The DOI matches its Crossref record; 29 of the 29 references it cites were found in a registry or an index.
Spectroscopic Evidence of Size-Dependent Buffering of Interfacial pH by Cation Hydrolysis during CO2 Electroreduction
Open accessAbstract
The nature of the electrolyte cation is known to affect the Faradaic efficiency and selectivity of CO 2 electroreduction. Singh et al. ( J. Am. Chem. Soc. 2016, 138, 13006–13012) recently attributed this effect to the buffering ability of cation hydrolysis at the electrical double layer. According to them, the p K a of hydrolysis decreases close to the cathode due to the polarization of the solvation water molecules sandwiched between the cation’s positive charge and the negative charge on the electrode surface. We have tested this hypothesis experimentally, by probing the pH at the gold-electrolyte interface in situ using ATR-SEIRAS. The ratio between the integrated intensity of the CO 2 and HCO 3 – bands, which has to be inversely proportional to the concentration of H +, provided a means to determining the pH change at the electrode–electrolyte interface in situ during the electroreduction of CO 2 . Our results confirm that the magnitude of the pH increase at the interface follows the trend Li + > Na + > K + > Cs +, adding strong experimental support to Singh’s et al.’s hypothesis. We show, however, that the pH buffering effect was overestimated by Singh et al., their overestimation being larger the larger the cation. Moreover, our results show that the activity trend of the alkali-metal cations can be inverted in the presence of impurities that alter the buffering effect of the electrolyte, although the electrolyte with maximum activity is always that for which the increase in the interfacial pH is smaller.
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Cites
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Progress and perspectives of electrochemical CO2 reduction on copper in aqueous electrolyte
Nitopi, S., Bertheussen, E., Scott, S. B., Liu, X., Engstfeld, A. K., Horch, S., Seger, B., Stephens, I. E. L., Chan, K., Hahn, C., et al. (2019) · Chemical Reviews · doi:10.1021/acs.chemrev.8b00705 · Cited by 5,223
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Birdja, Y. Y., Pérez-Gallent, E., Figueiredo, M. C., Göttle, A. J., Calle-Vallejo, F., & Koper, M. T. M. (2019) · Nature Energy · doi:10.1038/s41560-019-0450-y · Cited by 2,747
Rational catalyst and electrolyte design for CO2 electroreduction towards multicarbon products
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Metadata
- Authors
- Ayemoba, O., & Cuesta, A.
- Venue
- ACS Applied Materials & Interfaces
- Publisher
- American Chemical Society (ACS)
- Published
- 2017-08-15
- Volume
- 9
- Issue
- 33
- Pages
- 27377-27382
- ISSN
- 1944-8244 (ISSN-L)
- 1944-8252
- OpenAlex
- W2742615673
- Cited by
- 256
- References
- 29
- FWCI
- 3.77
- Type
- journal article
- Language
- en
- Open access
- green
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- Ayemoba, O., & Cuesta, A. (2017). Spectroscopic Evidence of Size-Dependent Buffering of Interfacial pH by Cation Hydrolysis during CO2 Electroreduction. ACS Applied Materials & Interfaces. https://doi.org/10.1021/acsami.7b07351
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