Abstract

Breathomics is a widely emerging tool for noninvasive disease diagnosis and focuses on the detection of various levels of volatile organic compounds and inorganic gases present in human breath. One of the rapid, easy-to-use, and noninvasive detection methods being investigated is a system that can measure exhaled breath ammonia levels and can be correlated to the functional state of protein metabolic pathways and the renal functioning system. In this work, we have demonstrated the development of an electrochemical nose system using ferrocene encapsulated into zeolitic imidazole framework, Fc@ZIF-8, which can be successfully used for the detection of ammonia levels in breath. This is the first report of an electrochemical gas sensor platform that uses a faradaic probe (that is ferrocene) encapsulated into a metal-organic framework cavity used for disease diagnosis by monitoring the levels of the target gas and can be used for breathomics applications. This work demonstrates that low levels of ammonia gas (up to 400 ppb) can be detected with high sensitivity and specificity. The morphological and structural characterization of the novel, synthesized Fc@ZIF-8 nanocomposite has been performed using powder X-ray diffraction, field emission scanning electron microscopy, Fourier transform infrared, ultraviolet-visible spectroscopy, and dynamic light scattering. Electrochemical characterization of the material has been performed using a standard glassy carbon electrode, and further application of the material has been shown using the in-house designed and reported spiral electrochemical notification coupled electrode, used for ammonia gas sensing. Cross-reactivity studies have also been performed to demonstrate sensor specificity toward the target gas. We demonstrate the first of its kind electrochemical bifunctional probe platform that can be used for sensing ammonia levels in breath, with high sensitivity and specificity, due to the hybrid material system-zinc-imidazole framework 8 (having excellent physisorption properties) and ferrocene (acting as a redox mediator). We envision that such a sensing system will allow noninvasive and early diagnosis of chronic kidney disease, thus leading to early treatment and a decrease in the mortality rate.

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