A first-principles study of hydrazine adsorption and decomposition on Pt(111) surface: The effect of partially dissociative H2O on decomposition process

IF 2.1 4区化学 Q3 CHEMISTRY, PHYSICAL

Surface Science Pub Date : 2024-12-12 DOI:10.1016/j.susc.2024.122680

Yaolin Zhao , Dayin Tong , Zhongcun Chen , Songtao Xiao

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Abstract

Density functional theory with dispersion correction (DFT-D3) is used to investigate the adsorption and decomposition of hydrazine (N₂H₄) on Pt(111) surface, and the effect of water on decomposition process is considered. The stable adsorption configurations and adsorption energies are obtained for hydrazine, water and intermediate species. The hydrazine decomposition is investigated in three kinds of pathways including intramolecular dehydrogenation and intermolecular dehydrogenation via H atom or OH group assistance. It is shown that the adsorption of water in partially dissociative conformation (H and OH radicals) is the most stable on Pt(111) surface for its largest adsorption energy. The OH group can greatly promote the decomposition of hydrazine by drastically decreasing the energy barriers of dehydrogenation reactions, which are closely related to the overall PDOS distribution shifts of their transition states. From thermodynamics and kinetics points of view, the favorable decomposition pathway of hydrazine may be N₂H₄+OH→N₂H₃+OH→NHNH+OH→NNH+OH→N₂.

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来源期刊

Surface Science 化学-物理：凝聚态物理

CiteScore

3.30

自引率

5.30%

发文量

137

审稿时长

25 days

期刊介绍： Surface Science is devoted to elucidating the fundamental aspects of chemistry and physics occurring at a wide range of surfaces and interfaces and to disseminating this knowledge fast. The journal welcomes a broad spectrum of topics, including but not limited to: • model systems (e.g. in Ultra High Vacuum) under well-controlled reactive conditions • nanoscale science and engineering, including manipulation of matter at the atomic/molecular scale and assembly phenomena • reactivity of surfaces as related to various applied areas including heterogeneous catalysis, chemistry at electrified interfaces, and semiconductors functionalization • phenomena at interfaces relevant to energy storage and conversion, and fuels production and utilization • surface reactivity for environmental protection and pollution remediation • interactions at surfaces of soft matter, including polymers and biomaterials. Both experimental and theoretical work, including modeling, is within the scope of the journal. Work published in Surface Science reaches a wide readership, from chemistry and physics to biology and materials science and engineering, providing an excellent forum for cross-fertilization of ideas and broad dissemination of scientific discoveries.