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Heterobimetallic Single-Source Precursors: A Springboard To The Synthesis Of Binary Intermetallics, Carena L. Daniels, Deyny L. Mendivelso-Perez, Bryan A. Rosales, Di You, Sumit Sahu, J. Stuart Jones, Emily A. Smith, François P. Gabbaï, Javier Vela 2019 Iowa State University

Heterobimetallic Single-Source Precursors: A Springboard To The Synthesis Of Binary Intermetallics, Carena L. Daniels, Deyny L. Mendivelso-Perez, Bryan A. Rosales, Di You, Sumit Sahu, J. Stuart Jones, Emily A. Smith, FrançOis P. Gabbaï, Javier Vela

Javier Vela-Becerra

Intermetallics are atomically ordered crystalline compounds containing two or more main group and transition metals. In addition to their rich crystal chemistry, intermetallics display unique properties of interest for a variety of applications, including superconductivity, hydrogen storage, and catalysis. Because of the presence of metals with a wide range of reduction potentials, the controlled synthesis of intermetallics can be difficult. Recently, soft chemical syntheses such as the modified polyol and ship-in-a-bottle methods have helped advance the preparation of these materials. However, phase-segregated products and complex multistep syntheses remain common. Here, we demonstrate the use of heterobimetallic single-source precursors for the ...


Energetics Of Cu Adsorption And Intercalation At Graphite Step Edges, Yong Han, Ann Lii-Rosales, Michael C. Tringides, James W. Evans, Patricia A. Thiel 2019 Iowa State University and Ames Laboratory

Energetics Of Cu Adsorption And Intercalation At Graphite Step Edges, Yong Han, Ann Lii-Rosales, Michael C. Tringides, James W. Evans, Patricia A. Thiel

Chemistry Publications

To assess the energetics of Cu intercalation on defective graphite, the chemical potentials and binding energies for Cu at graphite step edges are calculated for three main configurations: an isolated atom, a chain, and an atom attached to a chain. As expected, for Cu interacting directly with a graphite step edge, the strength of interaction depends on the stability of the step, with Cu binding more strongly at a less-stable step. However, the relationship is reversed when considering binding of a Cu atom attached to a chain. Taken together, these trends mean that if the graphite step is less stable ...


Energetics Of Cu Adsorption And Intercalation At Graphite Step Edges, Yong Han, Ann Lii-Rosales, Michael C. Tringides, James W. Evans, Patricia A. Thiel 2019 Iowa State University and Ames Laboratory

Energetics Of Cu Adsorption And Intercalation At Graphite Step Edges, Yong Han, Ann Lii-Rosales, Michael C. Tringides, James W. Evans, Patricia A. Thiel

James W. Evans

To assess the energetics of Cu intercalation on defective graphite, the chemical potentials and binding energies for Cu at graphite step edges are calculated for three main configurations: an isolated atom, a chain, and an atom attached to a chain. As expected, for Cu interacting directly with a graphite step edge, the strength of interaction depends on the stability of the step, with Cu binding more strongly at a less-stable step. However, the relationship is reversed when considering binding of a Cu atom attached to a chain. Taken together, these trends mean that if the graphite step is less stable ...


Squeezed Nanocrystals: Equilibrium Configuration Of Metal Clusters Embedded Beneath The Surface Of A Layered Material, Scott E. Julien, Ann Lii-Rosales, Kai-tak Wan, Yong Han, Michael C. Tringides, James W. Evans, Patricia A. Thiel 2019 Northeastern University

Squeezed Nanocrystals: Equilibrium Configuration Of Metal Clusters Embedded Beneath The Surface Of A Layered Material, Scott E. Julien, Ann Lii-Rosales, Kai-Tak Wan, Yong Han, Michael C. Tringides, James W. Evans, Patricia A. Thiel

Patricia A. Thiel

Shapes of functional metallic nanocrystals, typically synthesized either free in solution or supported on surfaces, are key for controlling properties. Here, we consider a novel new class of metallic nanocrystals, copper islands embedded near the surface of graphite, which can be considered a model system for metals embedded beneath surfaces of layered materials, or beneath supported membranes. We develop a continuum elasticity (CE) model for the equilibrium shape of these islands, and compare its predictions with experimental data. The CE model incorporates appropriate surface energy, adhesion energies, and strain energy. The agreement between the CE model and the data is ...


Energetics Of Cu Adsorption And Intercalation At Graphite Step Edges, Yong Han, Ann Lii-Rosales, Michael C. Tringides, James W. Evans, Patricia A. Thiel 2019 Iowa State University and Ames Laboratory

Energetics Of Cu Adsorption And Intercalation At Graphite Step Edges, Yong Han, Ann Lii-Rosales, Michael C. Tringides, James W. Evans, Patricia A. Thiel

Patricia A. Thiel

To assess the energetics of Cu intercalation on defective graphite, the chemical potentials and binding energies for Cu at graphite step edges are calculated for three main configurations: an isolated atom, a chain, and an atom attached to a chain. As expected, for Cu interacting directly with a graphite step edge, the strength of interaction depends on the stability of the step, with Cu binding more strongly at a less-stable step. However, the relationship is reversed when considering binding of a Cu atom attached to a chain. Taken together, these trends mean that if the graphite step is less stable ...


Kinetics, Energetics, And Size Dependence Of The Transformation From Pt To Ordered Ptsn Intermetallic Nanoparticles, Minda Chen, Yong Han, Tian Wei Goh, Rong Sun, Raghu V. Maligal‐Ganesh, Yuchen Pei, Chia‐ Kuang Tsung, James W. Evans, Wenyu Huang 2019 Iowa State University

Kinetics, Energetics, And Size Dependence Of The Transformation From Pt To Ordered Ptsn Intermetallic Nanoparticles, Minda Chen, Yong Han, Tian Wei Goh, Rong Sun, Raghu V. Maligal‐Ganesh, Yuchen Pei, Chia‐ Kuang Tsung, James W. Evans, Wenyu Huang

James W. Evans

The outstanding catalytic activity and chemical selectivity of intermetallic compounds make them excellent candidates for heterogeneous catalysis. However, the kinetics of their formation at the nanoscale is poorly understood or characterized, and precise control of their size, shape as well as composition during synthesis remains challenging. Here, using well-defined Pt nanoparticles (5 nm and 14 nm) encapsulated in mesoporous silica, we study the transformation kinetics from monometallic Pt to intermetallic PtSn at different temperatures by a series of time-evolution X-ray diffraction studies. Observations indicate an initial transformation stage mediated by Pt surface-controlled intermixing kinetics, followed by a second stage with ...


Toward Unraveling The Mechanisms Of “Green” Mechanochemical Reactions, Richard Chen, Mehmet Kerem Gokus 2019 Old Dominion University

Toward Unraveling The Mechanisms Of “Green” Mechanochemical Reactions, Richard Chen, Mehmet Kerem Gokus

Undergraduate Research Symposium

The mechanical processing of solids, such as milling or grinding powders, often leads to mechanochemical reactions. Mechanochemistry affords “green” synthetic routes avoiding or reducing the use of solvents, thus providing environmentally friendly and cost-effective synthetic alternatives for many materials. The solid-state reactants are usually ground together with small quantities of organic solvents, called “liquid assisted grinding” (LAG). LAG increases the reaction rates, it can yield products from otherwise unreactive mixtures, it increases the products crystallinity, and it selectively leads to crystal structures (polymorphs) of the products, depending on the quantities and physicochemical properties of the liquids used in LAG.

Mechanochemistry ...


On The Role Of Composition And Processing Parameters On The Microstructure Evolution Of Ti-Xmo Alloys, Michael Y. Mendoza, Peyman Samimi, David A. Brice, Iman Ghamarian, Matt Rolchigo, Richard Lesar, Peter Collins 2019 Iowa State University

On The Role Of Composition And Processing Parameters On The Microstructure Evolution Of Ti-Xmo Alloys, Michael Y. Mendoza, Peyman Samimi, David A. Brice, Iman Ghamarian, Matt Rolchigo, Richard Lesar, Peter Collins

Materials Science and Engineering Publications

Laser Engineered Net Shaping (LENS™) was used to produce a compositionally graded Ti-xMo (0 ≤ x ≤ 12 wt %) specimen and nine Ti-15Mo (fixed composition) specimens at different energy densities to understand the composition–processing–microstructure relationships operating using additive manufacturing. The gradient was used to evaluate the effect of composition on the prior-beta grain size. The specimens deposited using different energy densities were used to assess the processing parameters influence the microstructure evolutions. The gradient specimen did not show beta grain size reduction with the Mo content. The analysis from the perspective of the two grain refinement mechanisms based on a ...


Effect Of Dissolved Salts On The Physiochemical Properties Of Deep Eutectic Solvents, Eleanor Haeska, Megan Radtke 2019 South Dakota State University

Effect Of Dissolved Salts On The Physiochemical Properties Of Deep Eutectic Solvents, Eleanor Haeska, Megan Radtke

The Journal of Undergraduate Research

Green chemistry seeks to make chemical procedures safer, improve reaction efficiency, and utilize environmentally safe reagents. Deep eutectic solvents (DES) have recently become of great interest due to their eco-friendly nature and functionality as solvent for various chemical processes. One key characteristic of DES is their conductive nature and depressed melting point. This project sought to determine the effect of the addition of aqueous solutions of halides on the conductivity of two selected types of DES. Also assessed were the polarity and viscosity of the DES. It can be concluded that aqueous halides had no measureable effect on the conductivity ...


Kinetics Of The Γ–Δ Phase Transition In Energetic Nitramine-Octahydro-1,3,5,7-Tetranitro-1,3,5,7-Tetrazocine, P. Bowlan, B. F. Henson, L. Smilowitz, Valery I. Levitas, N. Suvorova, D. Oschwald 2019 Los Alamos National Laboratory

Kinetics Of The Γ–Δ Phase Transition In Energetic Nitramine-Octahydro-1,3,5,7-Tetranitro-1,3,5,7-Tetrazocine, P. Bowlan, B. F. Henson, L. Smilowitz, Valery I. Levitas, N. Suvorova, D. Oschwald

Aerospace Engineering Publications

The solid, secondary explosive nitramine-octahydro-1,3,5,7-tetranitro-1,3,5,7 or HMX has four different stable polymorphs which have different molecular conformations, crystalline structures, and densities, making structural phase transitions between these nontrivial. Previous studies of the kinetics of the βδ HMX structural transition found this to happen by a nucleation and growth mechanism, where growth was governed by the heat of fusion, or melting, even though the phase transition temperature is more than 100 K below the melting point. A theory known as virtual melting could easily justify this since the large volume difference in the two ...


Rapid Prototyping Of Reconfigurable Microfluidic Channels In Undercooled Metal Particle-Elastomer Composites, Boyce Chang, Mario Fratzl, Andrea Boyer, Andrew Martin, Henry C. Ahrenholtz, Isabelle De Moraes, Jean-Francis Bloch, Nora M. Dempsey, Martin M. Thuo 2019 Iowa State University

Rapid Prototyping Of Reconfigurable Microfluidic Channels In Undercooled Metal Particle-Elastomer Composites, Boyce Chang, Mario Fratzl, Andrea Boyer, Andrew Martin, Henry C. Ahrenholtz, Isabelle De Moraes, Jean-Francis Bloch, Nora M. Dempsey, Martin M. Thuo

Materials Science and Engineering Publications

Conventional fabrication of microfluidic channels/devices are faced with challenges such as single use channels and/or significant time consumption. We propose a flexible platform for fabricating microfluidic channels simply through indentation on a smart composite—the so-called ST3R (Stiffness tuning through thermodynamic relaxation) composite. The application of ST3R composite allows rapid fabrication of microfluidic channels by hand or with a prefabricated stamp, and precise prototyping of complex designs using a 2D plotter. Indenter geometry, applied stress, filler loading, and number of repeated indentations affect channel dimensions and/or shape. These channels further exhibit; i) Substantial improvement against swelling by ...


Oxidative Degradation Of Lignin And Investigation Of Utilization Of Lignin-Derived Materials As Building Blocks For Epoxy Resins, Zhen Fang 2019 University of Kentucky

Oxidative Degradation Of Lignin And Investigation Of Utilization Of Lignin-Derived Materials As Building Blocks For Epoxy Resins, Zhen Fang

Theses and Dissertations--Chemistry

Lignin, the second most abundant biopolymer on earth, is potentially a replaceable source for bulky fuels and chemical feedstocks. There have been numerous reports on methods for the oxidative cleavage of β-O-4 linkages but relatively few reports of how those methods affect other linkages that are present in lignin. We investigated how the β-1 and β-5 linkages respond under oxidative conditions proposed for lignin deconstruction based on their effect on β-O-4 linkages. Mechanochemical treatment of lignin can greatly improve the yield of monomer products and we applied a mechanochemical approach, using powerful ring-and-puck milling to promote lignin degradation. Along with ...


Squeezed Nanocrystals: Equilibrium Configuration Of Metal Clusters Embedded Beneath The Surface Of A Layered Material, Scott E. Julien, Ann Lii-Rosales, Kai-tak Wan, Yong Han, Michael C. Tringides, James W. Evans, Patricia A. Thiel 2019 Northeastern University

Squeezed Nanocrystals: Equilibrium Configuration Of Metal Clusters Embedded Beneath The Surface Of A Layered Material, Scott E. Julien, Ann Lii-Rosales, Kai-Tak Wan, Yong Han, Michael C. Tringides, James W. Evans, Patricia A. Thiel

Chemistry Publications

Shapes of functional metallic nanocrystals, typically synthesized either free in solution or supported on surfaces, are key for controlling properties. Here, we consider a novel new class of metallic nanocrystals, copper islands embedded near the surface of graphite, which can be considered a model system for metals embedded beneath surfaces of layered materials, or beneath supported membranes. We develop a continuum elasticity (CE) model for the equilibrium shape of these islands, and compare its predictions with experimental data. The CE model incorporates appropriate surface energy, adhesion energies, and strain energy. The agreement between the CE model and the data is ...


Kinetics, Energetics, And Size Dependence Of The Transformation From Pt To Ordered Ptsn Intermetallic Nanoparticles, Minda Chen, Yong Han, Tian Wei Goh, Rong Sun, Raghu V. Maligal‐Ganesh, Yuchen Pei, Chia‐ Kuang Tsung, James W. Evans, Wenyu Huang 2019 Iowa State University

Kinetics, Energetics, And Size Dependence Of The Transformation From Pt To Ordered Ptsn Intermetallic Nanoparticles, Minda Chen, Yong Han, Tian Wei Goh, Rong Sun, Raghu V. Maligal‐Ganesh, Yuchen Pei, Chia‐ Kuang Tsung, James W. Evans, Wenyu Huang

Chemistry Publications

The outstanding catalytic activity and chemical selectivity of intermetallic compounds make them excellent candidates for heterogeneous catalysis. However, the kinetics of their formation at the nanoscale is poorly understood or characterized, and precise control of their size, shape as well as composition during synthesis remains challenging. Here, using well-defined Pt nanoparticles (5 nm and 14 nm) encapsulated in mesoporous silica, we study the transformation kinetics from monometallic Pt to intermetallic PtSn at different temperatures by a series of time-evolution X-ray diffraction studies. Observations indicate an initial transformation stage mediated by Pt surface-controlled intermixing kinetics, followed by a second stage with ...


Atomic-Scale Structure Of Mesoporous Silica-Encapsulated Pt And Ptsn Nanoparticles Revealed By Dynamic Nuclear Polarization-Enhanced Si-29 Mas Nmr Spectroscopy, Evan Wenbo Zhao, Raghu Maligal-Ganesh, Frederic Mentink-Vigier, Tommy Yunpu Zhao, Yong Du, Yuchen Pei, Wenyu Huang, Clifford Russell Bowers 2019 University of Florida

Atomic-Scale Structure Of Mesoporous Silica-Encapsulated Pt And Ptsn Nanoparticles Revealed By Dynamic Nuclear Polarization-Enhanced Si-29 Mas Nmr Spectroscopy, Evan Wenbo Zhao, Raghu Maligal-Ganesh, Frederic Mentink-Vigier, Tommy Yunpu Zhao, Yong Du, Yuchen Pei, Wenyu Huang, Clifford Russell Bowers

Chemistry Publications

Mesoporous silica encapsulated Pt (Pt@mSiO2) and PtSn (PtSn@mSiO2) nanoparticles (NPs) are representatives of a novel class of heterogeneous catalysts with uniform particle size, enhanced catalytic properties, and superior thermal stability. In the ship-in-a-bottle synthesis, PtSn@mSiO2intermetallic NPs are derived from Pt@mSiO2 seeds where the mSiO2 shell is formed by polymerization of tetraethyl orthosilicate around a tetradecyltrimethylammonium bromide template, a surfactant used to template MCM-41. Incorporation of Sn into the Pt@mSiO2 seeds is accommodated by chemical etching of the mSiO2 shell. The effect of this etching on the atomic-scale structure of the mSiO2 has not been previously ...


Near Room Temperature Antiferromagnetic Ordering With A Potential Low Dimensional Magnetism In Almn2b2, Tej N. Lamichhane, Khusboo Rana, Qisheng Lin, Sergey L. Bud’ko, Yuji Furukawa, Paul C. Canfield 2019 Iowa State University and Ames Laboratory

Near Room Temperature Antiferromagnetic Ordering With A Potential Low Dimensional Magnetism In Almn2b2, Tej N. Lamichhane, Khusboo Rana, Qisheng Lin, Sergey L. Bud’Ko, Yuji Furukawa, Paul C. Canfield

Chemistry Publications

We present self flux growth and characterization of single crystalline AlMn2B2. It is an orthorhombic (space group Cmmm), layered material with a plate like morphology. The anisotropic bulk magnetization data, electrical transport and 11B nuclear magnetic resonance(NMR) data revealed an antiferromagnetic (AFM) transition at 313 ± 2 K. In the magnetization data, there is also a broad local maximum significantly above the AFM transition that could be a signature of low dimensional magnetic interactions in AlMn2B2.


Crystallographically Determined Etching And Its Relevance To The Metal-Assisted Catalytic Etching (Mace) Of Silicon Powders, Kurt W. Kolasinski, Bret A. Unger, Alexis T. Ernst, Mark Aindow 2019 West Chester University of Pennsylvania

Crystallographically Determined Etching And Its Relevance To The Metal-Assisted Catalytic Etching (Mace) Of Silicon Powders, Kurt W. Kolasinski, Bret A. Unger, Alexis T. Ernst, Mark Aindow

Chemistry Faculty Publications

Metal-assisted catalytic etching (MACE) using Ag nanoparticles as catalysts and H2O2 as oxidant has been performed on single-crystal Si wafers, single-crystal electronics grade Si powders, and polycrystalline metallurgical grade Si powders. The temperature dependence of the etch kinetics has been measured over the range 5–37◦C. Etching is found to proceed preferentially in a h001i direction with an activation energy of ∼0.4 eV on substrates with (001), (110), and (111) orientations. A quantitative model to explain the preference for etching in the h001i direction is developed and found to be consistent with the measured activation energies. Etching of ...


Heterobimetallic Single-Source Precursors: A Springboard To The Synthesis Of Binary Intermetallics, Carena L. Daniels, Deyny L. Mendivelso-Perez, Bryan A. Rosales, Di You, Sumit Sahu, J. Stuart Jones, Emily A. Smith, François P. Gabbaï, Javier Vela 2019 Iowa State University

Heterobimetallic Single-Source Precursors: A Springboard To The Synthesis Of Binary Intermetallics, Carena L. Daniels, Deyny L. Mendivelso-Perez, Bryan A. Rosales, Di You, Sumit Sahu, J. Stuart Jones, Emily A. Smith, FrançOis P. Gabbaï, Javier Vela

Chemistry Publications

Intermetallics are atomically ordered crystalline compounds containing two or more main group and transition metals. In addition to their rich crystal chemistry, intermetallics display unique properties of interest for a variety of applications, including superconductivity, hydrogen storage, and catalysis. Because of the presence of metals with a wide range of reduction potentials, the controlled synthesis of intermetallics can be difficult. Recently, soft chemical syntheses such as the modified polyol and ship-in-a-bottle methods have helped advance the preparation of these materials. However, phase-segregated products and complex multistep syntheses remain common. Here, we demonstrate the use of heterobimetallic single-source precursors for the ...


Photo-Isomerizable Complementary Hydrogen Bond Arrays, Jeffrey S. Pleizier 2018 The University of Western Ontario

Photo-Isomerizable Complementary Hydrogen Bond Arrays, Jeffrey S. Pleizier

Electronic Thesis and Dissertation Repository

The use of light as an external stimulus provides a non-invasive technique to induce large changes in physical and chemical properties of a substrate. The incorporation of a photochromic subunit into supramolecular polymeric systems therefore adds a potential "smart" quality for polymer manipulation. The azo moiety (-N=N-) is one of the most popular photochromic units as the trans to cis isomerization results in a large degree of spatial rearrangement. This present thesis exploits the azo group by its incorporation into complementary hydrogen bonded complexes. Hydrogen bonding acceptor groups attached to the periphery of the central azo photoswitch provided strong ...


Copper Grafted Titanium Dioxide In Hydrogels For Photocatalysts, Salem Amsaaed 2018 Atlanta University Center

Copper Grafted Titanium Dioxide In Hydrogels For Photocatalysts, Salem Amsaaed

Electronic Theses & Dissertations Collection for Atlanta University & Clark Atlanta University

This study are based on the premise that the incorporation of metal ions into nano titania-PHEMA [poly (2-hydroxyethyl methacrylate)] hydrogels would enhance the desirable properties in the photodecomposition of pollutants. The investigation are centered in the use of Cu(II) as metal ion of interest. The development of TiO2-PHEMA-Cu hydrogels was conducted, and the characterization of the materials by FT-IR, XRD and fluorescence was performed. The absorption of copper(II) from the solution was monitored by UV-Vis. The FT-IR are found too, be the most effective tool too, analyze the interaction of Cu(II) with PHEMA in the ...


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