TY - JOUR
T1 - Constructing Cu-Mn bimetallic synergistic sites in 2D metal-organic framework nanosheets to induce polarized charge distribution
T2 - Electronic structure transformation and evaluation of Fenton-like performance
AU - Wang, Sheng
AU - Yuan, Chi
AU - Lu, Qinyang
AU - Pei, Shangkun
AU - Lu, Yuxin
AU - Wu, Yukai
AU - Li, Xiang
AU - Wang, Bo
N1 - Publisher Copyright:
© 2024 Elsevier B.V.
PY - 2025/2/19
Y1 - 2025/2/19
N2 - Heterogeneous Fenton-like process based on H2O2 was an efficient method for the abatement of micropollutants in water. However, the mass transport resistance caused by the limited access between catalytic sites and target chemicals still restrict the decontamination efficiencies. Metal-organic frameworks (MOFs) with uniformed pores and anbundant metal sites shows great potentail in environmental remediation, Here, a novel two-dimensional nanosheet consisting of Cu and Mn bimetallic-oxygen clusters (CuMn-BDC, BDC refers to terephthalic acid organic ligand) was rationally designed and characterized. The introduction of second metal Mn changed the surface electronic distribution and accelerated the electron transfer of pristine Cu-based nanosheet, leading to improved catalytical acticities and removal effeciencies (kSA) for Sulfamethoxazole (SMX). The catalytic activity of CuMn-BDC obtained (5.76 × 10–4) was 3.95 times higher than that of Cu-BDC (1.46 × 10–4), demonstrating that the CuMn-BDC showed higher reaction rates than that of Cu-BDC when same amount of H2O2 was added. The interfacial micro-electric fields in bimetallic MOFs increased the interaction of organic pollutants and transfer the electron to activate H2O2. Several quenching experiments, electron paramagnetic resonance spectra and theoretical calculations were performed to study the reaction mechanism systematically. Further the powder was fabricated into membrane with higher water stablities. This study shed light on develop efficient 2D-MOFs catalyst for the abatement of micropollutants in water.
AB - Heterogeneous Fenton-like process based on H2O2 was an efficient method for the abatement of micropollutants in water. However, the mass transport resistance caused by the limited access between catalytic sites and target chemicals still restrict the decontamination efficiencies. Metal-organic frameworks (MOFs) with uniformed pores and anbundant metal sites shows great potentail in environmental remediation, Here, a novel two-dimensional nanosheet consisting of Cu and Mn bimetallic-oxygen clusters (CuMn-BDC, BDC refers to terephthalic acid organic ligand) was rationally designed and characterized. The introduction of second metal Mn changed the surface electronic distribution and accelerated the electron transfer of pristine Cu-based nanosheet, leading to improved catalytical acticities and removal effeciencies (kSA) for Sulfamethoxazole (SMX). The catalytic activity of CuMn-BDC obtained (5.76 × 10–4) was 3.95 times higher than that of Cu-BDC (1.46 × 10–4), demonstrating that the CuMn-BDC showed higher reaction rates than that of Cu-BDC when same amount of H2O2 was added. The interfacial micro-electric fields in bimetallic MOFs increased the interaction of organic pollutants and transfer the electron to activate H2O2. Several quenching experiments, electron paramagnetic resonance spectra and theoretical calculations were performed to study the reaction mechanism systematically. Further the powder was fabricated into membrane with higher water stablities. This study shed light on develop efficient 2D-MOFs catalyst for the abatement of micropollutants in water.
KW - Bimetallic MOF nanosheet
KW - Heterogeneous Fenton-like process
KW - Micropollutants
KW - Polarized electronic structure
UR - http://www.scopus.com/inward/record.url?scp=85203458389&partnerID=8YFLogxK
U2 - 10.1016/j.seppur.2024.129488
DO - 10.1016/j.seppur.2024.129488
M3 - Article
AN - SCOPUS:85203458389
SN - 1383-5866
VL - 354
JO - Separation and Purification Technology
JF - Separation and Purification Technology
M1 - 129488
ER -