Mediating the Competitive Adsorption of Propane and Oxygen via Pt-Sulfate Synergy for Enhanced Propane Combustion

丙烷 催化作用 吸附 氧气 化学 燃烧 化学工程 无机化学 材料科学 燃料电池 多相催化 过程(计算) 催化燃烧 碳氢化合物
作者
Han Zhao,Lu Liu,You‐Zeng Hao,Xiaoyang Zhu,Qian Zhou,Yi-Wei Xian,Wenzhi Jia,Lin Dong,Meng‐Fei Luo,Wei Tan,Jian Chen
出处
期刊:ACS Catalysis [American Chemical Society]
卷期号:15 (24): 21054-21065 被引量:5
标识
DOI:10.1021/acscatal.5c06403
摘要

Developing efficient catalysts for the low-temperature combustion of short-chain alkane VOCs remains challenging. One of the primary obstacles to further enhancing catalytic combustion performance is believed to be the inherently weak adsorption of alkanes, which leads to their loss in competitive adsorption against O 2 on reactive sites. Although sulfate-modified Pt catalysts have demonstrated potential for short-chain alkane combustion, the reaction mechanism on those catalysts, particularly concerning the adsorption behaviors of the reactants, remains unclear. Herein, starting from the preparation of sulfated ZrO 2 through an eco-friendly simultaneous pyrolysis strategy, an efficient supported Pt catalyst (Pt/ZrO 2 -5S) for propane combustion was prepared. Compared to Pt supported on bare ZrO 2 (Pt/ZrO 2 ), Pt/ZrO 2 -5S displayed significantly promoted activity for propane combustion, achieving a T 90 of 200 °C, which was 120 °C lower than that of Pt/ZrO 2 (320 °C). This dramatic improvement implied the critical role of Pt-sulfate synergy in altering propane adsorption/dissociation and oxygen adsorption. Further systematic characterizations, kinetic studies, and theoretical calculations disclosed that the sulfate species could efficiently facilitate the activation/cleavage of the C–H bond of propane and the adsorption of the resulting intermediate (e.g., C 3 H 7 *), while simultaneously weakening oxygen adsorption. The synergistic regulation of C 3 H 8 and O 2 adsorption for alleviating competitive adsorption provides a clear explanation for the superior activity on sulfate-modified Pt catalysts in propane combustion. This work offers fundamental insights into the design of efficient catalysts for alkane combustion through tailoring adsorption behavior.
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