构建三配位 Al (AlIII) 位点,促进 Pt/Al2O3 催化剂的丙烷完全氧化作用

IF 4.4 3区 化学 Q2 CHEMISTRY, PHYSICAL Catalysis Science & Technology Pub Date : 2024-06-10 DOI:10.1039/d4cy00582a
Yang You, Aijie Xu, Yao Lv, Lide Yang, Xuan Tang, Jie Tang, Yanglong Guo, Yao Cui, Wangcheng Zhan, Li Wang, Yun Guo, Sheng Dai
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引用次数: 0

摘要

丙烷的完全氧化在汽车排放控制和挥发性有机化合物消除领域引起了极大关注。然而,由于丙烷的稳定性,实现该反应的高活性具有挑战性。在此,我们利用一种简便的溶热法在合成的 ST-Al2O3 支持物上构建三配位的 Al (AlIII) 位点,以改变支持的铂物种的性质。研究表明,AlIII 位点有助于支撑铂位点的分散和电子富集。因此,Pt/ST-Al2O3 在完全氧化丙烷方面表现出卓越的活性,与商用 Pt/Al2O3 催化剂相比,翻转频率提高了 6.7 倍。同时,由于 Pt/ST-Al2O3 具有更强的 C-H 和 C-C 裂解能力,因此具有独特的反应路线,不仅在完全氧化丙烷方面,而且在完全氧化其他烷烃(CH4、C2H6 和 n-C4H10)方面也具有出色的活性。此外,AlIII 构建策略还成功地扩展到了更多情况,例如具有更高钯分散度和电子密度的 Pd/ST-Al2O3。这项工作为控制氧化物支持物以设计和合成先进的烷烃氧化催化剂提供了一种前景广阔的策略。
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Constructing tri-coordinated Al (AlIII) sites to boost complete propane oxidation of the Pt/Al2O3 catalyst
Complete oxidation of propane has drawn great attention in the fields of automotive emission control and volatile organic compound elimination. However, it is challenging to achieve high activity of this reaction due to the stability of propane. We here utilize a facile solvothermal method to construct tri-coordinated Al (AlIII) sites on the as-synthesized ST-Al2O3 support to alter the properties of supported Pt species. It is demonstrated that AlIII sites facilitate the dispersion and electron enrichment of supported Pt sites. Thus, Pt/ST-Al2O3 exhibits a superior activity toward complete propane oxidation, showing a 6.7-fold improvement in the turnover frequency over commercial Pt/Al2O3 catalysts. Meanwhile, Pt/ST-Al2O3 possesses a distinct reaction route originating from its stronger C–H and C–C cleavage capability, while having excellent activity not only in complete propane oxidation but also in the complete oxidation of other alkanes (CH4, C2H6, and n-C4H10). In addition, the AlIII construction strategy is successfully extended to more cases, e.g., Pd/ST-Al2O3 with higher Pd dispersion and electron density. This work provides a promising strategy for the control of the oxide support for advanced design and synthesis of alkane oxidation catalysts.
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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
期刊最新文献
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