Dr. Elizabeth Corson is a TomKat Center Postdoctoral Fellow in Sustainable Energy researching electrochemical nitrate reduction. She was a NSF Graduate Research Fellow at the University of California, Berkeley where she completed her Ph.D. in Chemical Engineering with Prof. Bryan McCloskey. She conducted her dissertation research on plasmon-enhanced electrochemical carbon dioxide reduction at the Joint Center for Artificial Photosynthesis (JCAP) at Lawrence Berkeley National Lab. Originally from Iowa, Elizabeth received her B.S. in Chemical Engineering from the Illinois Institute of Technology in Chicago.
William Tarpeh, Postdoctoral Research Mentor
William Tarpeh, Postdoctoral Faculty Sponsor
Catalytic Performance and Near-Surface X-ray Characterization of Titanium Hydride Electrodes for the Electrochemical Nitrate Reduction Reaction.
Journal of the American Chemical Society
The electrochemical nitrate reduction reaction (NO3RR) on titanium introduces significant surface reconstruction and forms titanium hydride (TiHx, 0 < x ≤ 2). With ex situ grazing-incidence X-ray diffraction (GIXRD) and X-ray absorption spectroscopy (XAS), we demonstrated near-surface TiH2 enrichment with increasing NO3RR applied potential and duration. This quantitative relationship facilitated electrochemical treatment of Ti to form TiH2/Ti electrodes for use in NO3RR, thereby decoupling hydride formation from NO3RR performance. A wide range of NO3RR activity and selectivity on TiH2/Ti electrodes between -0.4 and -1.0 VRHE was observed and analyzed with density functional theory (DFT) calculations on TiH2(111). This work underscores the importance of relating NO3RR performance with near-surface electrode structure to advance catalyst design and operation.
View details for DOI 10.1021/jacs.2c01274
View details for PubMedID 35315649
Effect of pressure and temperature on carbon dioxide reduction at a plasmonically active silver cathode
View details for DOI 10.1016/j.electacta.2021.137820
View details for Web of Science ID 000633032400003
Reduction of carbon dioxide at a plasmonically active copper-silver cathode
2020; 56 (69): 9970–73
Electrochemically deposited copper nanostructures were coated with silver to create a plasmonically active cathode for carbon dioxide (CO2) reduction. Illumination with 365 nm light, close to the peak plasmon resonance of silver, selectively enhanced 5 of the 14 typically observed copper CO2 reduction products while simultaneously suppressing hydrogen evolution. At low overpotentials, carbon monoxide was promoted in the light and at high overpotentials ethylene, methane, formate, and allyl alcohol were enhanced upon illumination; generally C1 products and C2/C3 products containing a double carbon bond were selectively promoted under illumination. Temperature-dependent product analysis in the dark showed that local heating is not the cause of these selectivity changes. While the exact plasmonic mechanism is still unknown, these results demonstrate the potential for enhancing CO2 reduction selectivity at copper electrodes using plasmonics.
View details for DOI 10.1039/d0cc03215h
View details for Web of Science ID 000563972400005
View details for PubMedID 32852004
In Situ ATR-SEIRAS of Carbon Dioxide Reduction at a Plasmonic Silver Cathode
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
2020; 142 (27): 11750–62
Illumination of a voltage-biased plasmonic Ag cathode during CO2 reduction results in a suppression of the H2 evolution reaction while enhancing CO2 reduction. This effect has been shown to be photonic rather than thermal, but the exact plasmonic mechanism is unknown. Here, we conduct an in situ ATR-SEIRAS (attenuated total reflectance-surface-enhanced infrared absorption spectroscopy) study of a sputtered thin film Ag cathode on a Ge ATR crystal in CO2-saturated 0.1 M KHCO3 over a range of potentials under both dark and illuminated (365 nm, 125 mW cm-2) conditions to elucidate the nature of this plasmonic enhancement. We find that the onset potential of CO2 reduction to adsorbed CO on the Ag surface is -0.25 VRHE and is identical in the light and the dark. As the production of gaseous CO is detected in the light near this onset potential but is not observed in the dark until -0.5 VRHE, we conclude that the light must be assisting the desorption of CO from the surface. Furthermore, the HCO3- wavenumber and peak area increase immediately upon illumination, precluding a thermal effect. We propose that the enhanced local electric field that results from the localized surface plasmon resonance (LSPR) is strengthening the HCO3- bond, further increasing the local pH. This would account for the decrease in H2 formation and increase the CO2 reduction products in the light.
View details for DOI 10.1021/jacs.0c01953
View details for Web of Science ID 000550639000019
View details for PubMedID 32469508
Important Considerations in Plasmon-Enhanced Electrochemical Conversion at Voltage-Biased Electrodes
2020; 23 (3): 100911
In this perspective we compare plasmon-enhanced electrochemical conversion (PEEC) with photoelectrochemistry (PEC). PEEC is the oxidation or reduction of a reactant at the illuminated surface of a plasmonic metal (or other conductive material) while a potential bias is applied. PEC uses solar light to generate photoexcited electron-hole pairs to drive an electrochemical reaction at a biased or unbiased semiconductor photoelectrode. The mechanism of photoexcitation of charge carriers is different between PEEC and PEC. Here we explore how this difference affects the response of PEEC and PEC systems to changes in light, temperature, and surface morphology of the photoelectrode.
View details for DOI 10.1016/j.isci.2020.100911
View details for Web of Science ID 000528358900034
View details for PubMedID 32113155
View details for PubMedCentralID PMC7047194
Directing Selectivity of Electrochemical Carbon Dioxide Reduction Using Plasmonics
ACS ENERGY LETTERS
2019; 4 (5): 1098–1105
View details for DOI 10.1021/acsenergylett.9b00515
View details for Web of Science ID 000468015600017
Surface-Plasmon-Assisted Photoelectrochemical Reduction of CO2 and NO3- on Nanostructured Silver Electrodes
ADVANCED ENERGY MATERIALS
2018; 8 (22)
View details for DOI 10.1002/aenm.201800363
View details for Web of Science ID 000440805400008
A temperature-controlled photoelectrochemical cell for quantitative product analysis
REVIEW OF SCIENTIFIC INSTRUMENTS
2018; 89 (5): 055112
In this study, we describe the design and operation of a temperature-controlled photoelectrochemical cell for analysis of gaseous and liquid products formed at an illuminated working electrode. This cell is specifically designed to quantitatively analyze photoelectrochemical processes that yield multiple gas and liquid products at low current densities and exhibit limiting reactant concentrations that prevent these processes from being studied in traditional single chamber electrolytic cells. The geometry of the cell presented in this paper enables front-illumination of the photoelectrode and maximizes the electrode surface area to electrolyte volume ratio to increase liquid product concentration and hence enhances ex situ spectroscopic sensitivity toward them. Gas is bubbled through the electrolyte in the working electrode chamber during operation to maintain a saturated reactant concentration and to continuously mix the electrolyte. Gaseous products are detected by an in-line gas chromatograph, and liquid products are analyzed ex situ by nuclear magnetic resonance. Cell performance was validated by examining carbon dioxide reduction on a silver foil electrode, showing comparable results both to those reported in the literature and identical experiments performed in a standard parallel-electrode electrochemical cell. To demonstrate a photoelectrochemical application of the cell, CO2 reduction experiments were carried out on a plasmonic nanostructured silver photocathode and showed different product distributions under dark and illuminated conditions.
View details for DOI 10.1063/1.5024802
View details for Web of Science ID 000433962700085
View details for PubMedID 29864888
CO2 capture by sub-ambient membrane operation
ELSEVIER SCIENCE BV. 2013: 993–1003
View details for DOI 10.1016/j.egypro.2013.05.195
View details for Web of Science ID 000345500501026