Abstract
The solution transport losses in a one-dimensional solar-driven water-splitting cell that operates in either concentrated acid, dilute acid, or buffered near-neutral pH electrolytes have been evaluated using a mathematical model that accounts for diffusion, migration and convective transport, as well as for bulk electrochemical reactions in the electrolyte. The Ohmic resistance loss, the Nernstian potential loss associated with pH gradients at the surface of the electrode, and electrodialysis in different electrolytes were assessed quantitatively in a stagnant cell as well as in a bubble-convected cell, in which convective mixing occurred due to product-gas evolution. In a stagnant cell that did not have convective mixing, small limiting current densities (-2) and significant polarization losses derived from pH gradients were present in dilute acid as well as in near-neutral pH buffered electrolytes. In contrast, bubble-convected cells exhibited a significant increase in the limiting current density, and a significant reduction of the concentration overpotentials. In a bubble-convected cell, minimal solution transport losses were present in membrane-free cells, in either buffered electrolytes or in unbuffered solutions with pH ≤ 1. However, membrane-free cells lack a mechanism for product-gas separation, presenting significant practical and engineering impediments to the deployment of such systems. To produce an intrinsically safe cell, an ion-exchange membrane was incorporated into the cell. The accompanying solution losses, especially the pH gradients at the electrode surfaces, were modeled and simulated for such a system. Hence this work describes the general conditions under which intrinsically safe, efficient solar-driven water-splitting cells can be operated.
| Original language | English |
|---|---|
| Pages (from-to) | 2760-2767 |
| Number of pages | 8 |
| Journal | Energy and Environmental Science |
| Volume | 8 |
| Issue number | 9 |
| DOIs | |
| Publication status | Published - Sep 1 2015 |
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ASJC Scopus subject areas
- Renewable Energy, Sustainability and the Environment
- Environmental Chemistry
- Pollution
- Nuclear Energy and Engineering
Cite this
An electrochemical engineering assessment of the operational conditions and constraints for solar-driven water-splitting systems at near-neutral pH. / Singh, Meenesh R.; Papadantonakis, Kimberly; Xiang, Chengxiang; Lewis, Nathan S.
In: Energy and Environmental Science, Vol. 8, No. 9, 01.09.2015, p. 2760-2767.Research output: Contribution to journal › Article
}
TY - JOUR
T1 - An electrochemical engineering assessment of the operational conditions and constraints for solar-driven water-splitting systems at near-neutral pH
AU - Singh, Meenesh R.
AU - Papadantonakis, Kimberly
AU - Xiang, Chengxiang
AU - Lewis, Nathan S
PY - 2015/9/1
Y1 - 2015/9/1
N2 - The solution transport losses in a one-dimensional solar-driven water-splitting cell that operates in either concentrated acid, dilute acid, or buffered near-neutral pH electrolytes have been evaluated using a mathematical model that accounts for diffusion, migration and convective transport, as well as for bulk electrochemical reactions in the electrolyte. The Ohmic resistance loss, the Nernstian potential loss associated with pH gradients at the surface of the electrode, and electrodialysis in different electrolytes were assessed quantitatively in a stagnant cell as well as in a bubble-convected cell, in which convective mixing occurred due to product-gas evolution. In a stagnant cell that did not have convective mixing, small limiting current densities (-2) and significant polarization losses derived from pH gradients were present in dilute acid as well as in near-neutral pH buffered electrolytes. In contrast, bubble-convected cells exhibited a significant increase in the limiting current density, and a significant reduction of the concentration overpotentials. In a bubble-convected cell, minimal solution transport losses were present in membrane-free cells, in either buffered electrolytes or in unbuffered solutions with pH ≤ 1. However, membrane-free cells lack a mechanism for product-gas separation, presenting significant practical and engineering impediments to the deployment of such systems. To produce an intrinsically safe cell, an ion-exchange membrane was incorporated into the cell. The accompanying solution losses, especially the pH gradients at the electrode surfaces, were modeled and simulated for such a system. Hence this work describes the general conditions under which intrinsically safe, efficient solar-driven water-splitting cells can be operated.
AB - The solution transport losses in a one-dimensional solar-driven water-splitting cell that operates in either concentrated acid, dilute acid, or buffered near-neutral pH electrolytes have been evaluated using a mathematical model that accounts for diffusion, migration and convective transport, as well as for bulk electrochemical reactions in the electrolyte. The Ohmic resistance loss, the Nernstian potential loss associated with pH gradients at the surface of the electrode, and electrodialysis in different electrolytes were assessed quantitatively in a stagnant cell as well as in a bubble-convected cell, in which convective mixing occurred due to product-gas evolution. In a stagnant cell that did not have convective mixing, small limiting current densities (-2) and significant polarization losses derived from pH gradients were present in dilute acid as well as in near-neutral pH buffered electrolytes. In contrast, bubble-convected cells exhibited a significant increase in the limiting current density, and a significant reduction of the concentration overpotentials. In a bubble-convected cell, minimal solution transport losses were present in membrane-free cells, in either buffered electrolytes or in unbuffered solutions with pH ≤ 1. However, membrane-free cells lack a mechanism for product-gas separation, presenting significant practical and engineering impediments to the deployment of such systems. To produce an intrinsically safe cell, an ion-exchange membrane was incorporated into the cell. The accompanying solution losses, especially the pH gradients at the electrode surfaces, were modeled and simulated for such a system. Hence this work describes the general conditions under which intrinsically safe, efficient solar-driven water-splitting cells can be operated.
UR - http://www.scopus.com/inward/record.url?scp=84940515656&partnerID=8YFLogxK
UR - http://www.scopus.com/inward/citedby.url?scp=84940515656&partnerID=8YFLogxK
U2 - 10.1039/c5ee01721a
DO - 10.1039/c5ee01721a
M3 - Article
AN - SCOPUS:84940515656
VL - 8
SP - 2760
EP - 2767
JO - Energy and Environmental Science
JF - Energy and Environmental Science
SN - 1754-5692
IS - 9
ER -