Highly Stable and Selective Sensing of Hydrogen Sulfide in Living Mouse Brain with NiN4 Single-Atom Catalyst-Based Galvanic Redox Potentiometry

Hydrogen sulfide (H₂S) is recognized as a gasotransmitter and multifunctional signaling molecule in the central nervous system. Despite its essential neurofunctions, the chemical dynamics of H₂S during physiological and pathological processes remains poorly understood, emphasizing the significance of H₂S sensor development. However, the broadly utilized electrochemical H₂S sensors suffer from low stability and sensitivity loss in vivo due to sulfur poisoning-caused electrode passivation. Herein, we report a high-performance H₂S sensor that combines single-atom catalyst strategy and galvanic redox potentiometry to overcome the issue. Atomically dispersed NiN₄ active sites on the sensing interface promote electrochemical H₂S oxidation at an extremely low potential to drive spontaneous bipolarization of a single carbon fiber. Bias-free potentiometric sensing at open-circuit condition minimizes sulfur accumulation on the electrode surface, thus significantly enhancing the stability and sensitivity. The resulting sensor displays high selectivity to H₂S against physiological interferents and enables real-time accurate quantification of H₂S-releasing behavior in the living mouse brain.