Journal
APPLIED CATALYSIS B-ENVIRONMENTAL
Volume 256, Issue -, Pages -Publisher
ELSEVIER
DOI: 10.1016/j.apcatb.2019.117844
Keywords
Methane oxidation; Spinel oxide; Electronic structure; Dissociative adsorbed oxygen; Lattice oxygen
Funding
- Singapore Ministry of Education [RG3/18(S), MOE2018-T22-027]
- Singapore National Research Foundation under its Campus for Research Excellence And Technological Enterprise (CREATE) program SinBeRISE
- Environmental Chemistry and Materials Centre (ECMC) under Nanyang Environment and Water Research Institute (NEWRI)
- Sustainable Earth division of the Nanyang Technological University's Interdisciplinary Graduate School (IGS)
- Facility for Analysis, Characterization, Testing and Simulation (FACTS) in Nanyang Technological University
- Nanjing Tech University Research Start-up Fund [38274017111]
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Exploring active and low-cost spinel catalysts for complete methane oxidation is essential for the development of efficient air purification technologies. Herein, a series of spinel oxides ZnNixCo2-xO4 (x = 0-0.8) were synthesized to investigate the origin of their electronic structure dependent activities and mechanisms for methane oxidation. The interplay between O p-band center and M-oct d-band center was found to be responsible for the methane oxidation activity. Ni-poor ZnNixCo2-xO4 spinels with the M-oct d-band center positioned higher relative to the O p-band center, exhibited greater metal character, indicative of a dissociative adsorbed oxygen featured suprafacial Eley-Rideal (E-R) model. In contrast, Ni-rich ZnNixCo2-xO4 with the O p-band center in a higher position relative to the M-oct d-band center, displayed greater oxygen character, predominated by the intrafacial Mars-van-Krevelen (Mv-K) mechanism featuring the involvement of lattice oxygen. These findings may provide steps towards the rational design of better spinel oxides for catalytic oxidation reactions.
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