MAPO-5 molecular sieves from alkylimidazolium bromide ionic liquids

IF 4.8 3区材料科学 Q1 CHEMISTRY, APPLIED

Microporous and Mesoporous Materials Pub Date : 2024-11-06 DOI:10.1016/j.micromeso.2024.113400

Susan C. Citrak , Beatriz Ehlke , Stacey I. Zones , Dan Xie , Son-Jong Hwang , Andrew S. Ichimura , Linjuan Zhang , Shibo Xi , Scott R.J. Oliver

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Abstract

The ionic liquids diisopropylimidazolium bromide (DIPI) and diisobutylimidazolium bromide (DIBU) were used both as solvents and structure-directing agents (SDAs) to obtain AlPO₄-5 and MnAPO-5 (Mn-AFI) molecular sieves. For increasing level of manganese, DIBU always yielded pure-phase Mn-AFI whereas DIPI led to amorphous product when more than 0.13 eq of Mn was added. Varying amounts of water, HF and metal led to AFI, cristobalite or tridymite phases. We also explored the use of nickel as the metal dopant, and although AFI phase were obtained under certain conditions, no framework incorporation of the metal was observed. Because of the vanishingly low vapor pressure of the ILs, the synthesis does not carry the risk of pressure build-up. The ILs were easily and fully recyclable and used for multiple syntheses. The MnAPO-5 material was characterized with powder X-ray diffraction (PXRD), thermogravimetric analysis (TGA), electron paramagnetic resonance (EPR), multinuclear solid-state nuclear magnetic resonance (SS-NMR) and X-ray absorption fine structure (XAFS). These findings provide new insight into the ionothermal synthesis of metal-doped AFI frameworks with possible implications in catalytic applications.

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来自烷基溴化咪唑离子液体的 MAPO-5 分子筛

使用离子液体二异丙基溴化咪唑（DIPI）和二异丁基溴化咪唑（DIBU）作为溶剂和结构引导剂（SDA），获得了 AlPO4-5 和 MnAPO-5 (Mn-AFI) 分子筛。随着锰含量的增加，DIBU 始终能得到纯相 Mn-AFI，而 DIPI 则会在锰含量超过 0.13 eq 时产生无定形产物。不同量的水、氢氟酸和金属会产生 AFI、嵴钙锰铁矿或三菱锰矿。我们还探索了使用镍作为金属掺杂剂，虽然在某些条件下获得了 AFI 相，但没有观察到金属的框架结合。由于 IL 的蒸气压非常低，因此合成过程不会产生压力升高的风险。ILs 易于完全回收并可用于多次合成。通过粉末 X 射线衍射 (PXRD)、热重分析 (TGA)、电子顺磁共振 (EPR)、多核固态核磁共振 (SS-NMR) 和 X 射线吸收精细结构 (XAFS) 对 MnAPO-5 材料进行了表征。这些发现为离子热合成掺杂金属的 AFI 框架提供了新的视角，并可能对催化应用产生影响。

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来源期刊

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.