利用zno辅助沸石间转化强化催化突破沸石合成障碍

IF 7.2 2区材料科学 Q2 CHEMISTRY, PHYSICAL

Chemistry of Materials Pub Date : 2025-05-27 DOI:10.1021/acs.chemmater.5c00431

Mostafa Torka Beydokhti, Gleb Ivanushkin, Ibrahim Khalil, Ahmed Sajid, Juna Bae, Aram Bugaev, Thibaut Donckels, Dieter Plessers, Michiel Dusselier

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引用次数: 0

摘要

沸石间转化（IZC）可以利用晶体的选择性溶解来克服向特殊相转变的动力学障碍。在ZnO的存在下，硅质丝光沸石（MOR）的受控溶解使我们能够“捕获”锌硅酸盐铁素体（FER）拓扑结构。结构表征证明，通过温和后处理实现的缺陷工程可以调整其组成和性能，从Si/Al和Si/Zn比分别为170和36的含锌FER到Si/Al比为170和Si/Zn比为700的高硅FER，这是在氢氧化物介质中一步合成难以达到的。酸洗的程度可以调节框架Zn向Lewis酸催化剂和几乎非酸性高硅对应物的方向发展。在此过程中，我们为锌杂原子对IZC动力学的影响和作用提供了丰富的新见解。由于Zn-FER通过IZC和后处理获得了独特的织构性质，并且表现出较少的Bro - nsted酸性，Zn-FER在CO2加氢制烃反应中对二甲醚（DME）的选择性增强，寿命长。

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Breaking Barriers in Zeolite Synthesis via ZnO-Assisted Interzeolite Conversion for Enhanced Catalysis

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Breaking Barriers in Zeolite Synthesis via ZnO-Assisted Interzeolite Conversion for Enhanced Catalysis

Interzeolite Conversion (IZC) can overcome kinetic hurdles toward exceptional phases by taking advantage of the selective dissolution of crystalline ones. Controlled dissolution of a siliceous mordenite (MOR) in the presence of ZnO enables us to ‘catch’ a zincosilicate ferrierite (FER) topology. Structural characterization proves that defect engineering achieved from a mild post-treatment can tune composition and properties ranging from a Zn-containing FER with Si/Al and Si/Zn ratios of 170 and 36 to a high-silica FER with a Si/Al ratio of 170 and Si/Zn ratio of 700, which is challenging to reach from one-step synthesis in hydroxide media. The extent of acid washing can regulate the framework Zn species toward a Lewis acid catalyst and an almost nonacidic high-silica counterpart. Along the way, we provide ample new insights into the influence and role of zinc heteroatom on the kinetics of IZC. Due to the custom textural properties obtained by IZC, post-treatment, and also by exhibiting Lewis acidity with less Bro̷nsted acidity, Zn-FER shows enhanced selectivity and long lifetime for dimethyl ether (DME) production in the CO₂ hydrogenation to hydrocarbons reaction.

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来源期刊

Chemistry of Materials 工程技术-材料科学：综合

CiteScore

14.10

自引率

5.80%

发文量

929

审稿时长

1.5 months

期刊介绍： The journal Chemistry of Materials focuses on publishing original research at the intersection of materials science and chemistry. The studies published in the journal involve chemistry as a prominent component and explore topics such as the design, synthesis, characterization, processing, understanding, and application of functional or potentially functional materials. The journal covers various areas of interest, including inorganic and organic solid-state chemistry, nanomaterials, biomaterials, thin films and polymers, and composite/hybrid materials. The journal particularly seeks papers that highlight the creation or development of innovative materials with novel optical, electrical, magnetic, catalytic, or mechanical properties. It is essential that manuscripts on these topics have a primary focus on the chemistry of materials and represent a significant advancement compared to prior research. Before external reviews are sought, submitted manuscripts undergo a review process by a minimum of two editors to ensure their appropriateness for the journal and the presence of sufficient evidence of a significant advance that will be of broad interest to the materials chemistry community.