Fabrication of Two Luminescent Imidazolyl Cadmium-Organic Frameworks and Their Sensing Mechanism for 2,6-Dichloro-4-nitroaniline
Fabrication of Two Luminescent Imidazolyl Cadmium-Organic Frameworks and Their Sensing Mechanism for 2,6-Dichloro-4-nitroaniline
复制标题
两种发光咪唑基镉有机框架的制备及其对2,6-二氯-4-硝基苯胺的传感机制
DOI：
10.1021/acsami.2c19766
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发表时间：
2023
期刊：
影响因子：
--
通讯作者：
Xiupei Yang
中科院分区：
文献类型：
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作者：
Yi Zhang;Yuhang Liu;Pran Gopal Karmaker;Lilei Zhang;Kaijing Yang;Lianfang Chen;Xiupei Yang
2，6-二氯-4-硝基苯胺，别名二氯仑（DCN），是一种广谱农药，可对人体造成不可逆的损害。因此，开发一种快速、简便的检测DCN的技术具有重要意义。发光金属有机骨架材料由于其优异的光学性能在传感和检测领域引起了广泛的关注。本研究开发了两种二维Cd-MOFs（CdMOF-1和CdMOF-2）用于环境中DCN残留的检测。这两种CdMOFs都具有优异的溶剂和酸碱稳定性，可以在短时间（30 s）内快速灵敏地响应DCN。CdMOFs不仅对DCN具有良好的选择性和抗干扰性，而且具有良好的可重复使用性。在DCN浓度为1-15 μ M和0.3 ~ 30 μM的条件下，CdMOF-1和CdMOF-2的荧光强度与DCN浓度呈良好的线性关系（R2= 0.999/0.991），检出限分别为0.36和0.12 μM。通过紫外-可见吸收光谱（UV-Vis）、X射线光电子能谱（XPS）、荧光寿命和密度泛函理论计算，揭示了DCN对两种Cd-MOFs的荧光猝灭机制为竞争吸收和光诱导电子转移，可能存在较弱的π-π相互作用。最后，通过两种荧光CdMOFs制作荧光试纸并对实际土壤进行检测，证明其可应用于实际现场，实现现场实时检测。
2,6-Dichloro-4-nitroaniline, alias dicloran (DCN), is a broad-spectrum pesticide that can cause irreversible damage to the human body. Therefore, it is of great significance to develop a technology for the rapid and convenient detection of DCN. Luminescent metal organic frameworks have attracted extensive attention in the field of sensing and detection due to their excellent optical properties. In this study, two kinds of 2D Cd-MOFs (CdMOF-1 and CdMOF-2) were developed for the detection of residual DCN in the environment. Both CdMOFs exhibit excellent solvent and acid–base stability and can respond to DCN quickly and sensitively in a short time (30 s). CdMOFs not only have good selectivity and anti-interference toward DCN but also have good reusability. Under the conditions of DCN concentrations of 1–15 and 0.3–30 μM, the change in fluorescence intensity of CdMOF-1 and CdMOF-2 showed a good linear relationship with DCN concentration (R2= 0.999/0.991), and the detection limits were 0.36 and 0.12 μM, respectively. Through ultraviolet–visible absorption spectroscopy (UV–Vis), X-ray photoelectron spectroscopy, fluorescence lifetime, and density functional theory calculations, it is revealed that the fluorescence quenching mechanisms of DCN for two kinds of Cd-MOFs are competitive absorption and photoinduced electron transfer, and there may be a weak π–π interaction. Finally, it is demonstrated that by using two types of fluorescent CdMOFs to make the fluorescent test paper and detect actual soil, these can be applied to the actual scene and achieve onsite real-time detection.