Green and continuous flow oxidation of ethylene sulfite to ethylene sulfate over highly selective titanium silicalite-1 catalyst

IF 4.8 2区 化学 Q2 CHEMISTRY, PHYSICAL
Huimin Li , Bin Wu , Zhimin Zhu , Chenyang Li , Zhihan Liu , Fuweng Zhang , Huidong Zheng , Longfei Yan
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引用次数: 0

Abstract

Ethylene sulfate (DTD) is a new type of solid electrolyte interphase (SEI) film-forming additive for lithium-ion batteries. DTD was typically synthesized in the industry by oxidation of ethylene sulfite (ES) with NaClO via a RuCl3-catalyzed reaction. However, this route generates significant amount of Cl-containing wastes, and the recovery of RuCl3 is costly and technically challenging. Herein, we present a green and heterogeneous route for synthesizing DTD from ES, utilizing the Titanium Silicalite-1 (TS-1) and H2O2 as catalysts and green oxidants, respectively. Our research reveals that the tetra-coordination framework of Ti in TS-1 serves as the main active site for the oxidation of ES, achieving a remarkable yield of DTD up to 92 % under optimized reaction conditions. Additionally, we developed a continuous green oxidation process for synthesizing DTD from ES, which is the first of its kind and has been successfully operated continuously for over 300 h. This work provides a cost-effective, green, and efficient route for synthesizing DTD from ES.
在高选择性硅酸钛-1催化剂上,亚硫酸乙烯绿色连续氧化制硫酸乙烯
硫酸乙酯(DTD)是一种新型的锂离子电池固体电解质间相成膜添加剂。在工业上,DTD通常是通过rucl3催化的反应,用NaClO氧化亚硫酸乙酯(ES)合成的。然而,这条路线会产生大量含cl的废物,并且RuCl3的回收成本高昂,技术上具有挑战性。本文提出了一种绿色多相的ES合成DTD的方法,分别以二氧化钛-1 (TS-1)和H2O2为催化剂和绿色氧化剂。我们的研究表明,Ti在TS-1中的四配位框架是ES氧化的主要活性位点,在优化的反应条件下,DTD的产率高达92 %。此外,我们开发了一种连续绿色氧化工艺,用于从ES合成DTD,这是同类工艺中的第一个,并已成功连续运行超过300 h。这项工作为从ES合成DTD提供了一条经济、绿色、高效的途径。
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来源期刊
Applied Catalysis A: General
Applied Catalysis A: General 化学-环境科学
CiteScore
9.00
自引率
5.50%
发文量
415
审稿时长
24 days
期刊介绍: Applied Catalysis A: General publishes original papers on all aspects of catalysis of basic and practical interest to chemical scientists in both industrial and academic fields, with an emphasis onnew understanding of catalysts and catalytic reactions, new catalytic materials, new techniques, and new processes, especially those that have potential practical implications. Papers that report results of a thorough study or optimization of systems or processes that are well understood, widely studied, or minor variations of known ones are discouraged. Authors should include statements in a separate section "Justification for Publication" of how the manuscript fits the scope of the journal in the cover letter to the editors. Submissions without such justification will be rejected without review.
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