Transition metal oxide manipulating ZrO2-based non-precious metal catalysts for enhanced CO2-mediated oxidative dehydrogenation of propane

Zelin Ma, Fang Wang, Luomeng Zhao, Zhuangzhuang Ma, Weihao Zhao, Shiyuan Wang, Shuang Yazhou, Jiulong Wang, Jie Jian, Pengfei Guo, Hongqiang Wang

科研成果: 期刊稿件文章同行评审

摘要

BACKGROUND: Developing highly stable and cost-effective catalysts for CO2-mediated oxidative dehydrogenation of propane (CO2-ODP) is critical to advancing sustainable propylene production. While ZrO2-based supports offer promising thermal stability and tunable acid–base properties, integrating transition metal oxides (TMOx) as active sites to optimize CO2 activation and propane conversion remains underexplored. RESULTS: Here, we systematically design a series of non-precious metal TMOx/ZrO2 catalysts (TM = Cr, Fe, Co, Ni, Cu, Zn) via a coprecipitation–gel method to uncover structure–activity relationships. Among them, CrOx/ZrO2 emerges as the optimal candidate, achieving notable C3H8/CO2 conversions of 46.24%/38.27% and 86.49%/27.03% C3H6 selectivity/yield at 600 °C. Characterization reveals that the coexistence of Cr3+/Cr4+ species (XPS) and mixed-phase Cr2O3/CrO2 (XRD/Raman) creates abundant oxygen vacancies and enhances CO2 adsorption (TPD), while HRTEM/EDX confirms uniform CrOx dispersion on ZrO2. Further optimizing the Cr/Zr ratio to 1:1 maximizes active site exposure while preventing excessive aggregation, thereby balancing redox activity and structural stability. CONCLUSIONS: This work elucidates how tailored TMOx/ZrO2 interfaces leverage synergistic electronic and geometric effects to drive CO2-ODP efficiency, offering a blueprint for designing high-performance non-precious metal catalysts for alkane valorization.

源语言英语
期刊Journal of Chemical Technology and Biotechnology
DOI
出版状态已接受/待刊 - 2025

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