The Dehydrogenation of H‐S Bond into Sulfur Species on Supported Pd Single Atoms Allows Highly Selective and Sensitive Hydrogen Sulfide Detection. Issue 52 (29th October 2021)

• Record Type: Journal Article
• Authors: Liu, Bo; Zhang, Linjuan; Luo, Yuanyuan; Gao, Lei; Duan, Guotao
• Is Part Of: Small. Volume 17:Issue 52(2021)
• Page Start: n/a
• Page End: n/a
• Publication Date: 2021-10-29
• Subjects: chemiresistive gas sensing -- DFT calculations -- H 2S -- kinetic reaction process -- Pd single atoms; Nanotechnology -- Periodicals; Nanoparticles -- Periodicals; Microtechnology -- Periodicals; 620.5
• DOI: 10.1002/smll.202105643
• Languages: English
• ISSNs: 1613-6810

Abstract

Abstract: The supported metal catalysts on scaffolds usually reveal multiple active sites, resulting in the occurrence of side reaction and being detrimental to the achievement of highly consistent catalysis. Single atom catalysts (SACs), possessed with highly consistent single active sites, have great potentials for overcoming such issues. Herein, the authors used SACs to modulate kinetic process of gas sensitive reaction. The supported Pd SACs, established by a metal organic frameworks‐templated approach, promoted greatly the detection capacity to hydrogen sulfide (H2 S) gas with a very high sensitivity and selectivity. Density functional theory calculations show that the supported Pd SACs not only increased the number of electrons transferring from H2 S molecules to Pd SACs, but strengthened surface affinity to H2 S. Moreover, the HS bonds of H2 S molecules absorbed on Pd atomic sites are more likely to be dehydrogenated directly into sulfur species. Significantly, quasi in situ XPS analysis confirmed the presence of sulfur species during H2 S detection process, which may be a major cause for such detection signal. Based on these results, a suitable sensing principle for H2 S gas driven by Pd SACs was put forward. This work will enrich catalytic electronics in chemiresistive gas sensing. Abstract : The effect of supported Pd single atoms on H2 S gas sensing behavior is investigated by combing density functional theory calculations with quasi in situ XPS analysis. The dehydrogenation of HS bonds into sulfur species on Pd atomic sites is a main cause for such H2 S sensing signal. A sensing model for H2 S on supported Pd atomic sites is proposed.