Photoelectron Storages in Functionalized Carbon Nitrides for Colorimetric Sensing of Oxygen

Colorimetric sensors have been widely used for centuries across diverse fields, thanks to their easy operation and uncompromisingly high sensitivity with no need for electricity. However, it is still a great challenge for conventional chromogenic systems to perform multiple measurements meanwhile maintaining high robustness. Here, we reported that carbon nitrides (CNs), the raw materials that are abundant, structure-tunable, and stable semiconductors with photoelectron storage capability, can be developed as a chromogenic system for colorimetric sensors. Beyond conventional metal oxides that only demonstrated a single blue-color switch after photoelectron storage, CN exhibited a multicolor switch under identical conditions owing to the unusual multiple photoelectron storage pathways. Mechanism studies revealed cyano and carbonyl groups in CN crucially elongated the centroid distance of electrons/holes, which exclusively stabilized the specific excited states that have different light absorption; meanwhile, the counter cations strengthened these processes. As a result, O-2, a proof-of-concept analyte, was quantitatively detected by the CN-derived colorimetric sensor, showing high reversibility in hundreds of cycles and adaptable sensitivity/detection range, outperforming most reported and commercial oxygen sensors. These intriguing features of CN are highly envisioned for the next generation of colorimetric sensors, especially in developing countries or fieldworks, to improve the detection reliability and lower the sensing cost.