Engineering topics
Goddard, William A.
Publications and source records attributed to Goddard, William A..
Addressing amorphization and transgranular fracture of B 4 C through Si doping and TiB 2 microparticle reinforcing
Over the last two decades, many studies have contributed to improving our understanding of the brittle failure mechanisms of boron carbide and provided a road map for inhibiting the underlying mechanisms and improving the mechanical response of boron carbide. This paper provides a review of the design and processing approaches utilized to address the amorphization and transgranular fracture of boron carbide, which are mainly based on what we have found through 9 years of work in the field of boron carbides as armor ceramics.
Predictions of Chemical Shifts for Reactive Intermediates in CO 2 Reduction under Operando Conditions
Not provided.
Design of robust 2,2′-bipyridine ligand linkers for the stable immobilization of molecular catalysts on silicon(111) surfaces
The attachment of the 2,2′-bipyridine (bpy) moieties to the surface of planar silicon(111) (photo)electrodes was investigated using ab initio simulations performed on a cluster model for methyl-terminated silicon.
Coarse-grained force-field for large scale molecular dynamics simulations of polyacrylamide and polyacrylamide-gels based on quantum mechanics
Developing a coarse-grained force field for polyacrylamide based on quantum mechanics equation of state.
Oxygen evolution reaction over catalytic single-site Co in a well-defined brookite TiO 2 nanorod surface
Efficient electrocatalysts for the oxygen evolution reaction (OER) are paramount to the development of electrochemical devices for clean energy and fuel conversion. However, the structural complexity of heterogeneous electrocatalysts makes it a great challenge to elucidate the surface catalytic sites and OER mechanisms. Here, we report that catalytic single-site Co in a well-defined brookite TiO 2 nanorod (210) surface (Co-TiO 2 ) presents turnover frequencies that are among the highest for Co-based heterogeneous catalysts reported to date, reaching 6.6 ± 1.2 and 181.4 ± 28 s -1 at 300 and 400 mV overpotentials, respectively. Based on grand canonical quantum mechanics calculations and the single-site Co atomic structure validated by in situ and ex situ spectroscopic probes, we have established a full description of the catalytic reaction kinetics for Co-TiO 2 as a function of applied potential, revealing an adsorbate evolution mechanism for the OER. The computationally predicted Tafel slope and turnover frequencies exhibit exceedingly good agreement with experiment.
Tailoring a Three-Phase Microenvironment for High-Performance Oxygen Reduction Reaction in Proton Exchange Membrane Fuel Cells
Despite tremendous progress in catalyst development for rate-limiting cathodic oxygen reduction reaction (ORR), reducing Pt usage while meeting performance requirements in practical proton exchange membrane fuel cells (PEMFCs) remains a challenge. The ORR in PEMFCs occurs at a catalyst–electrolyte–gas three-phase interface. A desirable interface should exhibit highly active and available catalytic sites, as well as allow efficient oxygen and proton feeding to the catalytic sites and timely removal of water to avoid interface flooding. In this work, we report the design of a three-phase microenvironment in PEFMCs, showing that carbon surface chemistry can be tuned to modulate its interaction with the ionomers and create favorable transport paths for rapid delivery of both reactants and products. With such an elaborate interfacial design, for the first time we have demonstrated PEMFCs with all key ORR catalyst performance metrics, including mass activity, rated power, and durability, surpassing the US Department of Energy targets.
A coarse-grain force field based on quantum mechanics (CGq FF) for molecular dynamics simulation of poly(ethylene glycol)- block -poly(ε-caprolactone) (PEG- b -PCL) micelles
In order to provide the means to predict from molecular dynamics (MD) simulations the structures of copolymer-based micelles in solution, we developed coarse grain force field (CGq FF) parameters for poly(ethylene glycol) (PEG) and for poly(ε-caprolactone) (PCL). A key advance here is the use of quantum mechanics to train the parameters describing the non-bonded (NB) interactions between the CG beads. The functional forms are the same as the MARTINI CG FF so standard MD codes can be used. Our CGq FF describes well the experimentally observed properties for the polymer–air and polymer–water interfaces, indicating the accuracy of the NB interactions. Additionally, the structural properties (density, radius of gyration ( R g ), and end-to-end distance ( h )) match both experiment and all atom (AA) simulations. We illustrate the application of this CGq FF by following the formation of a spherical micelle from 250 chains of PEG 23 - b -PCL 9 diblock copolymer, each block with molecular weight of 1000 Daltons (10 500 beads, corresponding to 123 250 atoms), in a water box with 119 139 water beads (426 553 water molecules).