Inverse Design, Development and Characterization of Catalytic Adsorbates at Semiconductor/Liquid Interfaces
Abstract
The development of efficient catalytic materials for selective CO2 reduction has beenhindered by a lack of understanding of the elementary steps coupling electron, proton and hydridetransfer at interfaces. Because of the complexity of the reactions in photoelectrochemical cells, adetailed mechanistic understanding can only be gained through an iterative approach of synthesis,in situ characterization of interfaces in operando and computational modeling for rigorousinterpretation of spectroscopic data and design of improved catalytic surfaces. The collaborativeteam of Batista (Yale University), Kubiak (University of California, San Diego) and Lian(Emory University) will implement a combination of synthetic, electrochemical, computational,and surface selective spectroscopic techniques to investigate electrochemical andphotoelectrochemical CO2 reduction intermediates in situ. The studieswill explore the molecular origins of overpotentials and will identify the interplay betweenthermodynamic and kinetic factors of reaction pathways at electrode surfaces to advance thedevelopment of electrocatalysts for CO2-to-fuel conversion. The first specific objective is to studythe structure and dynamics of molecular CO2 reduction catalysts immobilized on metal andsemiconductor electrodes by combining DFT, QM/MM and inverse design computationalmodeling, synthesis and in operando SFG spectro-electrochemical methods. The second specificobjective is to examine how hydricity controls selectivity of product formation during CO2reduction using a similar set of integrated experimental and theoretical methods. The thirdspecific objective is to investigate interfacial PCET mechanisms in quantum dot-model acceptorand quantum dot-catalysis complexes, with emphasis on identifying key factors controllingconcerted electron/proton transfer processes leading to low free energy reaction pathways.
Document Details
- Document Type
- DoD Grant Award
- Publication Date
- May 02, 2017
- Source ID
- FA95501710198
Entities
People
- Victor S Batista
Organizations
- Air Force Office of Scientific Research
- United States Air Force
- Yale University