TY - JOUR
T1 - ZIF-derived non-bonding Co/Zn coordinated hollow carbon nitride for enhanced removal of antibiotic contaminants by peroxymonosulfate activation
T2 - Performance and mechanism
AU - Li, Xi
AU - Wang, Shiwen
AU - Chen, Pei
AU - Xu, Baokang
AU - Zhang, Xiao
AU - Xu, Yanhua
AU - Zhou, Ru
AU - Yu, Yang
AU - Zheng, Huaili
AU - Yu, Peng
AU - Sun, Yongjun
N1 - Publisher Copyright:
© 2023
PY - 2023/5/15
Y1 - 2023/5/15
N2 - Co–Zn–N–C catalyst (MCZC) with neighboring Co and Zn pairs anchored on hollow carbon nitride was constructed by the direct etching of zeolitic imidazolate frameworks assembled with Co and Zn. Adequate characterizations and density functional theory (DFT) studies confirmed the successful construction of non-bonding Co and Zn pairs with enhanced electron transfer on Co sites by adjacent Zn sites. Based on the synergy of adjacent Co and Zn atom pairs, the MCZC/Perxymosulfate (PMS) system achieved 99.6% Tetracycline (TC) degradation in 24 min with a mineralization rate of 55.8% and PMS decomposition efficiency of 73.1%. DFT calculation based on the Fukui index identified the sites susceptible to attack by the active species. TC degradation pathways could be inferred, and reduced toxicity of intermediates was observed. This work provides new insights into the design of MOF-derived bimetallic catalysts and the importance of the interaction between adjacent metal active sites to catalytic performance.
AB - Co–Zn–N–C catalyst (MCZC) with neighboring Co and Zn pairs anchored on hollow carbon nitride was constructed by the direct etching of zeolitic imidazolate frameworks assembled with Co and Zn. Adequate characterizations and density functional theory (DFT) studies confirmed the successful construction of non-bonding Co and Zn pairs with enhanced electron transfer on Co sites by adjacent Zn sites. Based on the synergy of adjacent Co and Zn atom pairs, the MCZC/Perxymosulfate (PMS) system achieved 99.6% Tetracycline (TC) degradation in 24 min with a mineralization rate of 55.8% and PMS decomposition efficiency of 73.1%. DFT calculation based on the Fukui index identified the sites susceptible to attack by the active species. TC degradation pathways could be inferred, and reduced toxicity of intermediates was observed. This work provides new insights into the design of MOF-derived bimetallic catalysts and the importance of the interaction between adjacent metal active sites to catalytic performance.
KW - Antibiotic contaminants
KW - Bimetallic active sites
KW - Metal-organic frameworks
KW - Non-bonding interaction
KW - Peroxymonosulfate activation
UR - http://www.scopus.com/inward/record.url?scp=85146484020&partnerID=8YFLogxK
U2 - 10.1016/j.apcatb.2023.122401
DO - 10.1016/j.apcatb.2023.122401
M3 - 文章
AN - SCOPUS:85146484020
SN - 0926-3373
VL - 325
JO - Applied Catalysis B: Environmental
JF - Applied Catalysis B: Environmental
M1 - 122401
ER -