Directionally Exfoliated Ni/Co Hydroxide-Organic Framework Nanosheets for Enhanced Wearable Glucose Sensing.

We report two-dimensional (2D) Ni/Co-based metal hydroxide-organic framework nanosheets (Ni/Co-MHOF NSs) for the construction of an efficient electrochemical nonenzymatic glucose sensor. The nanosheet architecture maximizes the exposure of coordinatively unsaturated metal sites, which enables a largely improved electrocatalytic performance toward the glucose oxidation reaction. The as-designed nonenzymatic sensor exhibits a high sensitivity of 235.71 µA·mM-1·cm-2 and a wide linear range of 1-3000 µM. The sensor presents excellent selectivity against several potential interferences and a short response time of 3.0 s. Of interest, a high-performance flexible sensor is developed by depositing the Ni/Co-MHOF NSs on screen-printed electrodes, which reveal decent bending stability. The designed glucose sensor patch can attach to the human body and realize noninvasive glucose monitoring in human sweat. This work may shed light on the application of novel MHOFs in the field of wearable electrochemical sensing.

Complete Glucose Electrooxidation Enabled by Coordinatively Unsaturated Copper Sites in Metal-Organic Frameworks.

The electrocatalytic oxidation of glucose plays a vital role in biomass conversion, renewable energy, and biosensors, but significant challenges remain to achieve high selectivity and high activity simultaneously. In this study, we present a novel approach for achieving complete glucose electrooxidation utilizing Cu-based metal-hydroxide-organic framework (Cu-MHOF) featuring coordinatively unsaturated Cu active sites. In contrast to traditional Cu(OH)2 catalysts, the Cu-MHOF exhibits a remarkable 40-fold increase in electrocatalytic activity for glucose oxidation, enabling exclusive oxidation of glucose into formate and carbonate as the final products. The critical role of open metal sites in enhancing the adsorption affinity of glucose and key intermediates was confirmed by control experiments and density functional theory simulations. Subsequently, a miniaturized nonenzymatic glucose sensor was developed showing superior performance with a high sensitivity of 214.7 µA mM-1 cm-2 , a wide detection range from 0.1 µM to 22 mM, and a low detection limit of 0.086 µM. Our work provides a novel molecule-level strategy for designing catalytically active sites and could inspire the development of novel metal-organic framework for next-generation electrochemical devices.