Three-Dimensional Porous Carbon/Nitrogen Framework-Decorated Palladium Nanoparticles for Stable and Wide-Concentration-Range Hydrogen Sensing

ACS Appl Mater Interfaces. 2022 Apr 20;14(15):17911-17919. doi: 10.1021/acsami.1c24190. Epub 2022 Apr 6.

Abstract

Hydrogen (H2) as a high-energy-density carrier is of great potential in the upcoming hydrogen economy. Nevertheless, H2/air mixtures are explosive at H2 concentrations above 4 v/v % and reliable and wide-concentration-range H2 sensors are thus highly desired. Here, hydrogen sensing has been developed using palladium nanoparticles of ∼11.2 nm in diameter chemically decorated on the carbon/nitrogen three-dimensional porous framework of 308 m2 g-1 in specific surface area (Pd NPs@CN 3D framework). Theoretically, the Pd NPs and CN 3D framework are used to construct the Mott-Schottky heterojunctions, in which the CN 3D framework possesses a higher work function, promoting electron transfer to Pd NPs and therefore highly active dissociation of H2. Beneficially, the Pd NPs@CN 3D framework exhibits a wide concentration range of 200 ppm (S ≈ 0.2% and Tres ≈ 15 s) to 40 v/v % (S ≈ 73.8% and Tres ≈ 9 s) H2 sensing at room temperature. Remarkably, the H2 sensor prototype built with the Pd NPs@CN 3D framework shows excellent long-term stability that maintains reliable H2 sensing after 142 days. Such stable hydrogen sensing provides an experimental basis for the wide-concentration-range detection of H2 leakage in the future hydrogen economy.

Keywords: Pd NPs@CN 3D framework; hydrogen sensing; room temperature; stability; wide concentration range.