当前位置: X-MOL 学术Mol. Catal. › 论文详情
Our official English website, www.x-mol.net, welcomes your feedback! (Note: you will need to create a separate account there.)
Effect of Mg and Al on manganese oxides as catalysts for VOC oxidation
Molecular Catalysis ( IF 4.6 ) Pub Date : 2017-11-06 , DOI: 10.1016/j.mcat.2017.09.015
María Haidy Castaño , Rafael Molina , Sonia Moreno

Manganese mixed oxides with the compositions Mn-Mg-Al-O and Mn-O were synthesized by the self-combustion method. The effects of Mg and Al incorporation on the structural, textural, redox and catalytic properties of the manganese oxides were evaluated. The catalysts were characterized by X-ray diffraction (XRD), N2 adsorption, temperature-programed desorption of oxygen (O2-TPD), temperature-programmed reduction (H2-TPR), oxygen storage capacity (OSC), 18O/16O oxygen isotope exchange, and their catalytic performance was evaluated in the oxidation of toluene, ethyl acetate and 2-propanol. The analyses showed that the use of a glycine/nitrate ratio equal to 0.56 in the self-combustion favors the formation of the Mn3O4 phase and the incorporation of Mg and Al into the structure stabilizes this phase after a thermal process. In addition, the surface area increases, the particle size decreases, and the presence of electrophilic oxygens is favored, which increases the adsorption sites, exposes the active centers and facilitates the occurrence of redox cycles, leading to a better catalytic performance in the total conversion of the oxygenated compounds on the Mn-Mg-Al-O mixed oxide. In the oxide that only contains manganese, the presence of nucleophilic oxygens with great mobility was observed, leading to its good activity in the oxidation of the VOCs.

The catalytic tests showed that a high oxygen exchange capacity leads to lower temperatures of conversion of toluene, which suggests that, for the oxidation of aromatic compounds, the lattice oxygen plays a fundamental role in the catalytic activity. In contrast, in the oxidation of oxygenated compounds that require lower temperatures of conversion, the existence of surface oxygens such as O2 and O favors the catalytic process and therefore ensures superior activity in the transformation of ethyl acetate and 2-propanol on the Mn-Mg-Al-O mixed oxide.



中文翻译:

Mg和Al对锰氧化物作为VOC氧化催化剂的影响

通过自燃法合成了Mn-Mg-Al-O和Mn-O组成的锰混合氧化物。评估了镁和铝的掺入对锰氧化物的结构,组织,氧化还原和催化性能的影响。催化剂的特征在于X射线衍射(XRD),N 2吸附,氧气的程序升温脱附(O 2 -TPD),程序升温还原(H 2 -TPR),储氧量(OSC),18 O / 16O氧同位素交换,并在甲苯,乙酸乙酯和2-丙醇的氧化反应中评估了它们的催化性能。分析表明,在自燃中使用等于0.56的甘氨酸/硝酸盐比率有利于Mn 3 O 4的形成。在热处理之后,Mg和Al掺入到结构中使该相稳定。另外,表面积增加,粒度减小,并且亲电子氧的存在是有利的,这增加了吸附位点,暴露了活性中心并促进了氧化还原循环的发生,从而导致总转化率中更好的催化性能。含氧化合物对Mn-Mg-Al-O混合氧化物的影响。在仅包含锰的氧化物中,观察到亲核性氧具有很高的迁移率,从而使其在VOC的氧化中具有良好的活性。

催化试验表明,高的氧交换能力导致较低的甲苯转化温度,这表明,对于芳族化合物的氧化,晶格氧在催化活性中起着基本作用。与此相反,在需要转换的较低的温度下氧化化合物的氧化,面的存在是氧,例如O 2 -和O -有利于催化过程,因此可确保在转化优良活性乙酸乙酯和2-丙醇Mn-Mg-Al-O混合氧化物。

更新日期:2017-11-06
down
wechat
bug