The possible role of ammonia in a future energy infrastructure is discussed. The review is focused on the catalytic decomposition of ammonia as a key step. Other aspects, such as the catalytic removal of ammonia from gasification product gas or direct ammonia fuel cells, are highlighted as well. The more general question of the integration of ammonia in an infrastructure is also covered.

/pdf/ammonia-as-a-possible-element-in-an-energy-infrastructure-33hu5arllm.pdf

Ammonia as a possible element in an energy infrastructure: catalysts for ammonia decomposition

Whereas noble metal compounds have long been central in catalysis, Earth-abundant metal-based catalysts have in the same time remained undeveloped. Yet the efficacy of Earth-abundant metal catalysts was already shown at the very beginning of the 20th century with the Fe-catalyzed Haber–Bosch process of ammonia synthesis and later in the Fischer–Tropsch reaction. Nanoscience has revolutionized the world of catalysis since it was observed that very small Au nanoparticles (NPs) and other noble metal NPs are extraordinarily efficient. Therefore the development of Earth-abundant metals NPs is more recent, but it has appeared necessary due to their “greenness”. This review highlights catalysis by NPs of Earth-abundant transition metals that include Mn, Fe, Co, Ni, Cu, early transition metals (Ti, V, Cr, Zr, Nb and W) and their nanocomposites with emphasis on basic principles and literature reported during the last 5 years. A very large spectrum of catalytic reactions has been successfully disclosed, and catalysis has been examined for each metal starting with zero-valent metal NPs followed by oxides and other nanocomposites. The last section highlights the catalytic activities of bi- and trimetallic NPs. Indeed this later family is very promising and simultaneously benefits from increased stability, efficiency and selectivity, compared to monometallic NPs, due to synergistic substrate activation.

The recent development of efficient Earth-abundant transition-metal nanocatalysts

Inspired by natural processes, there is an enormous interest in light-driven water splitting to convert solar energy into electrical and chemical energy. This approach is thought to be able to eventually solve the main energy problem that society will face more dramatically in the near future. The water oxidation reaction is widely considered a major barrier for utilizing solar energy in artificial photosynthesis. Due to the relatively high overpotential and slow kinetics of the reaction, numerous efforts are made on the development of non-noble metal oxygen evolution catalysts such as transition metal oxides. Among them, cobalt-oxide-based materials have shown decent activity and thus present themselves as a promising candidate. In this perspective, we summarize the state of the art in synthesis of cobalt-oxide-based materials and application as water oxidation catalysts through electrochemical, photochemical, and photoelectrochemical approaches. Additionally, we state the future challenges that are crit...

Cobalt-Oxide-Based Materials as Water Oxidation Catalyst: Recent Progress and Challenges

Transition metal oxides are regarded as promising anode materials for lithium-ion batteries because of their high theoretical capacities compared with commercial graphite. Unfortunately, the implementation of such novel anodes is hampered by their large volume changes during the Li+ insertion and extraction process and their low electric conductivities. Herein, we report a specifically designed anode architecture to overcome such problems, that is, mesoporous peapod-like Co3O4@carbon nanotube arrays, which are constructed through a controllable nanocasting process. Co3O4 nanoparticles are confined exclusively in the intratubular pores of the nanotube arrays. The pores between the nanotubes are open, and thus render the Co3O4 nanoparticles accessible for effective electrolyte diffusion. Moreover, the carbon nanotubes act as a conductive network. As a result, the peapod-like Co3O4@carbon nanotube electrode shows a high specific capacity, excellent rate capacity, and very good cycling performance.

Controllable Synthesis of Mesoporous Peapod-like Co3O4@Carbon Nanotube Arrays for High-Performance Lithium-Ion Batteries†

Hydrogen storage materials for hydrogen and energy carriers

Uniform and highly dispersed γ-Fe2O3 nanoparticles with a diameter of ∼6 nm supported on CMK-5 carbons and C/SBA-15 composites were prepared via simple impregnation and thermal treatment. The nanostructures of these materials were characterized by XRD, Mossbauer spectroscopy, XPS, SEM, TEM, and nitrogen sorption. Due to the confinement effect of the mesoporous ordered matrices, γ-Fe2O3 nanoparticles were fully immobilized within the channels of the supports. Even at high Fe-loadings (up to about 12 wt %) on CMK-5 carbon no iron species were detected on the external surface of the carbon support by XPS analysis and electron microscopy. Fe2O3/CMK-5 showed the highest ammonia decomposition activity of all previously described Fe-based catalysts in this reaction. Complete ammonia decomposition was achieved at 700 °C and space velocities as high as 60 000 cm3 gcat−1 h−1. At a space velocity of 7500 cm3 gcat−1 h−1, complete ammonia conversion was maintained at 600 °C for 20 h. After the reaction, the immobilize...

Spatially and Size Selective Synthesis of Fe-Based Nanoparticles on Ordered Mesoporous Supports as Highly Active and Stable Catalysts for Ammonia Decomposition

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Spatially and Size Selective Synthesis of Fe-Based Nanoparticles on Ordered Mesoporous Supports as Highly Active and Stable Catalysts for Ammonia Decomposition