设计用于丙烷催化燃烧的有序介孔限制 Pt/Ti0.1AlOy 催化剂,New Journal of Chemistry

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设计用于丙烷催化燃烧的有序介孔限制 Pt/Ti0.1AlOy 催化剂
New Journal of Chemistry ( IF 2.7 ) Pub Date : 2023-02-02 , DOI: 10.1039/d2nj05893f
Liqiong Liu _{1,

2} , Weiliang Han ₂ , Fang Dong _{2,

3} , Hua Feng ₁ , Zhicheng Tang _{2,

4}

Affiliation

在这项工作中，成功构建了两种具有不同限制结构的有序介孔催化剂，用于丙烷的催化燃烧。值得注意的是，框架限制的 Pt/Ti _0.1 AlO _y -EISA 催化剂是使用一步蒸发诱导自组装 (EISA) 技术制备的，我们观察到 0.3%Pt/Ti _0.1 AlO _y -EISA 催化剂表现出优异的性能由于 Pt 纳米颗粒的分散和丰富的表面吸附氧物种 (O _ads ) 的双重作用，丙烷氧化的催化活性。为了进一步研究活性位点位置的影响，我们还制备了孔隙限制的 Pt/Ti _0.1 AlO _y-EISA催化剂，并证实骨架限制催化剂(0.3%Pt/Ti _0.1 AlO _y -EISA)在以下条件下表现出比孔限制的0.3%Pt/Ti _0.1 AlO _y -VI催化剂更好的活性和热稳定性相同的 Pt 负载。通过一系列表征研究，认为框架限制的 0.3%Pt/Ti _0.1 AlO _y -EISA 催化剂比孔限制的 0.3%Pt/Ti _0.1 AlO _{y催化剂具有更高的 Pt 分散度}-VI催化剂。有趣的是，孔隙限制催化剂比骨架限制催化剂具有更好的耐水性和抗硫性，因为孔隙在一定程度上保护了活性位点不被硫酸盐覆盖。_{硫酸盐增加了催化剂的酸度，从而提高了0.3%Pt/Ti 0.1} AlO _y -VI催化剂的耐水性和耐硫性。通过原位DRIFTS实验分析了丙烷催化燃烧过程的反应机理，提出朗缪尔欣谢尔伍德（LH）机理是可能的反应机理。

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Designing ordered mesoporous confined Pt/Ti0.1AlOy catalysts for the catalytic combustion of propane

In this work, two ordered mesoporous catalysts with different confined structures were successfully constructed for the catalytic combustion of propane. Notably, framework-confined Pt/Ti_0.1AlO_y-EISA catalysts were prepared using a one-step evaporation-induced self-assembly (EISA) technique, and we observed that the 0.3%Pt/Ti_0.1AlO_y-EISA catalyst exhibited superior catalytic activity for propane oxidation due to the dual effects of the dispersion of Pt nanoparticles and abundant surface adsorbed oxygen species (O_ads). To further investigate the influence of the location of the active sites, we also prepared pore-confined Pt/Ti_0.1AlO_y-EISA catalysts, and it was verified that the framework-confined catalyst (0.3%Pt/Ti_0.1AlO_y-EISA) shows better activity and thermal stability than the pore-confined 0.3%Pt/Ti_0.1AlO_y-VI catalyst under the same Pt loading. Through a series of characterization studies, it is considered that the framework-confined 0.3%Pt/Ti_0.1AlO_y-EISA catalyst has higher Pt dispersion than the pore-confined 0.3%Pt/Ti_0.1AlO_y-VI catalyst. Interestingly, the pore-confined catalyst has better water and sulfur resistance than the framework-confined catalyst, because the pores protect the active sites from being covered with sulfate to some extent. The sulfate increases the acidity of the catalyst, thereby improving the water and sulfur resistance of the 0.3%Pt/Ti_0.1AlO_y-VI catalyst. The reaction mechanism of the catalytic combustion process of propane was analyzed via in situ DRIFTS experiments, and the Langmuir Hinshelwood (L-H) mechanism was proposed to be the possible reaction mechanism.

更新日期：2023-02-02

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