Catalytic deoxygenation of stearic acid into olefins over Pt catalysts supported on MOF-derived metal oxides†

IF 4.4 3区 化学 Q2 CHEMISTRY, PHYSICAL Catalysis Science & Technology Pub Date : 2024-06-17 DOI:10.1039/d4cy00189c
Kok Bing Tan , Yiping Liu , Youting Wang , Sajid Ali , Wendong Wang , Jingru Li , Longmei Shang , Xing Yan , Xiaodong Zhang , Guowu Zhan
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Abstract

In this study, three different metal oxides derived from metal–organic frameworks (MOFs), including CeO2, ZrO2, and Fe2O3 were used as porous supports for loading Pt nanoparticles, and the supported catalysts (viz., Pt/CeO2, Pt/ZrO2, and Pt/Fe2O3) were evaluated for the catalytic deoxygenation of stearic acid to produce olefins by analytical pyrolysis-gas chromatography/mass spectrometry (Py-GC/MS). Interestingly, Pt/CeO2 and Pt/Fe2O3 catalysts demonstrated high selectivity for olefins or aromatics, respectively, with alkanes as minor products, while the Pt/ZrO2 catalyst demonstrated the lowest deoxygenation efficiency. Among them, the Pt/CeO2 catalyst demonstrated the highest deoxygenation efficiency due to its highest oxygen vacancy density and the largest specific surface area (53 m2 g−1). It also demonstrated the highest selectivity for olefins (41%) due to the in situ partial formation of the bimetallic PtCe phase during the catalytic reaction at high temperature, which facilitates the decarbonylation pathway and leads to the formation of olefins as the main product. In addition, experimental optimizations of the reaction parameters were conducted on the designed Pt/CeO2 catalyst to further enhance olefin selectivity. Importantly, the Pt/CeO2 catalyst also maintained high olefin selectivity and stearic acid conversion even after six consecutive cycles. Therefore, this work has provided an alternative route to produce olefins via the decarbonylation of stearic acid over a supported Pt/CeO2 catalyst.

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以 MOF 衍生金属氧化物为支撑的 Pt 催化剂催化硬脂酸脱氧生成烯烃
本研究采用三种不同的金属氧化物衍生金属有机框架 (MOF),包括 CeO2、ZrO2 和 Fe2O3,作为负载铂纳米颗粒的多孔载体,并通过分析热解-气相色谱/质谱法 (Py-GC/MS) 评估了载体催化剂(即 Pt/CeO2、Pt/ZrO2 和 Pt/Fe2O3)催化硬脂酸脱氧生成烯烃的情况。有趣的是,Pt/CeO2 和 Pt/Fe2O3 催化剂分别对烯烃或芳烃具有较高的选择性,烷烃则是次要产物,而 Pt/ZrO2 催化剂的脱氧效率最低。其中,Pt/CeO2 催化剂的脱氧效率最高,这是因为它具有最高的氧空位密度和最大的比表面积(53 m2 g-1)。由于在高温催化反应过程中原位部分形成了双金属 PtCe 相,从而促进了脱羰基化途径,并形成了作为主要产物的烯烃,因此它对烯烃的选择性也最高(41%)。此外,还对所设计的 Pt/CeO2 催化剂的反应参数进行了实验优化,以进一步提高烯烃的选择性。重要的是,Pt/CeO2 催化剂在连续循环六次后仍能保持较高的烯烃选择性和硬脂酸转化率。因此,这项研究为在支撑型 Pt/CeO2 催化剂上通过硬脂酸脱羰基反应生产烯烃提供了另一条途径。
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来源期刊
Catalysis Science & Technology
Catalysis Science & Technology CHEMISTRY, PHYSICAL-
CiteScore
8.70
自引率
6.00%
发文量
587
审稿时长
1.5 months
期刊介绍: A multidisciplinary journal focusing on cutting edge research across all fundamental science and technological aspects of catalysis. Editor-in-chief: Bert Weckhuysen Impact factor: 5.0 Time to first decision (peer reviewed only): 31 days
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