γ-氨基丁酸促进β沸石结晶及其在氨直接胺化异丁烯中的应用

IF 4.8 3区 材料科学 Q1 CHEMISTRY, APPLIED
Yijun Zhong , Dongpu Zhao , Weifeng Chu , Fucun Chen , Jie An , Yanan Wang , Wanling Shen , Shenglin Liu , Longya Xu
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引用次数: 0

摘要

沸石是石油炼制和精细化工过程中重要的催化剂。本文报道了一种通过添加γ-氨基丁酸(GABA)作为促进剂大大缩短β沸石结晶时间的新方法。通过XRD、SEM、TEM、TG-DTG、NH3-TPD、Py-IR、NMR等表征手段,系统研究了GABA对β分子筛合成的促进作用。结果表明,在140°C(初始Si/Al2 = 43)的水热合成条件下,GABA的加入使结晶时间从130 h显著缩短到18 h,同时将产物收率从51.7%提高到76.1%。Si/Al2比值从22.6增加到33.1,表明GABA调节了沸石成核过程中铝掺入动力学。GABA可以破坏TEA+和铝硅酸盐周围的水化层,从而加速5Rs结构的形成和成核过程。同时,TEAOH的Hoffmann分解也受到抑制。与常规合成的β沸石相比,快速合成的β沸石具有较高的产率和较高的Si/Al2比,由于其相对较高的弱酸位点,在异丁烯(i-C4H8)与氨(NH3)的直接胺化反应中表现出相当甚至更好的催化性能。
本文章由计算机程序翻译,如有差异,请以英文原文为准。

γ-Aminobutyric acid-promoted crystallization of Beta zeolite and its application for direct amination of isobutene with ammonia

γ-Aminobutyric acid-promoted crystallization of Beta zeolite and its application for direct amination of isobutene with ammonia
Beta zeolite is a significant catalyst used in petroleum refining and fine chemical course. We report a novel way to considerably shorten the crystallization time of Beta zeolite by adding γ-aminobutyric acid (GABA) as a ‘promoter’. The synthesis parameters are systematically investigated to unveil the promotion effect of GABA on Beta zeolite synthesis via a range of characterization skills, such as XRD, SEM, TEM, TG-DTG, NH3-TPD, Py-IR and NMR. The results demonstrate that under hydrothermal synthesis at 140 °C (initial Si/Al2 = 43), the addition of GABA has been shown to result in a significant reduction in crystallization time, from 130 h to 18 h, while concurrently enhancing product yield from 51.7 % to 76.1 %. The resulting Si/Al2 ratio increases from 22.6 to 33.1, suggesting that GABA regulates aluminum incorporation kinetics during zeolite nucleation. GABA can break the hydration layer round TEA+ and aluminosilicate, and consequently, the formation of 5Rs structure and the nucleation process are accelerated. Meanwhile, the Hoffmann decomposition of TEAOH is inhibited as well. In comparison with the conventionally synthesized counterpart, the fast-synthesized Beta zeolite possessing high product yield and high Si/Al2 ratio, exhibits comparable or even better catalytic performance in the direct amination of isobutene (i-C4H8) with ammonia (NH3), due to its relatively high concentration of weak acid site.
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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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