生物炭负载Gd-Mn莫来石氧化物协同臭氧催化氧化仲辛醇性能与机理

Performance and mechanism of synergistic catalytic oxidation of 2-octanol by Gd-Mn mullite oxide loaded on biochar and ozone

  • 摘要: 通过水热法制备了新型生物炭负载Gd-Mn莫来石氧化物(GdMn2O5和GdMn2O5/BC)用于协同臭氧高效催化氧化挥发性有机物(VOCs)废气。通过SEM、TEM、XRD、XPS和N2吸附脱附等手段对负载催化剂的结构、形貌和催化潜力进行了表征评估,研究工作条件和负载量对莫来石催化仲辛醇氧化降解性能的影响。结果表明,GdMn2O5催化氧化仲辛醇的T90 = 177℃,在201℃时完全降解,CO2转化率约为80%。生物炭负载莫来石催化剂可降低仲辛醇与臭氧氧化反应的活化能并增加催化剂表面的活性氧物种和氧空位数量。催化剂与臭氧协同作用下仲辛醇的催化氧化遵循马斯·范·克雷弗伦(MvK)催化机制,氧空位、晶格氧和活性氧物种的消耗-补充循环以及Mn4+和Mn3+之间的电子转移是发生催化反应的基础。

     

    Abstract: Some novel biochar-supported Gd-Mn mullite oxides (GdMn2O5 and GdMn2O5/BC) were prepared by the hydrothermal method for the efficient catalytic oxidation of volatile organic compounds (VOCs) waste gas in synergy with ozone. The structure, morphology and catalytic potential of the supported catalysts were characterized and evaluated by means of SEM, TEM, XRD, XPS and N2 adsorption-desorption. The effects of application conditions and supporter types on the catalytic performance of mullite for the oxidation and degradation of 2-octanol were investigated. The results show that the T90 for the catalytic oxidation of 2-octanol by GdMn2O5 is 177℃, and it is completely degraded at 201℃, with a CO2 conversion rate of approximately 80%. The biochar-supported mullite catalyst can reduce the activation energy of the oxidation reaction of 2-octanol with ozone and increase the number of active oxygen species and oxygen vacancies on the catalyst surface. The catalytic oxidation of 2-octanolunder the synergistic effect of the catalyst and ozone follows Mars-van Krevelen (MvK) mechanism.The consumption-supplementation cycle of oxygen vacancies, lattice oxygen and active oxygen species, as well as the electron transfer between Mn4+ and Mn3+ is the basis for the occurrence of the catalytic reaction.

     

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