Controlling Ni Distribution in PdNi Nanoalloys Decorated onto ZnO for Rapid and Robust ppb-Level H2S Sensing.

Rapid and robust ppb-level H2S sensing is of great importance for environmental monitoring, industrial safety, food quality control, and disease screening. However, improving the H2S sensing properties of semiconductor oxides under low-power conditions remains a significant challenge. In this work, an acid etching method was utilized to precisely control the elemental distribution in bimetallic nanoalloys. By tailoring the Ni distribution in PdNi alloy nanoparticles anchored on ZnO nanosheets, an ultralow detection limit of 5 ppb for H2S was achieved at a working temperature of 140 °C. More importantly, the sensor also demonstrated fast response and recovery kinetics, with its superior antipoisoning performance attributed to the oxidation of H2S into SO2 instead of sulfates or sulfites, as evidenced by in situ FTIR spectroscopy. Additionally, density functional theory calculations were performed to elucidate the synergistic effect of the PdNi alloy, revealing that Pd atoms act as electron donors while Ni atoms facilitate H2S adsorption. This study provides a viable strategy for optimizing noble metal-modified oxide-based gas sensors.