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Pt/Al2O3La2O3 catalysts stable at high temperature in air, prepared using a “one-pot” sol-gel process: Synthesis, characterization, and catalytic activity in the partial oxidation of CH4
Chemical Engineering Science ( IF 4.1 ) Pub Date : 2021-01-01 , DOI: 10.1016/j.ces.2020.115966
Kleper de O. Rocha , Wagner C. Macedo , Clélia M.P. Marques , José M.C. Bueno

Abstract Pt/Al2O3La2O3 catalysts were prepared by a “one-pot” sol-gel method, with different final synthesis temperatures. The catalysts were characterized by in situ X-ray absorption spectroscopy (XAS). The partial oxidation of methane (POM) reaction was used to evaluate catalyst stability. DRIFTS-CO analysis indicated the interaction of Pt with the support by Pt-O-(Al-O, La-O) bonds, which suppressed bridge CO adsorption. In situ POM-DXAS-MS analysis showed that after use in the POM reaction at about 1000 K and cooling to room temperature, the Pt/Al2O3La2O3 catalysts presented partial oxidation of Pt0, indicating the formation of a core-shell structure. The nanoparticles generated using the “one-pot” method showed higher Pt-O-Al type interaction with the support, relative to free Pt-O at the surface, resulting in high resistance to sintering in the POM reaction. The temperature used in the “one-pot” synthesis significantly influenced the Pt-O-Al interaction, which modified the resistance to sintering at 1073 K in air.

中文翻译:

Pt/Al2O3La2O3 催化剂在空气中的高温下稳定,使用“一锅”溶胶-凝胶工艺制备:CH4 部分氧化的合成、表征和催化活性

摘要 Pt/Al2O3La2O3 催化剂采用“一锅法”溶胶-凝胶法制备,具有不同的最终合成温度。催化剂通过原位X射线吸收光谱(XAS)表征。甲烷的部分氧化(POM)反应用于评估催化剂的稳定性。DRIFTS-CO 分析表明 Pt 与载体通过 Pt-O-(Al-O, La-O) 键相互作用,抑制了桥接 CO 吸附。原位 POM-DXAS-MS 分析表明,在约 1000 K 的 POM 反应中使用并冷却至室温后,Pt/Al2O3La2O3 催化剂呈现 Pt0 的部分氧化,表明形成了核壳结构。相对于表面的游离 Pt-O,使用“一锅”法生成的纳米颗粒显示出更高的 Pt-O-Al 型与载体的相互作用,导致在 POM 反应中具有很高的抗烧结性。“一锅法”合成中使用的温度显着影响了 Pt-O-Al 相互作用,从而改变了空气中 1073 K 的烧结电阻。
更新日期:2021-01-01
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