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用丝光沸石纳米晶体调节AlO纳米纤维中的催化酸度用于脱水反应。

Tuning the catalytic acidity in AlO nanofibers with mordenite nanocrystals for dehydration reactions.

作者信息

Rodriguez-Olguin M A, Cruz-Herbert R N, Atia H, Bosco M, Fornero E L, Eckelt R, De Haro Del Río D A, Aguirre A, Gardeniers J G E, Susarrey-Arce A

机构信息

Mesoscale Chemical Systems, MESA+ Institute, University of Twente PO. Box 217, 7500AE Enschede The Netherlands

Universidad Autónoma de Nuevo León, Facultad de Ciencias Químicas Pedro de Alba S/N San Nicolás de los Garza Nuevo León 64455 Mexico

出版信息

Catal Sci Technol. 2022 May 11;12(13):4243-4254. doi: 10.1039/d2cy00143h. eCollection 2022 Jul 4.

Abstract

Alumina (AlO) is one of the most used supports in the chemical industry due to its exceptional thermal stability, surface area, and acidic properties. Mesoscopic structured alumina with adequate acidic properties is important in catalysis to enhance the selectivity and conversion of certain reactions and processes. This study introduces a synthetic method based on electrospinning to produce AlO nanofibers (ANFs) with zeolite mordenite (MOR) nanocrystals (hereafter, hybrid ANFs) to tune the textural and surface acidity properties. The hybrid ANFs with electrospinning form a non-woven network with macropores. ANF-HMOR, , ANFs containing protonated mordenite (HMOR), shows the highest total acidity of 276 μmol g as determined with infrared spectroscopy using pyridine as a molecular probe (IR-Py). IR-Py results reveal that Lewis acid sites are prominently present in the hybrid ANFs. Brønsted acid sites are also observed in the hybrid ANFs and are associated with the HMOR presence. The functionality of hybrid ANFs is evaluated during methanol dehydration to dimethyl ether (DME). The proof of concept reaction reveals that ANF-HMOR is the more active and selective catalyst with 87% conversion and nearly 100% selectivity to DME at 573 K. The results demonstrate that the textural properties and the acid site type and content can be modulated in hybrid ANF structures, synergistically improving the selectivity and conversion during the methanol dehydration reaction. From a broader perspective, our results promote the utilization of hybrid structural materials as a means to tune chemical reactions selectively.

摘要

氧化铝(Al₂O₃)因其出色的热稳定性、表面积和酸性特性,是化学工业中最常用的载体之一。具有适当酸性特性的介观结构氧化铝在催化中对于提高某些反应和过程的选择性及转化率很重要。本研究介绍了一种基于静电纺丝的合成方法,以制备含有丝光沸石(MOR)纳米晶体的Al₂O₃纳米纤维(以下简称混合ANF),从而调节其结构和表面酸性特性。通过静电纺丝制备的混合ANF形成了具有大孔的非织造网络。ANF-HMOR(即含有质子化丝光沸石(HMOR)的ANF)在用吡啶作为分子探针的红外光谱法(IR-Py)测定时,显示出最高的总酸度为276 μmol/g。IR-Py结果表明,混合ANF中显著存在路易斯酸位点。在混合ANF中也观察到了布朗斯台德酸位点,且与HMOR的存在有关。在甲醇脱水制二甲醚(DME)过程中评估了混合ANF的功能。概念验证反应表明,ANF-HMOR是更具活性和选择性的催化剂,在573 K时对DME的转化率为87%,选择性接近100%。结果表明,在混合ANF结构中可以调节其结构特性以及酸位点类型和含量,协同提高甲醇脱水反应过程中的选择性和转化率。从更广泛的角度来看,我们的结果促进了混合结构材料作为一种选择性调节化学反应手段的应用。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/aa03/9252259/28daff90c5da/d2cy00143h-f1.jpg

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