Al-Modulated Y2O3 Multishelled Hollow Spheres for Ultrasensitive Acetone Cataluminescence Sensing and Catalytic Removal.

Abstract

Ultrasensitive detection and efficient removal of airborne acetone are vital for environmental monitoring; however, achieving both functions with a single material presents a significant challenge. Here, we developed a Y1.3Al0.7O3 bimetallic oxide multishelled hollow sphere (BMHS), which function as a high-performance cataluminescence (CTL) sensor for ultrasensitive acetone detection and as an efficient catalyst for acetone gas removal from air. Regulation aluminum distribution in the Y1.3Al0.7O3 BMHSs enabled the achievement of an ultrasensitive acetone detection limit of 412 ppt at a working temperature of 150 °C and wavelength of 620 nm. The sensor exhibited excellent sensitivity, selectivity, and repeatability for acetone detection, with spike recoveries ranging from 94.79% to 101.15% in acetone-spiked breath samples from three healthy volunteers. Meanwhile, the Y1.3Al0.7O3 BMHS catalyst achieves complete (100%) acetone removal efficiency without any inactivation during a 24 h continuous operation test. The superior catalytic performance is ascribed to the high specific surface area, abundant surface-adsorbed oxygen species, and the effects of aluminum doping. DFT calculations and in situ IR spectroscopy suggest that the incorporation of nonprecious aluminum (Al) effectively lowers the acetone adsorption energy compared to pure Y2O3 while also enhancing electron transport, thus significantly promoting catalytic oxidation of acetone and improving overall sensing performance. The proposed non-noble metal-doping strategy not only offers a promising approach to enhance the catalytic performance of bimetal oxide multishelled hollow spheres but also crucially addresses the challenge of integrating both detection and removal capabilities into a single functional material.

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