{"title":"沸石中碳点的密闭微环境调控,实现多模式、随时间变化的磷光颜色演变。","authors":"Siyu Zong, Bolun Wang, Jiani Zhang, Xiaowei Yu, Yida Zhou, Yuze Chen, Tianjun Zhang, Jiyang Li","doi":"10.1002/anie.202420156","DOIUrl":null,"url":null,"abstract":"<p><p>Matrix immobilization has been proven to be a favored method for enhancing the phosphorescence of carbon dots (CDs), however, it remains a significant challenge to realize time-dependent phosphorescence colors (TDPC) by embedding CDs with single emission center. In this study, we present a novel matrix-controlling strategy to regulate the microenvironment of CDs by doping limited Mn2+ in zeolite. The surrounding environment influences the surface state of the CDs, leading to the formation of different excitons. At low temperatures, Mn-coordinated CDs (C-CDs) show fast-decaying green phosphorescence, while non-coordinated CDs (NC-CDs) exhibit inherent slow-decaying blue phosphorescence. Notably, the energy transfer occurs between NC-CDs and Mn2+ to produce an ultrafast-decaying red phosphorescence, with the intensity of the red component increasing as the temperature rises. The interplay of these luminescent centers with distinct decay rates activates fascinating multi-mode TDPC behavior as the temperature changes, resulting in dynamic afterglow evolutions from red to green at 298 K, orange to green at 273 K, and green to cyan to blue at 77 K. Leveraging the diverse luminescence of CDs@MnAPO-5, a multi-dimensional dynamic afterglow color pattern was developed for advanced anti-counterfeiting applications.</p>","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":" ","pages":"e202420156"},"PeriodicalIF":16.1000,"publicationDate":"2024-11-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Confinement Microenvironment Regulation of Carbon Dots in Zeolite for Multi-Mode Time-Dependent Phosphorescence Color Evolution.\",\"authors\":\"Siyu Zong, Bolun Wang, Jiani Zhang, Xiaowei Yu, Yida Zhou, Yuze Chen, Tianjun Zhang, Jiyang Li\",\"doi\":\"10.1002/anie.202420156\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<p><p>Matrix immobilization has been proven to be a favored method for enhancing the phosphorescence of carbon dots (CDs), however, it remains a significant challenge to realize time-dependent phosphorescence colors (TDPC) by embedding CDs with single emission center. In this study, we present a novel matrix-controlling strategy to regulate the microenvironment of CDs by doping limited Mn2+ in zeolite. The surrounding environment influences the surface state of the CDs, leading to the formation of different excitons. At low temperatures, Mn-coordinated CDs (C-CDs) show fast-decaying green phosphorescence, while non-coordinated CDs (NC-CDs) exhibit inherent slow-decaying blue phosphorescence. Notably, the energy transfer occurs between NC-CDs and Mn2+ to produce an ultrafast-decaying red phosphorescence, with the intensity of the red component increasing as the temperature rises. The interplay of these luminescent centers with distinct decay rates activates fascinating multi-mode TDPC behavior as the temperature changes, resulting in dynamic afterglow evolutions from red to green at 298 K, orange to green at 273 K, and green to cyan to blue at 77 K. Leveraging the diverse luminescence of CDs@MnAPO-5, a multi-dimensional dynamic afterglow color pattern was developed for advanced anti-counterfeiting applications.</p>\",\"PeriodicalId\":125,\"journal\":{\"name\":\"Angewandte Chemie International Edition\",\"volume\":\" \",\"pages\":\"e202420156\"},\"PeriodicalIF\":16.1000,\"publicationDate\":\"2024-11-19\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Angewandte Chemie International Edition\",\"FirstCategoryId\":\"92\",\"ListUrlMain\":\"https://doi.org/10.1002/anie.202420156\",\"RegionNum\":1,\"RegionCategory\":\"化学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q1\",\"JCRName\":\"CHEMISTRY, MULTIDISCIPLINARY\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Angewandte Chemie International Edition","FirstCategoryId":"92","ListUrlMain":"https://doi.org/10.1002/anie.202420156","RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"CHEMISTRY, MULTIDISCIPLINARY","Score":null,"Total":0}
引用次数: 0
摘要
基质固定已被证明是增强碳点(CD)磷光的一种有效方法,然而,通过嵌入具有单发射中心的碳点来实现随时间变化的磷光颜色(TDPC)仍然是一项重大挑战。在这项研究中,我们提出了一种新颖的基质控制策略,通过在沸石中掺入有限的 Mn2+ 来调节 CD 的微环境。周围环境会影响光盘的表面状态,从而形成不同的激子。在低温条件下,锰配位光盘(C-CDs)显示出快速衰减的绿色磷光,而非配位光盘(NC-CDs)则显示出固有的缓慢衰减的蓝色磷光。值得注意的是,NC-CDs 和 Mn2+ 之间的能量转移会产生超快衰减的红色磷光,红色成分的强度会随着温度的升高而增加。随着温度的变化,这些具有不同衰减速率的发光中心相互作用,激活了迷人的多模式 TDPC 行为,从而产生了动态余辉演变:在 298 K 时从红色到绿色,在 273 K 时从橙色到绿色,在 77 K 时从绿色到青色再到蓝色。利用 CDs@MnAPO-5 的多种发光特性,开发出了一种多维动态余辉颜色模式,可用于先进的防伪应用。
Confinement Microenvironment Regulation of Carbon Dots in Zeolite for Multi-Mode Time-Dependent Phosphorescence Color Evolution.
Matrix immobilization has been proven to be a favored method for enhancing the phosphorescence of carbon dots (CDs), however, it remains a significant challenge to realize time-dependent phosphorescence colors (TDPC) by embedding CDs with single emission center. In this study, we present a novel matrix-controlling strategy to regulate the microenvironment of CDs by doping limited Mn2+ in zeolite. The surrounding environment influences the surface state of the CDs, leading to the formation of different excitons. At low temperatures, Mn-coordinated CDs (C-CDs) show fast-decaying green phosphorescence, while non-coordinated CDs (NC-CDs) exhibit inherent slow-decaying blue phosphorescence. Notably, the energy transfer occurs between NC-CDs and Mn2+ to produce an ultrafast-decaying red phosphorescence, with the intensity of the red component increasing as the temperature rises. The interplay of these luminescent centers with distinct decay rates activates fascinating multi-mode TDPC behavior as the temperature changes, resulting in dynamic afterglow evolutions from red to green at 298 K, orange to green at 273 K, and green to cyan to blue at 77 K. Leveraging the diverse luminescence of CDs@MnAPO-5, a multi-dimensional dynamic afterglow color pattern was developed for advanced anti-counterfeiting applications.
期刊介绍:
Angewandte Chemie, a journal of the German Chemical Society (GDCh), maintains a leading position among scholarly journals in general chemistry with an impressive Impact Factor of 16.6 (2022 Journal Citation Reports, Clarivate, 2023). Published weekly in a reader-friendly format, it features new articles almost every day. Established in 1887, Angewandte Chemie is a prominent chemistry journal, offering a dynamic blend of Review-type articles, Highlights, Communications, and Research Articles on a weekly basis, making it unique in the field.