Collaborative Research: In Situ Surface Spectroscopy of 2D Material-based Electrocatalysis and Photoelectrocatalysis

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Electrochemical and photoelectrochemical processes are important to a wide range of energy-related and environmental applications, including solar energy storage and carbon remediation. Photoelectrochemical hydrogen production is especially exciting for its potential to convert solar energy into carbon-free chemical fuels. The project will enable increased efficiency of photoelectrocatalytic reactions through study of the fundamental physical and chemical processes occurring in a class of ultrathin catalytic materials important for the sustainable production of fuels and chemicals.The study will investigate electrocatalysis (EC) and photoeletrocatalysis (PEC) in two-dimensional dichalcogenide materials using various forms of in situ linear, nonlinear, and ultrafast spectroscopy to characterize three critical factors in EC/PEC reactions: interfacial electrostatics (local (i.e., surface) electrostatic fields), interfacial dynamics and electrostatics (photoexcited charge carrier dynamics), and interfacial molecular structures (surface bound intermediate species) produced during the EC and PEC processes. Sum frequency generation (SFG), second harmonic generation (SHG), vibrational Stark Shift (VSS) spectroscopy, and transient absorption spectroscopy (TAS) will be employed to reveal key mechanistic information regarding the EC and PEC processes primarily for the reduction of CO2 to methanol and carbon monoxide. Spectroscopic data will be acquired in situ as a function of the electrochemical potential and electrolyte composition, and correlated with product yield and selectivity. The project includes educational and outreach activities that build upon the research to promote engagement of students in science, technology, engineering and mathematics (STEM) disciplines. These activities, which include workshop for high school science teachers, are directed at improving the education of promising high school students and encouraging their interest in STEM careers.This award reflects NSF's statutory mission and has been deemed worthy of support through evaluation using the Foundation's intellectual merit and broader impacts review criteria.