Abstract

This study reveals the effect of the catalytic 1D supports (carbon, ceria, alumina and titanate) for ruthenium particles on the low temperature release of hydrogen from ammonia. While the state-of-art literature presents Ru/carbon nanotubes (CNT) as the most active catalyst, we found in this work that ruthenium supported on ceria nanorods (Ru/CeO2) catalyst exhibited activity over 8 times higher than the Ru/CNT counterpart system. This enhanced activity is believed to be related to a strong metal-support interaction on the Ru/CeO2 catalysts promoting the formation of small (~ 3 nm) Ru particles. Addition of sodium as a promoter leads to the formation of smaller Ru particle sizes in addition to the modification of the electronic environment of Ru, enhancing the ammonia decomposition activity at low temperatures. This effect is particularly noticeable in the Ru–Na/CNT catalysts, facilitated by the high conductivity of the support, allowing distant electronic modification of the Ru active sites. This work provides novel insights in designing catalysts for hydrogen production from ammonia in our effort to enable the long-term energy storage in chemical bonds.

Highlights

  • The heavy reliance of our society on fossil fuels has raised serious environmental issues mainly related to the excessive carbon dioxide (­CO2) emissions into the atmosphere [1]

  • The feasibility of the ammonia economy depends on the development of new capabilities to release hydrogen at temperatures aligned to the operating temperature of proton exchange membrane fuel cells (PEMFCs), according to the US Department of Energy [6]

  • Commercial carbon nanotubes (CNT) and Titanate nanotubes (Ti-NT) have a hollow structure while ­CeO2 NR and ­Al2O3 NR have a solid interior

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Summary

Introduction

The heavy reliance of our society on fossil fuels has raised serious environmental issues mainly related to the excessive carbon dioxide (­CO2) emissions into the atmosphere [1] One reason for this situation is the challenging and fallingbehind development of new alternative renewable energy sources, such as solar, wind and biomass capable of meeting the current energy demands. The feasibility of the ammonia economy depends on the development of new capabilities to release hydrogen at temperatures aligned to the operating temperature of proton exchange membrane fuel cells (PEMFCs), according to the US Department of Energy [6] Such conditions will face thermodynamic limitations and the produced hydrogen will need to be purified to avoid the poisoning of the catalayst and membrane in the fuel cells using, for example, membranes [7]. CNTs are believed to be the best catalytic support due to its promotion of Ru

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