Computational Chemistry and Materials Group
Tackling challenges in making manufacturing of chemicals and fuels to have low-carbon emissions and be sustainable
Past Research
Electrochemical Water Splitting
Electrochemical hydrogen generation proceeds in tandem with oxygen evolution from water. The latter is more difficult and limits the former. How can we make it proceed faster?
Plasmonic Heterogeneous Catalysis
Reactions that occur slowly can be accelerated by light and ultra small nano-sized metal particles. What cases can this new technology be applied and is it competitive to thermally driven processes?
Quantum Mechanical Embedding
Computational cost of simulations is proportional to the size of the chemical system. Partitioning schemes make such simulations more manageable. How can this approach be made more accurate and systematic?
Ongoing Research
Electrochemical CO2 Reduction
Capture and valorization of carbon dioxide are the goals. Electricity makes the latter possible, but can it be made more efficient?
Aqueous Phase CO2 Sequestration
Sequestration of carbon dioxide can also be done using ocean water. How can we make this possible beyond laboratory scale?
Electrified NH3 Synthesis
Ammonia is one of the most important agricultural chemicals and also being considered for hydrogen storage and transport. How can it be produced more sustainably?
Elcetrochemical Water Splitting
We identified key species and pathways in the electrochemical oxygen evolution on doped nickel-based oxyhydroxides. We were able to codify doping strategies to improve the aqueous electrocatalytic oxygen evolving activity of this material, which we based on two central mechanistic features of its efficient water oxidation. We thus were able to demonstrate a mechanism-oriented design principle in the development of oxygen evolution catalysts.
Plasmonic Heterogeneous Catalysis
Our simulations furnished physical understanding and put forth reinterpretation of the effect of local surface plasmon resonances on heterogeneous catalysis. We addressed the kinetics of surface chemical reactions while considering electronically excited states. We concluded that plasmon resonances may lead to oscillating-dipole-induced local surface excitations making low-barrier, excited-state chemical reaction pathways available on the surface of plasmonic metals. This is in contrast to the energetic carrier injection and photothermal mechanism usually invoked to explain these phenomena.
Quantum Mechanical Embedding
Density functional embedding theory (DFET) enables one to perform accurate but computationally expensive quantum mechanical calculations on chemical systems through fragmentation. We introduced an extension of DFET to covalent and ionic compounds, where the original DFET method had been shown to be inadequate. The goal is to perform accurate embedded correlated wavefunction calculations and evaluate the absorption and emission behavior of, for example, hybrid organic-inorganic systems. In such systems, the fundamental electronic transitions usually are localized between the organic chromophore and the nearest transition metal cation of the inorganic component of the semiconductor, making such systems suitable for the localized description of excited states (excitons).
