A novel Cu-doped ZnO confined structure: Precisely preparation, and sensitization mechanism for ppb-level H2S gas detection

Abstract

It is still highly desired and challengeable to design H2S sensor with high selectivity and sensitivity due to its toxicity and new application in biomarkers like monitoring halitosis. Here, we reported a novel confined structure as highly sensitive and selective H2S gas sensor. The sensing material was prepared with a HKUST-1 templated method by atomic layer deposition (ALD) ZnO decorated on HKUST-1 and calcination. The gas sensor exhibits a high gas sensitivity (Ra/Rg = 2.67 @ 2 ppm) with excellent selectivity to H2S. Furthermore, the obtained sensor shows ppb-level detection ability (Ra/Rg = 1.13 @ 0.1 ppm). Apart from releasing electrons by the oxidization of H2S on oxygen vacancies with adsorbed oxygen species O2− on ZnO surface (Langmuir-Hinshelwood mechanism), the Cu was proved to be the active sites, and would react with surficial S species. The suggestion was confirmed by operando XAS (X-ray adsorption spectrum) measurements combined with DFT calculations (Mars-van Krevelen mechanism). This work provides valuable insights for developing efficient sensing materials and understanding the sensing mechanism.