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Comprehensive Structural and Microscopic Characterization of an Azine–Triazine-Functionalized Highly Crystalline Covalent Organic Framework and Its Selective Detection of Dichloran and 4-Nitroaniline
ACS Applied Materials & Interfaces ( IF 8.3 ) Pub Date : 2020-02-24 , DOI: 10.1021/acsami.9b17452 Prasenjit Das 1 , Gouri Chakraborty 1 , Sanjay K. Mandal 1
ACS Applied Materials & Interfaces ( IF 8.3 ) Pub Date : 2020-02-24 , DOI: 10.1021/acsami.9b17452 Prasenjit Das 1 , Gouri Chakraborty 1 , Sanjay K. Mandal 1
Affiliation
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In recent years, luminescent covalent organic frameworks (COFs) constructed with nitrogen-rich building units have been the target for selective detection of electron-deficient pollutants to serve for a clean environment. In order to contribute to these imperative applications, an azine–triazine-based COF (ANCOF) has been solvothermally synthesized and structurally characterized by a variety of analytical methods for comprehensive studies. ANCOF possesses micropores with a rare ABAB stacking, high thermal and chemical stabilities, and a Brunauer–Emmett–Teller surface area of 565 m2 g–1. On the other hand, ANCOF exhibits excellent luminescent property in the presence of different solvents marked by the wavelength shift due to polarity. Exploiting the bluish-white emission of ANCOF in aqueous medium, it has been found to be an excellent probe for the discriminative and selective detection of dichloran (DCNA) and 4-nitroaniline (4-NA) with detection limits of 142 and 89 ppb, respectively. A distinguishable color change for DCNA and 4-NA has been reflected by UV illumination, fluorescence microscopy, and a handy paper strip method. Time-resolved fluorescence studies, spectral overlap, density functional theory, and configurational bias Monte Carlo molecular simulation have been utilized to understand the mechanism of action and interaction of DCNA and 4-NA with the host ANCOF. The selectivity of ANCOF toward DCNA and 4-NA in the presence of other analytes and the recyclability after sensing experiments have been successfully demonstrated. Furthermore, the stability of ANCOF has been confirmed by powder X-ray diffraction and field emission scanning electron microscopy with good retention of crystallinity and morphology. To the best of our knowledge, this is the first COF employed for the detection of amine derivatives in aqueous solution combining both experimental and computational studies.
中文翻译：
叠氮基-三嗪功能化的高度结晶共价有机骨架的结构和微观表征，及其对二氯甲烷和4-硝基苯胺的选择性检测
近年来，使用富氮建筑单元构建的发光共价有机骨架（COF）已成为选择性检测电子不足的污染物以清洁环境的目标。为了促进这些必不可少的应用，已经对溶剂型溶剂合成了基于嗪-三嗪的COF（ANCOF）并通过多种分析方法对其结构进行了全面研究。ANCOF具有微孔，具有罕见的ABAB堆积，高的热稳定性和化学稳定性，并且Brunauer-Emmett-Teller表面积为565 m 2 g –1。另一方面，ANCOF在不同溶剂的存在下，由于极性引起的波长偏移而具有出色的发光性能。利用ANCOF在水介质中的蓝白色发射，已发现它是区分和选择性检测二氯乙烷（DCNA）和4-硝基苯胺（4-NA）的极佳探针，检测限为142和89 ppb，分别。DCNA和4-NA的明显颜色变化已通过紫外线照射，荧光显微镜和便捷的纸带方法得到反映。时间分辨荧光研究，光谱重叠，密度泛函理论和构型偏差蒙特卡洛分子模拟已用于了解DCNA和4-NA与宿主ANCOF的作用机理和相互作用。在其他分析物存在下，ANCOF对DCNA和4-NA的选择性以及传感实验后的可回收性已得到成功证明。此外，ANCOF的稳定性已通过粉末X射线衍射和场发射扫描电子显微镜得到了证实，并具有良好的结晶度和形态。据我们所知，这是结合实验和计算研究首次用于检测水溶液中胺衍生物的COF。
更新日期：2020-02-25
中文翻译：
叠氮基-三嗪功能化的高度结晶共价有机骨架的结构和微观表征，及其对二氯甲烷和4-硝基苯胺的选择性检测
近年来，使用富氮建筑单元构建的发光共价有机骨架（COF）已成为选择性检测电子不足的污染物以清洁环境的目标。为了促进这些必不可少的应用，已经对溶剂型溶剂合成了基于嗪-三嗪的COF（ANCOF）并通过多种分析方法对其结构进行了全面研究。ANCOF具有微孔，具有罕见的ABAB堆积，高的热稳定性和化学稳定性，并且Brunauer-Emmett-Teller表面积为565 m 2 g –1。另一方面，ANCOF在不同溶剂的存在下，由于极性引起的波长偏移而具有出色的发光性能。利用ANCOF在水介质中的蓝白色发射，已发现它是区分和选择性检测二氯乙烷（DCNA）和4-硝基苯胺（4-NA）的极佳探针，检测限为142和89 ppb，分别。DCNA和4-NA的明显颜色变化已通过紫外线照射，荧光显微镜和便捷的纸带方法得到反映。时间分辨荧光研究，光谱重叠，密度泛函理论和构型偏差蒙特卡洛分子模拟已用于了解DCNA和4-NA与宿主ANCOF的作用机理和相互作用。在其他分析物存在下，ANCOF对DCNA和4-NA的选择性以及传感实验后的可回收性已得到成功证明。此外，ANCOF的稳定性已通过粉末X射线衍射和场发射扫描电子显微镜得到了证实，并具有良好的结晶度和形态。据我们所知，这是结合实验和计算研究首次用于检测水溶液中胺衍生物的COF。
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