期刊
ACS APPLIED MATERIALS & INTERFACES
卷 13, 期 21, 页码 25153-25163出版社
AMER CHEMICAL SOC
DOI: 10.1021/acsami.1c05998
关键词
d(10)-MOFs; fluorescence turn-on; fast responsive detection; PET restriction; hydrogel; self-calibrating logic gate
资金
- Department of Higher Education, Science & Technology and Biotechnology, Govt. of West Bengal, India, sponsored project (GAP-225612) [78 (Sanc.)/ST/P/ST/ 6G-1/2018]
Two luminescent porous networks (CMERI-1 & CMERI-2) have been developed for efficient detection of formaldehyde (FA) in aqueous medium, with CMERI-1 showing better sensitivity and quicker response time due to facile imine formation. The detection limits of CMERI-1 & CMERI-2 for FA in water are below the intracellular concentration of formaldehyde, and a MOF-based hydrogel membrane for vapor-phase FA detection has been fabricated. The response mechanisms of MOFs are supported by density functional theory (DFT) and Fukui indices analysis, indicating their potential in real-world applications for food sample and water analyses.
Herein, two luminescent porous networks (CMERI-1 & CMERI-2) have been reported for the efficient detection of formaldehyde (FA) from aqueous medium. Judicious solvent screening using a high-throughput solvothermal procedure leads to two completely different metal-organic framework (MOFs) with different architectures. It is perceived that the framework CMERI-1 shows better sensitivity with a very short response time (1 min) in the realm of FA detection due to the facile imine (-N-CH-) formation, which is restricted in the case of CMERI-2. The fluorescence turn-on behavior is ascribed due to the inhibition of photoinduced electron transfer (PET) (from amine subunit to secondary building unit) process. The detection limits of CMERI-1 & CMERI-2 toward FA in aqueous medium were found to be 0.62 mu M (0.019 ppm) and 1.39 mu M (0.041 ppm), respectively, that lie far below the intracellular concentration of formaldehyde (100-400 mu M). In addition, MOF-based hydrogel membrane was fabricated, which shows vapor-phase detection of FA, which is hitherto unexplored in this realm. Moreover, the response mechanisms of MOFs are supported by density functional theory (DFT) and Fukui indices analysis. The high stability of the porous frameworks along with its interesting sensing features such as fast recognition phenomenon, appreciable detection limit, etc. instigated us to explore its real-world applicability in various food sample and water analyses. In view of the modular design principle of our polymeric probe, the proposed approach could open a new horizon to construct powerful sensing materials for the ultrafast detection of other industrial pollutants in the domain of supramolecular and analytical chemistry.
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