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Intermetallic compound PtMny-derived Pt―MnOx supported on mesoporous CeO2: Highly efficient catalysts for the combustion of toluene
Applied Catalysis A: General ( IF 5.5 ) Pub Date : 2020-03-04 , DOI: 10.1016/j.apcata.2020.117509
Xiaohang Fu , Yuxi Liu , Jiguang Deng , Lin Jing , Xing Zhang , Kunfeng Zhang , Zhuo Han , Xiyun Jiang , Hongxing Dai

Intermetallic compounds are a kind of important materials in heterogeneous catalysis. In this work, we first synthesized the PtMny intermetallic nanocrystals using the polyvinyl pyrrolidone-assisted ethylene glycol reduction method, and then loaded them on the surface of mesoporous CeO2 (meso-CeO2) derived from a KIT-6-templating route, generating the mPt―nMnOx/meso-CeO2 (m = 0―0.39 wt%, n = 0―1.21 wt%) catalysts after calcination at 500 °C in air. It is found that the as-obtained catalysts displayed an ordered mesoporous architecture with surface areas of 95―108 m2/g. The 0.37Pt―0.16MnOx/meso-CeO2 sample exhibited the best catalytic performance for toluene combustion (T50% =162 °C and T90% =171 °C at space velocity = 40,000 mL/(g h)). Kinetic analysis reveals that the apparent activation energy (57 kJ/mol) obtained over the best-performing 0.37Pt―0.16MnOx/meso-CeO2 sample was lower than those (63―75 kJ/mol) obtained over the other samples. Furthermore, the 0.37Pt―0.16MnOx/meso-CeO2 sample possessed good thermal stability and water-resistant performance. Benzyl alcohol, benzoic acid, and maleic anhydride were proven to be the main intermediates of toluene combustion, hence, toluene combustion might take place through a sequence of toluene → benzyl alcohol and benzoic acid → maleic anhydride → carbon dioxide and water, which might obey the Eley―Rideal reaction mechanism. It is concluded that loading of Pt and MnOx enhanced the adsorbed oxygen and Mn2+ species concentration and low-temperature reducibility, thus promoting toluene combustion over 0.37Pt―0.16MnOx/meso-CeO2.



中文翻译:

介孔CeO 2上负载的金属间化合物PtMn y衍生的Pt-MnO x:甲苯燃烧的高效催化剂

金属间化合物是非均相催化中的一种重要物质。在这项工作中,我们首先使用聚乙烯吡咯烷酮辅助的乙二醇还原法合成了PtMn y金属间纳米晶体,然后将其负载在源自KIT-6模板路线的介孔CeO 2(meso-CeO 2)的表面, 在空气中500°C煅烧后生成m Pt- n MnO x / meso-CeO 2m  = 0-0.39 wt%,n = 0-1.21 wt%)催化剂。发现所获得的催化剂表现出有序的介孔结构,表面积为95-108 m 2。/G。0.37Pt-0.16MnO x / meso-CeO 2样品表现出最佳的甲苯燃烧催化性能(在空速= 40,000 mL /(gh)时,T 50% = 162°C和T 90% = 171°C)。动力学分析表明,在性能最佳的0.37Pt-0.16MnO x / meso-CeO 2样品上获得的表观活化能(57 kJ / mol)低于在其他样品上获得的表观活化能(63-75 kJ / mol)。此外,0.37Pt〜0.16MnO x / meso-CeO 2样品具有良好的热稳定性和防水性能。苯甲醇,苯甲酸和马来酸酐被证明是甲苯燃烧的主要中间体,因此,甲苯燃烧可能通过甲苯→苯甲醇和苯甲酸→马来酸酐→二氧化碳和水的顺序发生。 Eley-Rideal反应机理。结论:负载Pt和MnO x可以提高吸附氧和Mn 2+的浓度,降低低温还原性,从而促进甲苯燃烧超过0.37Pt〜0.16MnO x / meso-CeO 2

更新日期:2020-03-04
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