New materials capable of storing hydrogen at high gravimetric and volumetric densities are required if hydrogen is to be widely employed as a clean alternative to hydrocarbon fuels in cars and other mobile applications. With exceptionally high surface areas and chemically-tunable structures, microporous metal–organic frameworks have recently emerged as some of the most promising candidate materials. In this critical review we provide an overview of the current status of hydrogen storage within such compounds. Particular emphasis is given to the relationships between structural features and the enthalpy of hydrogen adsorption, spectroscopic methods for probing framework–H2 interactions, and strategies for improving storage capacity (188 references).

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Hydrogen storage in metal–organic frameworks

The sensing ability of individual SnO2 nanowires and nanobelts configured as gas sensors was measured before and after functionalization with Pd catalyst particles. In situ deposition of Pd in the same reaction chamber in which the sensing measurements were carried out ensured that the observed modification in behavior was due to the Pd functionalization rather than the variation in properties from one nanowire to another. Changes in the conductance in the early stages of metal deposition (i.e., before metal percolation) indicated that the Pd nanoparticles on the nanowire surface created Schottky barrier-type junctions resulting in the formation of electron depletion regions within the nanowire, constricting the effective conduction channel and reducing the conductance. Pd-functionalized nanostructures exhibited a dramatic improvement in sensitivity toward oxygen and hydrogen due to the enhanced catalytic dissociation of the molecular adsorbate on the Pd nanoparticle surfaces and the subsequent diffusion ...

Enhanced gas sensing by individual SnO2 nanowires and nanobelts functionalized with Pd catalyst particles.

Hydrogen Spillover. Facts and Fiction

The use of well-defined materials in heterogeneous catalysis will open up numerous new opportunities for the development of advanced catalysts to address the global challenges in energy and the environment. This review surveys the roles of nanoparticles and isolated single atom sites in catalytic reactions. In the second section, the effects of size, shape, and metal-support interactions are discussed for nanostructured catalysts. Case studies are summarized to illustrate the dynamics of structure evolution of well-defined nanoparticles under certain reaction conditions. In the third section, we review the syntheses and catalytic applications of isolated single atomic sites anchored on different types of supports. In the final part, we conclude by highlighting the challenges and opportunities of well-defined materials for catalyst development and gaining a fundamental understanding of their active sites.

Well-Defined Materials for Heterogeneous Catalysis: From Nanoparticles to Isolated Single-Atom Sites.

The mechanism of hydrogen spillover is described using a precisely nanofabricated model system, explaining why it is slower on an aluminum oxide catalyst support than on a titanium oxide catalyst support.

S. Khoobiar

Papers

Particle to Particle Migration of Hydrogen Atoms on Platinum—Alumina Catalysts from Particle to Neighboring Particles