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Tailoring manganese oxide catalysts for the total oxidation of pollutants in gas and liquid phase
Applied Catalysis A: General ( IF 5.5 ) Pub Date : 2020-11-11 , DOI: 10.1016/j.apcata.2020.117917
Francesco Arena , Roberto Di Chio , Alessandra Palella , Lorenzo Spadaro , Leone Frusteri , Barbara Fazio , Sara Morandi , Gianmario Martra

Bare and ceria-promoted MnOx catalysts (0 ≤ χMn≤1) were prepared by redox-precipitation reactions of Mn(VII), Mn(II) and Ce(III) or Ce(IV) precursors in slightly acidic (pH, 4.5) or basic (pH, 8.0) environment to assess genesis, nature, and functionality of surface active sites. Both synthesis protocols yield nanostructured materials with large surface area and exposure of Mn sites, featuring high activity in the CO oxidation and the phenol wet-air-oxidation (CWAO) model reactions (T, 423 K). High oxide dispersion prompts an extensive incorporation of Mn(II) ions into ceria substitutional solid-solution structures, forming oxygen-vacancies with stronger oxidation activity than surface Mn(IV) sites. Basic structure-activity relationships indicate that the superior CO oxidation performance of the pristine α-MnO2 system relies on large exposure of very reducible Mn(IV) active sites, while O2-adsorption onto Mn(II)/O-vacancy active centres generates very reactive surface oxygen-species boosting the efficiency of composite MnCeOx catalysts in the CWAO of phenol.



中文翻译:

量身定制的氧化锰催化剂可完全氧化气相和液相中的污染物

裸和氧化铈促进的MnO的X催化剂(0≤χ≤1)的Mn的氧化还原沉淀反应(VII),锰(II)和Ce(III)或Ce制备(IV)在微酸性(pH为前体, 4.5)或基本(pH,8.0)环境以评估表面活性部位的起源,性质和功能。两种合成方案均产生纳米结构具有大表面积和Mn位点暴露的材料,在CO氧化和苯酚湿空气氧化(CWAO)模型反应中具有高活性(T,423 K)。较高的氧化物分散度促使Mn(II)离子广泛掺入二氧化铈替代固溶体结构中,形成的氧空位比表面Mn(IV)位置的氧化活性强。基本结构-活性关系表明,原始α-MnO的的优异的CO氧化性能2系统依赖于大曝光非常还原的Mn(IV)的活性位点,而ö 2 -adsorption到的Mn(II)/ O空位活性中心生成非常活泼的表面氧物种,从而提高了苯酚CWAO中复合MnCeO x催化剂的效率。

更新日期:2020-12-03
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