Journal
CHEMICAL ENGINEERING JOURNAL
Volume 371, Issue -, Pages 78-87Publisher
ELSEVIER SCIENCE SA
DOI: 10.1016/j.cej.2019.03.233
Keywords
Ethyl acetate oxidation; Sacrificial template method; Oxygen vacancy
Categories
Funding
- National Natural Science Foundation of China [51578245, 51878293, 21777047]
- National Key Research and Development Plan [2018YFB0605200]
- Natural Science Foundation of Guangdong Province, China [2016A030311003]
- Scientific Research Project of Guangzhou City [201804020026]
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Industrial volatile organic compounds (VOCs) are harmful to the environment and human health. Catalytic oxidation is the most effective method for end-of-pipe control. The challenges of VOC catalytic oxidation are the high space velocities and low oxidation temperatures. In this work, Mn cations were introduced into Ce-BTC supports by an impregnation method, after which the mixture was calcined. The as-synthesized CeO2-supported Mn catalyst MnOx-CeO2-s exhibited an outstanding activity for ethyl acetate (EtOAc) catalytic oxidation, which reached complete conversion at 210 degrees C (T-99 = 210 degrees C), even at a high space velocity (WHSV= 60,000 mL g(-1) h(-1)). With in situ UV Raman and other characterization methods, the Frankel oxygen vacancy (F-OV) was determined to be the crucial active site for EtOAc catalytic oxidation. The excellent low temperature activity of MnOx-CeO2-s benefited from the enhanced F-OVs concentration. The high temperature stability was attributed to the stable F-OVs recovery potential of the Ce-BTC-derived CeO2 support. The durability at a high space velocity was the result of the unique crossed channel structure inherited from Ce-BTC. These findings unraveled the crucial role of F-OVs in the EtOAc catalytic oxidation and the value of MOF-derived materials, which highlighted a feasible approach for the design of VOC-removal catalysts.
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