Abstract

The gas-detecting ability of nanostructured ZnO has led to significant attention being paid to the development of a unique and effective approach to its synthesis. However, its poor sensitivity, cross-sensitivity to humidity, long response/recovery times and poor selectivity hinder its practical use in environmental and health monitoring. In this context, the addition of noble metals, as dopants or catalysts to modify the ZnO surface has been examined to enhance its sensing performance. Herein, we report preparation of Pd-loaded ZnO nanoparticles via a chemical precipitation approach. Various Pd loadings were employed to produce surface-modified ZnO nanostructure sensors, and their resulting NH3 sensing capabilities both in dry and humid environments were investigated. Through a comparative gas sensing study between the pure and Pd-loaded ZnO sensors upon exposure to NH3 at an optimal operating temperature of 350 °C, the Pd-loaded ZnO sensors were found to exhibit enhanced sensor responses and fast response/recovery times. The influence of Pd loading and its successful incorporation into ZnO nanostructure was examined by X-ray diffraction, high resolution-transmission electron microscopy, and X-ray photoelectron spectroscopy. XPS studies demonstrated that in all samples, Pd existed in two chemical states, namely Pd° and Pd2+. The possible sensing mechanism related to NH3 gas is also discussed in detail.

Highlights

  • Due to the ongoing issue of elevated atmospheric pollution, the development of effective and inexpensive systems for the detection and quantification of environmentally hazardous gases is of particular importantance

  • ZnO NPs containing a range of Pd contents (i.e., 0.5, 0.75, and 1 mol%), their phase purities and crystal structures were examined using X-ray diffractomery (XRD)

  • Characterisation of the obtained ZnO NPs, both before and after Pd loading with 0.5, 0.75, and 1 mol% Pd was carried out, with X-ray diffraction revealing that the ZnO nanostructires are composed of a single phase würtzite structure, while high-resolution transmission electron microscopy confimed the random distribution of small Pd nanocrystals on the surface of ZnO nanoparticles

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Summary

Results and Discussion

Transition from Pd2+ to Pd0 oxidation state plays an important role as it can result in abundance of ionsorbed oxygen species and this is adventigeous the oxidation of NH3 resulting in enhanced sensor response Based on this finding, synergetic effects of higher surface area as a result of smaller crystallite/particle size achieved with Pd loading (as confirmed by XRD and TEM analysis) which led to large number of intrinsic defects may not be excluded as a possible cause for enhanced sensor response with Pd addition in this study. Reproducibility of the 0.75 mol% Pd-loaded ZnO based sensor was investigated by repeatedly subjecting it to 40 ppm of NH3 gas at an optimal operating temperature of 350 °C in both dry and humid atmospheres of 10 and 90% The five cycles showed good repeatability or stability behaviour further indicating good long-term stability fo this sensor

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