{"title":"Nb 改性 AFI 拓扑分子筛的原位合成及其对 4,6-二甲基二苯并噻吩加氢脱硫高效催化剂形成的调控作用","authors":"","doi":"10.1016/j.seppur.2024.129914","DOIUrl":null,"url":null,"abstract":"<div><div>Herein, molecular sieves with Nb and Si modified AFI-type structures were successfully synthesized in situ via a hydrothermal synthesis method. Subsequently, the corresponding NiW catalysts modified by the molecular sieve were obtained through incipient co-impregnation. The performance of NiW catalysts for 4,6-dimenthyldibenzothiophene (4,6-DMDBT) was comprehensively investigated. A series of characterizations demonstrated that Nb species were uniformly distributed within the AFI framework. This not only resulted in an increase in the acidic sites of both molecular sieves and hybrid-support (NbSAPO-5-alumina), but also effectively modulated the interaction between hybrid support and active metals. This led to a higher stacking numbers, which facilitated the sulfidation of W and Ni species, ultimately promoting the formation of more active edge sites on WS<sub>2</sub> slabs. This resulted in the catalyst NiW/NbSAPOA achieving a significantly higher desulfurization ratio of 95.8 % for 4,6-DMDBT at 280 ℃. Furthermore, the catalyst NiW/NbSAPOA exhibited the highest turnover frequency of 9.17 × 10<sup>−4</sup> s<sup>−1</sup>, and markedly enhanced selectivity for the direct desulfurization pathway in 4,6-DMDBT HDS.</div></div>","PeriodicalId":427,"journal":{"name":"Separation and Purification Technology","volume":null,"pages":null},"PeriodicalIF":8.1000,"publicationDate":"2024-09-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"In situ synthesis of Nb-modified AFI topology molecular sieve and its modulation on the formantion of high-efficiency catalyst for 4,6-dimethyldibenzothiophene hydrodesulfurization\",\"authors\":\"\",\"doi\":\"10.1016/j.seppur.2024.129914\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<div><div>Herein, molecular sieves with Nb and Si modified AFI-type structures were successfully synthesized in situ via a hydrothermal synthesis method. Subsequently, the corresponding NiW catalysts modified by the molecular sieve were obtained through incipient co-impregnation. The performance of NiW catalysts for 4,6-dimenthyldibenzothiophene (4,6-DMDBT) was comprehensively investigated. A series of characterizations demonstrated that Nb species were uniformly distributed within the AFI framework. This not only resulted in an increase in the acidic sites of both molecular sieves and hybrid-support (NbSAPO-5-alumina), but also effectively modulated the interaction between hybrid support and active metals. This led to a higher stacking numbers, which facilitated the sulfidation of W and Ni species, ultimately promoting the formation of more active edge sites on WS<sub>2</sub> slabs. This resulted in the catalyst NiW/NbSAPOA achieving a significantly higher desulfurization ratio of 95.8 % for 4,6-DMDBT at 280 ℃. Furthermore, the catalyst NiW/NbSAPOA exhibited the highest turnover frequency of 9.17 × 10<sup>−4</sup> s<sup>−1</sup>, and markedly enhanced selectivity for the direct desulfurization pathway in 4,6-DMDBT HDS.</div></div>\",\"PeriodicalId\":427,\"journal\":{\"name\":\"Separation and Purification Technology\",\"volume\":null,\"pages\":null},\"PeriodicalIF\":8.1000,\"publicationDate\":\"2024-09-28\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Separation and Purification Technology\",\"FirstCategoryId\":\"5\",\"ListUrlMain\":\"https://www.sciencedirect.com/science/article/pii/S1383586624036530\",\"RegionNum\":1,\"RegionCategory\":\"工程技术\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q1\",\"JCRName\":\"ENGINEERING, CHEMICAL\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Separation and Purification Technology","FirstCategoryId":"5","ListUrlMain":"https://www.sciencedirect.com/science/article/pii/S1383586624036530","RegionNum":1,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"ENGINEERING, CHEMICAL","Score":null,"Total":0}
引用次数: 0
摘要
在此,通过水热合成法成功地在原位合成了具有 Nb 和 Si 修饰 AFI 型结构的分子筛。随后,通过萌发共浸渍法获得了分子筛修饰的相应 NiW 催化剂。研究人员全面考察了 NiW 催化剂对 4,6-二甲基二苯并噻吩(4,6-DMDBT)的性能。一系列表征结果表明,铌物种均匀地分布在 AFI 框架中。这不仅增加了分子筛和混合支撑(NbSAPO-5-氧化铝)的酸性位点,还有效调节了混合支撑与活性金属之间的相互作用。这导致了更高的堆叠数,有利于 W 和 Ni 的硫化,最终促进在 WS2 板上形成更多的活性边缘位点。这使得催化剂 NiW/NbSAPOA 在 280 ℃ 下对 4,6-DMDBT 的脱硫率显著提高,达到 95.8%。此外,催化剂 NiW/NbSAPOA 的翻转频率最高,达到 9.17 × 10-4 s-1,并显著提高了 4,6-DMDBT 加氢脱硫过程中直接脱硫途径的选择性。
In situ synthesis of Nb-modified AFI topology molecular sieve and its modulation on the formantion of high-efficiency catalyst for 4,6-dimethyldibenzothiophene hydrodesulfurization
Herein, molecular sieves with Nb and Si modified AFI-type structures were successfully synthesized in situ via a hydrothermal synthesis method. Subsequently, the corresponding NiW catalysts modified by the molecular sieve were obtained through incipient co-impregnation. The performance of NiW catalysts for 4,6-dimenthyldibenzothiophene (4,6-DMDBT) was comprehensively investigated. A series of characterizations demonstrated that Nb species were uniformly distributed within the AFI framework. This not only resulted in an increase in the acidic sites of both molecular sieves and hybrid-support (NbSAPO-5-alumina), but also effectively modulated the interaction between hybrid support and active metals. This led to a higher stacking numbers, which facilitated the sulfidation of W and Ni species, ultimately promoting the formation of more active edge sites on WS2 slabs. This resulted in the catalyst NiW/NbSAPOA achieving a significantly higher desulfurization ratio of 95.8 % for 4,6-DMDBT at 280 ℃. Furthermore, the catalyst NiW/NbSAPOA exhibited the highest turnover frequency of 9.17 × 10−4 s−1, and markedly enhanced selectivity for the direct desulfurization pathway in 4,6-DMDBT HDS.
期刊介绍:
Separation and Purification Technology is a premier journal committed to sharing innovative methods for separation and purification in chemical and environmental engineering, encompassing both homogeneous solutions and heterogeneous mixtures. Our scope includes the separation and/or purification of liquids, vapors, and gases, as well as carbon capture and separation techniques. However, it's important to note that methods solely intended for analytical purposes are not within the scope of the journal. Additionally, disciplines such as soil science, polymer science, and metallurgy fall outside the purview of Separation and Purification Technology. Join us in advancing the field of separation and purification methods for sustainable solutions in chemical and environmental engineering.