首页|New insights of the initial processes of pyrene oxidation in the presence of Cu-based catalysts:Quantum-mechanical calculation and experimental evidence
New insights of the initial processes of pyrene oxidation in the presence of Cu-based catalysts:Quantum-mechanical calculation and experimental evidence
扫码查看
点击上方二维码区域，可以放大扫码查看
原文链接
NSTL
The oxidation and catalytic oxidation products of pyrene was analyzed by electron paramagnetic resonance(EPR),matrix-assisted laser desorption/ionization time-of-flight mass spectrometry(MALDI-TOF),Fourier-transform infrared spectroscopy(FT-IR),and gas chromatography-mass spectrometry(GC-MS).The in-situ transformation of Cu-based catalysts was analyzed.A qualitative model of pyrene oxidation with and without catalyst was built.CuO nanoparticles were in-situ formed as the active phases,and they decreased the polymerization and condensation of pyrene.The oxidation pathways of pyrene with and without CuO nanoparticles with the main product of 9-oxo-phenaleno-1-carbaldehyde were considered,which includes two elementary stages with the limiting Gibbs energy barrier of 227 kJ/mol.CuO increases the number of stages to diree and reduces the Gibbs activation energy by 20 % of the limiting stage of pyrene oxidation.These findings provide new insights into the initial oxidation of pyrene and its catalysis.The proposed model and methods using Density functional theory(DFT)calculation offer a new theoretical approach for investigating hydrocarbon oxidation as well as designing catalytic systems for accelerating their oxidation.
NSTL
