Enhanced Regulation of Selectivity by the Coupling Effects of Surface Acidity and Strain Effects via Precisely...

Loading a sensitizer and constructing a rational nanostructure have been reported to be effective approaches for enhancing the catalytic/sensing performance. However, the impact of the precise loading position on the catalytic/sensing performance is always overlooked. Here, we discovered that precisely changing the location of Pt clusters from the outside of Al₂O₃-ZnO nanocoils (O-PtAlZnNCs) to the inner side of the nanocoils (I-PtAlZnNCs) could change the sensing performance of the sensor from H₂S to acetone. Furthermore, precisely loading Pt inside of the confined space led to a high sensing performance and reduced the limit of detection (LOD) of acetone by a factor of 50 times (from 100 to 2 ppb). Combining X-ray photoelectron spectroscopy (XPS), NH₃-diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS), in situ X-ray absorption spectroscopy (XAS), and density functional theory (DFT) simulations, the enhancement of sensitivity and regulation of sensing selectivity are attributed to the coupling effects from enrichment of confined space and Al₂O₃ acid-base active sites as well as the regulation of electronic structure by location-dominated strain effects. This work not only provides a novel sight to precisely regulate the selectivity and obtain ultrasensitive materials but also serves as a useful instruction for further understanding and precisely designing specific sensors and catalysts with high performance.