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Study on Carbon Cycle of Hydrogen Supply System over Supported Pt Catalyst: Methylcyclohexane-Toluene-Hydrogen Cycle

Abstract

Owing to the importance of carbon cycle and universality of carbon loss in sustainable hydrogen supply system, Pt based catalysts were designed carefully for reversible methylcyclohexane-toluene-hydrogen (MTH) cycle. Through adjusting activity of Pt species toward C-H bonds to a middle level, higher selectivities of liquid organic hydrogen carriers (LOHCs) were achieved, which making MTH cycle closer to a closed carbon cycle. Specifically, in hydrogen generation process, we tried to enhance coking resistance as well as inhibit side-reactions such as disproportionation, de-alkylation and hydro-isomerization by Cu doping in Pt/S-1. Experimentally, selectivities of H2-rich and H2-lean LOHCs in MTH cycle reached to 99.9% with almost coke free. Moreover, Pt based catalysts exhibited excellent activity and durability in catalyzing MTH cycle. Hydrogen release rate reached to 445.3 mmol/gPt/min with 92.26% methylcyclohexane (MCH) conversion and hydrogen storage rate achieved to 1271 mmol/gPt/min with greater than 99.9% toluene conversion. Finally, through further investigating the geometric configuration and electronic environment of Cu and Pt species, we found that Pt was co-located and interacted with Cu by forming alloy. And the unique electron structure of Cu-Pt alloy facilitated electron transfer from Pt to Cu, decreasing electron density of Pt. As a consequence, over-dehydrogenation and hydrogenolysis in MTH cycle were inhibited.

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Supplementary files

Article information


Submitted
04 Oct 2019
Accepted
05 Jan 2020
First published
07 Jan 2020

Catal. Sci. Technol., 2020, Accepted Manuscript
Article type
Paper

Study on Carbon Cycle of Hydrogen Supply System over Supported Pt Catalyst: Methylcyclohexane-Toluene-Hydrogen Cycle

X. Zhang, N. He, L. Lin, Q. Zhu, G. Wang and H. Guo, Catal. Sci. Technol., 2020, Accepted Manuscript , DOI: 10.1039/C9CY01999E

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