Bidimensional Engineered Amorphous a-SnO2 Interfaces: Synthesis and Gas Sensing Response to H2S and Humidity

Two-dimensional (2D) transition metal dichalcogenides (TMDs) and metal chalcogenides (MCs), despite their excellent gas sensing properties, are subjected to spontaneous oxidation in ambient air, negatively affecting the sensor's signal reproducibility in the long run. Taking advantage of spontaneous oxidation, we synthesized fully amorphous a-SnO2 2D flakes (approximate to 30 nm thick) by annealing in air 2D SnSe2 for two weeks at temperatures below the crystallization temperature of SnO2 (T < 280 degrees C). These engineered a-SnO2 interfaces, preserving all the precursor's 2D surface-to-volume features, are stable in dry/wet air up to 250 degrees C, with excellent baseline and sensor's signal reproducibility to H2S (400 ppb to 1.5 ppm) and humidity (10-80% relative humidity (RH)) at 100 degrees C for one year. Specifically, by combined density functional theory and ab initio molecular dynamics, we demonstrated that H2S and H2O compete by dissociative chemisorption over the same a-SnO2 adsorption sites, disclosing the humidity cross-response to H2S sensing. Tests confirmed that humidity decreases the baseline resistance, hampers the H2S sensor's signal (i.e., relative response (RR) = Ra/Rg), and increases the limit of detection (LOD). At 1 ppm, the H2S sensor's signal decreases from an RR of 2.4 +/- 0.1 at 0% RH to 1.9 +/- 0.1 at 80% RH, while the LOD increases from 210 to 380 ppb. Utilizing a suitable thermal treatment, here, we report an amorphization procedure that can be easily extended to a large variety of TMDs and MCs, opening extraordinary applications for 2D layered amorphous metal oxide gas sensors.