配体保护和低温水热法合成包裹在 TON 沸石中的铂,用于糠醛到糠醇的形状选择性加氢反应

IF 10.7 2区 材料科学 Q1 CHEMISTRY, PHYSICAL Journal of Materials Chemistry A Pub Date : 2024-11-13 DOI:10.1039/d4ta07243j
Xuelin Wang, Congxin Wang, Wentao Bi, Wei Qu, Zhijian Tian
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引用次数: 0

摘要

将金属包封在沸石中是一种有效的方法,可以利用沸石微通道的空间限制提高金属/沸石催化剂在加氢反应中的催化选择性。在此,我们采用配体保护和低温水热结晶法合成了封装在具有 TON 拓扑结构的沸石(Pt@ZSM-22)中的铂。利用 XRD、SEM、TEM、TG-DSC-MS 和 13C CP/MAS NMR 对水热过程进行了跟踪研究。实验结果表明,金属前驱体([Pt(en)2]2+)的分解和还原通常发生在苛刻的水热条件下,而在较低的水热温度(140 °C)和配体(乙二胺)的保护下,金属前驱体([Pt(en)2]2+)的分解和还原得到了有效抑制。完整的[Pt(en)2]2+静电吸附在无定形硅酸盐纳米颗粒(沸石前体)上,并在这些纳米颗粒结晶时被包裹在 ZSM-22 晶体内部。通过直接用 H2 还原去除模板并还原 [Pt(en)2]2+,成功地获得了嵌入 ZSM-22 沸石内部的高度分散和均匀的铂粒子。为了评估封装 Pt@ZSM-22 的选择性氢化性能,研究人员进行了糠醛氢化成糠醇的反应。反应结果表明,在转化率为 99.5% 时,封装 Pt@ZSM-22 对糠醛醇的选择性高达 97.6%,优于支撑 Pt/ZSM-22。优异的糠醇选择性反映了 ZSM-22 一维微通道的空间限制所赋予的形状选择性。利用吸附糠醛的 CO-FT-IR、XPS、XAFS 和 FT-IR,揭示了 Pt@ZSM-22 的结构-活性关系。我们的工作不仅成功地实现了在具有一维直通道的沸石中直接水热合成金属封装,而且证明了这种催化剂在选择性催化中的巨大应用潜力。
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Ligand-protected and lowered-temperature hydrothermal synthesis of platinum encapsulated in TON zeolite for shape-selective hydrogenation of furfural to furfuryl alcohol
Encapsulating metal in zeolite is an effective tactic to up-regulate the catalytic selectivity of metal/zeolite catalysts in hydrogenation reaction by virtue of the spatial confinement of the zeolite microchannels. Herein, we present the synthesis of Pt encapsulated in zeolite with TON topology (Pt@ZSM-22) by adopting the ligand-protected and lowered-temperature hydrothermal crystallization. The XRD, SEM, TEM, TG-DSC-MS, and 13C CP/MAS NMR are used to track the hydrothermal process. The experimental results indicate the decomposition and reduction of metal precursor ([Pt(en)2]2+), which usually occurs at the harsh hydrothermal conditions, is effectively restrained at the lowered hydrothermal temperature (140 °C) and with the protection of the ligand (ethylenediamine). The intact [Pt(en)2]2+ is electrostatically adsorbed on the amorphous silicate nanoparticles (the zeolite precursor) and is encapsulated inside the ZSM-22 crystals as these nanoparticles are crystallized. The highly-dispersed and uniform Pt particles embedded inside the ZSM-22 zeolite are successfully obtained by adopting the direct H2 reduction to remove the template and reduce the [Pt(en)2]2+. The hydrogenation of furfural to furfuryl alcohol was conducted to evaluate the selective hydrogenation performance of the encapsulated Pt@ZSM-22. The reaction results reveal the furfuryl alcohol selectivity reaches as high as 97.6% at a conversion of 99.5% over the encapsulated Pt@ZSM-22, which is superior to the supported Pt/ZSM-22. The excellent furfuryl alcohol selectivity reflects the shape selectivity conferred by the spatial confinement of the one-dimensional microchannels of ZSM-22. The CO-FT-IR, XPS, XAFS and FT-IR of adsorbed furfural are used to disclose the structure-activity relationship of Pt@ZSM-22. Our work not only successfully realizes the direct hydrothermal synthesis of metal encapsulation in zeolite with 1D straight channels but also demonstrates the great application potentials of such catalysts in selective catalysis.
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来源期刊
Journal of Materials Chemistry A
Journal of Materials Chemistry A CHEMISTRY, PHYSICAL-ENERGY & FUELS
CiteScore
19.50
自引率
5.00%
发文量
1892
审稿时长
1.5 months
期刊介绍: The Journal of Materials Chemistry A, B & C covers a wide range of high-quality studies in the field of materials chemistry, with each section focusing on specific applications of the materials studied. Journal of Materials Chemistry A emphasizes applications in energy and sustainability, including topics such as artificial photosynthesis, batteries, and fuel cells. Journal of Materials Chemistry B focuses on applications in biology and medicine, while Journal of Materials Chemistry C covers applications in optical, magnetic, and electronic devices. Example topic areas within the scope of Journal of Materials Chemistry A include catalysis, green/sustainable materials, sensors, and water treatment, among others.
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