Ling Ding, Lou Gao, Di Pan, Ke Du, Jiayu Yu, Wanyi Li, Yahong Zhang and Yi Tang
{"title":"利用形状选择性 H-Beta 沸石减少外消旋乳酸生成中乳酸","authors":"Ling Ding, Lou Gao, Di Pan, Ke Du, Jiayu Yu, Wanyi Li, Yahong Zhang and Yi Tang","doi":"10.1039/D4CY01046A","DOIUrl":null,"url":null,"abstract":"<p >The utilization of racemic lactic acid (<em>rac</em>-LA) produced <em>via</em> chemocatalytic conversion for polylactic acid (PLA) synthesis remains limited due to the formation of undesired mesomeric lactide (<em>meso</em>-LD), a by-product that arises during the conversion process. This study proposes the use of shape-selective H-Beta zeolite to reduce the formation of <em>meso</em>-LD in lactide (LD) by leveraging its selectivity towards different lactic dimers (L<small><sub>2</sub></small>A) in a one-step catalytic conversion of <em>rac</em>-LA to LD. Experimental results from various LA solutions with different L<small><sub>2</sub></small>A content indicate that the L<small><sub>2</sub></small>A content is critical for maximizing the selectivity of racemic lactide (<small>D</small>/<small>L</small>-LD), thus confirming the shape-selective nature of H-Beta zeolite towards L<small><sub>2</sub></small>A. Additionally, it is found that increasing the reaction temperature and employing structurally reconstructed H-Beta zeolite with more regularized channels as a catalyst can further decrease <em>meso</em>-LD formation, and a LD yield of 60% with a <small>D</small>/<small>L</small>-LD/<em>meso</em>-LD ratio of 2.26 can be achieved under optimal catalyst and reaction conditions. Despite the coexistence of <small>D</small>/<small>L</small>-LD and <em>meso</em>-LD in the final product, this study marks a significant step towards controlling the stereoisomer distribution of LD synthesized from <em>rac</em>-LA derived from chemical conversion.</p>","PeriodicalId":4,"journal":{"name":"ACS Applied Energy Materials","volume":null,"pages":null},"PeriodicalIF":5.4000,"publicationDate":"2024-09-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Reducing meso-lactide formation from racemic lactic acid using shape-selective H-Beta zeolite†\",\"authors\":\"Ling Ding, Lou Gao, Di Pan, Ke Du, Jiayu Yu, Wanyi Li, Yahong Zhang and Yi Tang\",\"doi\":\"10.1039/D4CY01046A\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<p >The utilization of racemic lactic acid (<em>rac</em>-LA) produced <em>via</em> chemocatalytic conversion for polylactic acid (PLA) synthesis remains limited due to the formation of undesired mesomeric lactide (<em>meso</em>-LD), a by-product that arises during the conversion process. This study proposes the use of shape-selective H-Beta zeolite to reduce the formation of <em>meso</em>-LD in lactide (LD) by leveraging its selectivity towards different lactic dimers (L<small><sub>2</sub></small>A) in a one-step catalytic conversion of <em>rac</em>-LA to LD. Experimental results from various LA solutions with different L<small><sub>2</sub></small>A content indicate that the L<small><sub>2</sub></small>A content is critical for maximizing the selectivity of racemic lactide (<small>D</small>/<small>L</small>-LD), thus confirming the shape-selective nature of H-Beta zeolite towards L<small><sub>2</sub></small>A. Additionally, it is found that increasing the reaction temperature and employing structurally reconstructed H-Beta zeolite with more regularized channels as a catalyst can further decrease <em>meso</em>-LD formation, and a LD yield of 60% with a <small>D</small>/<small>L</small>-LD/<em>meso</em>-LD ratio of 2.26 can be achieved under optimal catalyst and reaction conditions. Despite the coexistence of <small>D</small>/<small>L</small>-LD and <em>meso</em>-LD in the final product, this study marks a significant step towards controlling the stereoisomer distribution of LD synthesized from <em>rac</em>-LA derived from chemical conversion.</p>\",\"PeriodicalId\":4,\"journal\":{\"name\":\"ACS Applied Energy Materials\",\"volume\":null,\"pages\":null},\"PeriodicalIF\":5.4000,\"publicationDate\":\"2024-09-03\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"ACS Applied Energy Materials\",\"FirstCategoryId\":\"92\",\"ListUrlMain\":\"https://pubs.rsc.org/en/content/articlelanding/2024/cy/d4cy01046a\",\"RegionNum\":3,\"RegionCategory\":\"材料科学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q2\",\"JCRName\":\"CHEMISTRY, PHYSICAL\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"ACS Applied Energy Materials","FirstCategoryId":"92","ListUrlMain":"https://pubs.rsc.org/en/content/articlelanding/2024/cy/d4cy01046a","RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q2","JCRName":"CHEMISTRY, PHYSICAL","Score":null,"Total":0}
Reducing meso-lactide formation from racemic lactic acid using shape-selective H-Beta zeolite†
The utilization of racemic lactic acid (rac-LA) produced via chemocatalytic conversion for polylactic acid (PLA) synthesis remains limited due to the formation of undesired mesomeric lactide (meso-LD), a by-product that arises during the conversion process. This study proposes the use of shape-selective H-Beta zeolite to reduce the formation of meso-LD in lactide (LD) by leveraging its selectivity towards different lactic dimers (L2A) in a one-step catalytic conversion of rac-LA to LD. Experimental results from various LA solutions with different L2A content indicate that the L2A content is critical for maximizing the selectivity of racemic lactide (D/L-LD), thus confirming the shape-selective nature of H-Beta zeolite towards L2A. Additionally, it is found that increasing the reaction temperature and employing structurally reconstructed H-Beta zeolite with more regularized channels as a catalyst can further decrease meso-LD formation, and a LD yield of 60% with a D/L-LD/meso-LD ratio of 2.26 can be achieved under optimal catalyst and reaction conditions. Despite the coexistence of D/L-LD and meso-LD in the final product, this study marks a significant step towards controlling the stereoisomer distribution of LD synthesized from rac-LA derived from chemical conversion.
期刊介绍:
ACS Applied Energy Materials is an interdisciplinary journal publishing original research covering all aspects of materials, engineering, chemistry, physics and biology relevant to energy conversion and storage. The journal is devoted to reports of new and original experimental and theoretical research of an applied nature that integrate knowledge in the areas of materials, engineering, physics, bioscience, and chemistry into important energy applications.