Dynamic active-site induced by host-guest interactions boost the Fenton-like reaction for organic wastewater treatment.
Dongpeng ZhangYanxiao LiPengfei WangJinyong QuYi LiSihui ZhanPublished in: Nature communications (2023)
In heterogeneous catalysis, uncovering the dynamic evolution of active sites in the working conditions is crucial to realizing increased activity and enhanced stability of catalyst in Fenton-like activation. Herein, we capture the dynamic changes in the unit cell of Co/La-SrTiO 3 catalyst during the exemplary peroxymonosulfate activation process using X-ray absorption spectroscopy and in situ Raman spectroscopy, revealing the substrate tuned its structural evolution, which is the reversible stretching vibration of O-Sr-O and Co/Ti-O bonds in different orientations. This process effectively promotes the generation of key SO 5 * intermediates, which is beneficial to the formation of 1 O 2 and SO 4 •- from persulfate on the Co active site. Density functional theory and X-ray absorption spectroscopy show that the optimized structural distortion enhanced the metal-oxygen bond strength by tuning the e g orbitals and increased the number of transferred electrons to peroxymonosulfate by about 3-fold, achieving excellent efficiency and stability in removing organic pollutants.
Keyphrases
- wastewater treatment
- density functional theory
- high resolution
- raman spectroscopy
- antibiotic resistance genes
- molecular dynamics
- ionic liquid
- visible light
- single molecule
- room temperature
- highly efficient
- reduced graphene oxide
- dual energy
- single cell
- hydrogen peroxide
- electron microscopy
- carbon dioxide
- magnetic resonance imaging
- computed tomography
- metal organic framework
- cell therapy
- mass spectrometry
- stem cells
- solid state
- gold nanoparticles
- nitric oxide