Yijun Zhong , Dongpu Zhao , Weifeng Chu , Fucun Chen , Jie An , Yanan Wang , Wanling Shen , Shenglin Liu , Longya Xu
{"title":"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","authors":"Yijun Zhong , Dongpu Zhao , Weifeng Chu , Fucun Chen , Jie An , Yanan Wang , Wanling Shen , Shenglin Liu , Longya Xu","doi":"10.1016/j.micromeso.2025.113648","DOIUrl":null,"url":null,"abstract":"<div><div>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, NH<sub>3</sub>-TPD, Py-IR and NMR. The results demonstrate that under hydrothermal synthesis at 140 °C (initial Si/Al<sub>2</sub> = 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/Al<sub>2</sub> 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<sup>+</sup> 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/Al<sub>2</sub> ratio, exhibits comparable or even better catalytic performance in the direct amination of isobutene (<em>i</em>-C<sub>4</sub>H<sub>8</sub>) with ammonia (NH<sub>3</sub>), due to its relatively high concentration of weak acid site.</div></div>","PeriodicalId":392,"journal":{"name":"Microporous and Mesoporous Materials","volume":"392 ","pages":"Article 113648"},"PeriodicalIF":4.8000,"publicationDate":"2025-04-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"γ-Aminobutyric acid-promoted crystallization of Beta zeolite and its application for direct amination of isobutene with ammonia\",\"authors\":\"Yijun Zhong , Dongpu Zhao , Weifeng Chu , Fucun Chen , Jie An , Yanan Wang , Wanling Shen , Shenglin Liu , Longya Xu\",\"doi\":\"10.1016/j.micromeso.2025.113648\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<div><div>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, NH<sub>3</sub>-TPD, Py-IR and NMR. The results demonstrate that under hydrothermal synthesis at 140 °C (initial Si/Al<sub>2</sub> = 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/Al<sub>2</sub> 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<sup>+</sup> 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/Al<sub>2</sub> ratio, exhibits comparable or even better catalytic performance in the direct amination of isobutene (<em>i</em>-C<sub>4</sub>H<sub>8</sub>) with ammonia (NH<sub>3</sub>), due to its relatively high concentration of weak acid site.</div></div>\",\"PeriodicalId\":392,\"journal\":{\"name\":\"Microporous and Mesoporous Materials\",\"volume\":\"392 \",\"pages\":\"Article 113648\"},\"PeriodicalIF\":4.8000,\"publicationDate\":\"2025-04-17\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Microporous and Mesoporous Materials\",\"FirstCategoryId\":\"88\",\"ListUrlMain\":\"https://www.sciencedirect.com/science/article/pii/S1387181125001623\",\"RegionNum\":3,\"RegionCategory\":\"材料科学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q1\",\"JCRName\":\"CHEMISTRY, APPLIED\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Microporous and Mesoporous Materials","FirstCategoryId":"88","ListUrlMain":"https://www.sciencedirect.com/science/article/pii/S1387181125001623","RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"CHEMISTRY, APPLIED","Score":null,"Total":0}
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.
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.