Abstract
Series of ZSM-5 zeolites with diverse contents and locations of Al pairs were synthesized, and Co2+ ions were subsequently anchored at the Al pairs of ZSM-5 zeolites by wet ion-exchange with H protons. The Co-ZSM-5 sample derived from the mixtures of AlCl3 and TEOS of Si/Al=30.3 showed the best deN2O performance. Analysis on Co (Ⅱ) ion exchange capacity demonstrated the content of Al pairs followed the sequence: AlCl3 (0.84) > Al(NO3)3 (0.73) > aluminum isopropoxide (0.65) and TEOS (0.84) > silicic acid (0.57). More Al pairs coordinated with protons or cobalt ions were essentially associated with better performances for N2O catalytic dissociation. Moreover, Si source had a significant effect on the location of Al pairs determined by UV–vis–DRS of bare Co (Ⅱ), Al pairs of ZSM-5 zeolite synthesized from TEOS were enriched in the sinusoidal channel (γ site), whereas those synthesized from silicic acid were concentrated in the channel intersections (6-MRs β site). The theoretical calculation revealed that the O2 desorption at γ-site Co2+ of ZSM-5 zeolite required to overcome less energy barrier (23.8 kcal/mol) than that at β-site one.
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