用于甲烷燃烧的具有 Pd-Co 复合界面的高活性、高稳定性 Pd/15CoAlOx 催化剂

Jieying Cai, Shenghai Wu, Miaomiao Liu, Yan Zhang, Meng Wang, Yun Liu, Yunbo Yu, Wenpo Shan
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摘要

合成了一系列用于燃烧 CH 的 Pd/yCoAlO(其中 y 代表 Co/AlO 质量比,范围为 0 至 20.0 wt%)催化剂,其中 Pd/15CoAlO 催化剂具有优异的活性、稳定性和耐水性。HRTEM、XRD 和拉曼结果表明,Pd/15CoAlO 催化剂由 CoAlO 和 CoO 两相组成。H-TPR、O-TPD 和原位 DRIFTS 显示,以 Pd-Co 复合界面为特征的 Pd/15CoAlO 加强了 PdO 的锚定,促进了 Pd-Co 界面之间的电子转移。此外,活性氧物种在界面上富集,促进了从甲氧基到甲酸酯而不是从甲基到甲酸酯的反应途径。多种表征和分析表明,Pd/15CoAlO 的 MSI 弱于 Pd-CoO 界面,但强于在 Pd-AlO 界面观察到的 MSI。适当程度的相互作用避免了钯的过度氧化,确保了大量不饱和钯位点的存在。
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A highly active and stable Pd/15CoAlOx catalyst with Pd-Co composite interfaces for methane combustion
A series of Pd/yCoAlO (where y represents the Co/AlO mass ratio, ranging from 0 to 20.0 wt%) catalysts for CH combustion were synthesized, among which the Pd/15CoAlO catalyst exhibited excellent activity, stability and water resistance. HRTEM, XRD, and Raman results indicated that the Pd/15CoAlO catalyst comprised two phases, namely CoAlO and CoO. H-TPR, O-TPD, and in-situ DRIFTS revealed that Pd/15CoAlO featuring Pd-Co composite interfaces strengthened the anchoring of PdO and facilitated electron transfer between Pd-Co interfaces. Moreover, active oxygen species were enriched at the interface, which promoted the reaction pathway involving the change from methoxy to formate, rather than from methyl to formate. Multiple characterizations and analyses indicated that Pd/15CoAlO exhibited a MSI weaker than the Pd-CoO interface but stronger than that observed at the Pd-AlO interface. The appropriate level of interaction avoided the excessive oxidation of Pd, ensuring the presence of a substantial quantity of unsaturated Pd sites.
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