{"title":"封闭在 Beta 沸石中的沸石框架 Ta 和 MoO3 可协同提高氧化脱硫的活性和稳定性。","authors":"Zhiguo Zhu, Songcheng Bo, Xueyun Wang, Fengyuan Zuo, Ting Su, Kaixuan Yang, Hongying Lü","doi":"10.1021/acs.langmuir.4c02369","DOIUrl":null,"url":null,"abstract":"<p><p>Oxidative desulfurization (ODS), as a novel desulfurization technique of fuel oil, possesses high desulfurization efficiency for aromatic sulfide and low cost, making it a promising approach. The key to the technology lies in the rational design of catalysts with high activity and stability. Polyoxometalates, which are environmentally friendly, cost-effective, and abundantly available, face constraints in the development of ODS applications due to their low specific surface area and difficulty in regeneration. Introducing metal oxides into carriers with large specific surface areas to obtain heterogeneous catalysts is an effective solution to this problem. Beta zeolites, with regular three-dimensional channel systems, large specific surface area, and superior thermal/hydrothermal stability, are usually used as carriers. In this work, we developed a strategy to enhance zeolite carrier utilization efficiency by introducing Ta<sup>5+</sup> species into the rigid framework of zeolites containing confined MoO<sub>3</sub>. The Ta species in the zeolite framework and the confined MoO<sub>3</sub> produce a synergistic effect, exhibiting extremely high catalytic activity for the aerobic oxidative desulfurization of various organic aromatic sulfur compounds under mild conditions (90 °C and atmospheric pressure) in a deep eutectic solvent, surpassing common heterogeneous catalysts for oxidative desulfurization. Moreover, it can resist the adverse effects of interferents, such as naphthalene and indole. Additionally, the confined nature of Beta zeolite endows it with exceptional stability, demonstrating distinctive recyclability.</p>","PeriodicalId":50,"journal":{"name":"Langmuir","volume":" ","pages":"18706-18716"},"PeriodicalIF":3.9000,"publicationDate":"2024-09-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Zeolitic Framework Ta and MoO<sub>3</sub> Confined in Beta Zeolite Cooperatively Enhance Activity and Stability for Oxidative Desulfurization.\",\"authors\":\"Zhiguo Zhu, Songcheng Bo, Xueyun Wang, Fengyuan Zuo, Ting Su, Kaixuan Yang, Hongying Lü\",\"doi\":\"10.1021/acs.langmuir.4c02369\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<p><p>Oxidative desulfurization (ODS), as a novel desulfurization technique of fuel oil, possesses high desulfurization efficiency for aromatic sulfide and low cost, making it a promising approach. The key to the technology lies in the rational design of catalysts with high activity and stability. Polyoxometalates, which are environmentally friendly, cost-effective, and abundantly available, face constraints in the development of ODS applications due to their low specific surface area and difficulty in regeneration. Introducing metal oxides into carriers with large specific surface areas to obtain heterogeneous catalysts is an effective solution to this problem. Beta zeolites, with regular three-dimensional channel systems, large specific surface area, and superior thermal/hydrothermal stability, are usually used as carriers. In this work, we developed a strategy to enhance zeolite carrier utilization efficiency by introducing Ta<sup>5+</sup> species into the rigid framework of zeolites containing confined MoO<sub>3</sub>. The Ta species in the zeolite framework and the confined MoO<sub>3</sub> produce a synergistic effect, exhibiting extremely high catalytic activity for the aerobic oxidative desulfurization of various organic aromatic sulfur compounds under mild conditions (90 °C and atmospheric pressure) in a deep eutectic solvent, surpassing common heterogeneous catalysts for oxidative desulfurization. Moreover, it can resist the adverse effects of interferents, such as naphthalene and indole. Additionally, the confined nature of Beta zeolite endows it with exceptional stability, demonstrating distinctive recyclability.</p>\",\"PeriodicalId\":50,\"journal\":{\"name\":\"Langmuir\",\"volume\":\" \",\"pages\":\"18706-18716\"},\"PeriodicalIF\":3.9000,\"publicationDate\":\"2024-09-03\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Langmuir\",\"FirstCategoryId\":\"92\",\"ListUrlMain\":\"https://doi.org/10.1021/acs.langmuir.4c02369\",\"RegionNum\":2,\"RegionCategory\":\"化学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"2024/8/19 0:00:00\",\"PubModel\":\"Epub\",\"JCR\":\"Q2\",\"JCRName\":\"CHEMISTRY, MULTIDISCIPLINARY\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Langmuir","FirstCategoryId":"92","ListUrlMain":"https://doi.org/10.1021/acs.langmuir.4c02369","RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"2024/8/19 0:00:00","PubModel":"Epub","JCR":"Q2","JCRName":"CHEMISTRY, MULTIDISCIPLINARY","Score":null,"Total":0}
Zeolitic Framework Ta and MoO3 Confined in Beta Zeolite Cooperatively Enhance Activity and Stability for Oxidative Desulfurization.
Oxidative desulfurization (ODS), as a novel desulfurization technique of fuel oil, possesses high desulfurization efficiency for aromatic sulfide and low cost, making it a promising approach. The key to the technology lies in the rational design of catalysts with high activity and stability. Polyoxometalates, which are environmentally friendly, cost-effective, and abundantly available, face constraints in the development of ODS applications due to their low specific surface area and difficulty in regeneration. Introducing metal oxides into carriers with large specific surface areas to obtain heterogeneous catalysts is an effective solution to this problem. Beta zeolites, with regular three-dimensional channel systems, large specific surface area, and superior thermal/hydrothermal stability, are usually used as carriers. In this work, we developed a strategy to enhance zeolite carrier utilization efficiency by introducing Ta5+ species into the rigid framework of zeolites containing confined MoO3. The Ta species in the zeolite framework and the confined MoO3 produce a synergistic effect, exhibiting extremely high catalytic activity for the aerobic oxidative desulfurization of various organic aromatic sulfur compounds under mild conditions (90 °C and atmospheric pressure) in a deep eutectic solvent, surpassing common heterogeneous catalysts for oxidative desulfurization. Moreover, it can resist the adverse effects of interferents, such as naphthalene and indole. Additionally, the confined nature of Beta zeolite endows it with exceptional stability, demonstrating distinctive recyclability.
期刊介绍:
Langmuir is an interdisciplinary journal publishing articles in the following subject categories:
Colloids: surfactants and self-assembly, dispersions, emulsions, foams
Interfaces: adsorption, reactions, films, forces
Biological Interfaces: biocolloids, biomolecular and biomimetic materials
Materials: nano- and mesostructured materials, polymers, gels, liquid crystals
Electrochemistry: interfacial charge transfer, charge transport, electrocatalysis, electrokinetic phenomena, bioelectrochemistry
Devices and Applications: sensors, fluidics, patterning, catalysis, photonic crystals
However, when high-impact, original work is submitted that does not fit within the above categories, decisions to accept or decline such papers will be based on one criteria: What Would Irving Do?
Langmuir ranks #2 in citations out of 136 journals in the category of Physical Chemistry with 113,157 total citations. The journal received an Impact Factor of 4.384*.
This journal is also indexed in the categories of Materials Science (ranked #1) and Multidisciplinary Chemistry (ranked #5).