Redispersing Ir Nanoparticles via a Carbon-Assisted Pyrolysis Process to Break the Activity-Stability Trade-Off of H2 Sensors.

Oxide semiconductor-supported metal nanoparticles often suffer from a high-temperature gas sensing process, resulting in agglomeration and coalescence, which significantly decrease their surface activity and stability. Here, we develop an in situ pyrolysis strategy to redisperse commercial Ir particles (∼15.6 nm) into monodisperse Ir species (∼5.4 nm) on ZnO supports, exhibiting excellent sintering-resistant properties and H2 sensing. We find that large-size Ir nanoparticles can undergo an unexpected splitting decomposition process and spontaneously migrate along the encapsulated carbon layer surface during high-temperature pyrolysis of ZIF-8. This resultant monodisperse status can be integrally reserved, accompanying further oxidation sintering. The final Irred/ZnO-450-based sensor exhibits outstanding stability, H2 response (10-2000 ppm), fast response/recovery capability (7/9.7 s@100 ppm), and good moisture resistance. In situ Raman and ex situ XPS further experimentally verify that highly dispersive Ir species can promote the electron transfer process during the gas sensing process. Our strategy thus provides important insights into the design of agglomeration-resistant gas sensing materials for highly effective H2 detection.