Issue 19, 2024

Activating S surfaces by reversing the electron supply direction for fast hydrogen sensing

Abstract

The nature of a built-in electric field within supported metal catalysts plays a crucial role in regulating gas adsorption and electron transfer during the gas-sensing process. Herein, we found an electron-supply redeployment phenomenon involving the reversal of direction of a built-in electric field between the metal palladium species and the outer S atoms in ZnS, resulting in a marked hydrogen sensing difference. It was found that Pd nanoparticles embedded into Pd NP-ZnS can induce spontaneous electron transfer from S atoms to Pd species to generate an electron-deficient sulfur (S(2−δ)−) surface. Conversely, atomically dispersed Pd species (Pd1-ZnS) prefer to generate electron-rich sulfur (S(2+δ)−) sites and thus reverse the built-in electric field. Theoretical calculations demonstrate that the electron-rich S (S(2+δ)−) surface can reduce the occupancy of antibonding orbitals in the S–Hads bond and enhance the bond energy of S–Hads, thus increasing the adsorption of hydrogen. Additionally, in situ Raman, ex situ X-ray photoelectron spectroscopy and DFT analysis demonstrate that S(2+δ)− sites in Pd1-ZnS samples can undergo strong electron transfer with hydrogen during the sensing process. Ultimately, Pd1-ZnS sensors exhibit extremely high response values (9.66/20 ppm) and fast response recovery times (5.1 s/1.8 s to 400 ppm) for hydrogen gas at a working temperature of 170 °C.

Graphical abstract: Activating S surfaces by reversing the electron supply direction for fast hydrogen sensing

Supplementary files

Article information

Article type
Research Article
Submitted
20 Jun 2024
Accepted
16 Aug 2024
First published
22 Aug 2024

Inorg. Chem. Front., 2024,11, 6406-6417

Activating S surfaces by reversing the electron supply direction for fast hydrogen sensing

X. Jia, M. Li, Y. Li, P. Qiao, X. Wang, Y. Jiang, M. Guo, P. Hu, B. Lu, B. An, Z. Xue and J. Xu, Inorg. Chem. Front., 2024, 11, 6406 DOI: 10.1039/D4QI01552E

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