doped g-C3N4 Nano Sheet Decorated Magnetic -Fe2O3@SiO2 Core-Shell Hollow Spheres through a Novel Hydrothermal Procedure: Investigation of the Catalytic activity for A3, KA2 Coupling Reactions and [3+2] Cycloaddition
    Sadjadi, Samahe
    Malmir, Masoumeh
    Heravi, Majid M.
    APPLIED ORGANOMETALLIC CHEMISTRY, 2018, 32 (08)