Repetitive pulsed gas-liquid discharge in different atmospheres: from discharge characteristics to plasma-liquid interactions

Gas-liquid discharges enable efficient plasma-liquid interactions and thus have promising applications, but many concerns remain unanswered regarding working gas, an important influencing factor. Investigations of a pulsed needle-to-water gas-liquid discharge in Ar, He, and N2 are carried out in this study. Voltage-current waveforms and intensified charge-coupled device (ICCD) images were combined to explore discharge modes and evolution processes. Experimental results demonstrate that the Ar tip spark discharge develops all the way to liquid compared with the He and N2 discharges concentrated in the tube, considerably increasing the plasma-liquid interaction efficiency. According to the optical emission spectra (OES), plasma properties are found to be strongly influenced by interactions between gas particles and interfering particles (H2O, etc.). For instance, excess water vapor causes quenching of excited species, resulting in OH (A-X) in Ar and NO (A-X) in N2 concentrated in the middle region with weak discharge. By adding dimethyl sulfoxide, it is demonstrated that OH dominates H2O2 production in Ar and contributes to both NO2- and NO3- generation in Ar and He, whereas in N2 it only affects NO3- generation. This study advances the "bridge building" between practical application and gas-liquid discharge employing different working gases. Intense Ar spark discharge leads to the most efficient plasma-liquid interactions, energetic He particles give rise to multiple synthesis pathways for H2O2, and OH plays different roles in aqueous physicochemical reactions in different atmospheres.