화학공학소재연구정보센터
홈 로그인 로그아웃 연락처 사이트맵
Korean Journal of Chemical Engineering, Vol.39, No.4, 920-927, April, 2022
DOI10.1007/s11814-021-1001-3  Export Citation
The effect of Zn doping on active Cu species and its location of Cu-exchanged mordenite for the stepwise oxidation of methane to methanol
Nutchapon Chotigkrai1, †, Phakpum Tannititam1, Sunthon Piticharoenphun1, Narit Triamnak2, Supareak Praserthdam3, 4, and Piyasan Praserthdam3, 4
  • 1Department of Chemical Engineering, Faculty of Engineering and Industrial Technology, Silpakorn University, Nakhon Pathom, Thailand 73000
  • 2Department of Materials Science and Engineering, Faculty of Engineering and Industrial Technology, Silpakorn University, Nakhon Pathom, Thailand 73000
  • 3Department of Chemical Engineering, Faculty of Engineering, Chulalongkorn University, Bangkok, Thailand 10310
  • 4Center of Excellence on Catalysis and Catalytic Reaction Engineering, Chulalongkorn University, Bangkok, Thailand 10330
E-mail:
The effect of Zn doping (0.5-3wt%) on Cu-exchanged mordenite (Cu-MOR) was investigated during the stepwise oxidation of methane to methanol. The strong interaction between Cu and ZnOx stabilized the highly-dispersed state of Cu2+ but reduced the Cu2+ bounded to extra-framework oxygen (active site), as demonstrated by the H2- TPR and XPS results. The Cu/Al and Zn/Al ratios suggested that Zn preferably bonded to the sites in the 8-MR channel, which led to highly dispersed Cu2+ anchored onto the highly accessible sites (12-MR and 8-MR side pocket). The reactivity indicated that highly dispersed Cu2+ can be gradually transformed into active Cu2+ species during contact with methane. Bimetallic Cu-ZnOx was also able to activate methane, resulting in a product complex. Although Zndoped Cu-MOR catalysts gave a lower methanol yield at 2 h, a higher methanol yield could be achieved at saturation methane loading time. Interestingly, 3 wt% Zn doping on Cu-MOR showed superior activity due to the increase of methanol yield up to 20% at 5 h of methane loading time. This work paves the way for the design of highly dispersed Cu2+ in the 12-MR channel of mordenite zeolite via the control of strong Cu-ZnOx interaction.
Keywords:Copper-zinc;Highly Dispersed Copper(II);Copper Mordenite;Copper Reduction;Methane to Methanol
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