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Published on: August 17, 2019
Brønsted Acid-Driven Dynamic LMCT Sites Transform Pt/Zeolite Into a Light-Responsive Oxidation Platform
Xiaowei Han1, Tangxuan Chen1, Qingqing Zhang1
1State Key Laboratory of Green Chemical Engineering and Industrial Catalysis, Institute of Fine Chemicals, School of Chemistry and Molecular Engineering, East China University of Science and Technology, Shanghai, P. R. China.
This study enhances photocatalysis for efficient oxidation by creating dynamic ligand-to-metal charge transfer (LMCT) sites on Pt/zeolite catalysts. This approach boosts oxygen activation and pollutant degradation using visible light and photothermal effects.
Area of Science:
- Catalysis
- Materials Science
- Environmental Chemistry
Background:
- Photocatalysis offers low-temperature oxidation but struggles with inefficient oxygen activation and intermediate utilization compared to thermal catalysis.
- Conventional Pt/zeolite catalysts have limitations in harnessing light energy for oxidation reactions.
Purpose of the Study:
- To develop a photothermal-photoelectronic platform for enhanced catalytic oxidation.
- To improve oxygen activation and utilization of surface intermediates in photocatalysis.
- To achieve efficient degradation of aromatic hydrocarbons using visible light.
Main Methods:
- Transformation of Pt/zeolite into a photothermal-photoelectronic platform using Brønsted acid-mediated dynamic ligand-to-metal charge transfer (LMCT) sites.
- Utilizing toluene oxidation over Pt/ZSM-5 as a model system.
- Investigating UV-enabled intermediate formation and visible-light-triggered LMCT excitation.
Main Results:
- Formation of Pt-O-CH2-Ar complexes via acid-assisted deprotonation of benzyl alcohol under UV irradiation.
- Demonstration of visible-light absorption and O2 activation through the LMCT mechanism by these complexes.
- Complete degradation of 1000 ppm toluene under light-only conditions with high efficiency (240-480 L g-1 h-1) using only 0.5 wt.% Pt.
Conclusions:
- A novel strategy merges photothermal and photoelectronic effects for superior catalytic oxidation.
- Dynamic intermediate coordination effectively boosts light-driven O2 activation.
- The approach offers a general method for energy-efficient oxidation of aromatic hydrocarbons.
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