Development of a Photoelectrochemical Microelectrode Using an Organic Probe for Monitoring Hydrogen Sulfide in Living Brains

Hydrogen sulfide (H2S) is an important bioactive molecule that plays a significant role in various functions, particularly in the living brain, where it is closely linked to cognition, memory, and several neurological diseases. Consequently, developing effective detection methods for H2S is essential for studying brain functions and the underlying mechanisms of these diseases. This study aims to construct a novel photoelectrochemical (PEC) microelectrode Ti/TiO2@HSP for the quantitative monitoring of H2S levels in the living brain. The PEC microelectrode Ti/TiO2@HSP is formed by covalently bonding a specifically designed organic PEC probe HSP, which possesses a D-π–A structure, to the surface of TiO2 nanotubes generated via in situ anodic oxidation of titanium wire. The PEC probe HSP can effectively react with H2S and generate significant photocurrent response under long-wavelength excitation light (560 nm), thereby achieving quantitative detection of H2S. The sensor demonstrates high sensitivity and good selectivity. In vivo experiments utilizing the PEC microelectrode Ti/TiO2@HSP enable the monitoring of dynamic changes in H2S levels across various regions of the mouse brain. The findings reveal that in normal mice, the concentration of H2S in the hippocampus is significantly higher than in the striatum and cerebral cortex. Additionally, following propargylglycine drug stimulation, H2S concentrations in different brain regions were observed to decrease, with the most substantial reduction noted in the hippocampus. This suggests that cystathionine γ-lyase (CSE) is the primary enzyme responsible for H2S production in this area, while the striatum exhibits a less pronounced decrease in H2S concentration, indicating a reliance on alternative enzymatic pathways for H2S production. Therefore, this study not only successfully develops a high-performance H2S detection sensor but also provides new experimental tools and theoretical foundations for further exploring the roles of H2S in neurophysiological and pathological processes.