Synergistic multiple active species for the photocatalytic degradation of contaminants by imidazole-modified g-C3N4 coordination with iron phthalocyanine in the presence of peroxymonosulfate

被引:109
作者
Dong, Lulu [1 ]
Xu, Tiefeng [1 ]
Chen, Wenxing [1 ]
Lu, Wangyang [1 ]
机构
[1] Zhejiang Sci Tech Univ, Natl Engn Lab Text Fiber Mat & Proc Technol Zheji, Hangzhou 310018, Zhejiang, Peoples R China
基金
中国国家自然科学基金;
关键词
g-C3N4; Axial coordination; Peroxymonosulfate; Visible-light; Mechanism; ZERO-VALENT IRON; CARBON NITRIDE; DOPED G-C3N4; HETEROGENEOUS CATALYSTS; EMERGING CONTAMINANTS; HYDROGEN EVOLUTION; ADVANCED OXIDATION; FACILE SYNTHESIS; SINGLET OXYGEN; ELECTRO-FENTON;
D O I
10.1016/j.cej.2018.09.094
中图分类号
X [环境科学、安全科学];
学科分类号
08 ; 0830 ;
摘要
Utilizing peroxymonosulfate (PMS)-based advanced oxidation processes to remove emerging contaminants in water has received widespread attention. In this study, g-C3N4-IMA-FePcCl16 that was fabricated by axial coordination was applied to activate PMS for carbamazepine (CBZ) degradation. The introduction of imidazole-based ligand (IMA) and iron hexadecachlorophthalocyanine (FePcCl16) facilitates the photogenerated electron-hole pairs separation of g-C3N4 and broadens the visible-light response range. The coordination structure was characterized by X-ray diffraction and X-ray photoelectron spectroscopy. Photocatalytic experiments demonstrated that g-C3N4-IMA-FePcCl16 can highly effective eliminate CBZ with a removal of similar to 95% within 25 min in the presence of PMS. The effects of various experimental parameters on the CBZ degradation were investigated, such as the loading amount of FePcCl16, pH, PMS dosage and anions. It is noteworthy that Cl- has a positive effect on the degradation of CBZ. Another interesting finding is that the degradation of CBZ is attributed to the synergistic effect of multiple active species, which is confirmed by gas chromatography-mass spectrometry, electron paramagnetic resonance and radical quenching tests. Superoxide radicals (O-2(center dot-)) and singlet oxygen (O-1(2)) are the dominated active species. This work offers a novel idea for the rational design of high-efficiency photocatalysts for wastewater remediation.
引用
收藏
页码:198 / 208
页数:11
相关论文
共 62 条
[1]   Combination of UVC-LEDs and ultrasound for peroxymonosulfate activation to degrade synthetic dye: influence of promotional and inhibitory agents and application for real wastewater [J].
Ahmadi, Mehdi ;
Ghanbari, Farshid .
ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH, 2018, 25 (06) :6003-6014
[2]   Medium pressure UV-activated peroxymonosulfate for ciprofloxacin degradation: Kinetics, mechanism, and genotoxicity [J].
Ao, Xiuwei ;
Liu, Wenjun ;
Sun, Wenjun ;
Cai, Meiquan ;
Ye, Zi ;
Yang, Chao ;
Lu, Zedong ;
Li, Chen .
CHEMICAL ENGINEERING JOURNAL, 2018, 345 :87-97
[3]   Synthesis of porous carbon-doped g-C3N4 nanosheets with enhanced visible-light photocatalytic activity [J].
Bao, Nan ;
Hu, Xinde ;
Zhang, Qingzhe ;
Miao, Xinhan ;
Jie, Xiuyan ;
Zhou, Shuai .
APPLIED SURFACE SCIENCE, 2017, 403 :682-690
[4]   Facile synthesis of highly dispersed Fe(II)-doped g-C3N4 and its application in Fenton-like catalysis [J].
Bicalho, H. A. ;
Lopez, J. L. ;
Binatti, I. ;
Batista, P. F. R. ;
Ardisson, J. D. ;
Resende, R. R. ;
Lorencon, E. .
MOLECULAR CATALYSIS, 2017, 435 :156-165
[5]   Fast Photoelectron Transfer in (Cring)-C3N4 Plane Heterostructural Nanosheets for Overall Water Splitting [J].
Che, Wei ;
Cheng, Weiren ;
Yao, Tao ;
Tang, Fumin ;
Liu, Wei ;
Su, Hui ;
Huang, Yuanyuan ;
Liu, Qinghua ;
Liu, Jinkun ;
Hu, Fengchun ;
Pan, Zhiyun ;
Sun, Zhihu ;
Wei, Shiqiang .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2017, 139 (08) :3021-3026
[6]   Visible light photoactivity enhancement via CuTCPP hybridized g-C3N4 nanocomposite [J].
Chen, Daimei ;
Wang, Kewei ;
Hong, Wangzhi ;
Zong, Ruilong ;
Yao, Wenqing ;
Zhu, Yongfa .
APPLIED CATALYSIS B-ENVIRONMENTAL, 2015, 166 :366-373
[7]   Highly efficient removal of organic contaminants based on peroxymonosulfate activation by iron phthalocyanine: mechanism and the bicarbonate ion enhancement effect [J].
Dai, Dejun ;
Yang, Zhiyuan ;
Yao, Yuyuan ;
Chen, Likun ;
Jia, Guosheng ;
Luo, Lianshun .
CATALYSIS SCIENCE & TECHNOLOGY, 2017, 7 (04) :934-942
[8]   Mesoporous manganese Cobaltite nanocages as effective and reusable heterogeneous peroxymonosulfate activators for Carbamazepine degradation [J].
Deng, Jing ;
Cheng, Yong-qing ;
Lu, Yu-an ;
Crittenden, John C. ;
Zhou, Shi-qing ;
Gao, Nai-yun ;
Li, Jun .
CHEMICAL ENGINEERING JOURNAL, 2017, 330 :505-517
[9]   A direct Z-scheme g-C3N4/SnS2 photocatalyst with superior visible-light CO2 reduction performance [J].
Di, Tingmin ;
Zhu, Bicheng ;
Cheng, Bei ;
Yu, Jiaguo ;
Xu, Jingsan .
JOURNAL OF CATALYSIS, 2017, 352 :532-541
[10]   In Situ Construction of g-C3N4/g-C3N4 Metal-Free Heterojunction for Enhanced Visible-Light Photocatalysis [J].
Dong, Fan ;
Zhao, Zaiwang ;
Xiong, Ting ;
Ni, Zilin ;
Zhang, Wendong ;
Sun, Yanjuan ;
Ho, Wing-Kei .
ACS APPLIED MATERIALS & INTERFACES, 2013, 5 (21) :11392-11401