富氮孔分区 MOF 中的位点记忆触发可逆首字母缩略词加密，用于多平台上洛克沙胂和二氯兰的超灵敏监测,ACS Applied Materials & Interfaces

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富氮孔分区 MOF 中的位点记忆触发可逆首字母缩略词加密，用于多平台上洛克沙胂和二氯兰的超灵敏监测
ACS Applied Materials & Interfaces ( IF 8.3 ) Pub Date : 2023-11-15 , DOI: 10.1021/acsami.3c11197
Nilanjan Seal _{1,

2} , Partha Pratim Mondal ₂ , Athulya S Palakkal ₃ , Renjith S Pillai ₄ , Subhadip Neogi _{1,

2}

Affiliation

荧光金属有机框架（MOF）中的刺激响应发射颜色调制有望实现基于发光墨水的安全应用，而特定于任务的功能工程孔可以帮助快速响应、有辨别力和超低检测有害有机芳香族化合物。水相。考虑到实际适用性，加密和解密状态之间的自校准荧光开关最适合防伪措施，而通过多个平台上的重复和方便的方法对有机毒素进行基于图像的监测则支持现场感官潜力。_{在此，我们从–NH 2}挂钩的吡啶基连接体和三羧酸酯配体构建了一种基于混合配体的化学稳定的双层柱MOF，该配体包含带负电的[Cd ₃ (μ ₂ -OH)(COO) ₆ ]节点并显示出孔-通过富含氮的侧翼有机支柱进行空间分隔。由于存在自校准三唑胺部分接枝的辅助连接体，这种阴离子 MOF 在酸和碱交替存在的情况下描绘了质子化加密和去质子化解密结构域之间的可逆和多环氟交换。这种 pH 值触发的位点特异性发光变化可用于构建高度再生的防伪标签，以实现生动的首字母缩略词加密。该材料的强烈荧光特征被进一步利用，以高度可回收的方式对有害饲料添加剂洛克沙胂 (ROX) 和二氯喃 (DCNA) 农药进行极其选择性和快速响应的传感，具有显着的猝灭和纳摩尔检测限（ROX：52 ppb；DCNA）：26.8ppb）。值得注意的是，通过方便的纸条方法以及在蔬菜表面进行实时监测，成功地证明了对这两种有机毒素的超灵敏荧光检测。综合密度泛函理论研究除了证明 MOF-分析物超分子相互作用外，还通过该富电子框架中每种目标分析物重新分配分子轨道能级来验证电子转移机制。

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Site-Memory-Triggered Reversible Acronym Encryption in a Nitrogen-Rich Pore-Partitioned MOF for Ultrasensitive Monitoring of Roxarsone and Dichloran over Multiple Platform

Stimuli-responsive emission color modulation in fluorescent metal–organic frameworks (MOFs) promises luminescence-ink-based security application, while task-specific functionality-engineered pores can aid fast-responsive, discriminative, and ultralow detection of harmful organo-aromatics in the aqueous phase. Considering practical applicability, a self-calibrated fluoro-switch between encrypted and decrypted states is best suited for antiforgery measures, whereas image-based monitoring of organo-toxins by repetitive and handy methods over multiple platforms endorses in-field sensory potential. Herein, we constructed a mixed-ligand based chemically stable and bilayered-pillar MOF from –NH₂-hooked pyridyl linker and tricarboxylate ligand that embraces negatively charged [Cd₃(μ₂-OH)(COO)₆] node and shows pore-space-partitioning by nitrogen-rich flanked organic struts. Owing to the presence of a self-calibrating triazolylamine moiety-grafted auxiliary linker, this anionic MOF delineates reversible and multicyclic fluoro-swapping between protonated-encrypted and deprotonated-decrypted domains in the alternative presence of acid and base. Such pH-triggered, site-specific luminescence variation is utilized to construct highly regenerative anticounterfeiting labels for vivid acronym encryption. The intense fluorescence signature of the material is further harnessed in extremely selective and quick responsive sensing of harmful feed additive roxarsone (ROX) and dichloran (DCNA) pesticide in highly recyclable fashion with significant quenching and nanomolar limits of detection (ROX: 52 ppb; DCNA: 26.8 ppb). Notably, the ultrasensitive fluoro-detection of both these organo-toxins is successfully demonstrated via a handy paper-strip method as well as on the vegetable surface for real-time monitoring. Comprehensive density functional theory studies validate the electron transfer mechanism through redistribution of molecular orbital energy levels by each of the targeted analytes in this electron-rich framework besides evidencing MOF-analyte supramolecular interactions.

更新日期：2023-11-15

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