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 Title: KEY INTERMEDIATES OF CARBON DIOXIDE REDUCTION ON SILVER FROM VIBRATIONAL NANOSPECTROSCOPY Author(s): Jain, Prashant Subject(s): Mini-symposium: Multiple Potential Energy Surfaces Abstract: The design of efficacious, selective heterogeneous catalysts relies on the knowledge of the nature of active sites and reactive intermediates involved in the catalytic transformation. This is also true in the case of carbon dioxide reduction, an important scientific and technological problem. With the goal of furthering mechanistic understanding of a complex transformation that yields multiple products, we are employing surface enhanced Raman scattering (SERS) to image carbon dioxide photoreduction on individual Ag nanoparticles within a heterogeneous dispersion. The lack of ensemble-averaging is allowing us to detect fleeting intermediates in the adsorption and catalytic photoreduction processes. In particular, we have detected on some sites physisorbed CO$_{2}$ and at others chemisorbed CO$_{2}$$^{-}$ anion radical, a critical intermediate in carbon dioxide reduction. The primary product formed also appears to vary from one catalytic nanoparticle to another: CO, formaldehyde, or formic acid. The origin of such heterogeneities in adsorption and photoreduction behavior are being traced to differences in nanoparticle structure or surface composition, from which structure/activity relationships will be established, with aid from electronic structure theory. This single-nanoparticle approach is providing molecular-level insights into a broad range of industrially and environmentally relevant catalytic transformations. Issue Date: 6/21/2017 Publisher: International Symposium on Molecular Spectroscopy Citation Info: APS Genre: CONFERENCE PAPER/PRESENTATION Type: Text Language: English URI: http://hdl.handle.net/2142/97146 DOI: 10.15278/isms.2017.WB09 Date Available in IDEALS: 2017-07-272018-01-29
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