在 Pt@Sn-MFI 沸石上增强甘油对二羟基丙酮的选择性氧化作用

IF 3.8 3区工程技术 Q2 ENGINEERING, CHEMICAL

Industrial & Engineering Chemistry Research Pub Date : 2024-09-19 DOI:10.1021/acs.iecr.4c01831

Shiwei Wang, Tianhao Li, Yanle Li, Hongfeng Yin, Ziqi Tian, Hongbo Yu

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引用次数: 0

摘要

在将生物柴油生产过程中产生的甘油（GL）选择性氧化为高价值的二羟基丙酮（DHA）的过程中，支撑铂纳米颗粒（NPs）表现出卓越的活性。然而，由于 GL 中的主 -OH 优先氧化，它们对 DHA 的选择性并不令人满意。本研究采用原位封装策略合成了具有 4.0 nm Pt NPs 和不同 Si/Sn 比率的 Pt@Sn-MFI。优化后的 Pt@Sn-MFI-80 催化剂对 DHA 的选择性为 74.8%，60 °C 时的 GL 转化率为 43.5%。我们的实验和密度泛函理论（DFT）计算表明，优异的选择性归因于铂和锡-MFI 之间的协同效应。Sn-MFI 使铂氮氧化物进入贫电子状态，从而抑制了甘油醛 (GLD) 的进一步氧化；然后，Sn-MFI 触发 GLD 异构化生成 DHA。核壳结构不仅保证了铂和 Sn-MFI 的亲密接触，还增强了活性铂 NPs 的稳定性。

本文章由计算机程序翻译，如有差异，请以英文原文为准。

Enhanced Selective Oxidation of Glycerol to Dihydroxyacetone over Pt@Sn-MFI Zeolites

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Enhanced Selective Oxidation of Glycerol to Dihydroxyacetone over Pt@Sn-MFI Zeolites

Supported Pt nanoparticles (NPs) exhibit excellent activity for the selective oxidation of glycerol (GL) derived from biodiesel production to high-value dihydroxyacetone (DHA). However, their selectivity to DHA is not satisfactory due to the preferential oxidation of the primary −OH in GL. In this study, Pt@Sn-MFI with ∼4.0 nm Pt NPs and different Si/Sn ratios were synthesized by an in situ encapsulation strategy. The optimized Pt@Sn-MFI-80 catalyst presents a 74.8% selectivity to DHA with a GL conversion of 43.5% at 60 °C. Our experiments and density functional theory (DFT) calculations indicated that the excellent selectivity was ascribed to the synergistic effect between Pt and Sn-MFI. Sn-MFI turned Pt NPs into an electronic-poor state so that suppressed further oxidation of glyceraldehyde (GLD); then, Sn-MFI triggered isomerization of GLD to generate DHA. The core–shell structure not only guaranteed an intimate contact between Pt and Sn-MFI but also enhanced the stability of the active Pt NPs.

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来源期刊

Industrial & Engineering Chemistry Research 工程技术-工程：化工

CiteScore

7.40

自引率

7.10%

发文量

1467

审稿时长

2.8 months

期刊介绍： ndustrial & Engineering Chemistry, with variations in title and format, has been published since 1909 by the American Chemical Society. Industrial & Engineering Chemistry Research is a weekly publication that reports industrial and academic research in the broad fields of applied chemistry and chemical engineering with special focus on fundamentals, processes, and products.