Rational Design of Solid-Electrolyte Interfaces for Biofuel Production and Energy Storage
EMSL Project ID
49277
Abstract
Structure-activity relationships determined from molecular-level investigation of mesoscale assemblies of well-defined clusters are critical to the rational development of improved devices for heterogeneous biofuel production and catalytic conversion as well as energy storage. Currently, the rational design of cathode and anode materials with tunable electronic properties that match the highest occupied molecular orbital (HOMO) and lowest unoccupied molecular orbital (LUMO) levels of electrolytes is one of the major limiting factors in this area of research. A combined theoretical and experimental approach will be employed to model, prepare, and characterize the properties of arrays of well-defined molecular clusters on surfaces for application in heterogeneous catalytic biofuel production and energy storage. Specifically, soft landing of mass selected ions at EMSL will provide atomically precise control over the size, charge state, and composition of Keggin anions supported on conductive electrodes such as metal oxide layers, graphene, and carbon nanotube paper. Mesocale assemblies of clusters will be examined in the absence of contaminants and counterions using spatially resolved electrochemical cell microscopy. Species exhibiting superior performance will be fully characterized using the cutting-edge microscopy and spectroscopy tools available at EMSL. Theoretical calculations will be employed to understand how interaction with the electrode surface and neighboring clusters determines the redox properties and stability of clusters in extended arrays. This multidisciplinary project involving researchers from around the world is relevant to the EMSL science theme of Energy Materials and Processes (EMP) including 1) Physical and chemical properties of interfaces relevant to degradation of biomass; 2) Dynamic and emergent processes occurring at solvent-mediated interfaces.
Project Details
Project type
Large-Scale EMSL Research
Start Date
2016-10-01
End Date
2018-09-30
Status
Closed
Released Data Link
Team
Principal Investigator
Co-Investigator(s)
Team Members
Related Publications
Prabhakaran V, BL Mehdi, JJ Ditto, MH Engelhard, B Wang, KDD Gunaratne, DC Johnson, ND Browning, GE Johnson, and J Laskin. 2016. "Rational Design of Efficient Electrode-Electrolyte Interfaces for Solid-State Energy Storage Using Ion Soft-Landing." Nature Communications 7:Article No. 11399. doi:10.1038/ncomms11399
Prabhakaran V, GE Johnson, B Wang, and J Laskin. 2016. "In situ solid-state electrochemistry of mass selected ions at well-defined electrode-electrolyte interfaces." Proceedings of the National Academy of Sciences of the United States of America 113(47):13324-13329. doi:10.1073/pnas.1608730113
Prabhakaran V., Z. Lang, A. Clotet, J.M. Poblet, G.E. Johnson, and J. Laskin. 2019. "Controlling the Activity and Stability of Electrochemical Interfaces Using Atom-by-Atom Metal Substitution of Redox Species." ACS Nano 13, no. 1:458-466. PNNL-SA-132145. doi:10.1021/acsnano.8b06813
Su P., V. Prabhakaran, G.E. Johnson, and J. Laskin. 2018. "In situ Infrared Spectroelectrochemistry for Understanding Structural Transformations of Precisely-Defined Ions at Electrochemical Interfaces." Analytical Chemistry 90, no. 18:10935-10942. PNNL-SA-137370. doi:10.1021/acs.analchem.8b02440