Brian B. Laird
3189A ISB (CDS1)
1567 Irving Hill Rd
Lawrence, KS 66045
1567 Irving Hill Rd
Lawrence, KS 66045
Gray-Little Hall, room #3189A
Theoretical and computational chemistry The ultimate goal of materials chemistry is the understanding of the macroscopic properties of materials in terms of the microscopic molecular interactions. This is a common theme in all of the natural sciences. The differences between the various scientific disciplines (chemistry, biology, physics, materials sciences, etc.) often disappear as the traditional macroscopic phenomenology is replaced by a more molecular approach. At present, most of what is known about the chemical and physical properties of materials is still largely empirical, especially in the case of amorphous, macromolecular or interfacial systems. The development of a microscopic theoretical description for a variety of such complex systems is the primary focus of our research. Several representative projects are listed below. They are all projects in which great advantage will be gained by exploiting the natural symbiosis between analytical and computer-simulation techniques.
1) Crystal-melt interfaces of complex systems: The structure and dynamics of an interface between a crystal and its melt are of paramount importance in studies of crystal growth and nucleation. Experimental study is difficult as such an interface lies sandwiched between two dense phases, and experimental data is lacking, increasing the value of computer simulations to the study of such systems. Most previous studies have involved simple, one-component model systems. Using molecular-dynamics computer simulations and classical density-functional theories, we are currently concentrating on more complex systems such as multicomponent systems (for example, alloys) and molecular systems, such as succinonitrile and pivalic acid, for which extensive data relating to crystal growth and interfacial properties have been collected from microgravity experiments aboard the Space Shuttle.
2) Fundamental Investigations into Gas Expanded Solvent Media for Green Chemistry: This project is part of the research mission of the newly formed Center for Environmentally Beneficial Catalysis, an NSF funded Engineering Research Center headquartered at the University of Kansas. In this project we seek a fundamental understanding, through molecular simulation, of the thermodynamics, transport properties and molecular-level structure of gas-expanded solvent systems - a new class of solvent media in which a traditional industrial organic solvents, such as acetonitrile, are expanded by an order of magnitude in volume (without phase separation) by 2. In these new media, dense CO2 significantly replaces the traditional solvent (up to 80% by volume), such that the retained solvent maintains the catalyst solubility and other advantages provided by the traditional solvent (for example, rate enhancement due to polarity). Further, solubility is increased for O2 Thus, gas-expanded solvents combine the environmentally beneficial nature of supercritical (sc) solvents (such as sc-CO2) and the advantages of traditional solvents in an optimal manner, thereby deriving many reaction and environmental/economic advantages not possible with either the neat solvent or sc-fluid. Due to their novelty, these gas-expanded solvent systems have received little attention from the molecular simulation community. To complement the current experimental effort, this project represents a parallel program of modeling efforts to gain a fundamental molecular-level understanding of the physico-chemical properties of gas-expanded solvents, with particular attention to those systems utilizing CO2 as the expansion gas. provide guidance to the experimental program to rationally chose optimum solvents provide guidance to the experimental program in the optimization of catalyst performance in expanded media.
3) Algorithms for Molecular Modeling: Molecular-dynamics computer simulation has become an invaluable tool in chemistry, chemical engineering, physics, materials science and biology; however, its uses are still limited by the relatively small system sizes and short time scales that can be simulated at present. Progress in this area therefore comes from advances in computer technology and in the development of efficient and stable algorithms. The latter is the goal of an ongoing multidisciplinary project in collaboration with Prof. Ben Leimkuhler, an applied mathematician at the University of Leicester.
- Computational materials science
- computational chemistry
- solid- liquid interfaces
- algorithms for molecular simulation
- phase transitions
- properties of glasses and supercooled liquids
- general liquid-state theory (equilibrium and non-equilibrium)
- inhomogeneous fluids
- physical chemistry
- general chemistry
- statistical mechanics
- quantum mechanics
Selected Publications —
Radetic, T., E Johnson, David Olmstead, Yang Yang, Brian B Laird, Mark D Asta, and Ulrich Dahmen. “Step-Controlled Brownian Motion of Nano-Sized Liquid Pb Inclusions in a Solid Al Matrix.” Journal Articles. Acta Materialia 141 (August 19, 2017): 427–33. https://doi.org/10.1016/j.actamat.2017.09.040.
Wang, Zhenxing, Jesse L Kern, and Brian B Laird. “The Phase Equilibrium, Transport and Local Liquid Structure of the Methanol/Water/Ethylene Ternary System: A Molecular Simulation Study.” Journal Articles. Fluid Phase Equilibria 429 (November 15, 2016): 275-280Gas-expanded liquids have received significant interest as catalytic reaction media. While most GXL studies involve CO2 as the expansion gas, there is growing interest in non-CO2 based GXLs, especially when the expansion gas is also a reactant. In this work, we focus on ethylene as an expansion gas, motivated by recent experimental studies on the catalytic epoxidation of ethylene using ethylene-expanded methanol/H2O2/water mixtures within metal doped silica mesopores. Reported simulation studies on GXLs, even for bulk properties, have been primarily limited to single-component or binary systems. Here we extend the use of simulation to the study of a bulk ternary GXL system-namely, ethylene-expanded mixtures of methanol and water mixtures. We investigate the phase behavior and transport properties in the liquid phase with respect to temperature, pressure and water content. The model force fields are validated by comparing compositions and transport properties to existing experiments. In addition, we study local liquid solvation structure as a function of composition.
Wang, Zhenxing, David Olmsted, Mark D Asta `, and Brian B Laird. “Electric Potential Calculation in Molecular Simulation of Electric Double Layer Capacitors.” Journal Articles. Journal of Physics: Condensed Matter 28, no. 46 (August 14, 2016): 464006. https://doi.org/10.1088/0953-8984/28/46/464006.
Palafox-Hernandez, J. Pablo, and Brian B. Laird. “Orientation Dependence of Heterogeneous Nucleation at the Cu-Pb Solid-Liquid Interface.” Journal Articles. Journal of Chemical Physics 145 (August 23, 2016): 211914.
Kern, Jesse L, Thomas J Flynn, Zhenxing Wang, Ward H Thompson, and Brian B Laird. “Molecular Simulation of Ethylene-Expanded Methanol: Phase Behavior, Structure, and Transport Properties.” Journal Articles. Fluid Phase Equilibria 411 (March 15, 2016): 81–87. http://www.sciencedirect.com/science/article/pii/S0378381215302636.
Davidchack, Ruslan L, Brian B Laird, and Roland Roth. “Hard Spheres at a Planar Hard Wall: Simulations and Density Functional Theory.” Journal Articles. Condensed Matter Physics 19, no. 2 (February 2016): 23001:1-10.
Steenbergen, Krista G, Jesse Kern, Zhenxing Wang, Ward H Thompson, and Brian B Laird. “Tunability of Gas-Expanded Liquids under Confinement: Phase Equilibrium and Transport Properties of Ethylene-Expanded Methanol in Mesoporous Silica.” Journal Articles. Journal of Physical Chemistry C 120 (February 8, 2016): 510–19. https://doi.org/10.1021/acs.jpcc.5b12750.
Davidchack, Ruslan L, Brian B Laird, and Roland Roth. “Parameterising the Surface Free Energy and Excess Adsorption of a Hard-Sphere Fluid at a Planar Hard Wall.” Journal Articles. Molecular Physics 113, no. 9–10 (2015): 1091–96. https://doi.org/10.1080/00268976.2014.986240.
Wang, Zhenxing, Yang Yang, David L Olmsted, Mark Asta, and Brian B Laird. “Evaluation of the Constant Potential Method in Simulating Electric Double-Layer Capacitors (Feature Article).” Journal Articles. Journal of Chemical Physics 184102 (October 10, 2014): 184192. https://doi.org/10.1063 1.4899176.
Yang, Yang, and Brian B Laird. “Thermodynamics and Intrinsic Structure of the Al–Pb Liquid–Liquid Interface: A Molecular Dynamics Simulation Study.” Journal Articles. Journal of Physical Chemistry B 118, no. 28 (June 17, 2014): 8373–8380. https://doi.org/10.1021/jp5019313.
Kern, Jesse L, and Brian B Laird. “Calculation of the Interfacial Free Energy of a Binary Hard-Sphere Fluid at a Planar Hard Wall.” Journal Articles. Journal of Chemical Physics 140 (January 8, 2014): 024703. https://doi.org/10.1063/1.4858433.
Grants & Other Funded Activity —
Thermodynamics and Structure of Chemically Heterogeneous Solid-Liquid Interfaces. National Science Foundation. $420000.00. Submitted 9/30/2014 (12/1/2015 - 11/30/2019). Federal. Status: Funded
NSMDS: Sustainable chemical innovations by an integrated design approach. CHE-1339661. National Science Foundation, Environmental Protection Agency. $4400000.00. Submitted 3/18/2013 (10/1/2013 - 9/30/2017). Federal. Status: Funded
Energy Frontier Research Center on Molecularly Assembled Material Architectures for Solar Energy Production, Storage, and Carbon Capture. Department of Energy. $750000.00. (8/1/2009 - 7/31/2015). Federal. Status: Funded. $750,000 out of $11,500,000 for center for each of the 10 principal and co-principal investigators, including B. Laird