Junction-Amplified Porous SnO2-Co3O4 Nanospheres for ppb-Level Low-Temperature Acetone Detection and Wearable-Integrated Breath Monitoring

材料科学 多孔性 工作(物理) 丙酮 纳米技术 调制(音乐) 化学工程 转导(生物物理学) 还原(数学) 氧化还原 光电子学 曲面(拓扑) 电极 化学 多孔介质 高电阻
作者
Jian Hou,Dalei Zu,Zhaoyang Li,Zhiyong Chen,Jun‐Hyun Kim,C LEE,Muhammad Hilal,Zhicheng Cai
出处
期刊:ACS Sensors [American Chemical Society]
卷期号:11 (7): 5998-6013 被引量:1
标识
DOI:10.1021/acssensors.6c00930
摘要

Porous oxide heterostructures are attractive for breath acetone sensing, yet low-temperature operation in humidity-rich environments is often constrained by insufficient signal gain and interfacial transport loss. Here, we report junction-rich porous SnO2-Co3O4 nanospheres synthesized via a glucose-templated route, in which the Sn:Co precursor ratio is systematically programmed to tune phase composition, heterointerface density, and the dominant carrier type across an n-to-p transition. The optimized sample (SnCo-3) exhibits the lowest optimal operating temperature and the highest acetone response, enabling ppb-level detection at 125 °C with a theoretical limit of detection of 43 ppb. Beyond an adsorption-only interpretation, we build a correlative mechanistic framework connecting the electronic structure and transport kinetics to the chemiresistive output. UV-vis spectroscopy, Mott-Schottky analysis, and valence-band XPS jointly constrain band positions and Fermi-level evolution, while electrochemical impedance spectroscopy reveals reduced interfacial transport loss for SnCo-3. Together with O 1s oxygen-chemistry analysis, these results indicate that the superior performance arises from an electronically well-coupled p-n junction network that enhances band-bending tunability while maintaining continuous charge-transport pathways. In this optimized regime, the junction barriers serve as modulation-sensitive transduction sites rather than transport-blocking interfaces, allowing surface redox events to be converted into amplified resistance modulation with reduced interfacial transport loss. The sensor further shows robust repeatability, long-term stability, and humidity-dependent response trends relevant to breath conditions, and SnCo-3 is integrated on a flexible platform for wearable-oriented evaluation. This work offers a mechanism-guided strategy to design low-temperature chemiresistive breath sensors by jointly optimizing junction gain and interfacial transport.
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