Engineering polyhedral high entropy oxide with high-index facets via mechanochemistry-assisted strategy for efficient oxidative desulfurization
2023
Deng, Chang | Wu, Peiwen | Li, Hongping | Zhu, Haonan | Chao, Yanhong | Tao, Duanjian | Chen, Ziran | Hua, Mingqing | Liu, Jixing | Liu, Jianjun | Zhu, Wenshuai
High entropy oxides are promising catalysts for numerous catalytic oxidation processes with oxygen as the oxidant. However, most of them often show bulk morphologies, which hinders the full exposure of active sites. In this work, a unique 26-faceted polyhedral high entropy oxide MnNiCuZnCoOₓ-1000 (P-HEO) with highly active site exposure is fabricated via a mechanochemistry-assisted strategy. By employing such a strategy, the supersaturation of P-HEO during the crystal growth process is effectively reduced to form high-index facets, which is proved to be beneficial to the formation of high-index facets. Characterization results indicate that more oxygen vacancies are generated in P-HEO compared with the bulk counterparts. Density functional theory calculations reveal that the high-index facets {−211} can facilitate adsorption and activation of O₂ because of the higher adsorption energy −2.23 eV compared with that of (111) surfaces (-1.79 eV), which induces significantly enhanced activity for organic sulfides oxidation. Interestingly, the synthesized P-HEO with high-index facets shows a 98.4% removal rate of dibenzothiophene from model oil within 8 h at 120 °C, which is much higher than that of the bulk counterparts (33.5%).
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