The Goldsmith Lab performs interdisciplinary research using state-of-the-art electronic-structure theory and molecular simulation, as well as data analytics tools,
to understand catalysts and materials under realistic conditions, and to help generate a platform for their design and use in sustainable fuel production, energy storage, and pollution reduction.
See the posters below for more information about our current research thrusts and recent research highlights.
Catalysts and materials for a sustainable future
Click the poster for info about some of our research group thrusts, namely: (i) The investigation of amorphous materials for their use as catalysts and supports for alternative fuel production and pollution reduction;
(ii) Understanding nanoclusters and atomically dispersed metal-complexes supported by metal oxides for natural gas conversion;
(iii) Homogeneous organometallic complexes as C-H activation catalysts; and (iv) Using machine learning to accelerate discovery of catalysts and materials. We also have collaborative electrocatalysis projects for flow batteries and wastewater remediation.
Data analytics to discover materials insights
As part of the Novel Materials Discovery Laboratory, a major goal is to develop data analytics tools to uncover scientific insights from large materials repositories.
Dr. Goldsmith's group is using subgroup discovery to find and describe interesting local patterns in materials-science data.
While at the FHI Theory Department and in collaboration with Dr. Boley, two illustrative examples were considered to: (1) discover interpretable models that classify the octet binary
materials as either zincblende or rocksalt, and (2) elucidate structure-property relationships of gold clusters in the gas phase. Read here and here.
Understanding gold clusters in the gas phase
With the L. M. Ghiringhelli Group, we are examining the (meta)stable structures of gold clusters present at finite temperature using van der Waals (vdW) corrected density-functional theory and replica-exchange ab initio molecular dynamics. Inclusion of many-body vdW interactions is needed for predicting accurate isomer energetics, and its importance grows as the cluster size increases. Temperature effects are observed to typically stabilize three-dimensional structures over planar structures at finite temperature.
Gold cluster structures are assigned using far-IR spectroscopy obtained by the Fieleke Group and theoretical predictions.
Synthesis and characterization of Cu-hydride clusters
Copper hydrides have attracted interest for their ability to catalyze the reduction of unsaturated carbonyls, electron deficient alkenes, alkynes, and even CO2. Here, atomically precise copper hydride clusters [Cu14H12(phen)6(PPh3)4]Cl]2, [Cu18H17(PPh3)10]Cl, and [Cu25H22(PPh3)12]Cl were synthesized and characterized in collaboration with the Hayton group.
Most remarkably, the [Cu25H22(PPh3)12]Cl is the first copper nanocluster with metallic copper character. Generally, these homogeneous copper clusters represent an opportunity to study the reactivity of Cu nanoclusters, particularly for CO2 reduction.
Read here and here.
Route to renewable high-density fuels
Together with Benjamin Harvey and colleagues at China Lake (US Navy, Naval Air Warfare Center Weapons Division), we demonstrated that linalool, a linear terpene alcohol, can be selectively converted by ruthenium metathesis catalysts under solvent-free conditions to 1-methyl-cyclopent-2-enol and isobutylene in quantitative yield. Dehydration of the alcohol under mild conditions followed by low-temperature thermal dimerization yields methylcyclopentadiene dimer,
which can be readily converted into a high-density fuel.
Single atom formation under reaction conditions
Highly active and selective single atom catalysts can spontaneously form from their nanocluster hosts under reaction conditions.
In collaboration with the Wei-Xue Li Group, we conducted an ab initio thermodynamics study to understand the effects of CO and NO reactants on the disintegration of
metal-oxide supported Rh, Pd, and Pt nanoparticles into single atom complexes. Read article here. Ongoing work is being performed to gain a deeper understanding of the interplay between single atoms and nanoclusters under catalytic conditions.