TY - JOUR
T1 - Highly dispersive Ru confined in porous ultrathin g-C3N4 nanosheets as an efficient peroxymonosulfate activator for removal of organic pollutants
AU - Yin, Yu
AU - Liu, Mengxuan
AU - Shi, Lei
AU - Zhang, Shu
AU - Hirani, Rajan Arjan Kalyan
AU - Zhu, Chengzhang
AU - Chen, Chuanxiang
AU - Yuan, Aihua
AU - Duan, Xiaoguang
AU - Wang, Shaobin
AU - Sun, Hongqi
N1 - Funding Information:
This work is financially supported by the National Natural Science Foundation of China (51602133). The authors also show great appreciate to the Centre for Microscopy, Characterization and Analysis (CMCA) of the University of Western Australia for providing HAADF-STEM and element mapping imaging.
Funding Information:
This work is financially supported by the National Natural Science Foundation of China (51602133). The authors also show great appreciate to the Centre for Microscopy, Characterization and Analysis (CMCA) of the University of Western Australia for providing HAADF-STEM and element mapping imaging. Supported metal catalysts have been widely used in advanced oxidation processes (AOPs) for removal of various toxic organic pollutants. However, the activity is still far from satisfactory, mainly due to the restriction by the agglomeration of active metal species. In this work, a strategy is developed to prepare a supporting material of porous ultrathin g-C3N4 nanosheets to endow the high dispersion of active Ru sites without any aggregation. The efficiency for 2,4,6-trichlorophenol removal via peroxymonosulfate activation was thus dramatically improved as compared to Ru aggregating materials. Moreover, excellent performances in degradation of various contaminants were also demonstrated.
Publisher Copyright:
© 2022 Elsevier B.V.
PY - 2022/8/5
Y1 - 2022/8/5
N2 - Ru species were loaded on a two-dimensional (2D) material of graphitic carbon nitride (2D g-C3N4) to serve as the efficient AOP catalysts. The catalytic activity was closely related to the dispersion degree of Ru, as determined by the inherent nanoarchitecture of the supporting material. Ultrathin g-C3N4 nanosheets with a unique porous structure were fabricated by further thermally oxidizing and etching bulk g-C3N4 (bCN) in air. Homogeneous dispersion of Ru species was successfully achieved on the porous few-layered g-C3N4 nanosheets (pCN) by stirring, washing, freeze drying and annealing processes to obtain Ru-pCN catalysts, whereas bCN or multilayered g-C3N4 (mCN) led to the aggregation of Ru nanoparticles in Ru-bCN and Ru-mCN materials. The conventional impregnation method also caused the resulting Ru-pCN-imp catalyst with undesirable Ru aggregation in spite of employing pCN. The optimal 4.4Ru-pCN removed 100% of 2,4,6-trichlorophenol (TCP) within only 3 min, superior to its counterpart samples, and exhibited remarkable degradation efficiencies for methyl orange, neutral red, 4-chlorophenol, tetracycline and oxytetracycline. Mechanistic studies suggested that four radicals, e.g., •OH, SO4• −, O2• − and 1O2 were generated during the peroxymonosulfate (PMS) activation, in which SO4• − and 1O2 played a major role.
AB - Ru species were loaded on a two-dimensional (2D) material of graphitic carbon nitride (2D g-C3N4) to serve as the efficient AOP catalysts. The catalytic activity was closely related to the dispersion degree of Ru, as determined by the inherent nanoarchitecture of the supporting material. Ultrathin g-C3N4 nanosheets with a unique porous structure were fabricated by further thermally oxidizing and etching bulk g-C3N4 (bCN) in air. Homogeneous dispersion of Ru species was successfully achieved on the porous few-layered g-C3N4 nanosheets (pCN) by stirring, washing, freeze drying and annealing processes to obtain Ru-pCN catalysts, whereas bCN or multilayered g-C3N4 (mCN) led to the aggregation of Ru nanoparticles in Ru-bCN and Ru-mCN materials. The conventional impregnation method also caused the resulting Ru-pCN-imp catalyst with undesirable Ru aggregation in spite of employing pCN. The optimal 4.4Ru-pCN removed 100% of 2,4,6-trichlorophenol (TCP) within only 3 min, superior to its counterpart samples, and exhibited remarkable degradation efficiencies for methyl orange, neutral red, 4-chlorophenol, tetracycline and oxytetracycline. Mechanistic studies suggested that four radicals, e.g., •OH, SO4• −, O2• − and 1O2 were generated during the peroxymonosulfate (PMS) activation, in which SO4• − and 1O2 played a major role.
KW - AOPs
KW - Carbon nitride
KW - Non-radical
KW - PMS
KW - Sulfate radical
UR - https://www.scopus.com/pages/publications/85129272844
U2 - 10.1016/j.jhazmat.2022.128939
DO - 10.1016/j.jhazmat.2022.128939
M3 - Article
C2 - 35483264
AN - SCOPUS:85129272844
SN - 0304-3894
VL - 435
JO - Journal of Hazardous Materials
JF - Journal of Hazardous Materials
M1 - 128939
ER -