Journal
CHEMICAL ENGINEERING JOURNAL
Volume 446, Issue -, Pages -Publisher
ELSEVIER SCIENCE SA
DOI: 10.1016/j.cej.2022.137364
Keywords
Cu2S@MoS2; H2O2 activation; Sulfur vacancy; Density functional theory; Mechanism analysis
Categories
Funding
- Science and Technology Innovation Program of Hunan Province [2021RC3039]
- Natural Science Foundation of Hunan Province [2021JJ40069]
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This study synthesized a series of hollow Cu2S@MoS2-x nanoboxes with excellent catalytic activity for contaminant degradation using H2O2 activation. The dominant reactive oxygen species produced during activation were identified as center dot OH and O-1(2). The Cu2S@MoS2-2 system showed improved reaction rate and higher yield of O-1(2) compared to Cu2S/H2O2 system, demonstrating its potential as a reliable candidate for refractory organics degradation.
This work synthesized a series of hollow Cu2S@MoS2-x nanoboxes by using Cu2O nanocubes as precursor. Electron paramagnetic resonance (EPR) and X-ray absorption spectroscopy (XAS) analysis identified the existence of Sv in Cu2S@MoS2-x. Sulfadiazine (SDZ), a typical antibiotic, was selected as the target contaminant to evaluate the catalytic activity of Cu2S@MoS2-x via H2O2 activation. With adding 0.2 g/L Cu2S@MoS2-2 and 5 mM H2O2, 95.9% of SDZ (20 mu M) was removed in 60 min and the reaction rate constant obtained by Cu2S@-MoS2-2 (0.239 min(-1)) was improved by 4 times and 10 times in contrast with Cu2S (0.0622 min-1) and MoS2 (0.0219 min(-1)). EPR analysis and radical scavenger tests confirmed center dot OH and O-1(2) as the dominated reactive oxygen species (ROS). In Cu2S@MoS2-2 activated H2O2 system, the yield of O-1(2) was 6.12 x 10(-14) mol/L, more than 8 times that in Cu2S/H2O2 system (0.73 x 10(-14) mol/L). Density functional theory (DFT) calculation revealed that the Cu atoms exposed by the formation of Sv on Cu2S@MoS2-2 were the preferred adsorption sites for O-2, which further achieved the conversion of O-2 to center dot O-2(-) . In the activation process, Cu2S mainly produced center dot OH through sulfur-enhanced Fenton process, while MoS2 shell accounted for the O-2 production. Thereafter, the obtained O-2 acquired electrons from the Cu atoms exposed by Sv to produce center dot O-2(-) , followed by the generation of O-1(2). The cooperation between MoS2 and Cu2S resulted in the superior catalytic activity. The excellent recyclability, stability, and adaptability demonstrated Cu2S@MoS2-2 as a reliable candidate for activating H2O2 toward refractory organics degradation.
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