The total reorganization energy, λ, for interfacial electron transfer, ET, from a conductive electrode to redox-active molecules at fixed positions within the electric double layer, EDL, has been determined experimentally. Conductive indium–tin-oxide (ITO, In2O3:Sn) mesoporous films were functionalized with 4-[N,N-di(p-tolyl)-amino]benzylphosphonic … Read more

A new approach is described for the preparation of water oxidation photoanodes in a Dye-Sensitized Photoelectrosynthesis Cell (DSPEC) for water splitting. It is based on a chromophore (C) – catalyst (Cat) assembly prepared by a self-assembled bilayer (SAB) on a … Read more

Congratulations to Eric Assaf, 3rd year graduate student in the Miller group and member of the AMPED EFRC Catalysis Team, who has been accepted to the editorial board of the DOE EFRC quarterly newsletter Frontiers in Energy Research. This newsletter … Read more

Molecular excited states at conductive and semiconductive interfaces were found to transfer an electron to the oxide (injection) or accept an electron from the oxide (hole transfer). The direction of this electron transfer was determined by the metal oxide electronic … Read more

In the development of photoelectrochemical cells for water splitting or CO2 reduction, a major challenge is O2 evolution at photoelectrodes that, in behavior, mimic photosystem II. At an appropriate semiconductor electrode, a water oxidation catalyst must be integrated with a visible … Read more

A study of SnO2/TiO2 core/shell films was undertaken to investigate the influence of shell thickness and post deposition sintering on electron localization and transport properties. Electrochemical reduction of the materials resulted in the appearance of a broad visible –near IR … Read more

The atomic layer deposition of tetrakisdimethylamidotin(IV) and water on mesoporous thin films of nanocrystalline anatase TiO2, rutile SnO2, and rutile TiO2 was investigated. For all deposition conditions tested, highly oxygen deficient coatings were created, and purge time and temperature were … Read more

The reorganization energy, λ, for interfacial electron transfer (ET) and for proton-coupled electron transfer (PCET) between a water oxidation catalyst and a conductive In2O3:Sn (ITO) oxide were extracted from kinetic data by application of Marcus–Gerischer theory. Specifically, light excitation of … Read more

The AMPED EFRC just achieved 3 major milestones in publications: 300th paper – complete list here h-Index of 62 More than 17,000 citations Major congratulations to all current and former Center members on your very impressive scientific accomplishments.    

Excited electron transfer across semiconductor-molecule heterogeneous interfaces is central to various future electronic and optoelectronic devices. At the same time, first-principles modeling of such dynamical processes remains as a great challenge in theoretical chemistry and condensed matter physics for developing … Read more

In artificial photosynthesis, the sun drives water splitting into H2 and O2 or converts CO2 into a useful form of carbon. In most schemes, water oxidation is typically the limiting half-reaction. Here, we introduce a molecular approach to the design … Read more

A comprehensive mechanistic study of electrocatalytic CO2 reduction by ruthenium 2,2′:6′,2″-terpyridine (tpy) pyridyl-carbene catalysts reveals the importance of stereochemical control to locate the strongly donating N-heterocyclic carbene ligand trans to the site of CO2 activation.  Computational studies were undertaken to … Read more

AMPED EFRC graduate student Matthew Brady has been selected to receive a U.S. Department of Energy (DOE) Office of Science Graduate Student Research (SCGSR) award.  Matt’s selection is in recognition of his outstanding academic accomplishments and the merit of the research … Read more

This paper describes the preparation and characterization of a photocathode assembly for CO2 reduction to CO in 0.1M LiClO4 acetonitrile. The assembly was formed on 1.0 µm thick mesoporous films of NiO using a layer-by-layer procedure based on Zr(IV)-phosphonate bridging … Read more

AMPED EFRC graduate student Leah Bowers is one of five 2019 recipients of the UNC University Award for the Advancement of Women. The award recognizes people on campus who have elevated the status of women, helped improve campus policies and … Read more