Inhibited proton transfer enhances Au-catalyzed CO 2 -to-fuels selectivity
Abstract
Renewable electricity can be stored in the energy-dense bonds of carbon-based fuels via the electroreduction of CO 2 . CO 2 reduction in aqueous electrolytes suffers efficiency losses because of the simultaneous reduction of water to H 2 . Rational design of selective CO 2 -to-fuels catalysts requires direct knowledge of the electrode surface structure during turnover and how electrons and protons couple to direct product selectivity. Using model Au catalysts, we uncover the complex heterogeneity in CO surface binding equilibria and the differential proton coupling requirements for CO vs. H 2 production. We assemble the spectroscopic and kinetic data to construct a mechanistic model that predicts that impeding proton transfer to the surface is an effective strategy for improving CO 2 -to-fuels catalyst selectivity.
Document Details
- Document Type
- Pub Defense Publication
- Publication Date
- Jul 22, 2016
- Source ID
- 10.1073/pnas.1602984113
Entities
People
- Anna Wuttig
- Kenta Motobayashi
- Masatoshi Osawa
- Momo Yaguchi
- Yogesh Surendranath
Organizations
- Air Force Office of Scientific Research
- Hokkaido University
- Massachusetts Institute of Technology