Synthesis of Nb2O5 based solid superacid materials for catalytic combustion of chlorinated VOCs

Synthesis of Nb2O5 based solid superacid materials for catalytic combustion of chlorinated VOCs
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Nb2O5基固体超强酸材料的合成用于催化燃烧氯化VOCs

DOI:
10.1016/j.apcatb.2018.07.061
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发表时间:
2018-12
期刊:
Applied Catalysis B: Environmental
影响因子:
--
通讯作者:
Chenze Qi
Chenze Qi
中科院分区:
其他
文献类型:
--
作者:
Peng Yang;Shaokang Fan;Zhenyang Chen;Guofang Bao;Shufeng Zuo;Chenze Qi

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以柠檬酸为交联剂,采用溶胶-凝胶法合成了Nb 2 O 5基固体超强酸(Nb 2 O 5-MOx,M = Ti,W,Zr,Si,Al和Ca),并将其用于催化燃烧氯代VOCs污染物1,2-二氯乙烷(简称:DCE)。结构-性能关系的研究结果表明,Nb 2 O 5-MOx形成了介孔和非晶态结构,金属元素高度分散,有助于增强金属-金属相互作用,改善催化剂的物化性能。其固有催化活性顺序为:Nb_2O_5-WO_3> Nb_2O_5-ZrO_2> Nb_2O_5-TiO_2> Nb_2O_5-SiO_2> Nb_2O_5-Al_2O_3> Nb_2O_5> Nb_2O_5-CaO。存在协同催化效应:介孔和表面酸性促进反应物中C单键Cl键的吸附、活化和破坏,生成HCl和副产物C2 H3Cl(或碳正离子中间体),氧化还原中心促进副产物/中间体的深度氧化,转化为CO2和H2O。其中,Nb 2 O 5-TiO 2催化剂表现出最高的表观催化降解活性。它还表现出良好的热稳定性和对DCE破坏的耐久性以及良好的抗水蒸气性。
Nb2O5based solid superacids (Nb2O5-MOx, M = Ti, W, Zr, Si, Al and Ca, respectively) were synthesized by sol-gel method using citric acid as the cross-linking agent, and then were investigated for catalytic combustion of 1,2-dichloroethane (abbreviation: DCE), one of the typical examples for chlorinated VOCs pollutants. The research results of the structure-performance relationship show that mesopore and amorphous state structure are formed for Nb2O5-MOx, and the metal elements are highly dispersed, which contribute to enhancing the metal-metal interaction and modifying the physicochemical properties of the catalysts. The order for the inherent catalytic activity is: Nb2O5-WO3>Nb2O5-ZrO2>Nb2O5-TiO2>Nb2O5-SiO2>Nb2O5-Al2O3>Nb2O5>Nb2O5-CaO. There exists synergistic catalytic effect: the mesopore and surface acidity facilitate the adsorption, activation and destruction of the Csingle bondCl bond in the reactants to form HCl and byproduct C2H3Cl (or carbocation intermediate), and then the redox sites promote deep oxidation of the byproduct/intermediate to convert to CO2and H2O. Especially, the Nb2O5-TiO2catalyst represents the highest apparent catalytic degradation activity. It also represents good thermal stability and durability for DCE destruction as well as good resistance to water vapor.
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