原子分散锌位限制在层状硅-2沸石与丙烷脱氢增强的稳定性

IF 4.5 3区 材料科学 Q1 CHEMISTRY, APPLIED Microporous and Mesoporous Materials Pub Date : 2025-03-15 Epub Date: 2025-01-08 DOI:10.1016/j.micromeso.2025.113503
Jun Zhao , Zhaopeng Liu , Dehui Wang , Lei Zhao , Diandian Shi , Zhiyu He , Feng Shao , Peng Lu , Valentin Valtchev
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引用次数: 0

摘要

制备成本低、环境友好的非氧化丙烷脱氢(PDH)催化剂以替代铂基和铬基催化剂是人们多年来一直追求的目标。锌基催化剂在PDH过程中表现出了很大的潜力,但其活性和稳定性仍有待提高。在此,我们报道了一种锌基沸石催化剂,其原子锌活性位点高度分散并限制在层状纯硅沸石(硅石-2)中,通过一锅水热合成法使用配体保护方法。利用互补表征技术明确证实了分离的Zn2+物种的原子分散及其在纯硅LS-2-150沸石中被Si - OH成功捕获和稳定。在PDH反应(550℃,WHSV = 2.4 h−1)中,优化后的zn2.65% @LS-2具有良好的初始活性(丙烷转化率为32.2%,丙烯选择性为90.1%)和良好的催化稳定性(失活率为0.0087 h−1)。因此,这项工作提出了一种高活性和更耐用的锌基沸石催化剂,有望用于PDH应用。
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Atomically dispersed zinc sites confined in a layered silicalite-2 zeolite with enhanced stability for propane dehydrogenation
The goal of obtaining non-oxidative propane dehydrogenation (PDH) catalysts with low cost and environmental friendliness as alternatives to Pt and Cr-based catalysts, has been pursued for years. Zn-based catalysts have demonstrated great potential in the PDH process, but their activity and stability still need to be improved. Herein, we report a Zn-based zeolite catalyst with atomic Zn active sites that are highly dispersed and confined in a layered-like pure silica zeolite (Silicalite-2), via one-pot hydrothermal synthesis using a ligand-protection method. The atomic dispersion of isolated Zn2+ species and their successful trapping and stabilizing by Si−OH in pure-silica LS-2-150 zeolite are unambiguously corroborated using complementary characterization techniques. In PDH reaction (550 °C, WHSV = 2.4 h−1), the optimized Zn2.65 %@LS-2 exhibits excellent initial activity (the propane conversion at 32.2 % and the propene selectivity at 90.1 %) and good catalytic stability after 6 cycles for 60 h on stream (the deactivation rate of 0.0087 h−1). Thus, this work presents a highly active and more durable Zn-based zeolite catalyst that is promising for PDH applications.
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来源期刊
Microporous and Mesoporous Materials
Microporous and Mesoporous Materials 化学-材料科学:综合
CiteScore
10.70
自引率
5.80%
发文量
649
审稿时长
26 days
期刊介绍: Microporous and Mesoporous Materials covers novel and significant aspects of porous solids classified as either microporous (pore size up to 2 nm) or mesoporous (pore size 2 to 50 nm). The porosity should have a specific impact on the material properties or application. Typical examples are zeolites and zeolite-like materials, pillared materials, clathrasils and clathrates, carbon molecular sieves, ordered mesoporous materials, organic/inorganic porous hybrid materials, or porous metal oxides. Both natural and synthetic porous materials are within the scope of the journal. Topics which are particularly of interest include: All aspects of natural microporous and mesoporous solids The synthesis of crystalline or amorphous porous materials The physico-chemical characterization of microporous and mesoporous solids, especially spectroscopic and microscopic The modification of microporous and mesoporous solids, for example by ion exchange or solid-state reactions All topics related to diffusion of mobile species in the pores of microporous and mesoporous materials Adsorption (and other separation techniques) using microporous or mesoporous adsorbents Catalysis by microporous and mesoporous materials Host/guest interactions Theoretical chemistry and modelling of host/guest interactions All topics related to the application of microporous and mesoporous materials in industrial catalysis, separation technology, environmental protection, electrochemistry, membranes, sensors, optical devices, etc.
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