Key intermediates of carbon dioxide reduction on silver from vibrational nanospectroscopy

Jain, Prashant

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https://hdl.handle.net/2142/97146 Copy

Description

Title

Key intermediates of carbon dioxide reduction on silver from vibrational nanospectroscopy

Author(s)

Jain, Prashant

Issue Date

2017-06-21

Keyword(s)

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.

Publisher

International Symposium on Molecular Spectroscopy

Type of Resource

text

Language

eng

Permalink

http://hdl.handle.net/2142/97146

DOI

https://doi.org/10.15278/isms.2017.WB09

Copyright and License Information

Copyright 2017 Prashant Jain

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