A5037264129- Catalytic Processes in Materials Science
- Catalysis and Oxidation Reactions
- Advanced Chemical Physics Studies
- Ammonia Synthesis and Nitrogen Reduction
- Electrocatalysts for Energy Conversion
- Zeolite Catalysis and Synthesis
- Atmospheric chemistry and aerosols
- Atmospheric Ozone and Climate
- Ionic liquids properties and applications
- Plasma Applications and Diagnostics
- Gas Sensing Nanomaterials and Sensors
- Machine Learning in Materials Science
- nanoparticles nucleation surface interactions
- Inorganic and Organometallic Chemistry
- Metal-Organic Frameworks: Synthesis and Applications
- Catalysis and Hydrodesulfurization Studies
- Carbon dioxide utilization in catalysis
- Radioactive element chemistry and processing
- Molecular Junctions and Nanostructures
- Phase Equilibria and Thermodynamics
- CO2 Reduction Techniques and Catalysts
- Advanced Data Storage Technologies
- Nanomaterials for catalytic reactions
- Industrial Gas Emission Control
- Spectroscopy and Laser Applications
University of Notre Dame
2016-2025
Notre Dame of Dadiangas University
2017-2023
Dutch Institute for Fundamental Energy Research
2021
Eindhoven University of Technology
2021
Purdue University West Lafayette
2014-2021
Klinikum im Friedrichshain
2015
History of Science Society
2014
University of Illinois Urbana-Champaign
1997-2013
Freeport-McMoRan (United States)
2013
Urbana University
2011
Amino acid ionic liquid trihexyl(tetradecyl)phosphonium methioninate [P66614][Met] and prolinate [P66614][Pro] absorb CO2 in nearly 1:1 stoichiometry, surpassing by up to a factor of 2 the capture efficiency previously reported aqueous amine absorbants for CO2. Room temperature isotherms are obtained barometric measurements an accurately calibrated stirred cell, product identity is confirmed using situ IR. Density functional theory (DFT) calculations support reaction stoichiometry predict...
Copper ions exchanged into zeolites are active for the selective catalytic reduction (SCR) of nitrogen oxides (NO x ) with ammonia (NH3), but low-temperature rate dependence on copper (Cu) volumetric density is inconsistent reaction at single sites. We combine steady-state and transient kinetic measurements, x-ray absorption spectroscopy, first-principles calculations to demonstrate that under conditions, mobilized Cu can travel through zeolite windows form ion pairs participate in an oxygen...
The relationships among the macroscopic compositional parameters of a Cu-exchanged SSZ-13 zeolite catalyst, types and numbers Cu active sites, activity for selective catalytic reduction (SCR) NOx with NH3 are established through experimental interrogation computational analysis materials across catalyst composition space. Density functional theory, stochastic models, characterizations demonstrate that within synthesis protocols applied here Si:Al ratios, volumetric density six-membered-rings...
Aluminas and their surface chemistry play a vital role in many areas of modern technology. The behavior adsorbed water is particularly important poorly understood. Simulations hydrated alpha-alumina (0001) surfaces with ab initio molecular dynamics elucidate aspects this problem, especially the complex dissociation related reactions. At low coverage, free energy profiles established that molecularly metastable dissociates readily, even absence defects, by kinetically preferred pathway....
Abstract Plasma catalysis is gaining increasing interest for various gas conversion applications, such as CO 2 into value-added chemicals and fuels, CH 4 activation hydrogen, higher hydrocarbons or oxygenates, NH 3 synthesis. Other applications are already more established, air pollution control, e.g. volatile organic compound remediation, particulate matter NO x removal. In addition, plasma also very promising catalyst synthesis treatment. clearly has benefits over ‘conventional’ catalysis,...
Abstract Mixed halide hybrid perovskites, CH 3 NH Pb(I 1− x Br ) , represent good candidates for low-cost, high efficiency photovoltaic, and light-emitting devices. Their band gaps can be tuned from 1.6 to 2.3 eV, by changing the anion identity. Unfortunately, mixed perovskites undergo phase separation under illumination. This leads iodide- bromide-rich domains along with corresponding changes material’s optical/electrical response. Here, using combined spectroscopic measurements theoretical...
The discovery of materials that combine selectively, controllably, and reversibly with CO2 is a key challenge for realizing practical carbon capture from flue gas other point sources. We report the design ionic liquids (ILs) properties tailored to this separation problem. Atomistic simulations predict suitably substituted aprotic heterocyclic anions, or "AHAs," bind energies can be controlled over wide range suitable separations. Further, unlike all previously known CO2-binding ILs, AHA IL...
Mixed halide lead perovskites (e.g., CH3NH3PbBrxI3–x) undergo phase segregation creating iodide-rich and bromide-rich domains when subjected to visible irradiation. This intriguing aspect of ion movement in mixed films is now being tracked through excited-state behavior using emission transient absorption spectroscopy tools. These experiments have allowed us establish the time scale with which such separation occurs under laser irradiation (405 nm, 25 mW/cm2 1.7 W/cm2) as well dark recovery....
Operando X-ray absorption experiments and density functional theory (DFT) calculations are reported that elucidate the role of copper redox chemistry in selective catalytic reduction (SCR) NO over Cu-exchanged SSZ-13. Catalysts prepared to contain only isolated, exchanged Cu(II) ions evidence both Cu(I) under standard SCR conditions at 473 K. Reactant cutoff show NH3 together necessary for Cu(I). DFT NO-assisted dissociation is energetically favorable accounts observed reduction. The predict...
We report a plane-wave, supercell density functional theory (DFT) investigation of the adsorption and dissociation water on (111) surfaces Cu, Au, Pt, Pd, Ni, five metals potential interest in context gas shift (WGS) catalysis. Binding energies, preferred sites, configurations for H2O its products (OH, H, O) are determined all metals, as minimum energy paths (MEPs) activation energies H−OH O−H dissociation. Results compared with diverse computational literature over these metals. Both steps...
Ionic liquids (ILs) with aprotic heterocyclic anions, or AHAs, can bind CO2 reaction enthalpies that are suitable for gas separations and without suffering large viscosity increases. In the present work, we have synthesized ILs bearing an alkyl-phosphonium cation indazolide, imidazolide, pyrrolide, pyrazolide triazolide-based anions span a wide range of predicted CO2. Each AHA-based IL was characterized by NMR spectroscopy their physical properties (viscosity, glass transition, thermal...
Abstract Substituted iminodiacetic acids of the general formula RN(CH 2 ‐COOH) have been synthesized and their coordination tendency with 12 different metal cations investigated. The groups R 13 complexing agents are tabulated on page 1147–1148 this paper. Most them carry donor atoms in such a position, that third chelate ring may be formed when anion acid combines metal. It could proved oxygen, sulfur nitrogen atom aliphatically bound HO, CH 3 O, HS, S, (−) NH , OOC, H NCO actually...
Chemical kinetic modeling in heterogeneous catalysis is advancing its ability to provide qualitatively or even quantitatively accurate prediction of real-world behavior because new advances the physical and chemical representations catalytic systems, estimation relevant parameters, capabilities modeling. This Perspective describes current trends future areas advancement modeling, simulation, parameter estimation: ranging from elementary step calculations multiscale role advanced statistical...
We combine experiment and theory to investigate the cooperation or competition between organic inorganic structure-directing agents (SDAs) for occupancy within microporous voids of chabazite (CHA) zeolites rationalize effects SDA siting on biasing framework Al arrangement (Al–O(−Si–O)x–Al, x = 1–3) among CHA essentially fixed composition (Si/Al 15). crystallized using mixtures TMAda+ Na+ contain one occluded per cage co-occluded in an amount linearly proportional number 6-MR paired sites,...
We present a more detailed account of our recently reported [Hass, K. C.; Schneider, W. F.; Curioni, A.; Andreoni, Science 1998, 282, 265] first-principles molecular dynamics investigation the static and dynamical behavior adsorbed H2O on α-Al2O3 (0001). Al-terminated surfaces with varying degrees coverage are modeled using large periodic supercells. A predicted relaxation clean surface agrees well previous density functional theory calculations. Both dissociative adsorption modes...
The reactivity of heterogeneous metal catalysts can be a strong function the coverage adsorbates. For example, Pt-catalyzed NO oxidation to NO2 requires high concentrations chemisorbed (surface-bound) O, but development surface oxides is detrimental reaction kinetics. Quantifying structures, properties, and especially conditions that produce various adsorbate coverages essential developing qualitatively quantitatively correct models reactivity. In this work, we examine these ideas in context...