Details

Autor(en) / Beteiligte

• Dunwell, Marco
• Lu, Qi
• Heyes, Jeffrey M
• Rosen, Jonathan
• Chen, Jingguang G
• Yan, Yushan
• Jiao, Feng
• Xu, Bingjun

Titel

The Central Role of Bicarbonate in the Electrochemical Reduction of Carbon Dioxide on Gold

Ist Teil von

• Journal of the American Chemical Society, 2017-03, Vol.139 (10), p.3774-3783

Ort / Verlag

United States: American Chemical Society

Erscheinungsjahr

2017

Quelle

Alma/SFX Local Collection

Beschreibungen/Notizen

• Much effort has been devoted in the development of efficient catalysts for electrochemical reduction of CO2. Molecular level understanding of electrode-mediated process, particularly the role of bicarbonate in increasing CO2 reduction rates, is still lacking due to the difficulty of directly probing the electrochemical interface. We developed a protocol to observe normally invisible reaction intermediates with a surface enhanced spectroscopy by applying square-wave potential profiles. Further, we demonstrate that bicarbonate, through equilibrium exchange with dissolved CO2, rather than the supplied CO2, is the primary source of carbon in the CO formed at the Au electrode by a combination of in situ spectroscopic, isotopic labeling, and mass spectroscopic investigations. We propose that bicarbonate enhances the rate of CO production on Au by increasing the effective concentration of dissolved CO2 near the electrode surface through rapid equilibrium between bicarbonate and dissolved CO2.