期刊
ACS NANO
卷 17, 期 18, 页码 17790-17798出版社
AMER CHEMICAL SOC
DOI: 10.1021/acsnano.3c03034
关键词
oxygen vacancies; adsorbed oxygen species; gas sensors; metal oxides; gas mixtures identification; chemisorption; density functional theory
This study proposes a method to manipulate the amount of surface oxygen on metal oxide surfaces by electrically controlling the electron concentration of the metal oxide. The method is effective, repeatable, and does not require severe settings. It can selectively increase oxidizing and reducing gas reactions by reconfiguring the oxygen vacancies on the metal oxide surfaces. The proposed method is applied to gas sensors and overcomes their existing limitations, making the sensors insensitive to certain gases in mixed-gas environments and providing a rapid and linear response to target gas concentrations.
Oxygen vacancies and adsorbed oxygen species on metal oxide surfaces play important roles in various fields. However, existing methods for manipulating surface oxygen require severe settings and are ineffective for repetitive manipulation. We present a method to manipulate the amount of surface oxygen by modifying the oxygen adsorption energy by electrically controlling the electron concentration of the metal oxide. The surface oxygen control ability of the method is verified using first-principles calculations based on density functional theory (DFT), X-ray photoelectron spectroscopy (XPS), and electrical resistance analysis. The presented method is implemented by fabricating oxide thin film transistors with embedded microheaters. The method can reconfigure the oxygen vacancies on the In2O3, SnO2, and IGZO surfaces so that specific chemisorption dominates. The method can selectively increase oxidizing (e.g., NO and NO) and reducing gas (e.g., H2S, NH3, and CO) reactions by electrically controlling the metal oxide surface to be oxygen vacancy-rich or adsorbed oxygen species-rich. The proposed method is applied to gas sensors and overcomes their existing limitations. The method makes the sensor insensitive to one gas (e.g., H2S) in mixed-gas environments (e.g., NO2+H2S) and provides a linear response (R-2 = 0.998) to the target gas (e.g., NO2) concentration within 3 s. We believe that the proposed method is applicable to applications utilizing metal oxide surfaces.
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