Spin Meets the Light: Emergence of Paramagnetic Metal‐organic Frameworks (PMOFs) for Optical and Electrochemical Sensing Over the Last Five Years

ABSTRACT Ensuring environmental and human healthcare safety is one of the burgeoning challenges faced by researchers worldwide. In this context, judicious coupling of analytical performances obtained from the usage of reticular metal‐organic frameworks (MOFs) assisted with point‐of‐care‐testing (POCT) devices has revolutionized the stimuli‐responsive host‐guest recognition arena. However, exploration of the potential of MOFs containing a paramagnetic metal node is still an under‐niche area. These kinds of frameworks are of paramount importance because the presence of unpaired electrons on the metal centres can regulate the electronic and photophysical properties along with the corresponding optical and/or electrochemical responses. The present review deals with the strategic exploration of paramagnetic MOFs along with their allied composites in the domain of sensing, predominantly focused on the last quinquennial period (2020‐2025). The design principle, along with their in‐depth sensing mechanisms, sensitivity via chromo‐fluorogenic, electrochemical, chemiluminescent, etc., readouts have been presented. Ultimately, despite of significant research progress, the critical bottlenecks of the current research strategy, like device dependence, lack of standard calibration and validation methods, sampling error, photobleaching, reproducibility, biocompatibility, etc. as well as future research directions in light with artificial intelligence‐machine learning‐internet of things (AI‐ML‐IoT)‐assisted data analysis and cloud storage have been briefly elaborated for accelerating the transition of paramagnetic MOFs‐based sensors toward smart and real‐time environmental and healthcare monitoring, especially in resource‐constraint area.