Mei Xu, Fengtao Yu*, Yiping Liu, Wanru Li, Chuangye Li, Fangru Song, Guihong Wu, Zhenzhen Xu and Jianding Qiu*,
{"title":"将铀亲和性 \"钩子 \"集成到共轭聚合物中,实现巨型内置电场,促进海水中铀的光催化提取","authors":"Mei Xu, Fengtao Yu*, Yiping Liu, Wanru Li, Chuangye Li, Fangru Song, Guihong Wu, Zhenzhen Xu and Jianding Qiu*, ","doi":"10.1021/acs.macromol.4c00717","DOIUrl":null,"url":null,"abstract":"<p >Insufficient charge separation and sluggish exciton transport seriously restrict the practical application of photocatalytic uranium extraction from seawater. In this study, a D-π-A conjugated microporous polymer is synthesized using perylene, phosphonate-containing fluorene, and benzothiadiazole as D, π-linker, and A units, respectively, as novel uranium extraction photocatalysts. Both experimental and theoretical studies have demonstrated that the D-π-A structure simultaneously expands π-electron delocalization and promotes intramolecular charge transfer, thus accelerating the photocatalytic reaction. More importantly, phosphate ester and benzothiadiazole together act as uranyl-affinity “hooks” in the skeleton, adding the asymmetry and expanding the built-in electric field, thereby enhancing the driving force of photogenerated charge separation and elevating the charge separation efficiency (84.8%). The results show that the photocatalytic uranium extraction capacity of CMP-D-π′-A reaches 11.68 ± 0.21 mg g<sup>–1</sup>, exceeding most reported photocatalysts. These findings provide a promising avenue for the development of uranium extraction materials through regulating the interfacial electric field.</p>","PeriodicalId":51,"journal":{"name":"Macromolecules","volume":null,"pages":null},"PeriodicalIF":5.1000,"publicationDate":"2024-06-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Integrating Uranyl-Affinity “Hooks” into Conjugated Polymers Achieving Giant Built-in Electric Field for Boosting Photocatalytic Uranium Extraction from Seawater\",\"authors\":\"Mei Xu, Fengtao Yu*, Yiping Liu, Wanru Li, Chuangye Li, Fangru Song, Guihong Wu, Zhenzhen Xu and Jianding Qiu*, \",\"doi\":\"10.1021/acs.macromol.4c00717\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<p >Insufficient charge separation and sluggish exciton transport seriously restrict the practical application of photocatalytic uranium extraction from seawater. In this study, a D-π-A conjugated microporous polymer is synthesized using perylene, phosphonate-containing fluorene, and benzothiadiazole as D, π-linker, and A units, respectively, as novel uranium extraction photocatalysts. Both experimental and theoretical studies have demonstrated that the D-π-A structure simultaneously expands π-electron delocalization and promotes intramolecular charge transfer, thus accelerating the photocatalytic reaction. More importantly, phosphate ester and benzothiadiazole together act as uranyl-affinity “hooks” in the skeleton, adding the asymmetry and expanding the built-in electric field, thereby enhancing the driving force of photogenerated charge separation and elevating the charge separation efficiency (84.8%). The results show that the photocatalytic uranium extraction capacity of CMP-D-π′-A reaches 11.68 ± 0.21 mg g<sup>–1</sup>, exceeding most reported photocatalysts. These findings provide a promising avenue for the development of uranium extraction materials through regulating the interfacial electric field.</p>\",\"PeriodicalId\":51,\"journal\":{\"name\":\"Macromolecules\",\"volume\":null,\"pages\":null},\"PeriodicalIF\":5.1000,\"publicationDate\":\"2024-06-10\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Macromolecules\",\"FirstCategoryId\":\"92\",\"ListUrlMain\":\"https://pubs.acs.org/doi/10.1021/acs.macromol.4c00717\",\"RegionNum\":1,\"RegionCategory\":\"化学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q1\",\"JCRName\":\"POLYMER SCIENCE\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Macromolecules","FirstCategoryId":"92","ListUrlMain":"https://pubs.acs.org/doi/10.1021/acs.macromol.4c00717","RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"POLYMER SCIENCE","Score":null,"Total":0}
Integrating Uranyl-Affinity “Hooks” into Conjugated Polymers Achieving Giant Built-in Electric Field for Boosting Photocatalytic Uranium Extraction from Seawater
Insufficient charge separation and sluggish exciton transport seriously restrict the practical application of photocatalytic uranium extraction from seawater. In this study, a D-π-A conjugated microporous polymer is synthesized using perylene, phosphonate-containing fluorene, and benzothiadiazole as D, π-linker, and A units, respectively, as novel uranium extraction photocatalysts. Both experimental and theoretical studies have demonstrated that the D-π-A structure simultaneously expands π-electron delocalization and promotes intramolecular charge transfer, thus accelerating the photocatalytic reaction. More importantly, phosphate ester and benzothiadiazole together act as uranyl-affinity “hooks” in the skeleton, adding the asymmetry and expanding the built-in electric field, thereby enhancing the driving force of photogenerated charge separation and elevating the charge separation efficiency (84.8%). The results show that the photocatalytic uranium extraction capacity of CMP-D-π′-A reaches 11.68 ± 0.21 mg g–1, exceeding most reported photocatalysts. These findings provide a promising avenue for the development of uranium extraction materials through regulating the interfacial electric field.
期刊介绍:
Macromolecules publishes original, fundamental, and impactful research on all aspects of polymer science. Topics of interest include synthesis (e.g., controlled polymerizations, polymerization catalysis, post polymerization modification, new monomer structures and polymer architectures, and polymerization mechanisms/kinetics analysis); phase behavior, thermodynamics, dynamic, and ordering/disordering phenomena (e.g., self-assembly, gelation, crystallization, solution/melt/solid-state characteristics); structure and properties (e.g., mechanical and rheological properties, surface/interfacial characteristics, electronic and transport properties); new state of the art characterization (e.g., spectroscopy, scattering, microscopy, rheology), simulation (e.g., Monte Carlo, molecular dynamics, multi-scale/coarse-grained modeling), and theoretical methods. Renewable/sustainable polymers, polymer networks, responsive polymers, electro-, magneto- and opto-active macromolecules, inorganic polymers, charge-transporting polymers (ion-containing, semiconducting, and conducting), nanostructured polymers, and polymer composites are also of interest. Typical papers published in Macromolecules showcase important and innovative concepts, experimental methods/observations, and theoretical/computational approaches that demonstrate a fundamental advance in the understanding of polymers.