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Highly active SBA-15-confined Pd catalyst with short rod-like micro-mesoporous hybrid nanostructure for n-butylamine low-temperature destruction
Molecular Catalysis ( IF 4.6 ) Pub Date : 2018-06-22 , DOI: 10.1016/j.mcat.2018.06.016
Mudi Ma , Huang Huang , Changwei Chen , Qing Zhu , Lin Yue , Reem Albilali , Chi He

Catalytic destruction of nitrogen-containing volatile organic compounds (NVOCs) is rarely reported although they can make great harm to the environment and public health. In the present work, a series of short rod-like micro-mesoporous composite SBA-15 materials (SBA-15-r) with developed porosity and enhanced mass transfer performance were rationally designed and synthesized, and highly dispersed and thermally stable Pd nanoparticles were successfully introduced into the mesopore channels of SBA-15-r via an extraordinary incipient wetness impregnation with the assistance of furfuryl alcohol and trimethylbenzene. The correlation between catalyst property and catalytic performance in n-butylamine destruction was elucidated. 29Si MAS NMR and FT-IR results show that phosphorus is incorporated into the skeleton of SBA-15-r through a POSi connection, altering the structural property of support. All Pd/SBA-15-r materials are highly active and stable catalysts with n-butylamine totally converted at 280 °C. Amongst, Pd/S-5 possesses the best n-butylamine oxidation activity and lowest NOx formation rate ascribable to the largest surface area and highest porosity which can promote the dispersion of Pd active sites and accelerate the oxidation process and product diffusion, inhibiting the formation of reaction byproducts. Moreover, the structural micropores over Pd/SBA-15-r catalysts play an important positive role in NOx formation control. The n-butylamine destruction mechanism were further discussed according to the results of gas chromatography and in situ DRIFTS. We believe that the present work provides new insights into the design and application of high-efficient catalysts based on hierarchical materials in NVOC elimination.



中文翻译:

具有短棒状微介孔杂化纳米结构的高活性SBA-15受限Pd催化剂,可用于丁胺的低温破坏

尽管含氮挥发性有机化合物会对环境和公众健康造成极大伤害,但很少有人报道过催化破坏含氮挥发性有机化合物的现象。在本工作中,合理设计和合成了一系列孔隙率高,传质增强的短棒状微孔复合SBA-15材料(SBA-15-r),并制备了高度分散和热稳定的Pd纳米粒子。在糠醇和三甲基苯的辅助下,通过异常的初湿浸渍成功地将SBA-15-r的介孔通道引入了SBA-15-r 。阐明了催化剂性能与催化性能在丁胺破坏中的相关性。29Si MAS NMR和FT-IR结果表明,磷通过P O Si连接结合到SBA-15-r的骨架中,从而改变了载体的结构性质。所有Pd / SBA-15-r材料均为高活性和稳定的催化剂,丁胺在280°C时完全转化。当中,将Pd / S-5具有最好Ñ丁胺氧化活性和最低NO X形成速率归因于最大的表面积和孔隙率最高可促进钯活性位点的分散性和加速氧化过程和产品中的扩散,抑制了反应副产物的形成。此外,Pd / SBA-15-r催化剂上的结构微孔在NO x中起着重要的积极作用。编队控制。所述Ñ丁胺破坏机理是根据气相色谱法的,结果进一步讨论的原位DRIFTS。我们相信,目前的工作为基于NVOC消除中分层材料的高效催化剂的设计和应用提供了新的见识。

更新日期:2018-06-22
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