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Homogeneous and Interfacial Catalysis in 3D Controlled Environment

This collaborative research effort is geared toward bringing together the best features of homogeneous and heterogeneous catalysis for developing new catalytic principles. Novel silica-based, single-site mesoporous catalysts with controlled, nanostructured morphology and surface properties will be prepared. The control of specific chemical properties, spatial distribution, and concentrations of various catalytic functional groups on the pore walls will be achieved. The catalytic activity of these single-site heterogeneous catalysts will be examined. Detailed mechanistic studies of such systems will be carried out in an effort to recognize the key factors that determine selectivity, reactivity and kinetics of both homogeneous and heterogeneous catalytic reactions.

This research is supported by the U.S. Department of Energy, Office of Basic Energy Sciences, Division of Chemical Sciences, Geosciences, and Biosciences through the Ames Laboratory.  The Ames Laboratory is operated for the U.S. Department of Energy by Iowa State University under Contract No. DE-AC02-07CH11358

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  • Temperature programmed surface reaction profiles of 2-propanol on CeO2 and Ce-Na for m/z=58.

    Researchers have discovered that sodium modification of ceria leads to boost in ceria catalytic activity for the formation of hydrogen from an alcohol that can be derived from renewable resources, isopropanol.  Infiltrating sodium carbonates into ceria disrupts its structure resulting in an increase in the number of surface oxygen vacancies.

  • Bimodal coordination of methionine observed on alumina in the presence of a Pd catalyst using dynamic nuclear polarization surface-enhanced NMR spectroscopy.

    Researchers have discovered a core deactivation mechanism of noble metal catalysts that are used in biorefining and catalytic automobile converters.

  • Schematic of the Pt atom inside the MOF structure, and its corresponding wideline spectrum acquired using DNP NMR

    Researchers have uncovered the atomic-scale geometry of platinum ions with unprecedented precision within metal organic frameworks (MOFs)—a growing class of porous materials that consist of organic ligands and inorganic components.  Due to the immense structural diversity and large surface areas of MOFs, often exceeding the size of a professional football field per gram of material, many uses of MOFs have been discovered in purification, separation, capture, and storage of gases, especially hydrogen, carbon dioxide and methane, as well as applications as catalysts and sensors.

  • Schematic of interaction of methionine with Pd dispersed on alumina and the cooresponding DNP NMR signal

    For the first time researchers have found a way to study highly-dispersed metal nanoparticles and their reactions using dynamic nuclear polarization (DNP) surface-enhanced nuclear magnetic resonance spectroscopy (SENS). Nuclear magnetic resonance (NMR) spectroscopy is a researcher’s equivalent to a physician’s MRI, only in this case the patient is not a person but a material. Now researchers have demonstrated new DNP-based measurements that extend solid-state NMR well beyond its current capabilities and into the realm of probing noble metal nanoparticles. The characterizatio

  • The proximity of the two metals leads to extraordinarily synergistic behavior and researchers observed a 99% conversion of fatty acids into fatty alcohols compared to a mere 8% conversion rate when the same oxides were on separate particles.

    An ingenious method of putting copper and iron in the same nanoparticle has led to a powerful new catalyst that converts waste feedstocks into valuable fatty alcohols.

  • Oxygen is one of the most ubiquitous elements in chemistry and materials science, yet one of the most elusive elements for spectroscopic investigation by solid-state Nuclear Magnetic Resonance (SSNMR). Used to determine the structure of materials and chemicals on the atomic scale, SSNMR requires nuclei that have magnetic moments. Yet, less than four of every 10,000 oxygen nuclei are 17O, the only NMR-active isotope of oxygen.

  • By simply changing the solvent, organic reactions vital for producing the starting materials for many major industrial processes have been found to be faster and able to yield the desired product with close to 100% selectivity.

  • Researchers have studied the effect of concentration on the activity and selectivity in a zirconium-catalyzed hydroamination reaction.  In this important reaction for the efficient and atom economical synthesis of valuable amine compounds, the nitrogen-hydrogen bond adds across a carbon double bond to give a new nitrogen-carbon bond.  Varying concentrations allows for the systematic tuning of a homogeneous 3D environment, impacting the selectivity.

  • If nanostructures were authors, cadmium selenide (CdSe) nanorods would be Hemingway.  Like him, they can endure the heat (up to 662 °F for long periods of time) and don’t break down (in the presence of oxygen or oxygen-like molecules).  CdSe nanorods are one of the II-VI semiconductor nanostructures that are used in various energy conversion applications, including photocatalysis.  Using this material, solar energy can be transformed into hydrogen fuel.

  • New research provides insight into design guidelines for the ideal pore width in nanoporous catalytic materials.  Nanoporous materials have long narrow aisles, or pores, around 2 nm in diameter.  In designing these lab-synthesized materials, researchers strive for the greatest amount of surface area to maximize reaction yield while still allowing molecules to pass each other.  Within a single pore molecules have to squeeze past each other, like shoppers in a crowded supermarket aisle.

Publications


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