Abstract
Nano-scale confinements within mesoporous systems develop overlapping electric double layers (EDL) such that the existing theoretical models cannot predict the electric potential distributions and resulting surface charges. In addition, ionic conditions undergo local variation through connections between the pore voids and pore throats. For the first time in literature, we studied the charging behavior of mesoporous silica in terms of the pore to throat size ratio (Rpt) to characterize the pore connectivity effects, in addition to porosity (є) and pore size (H). Both local and average surface charge densities inside mesoporous silica were examined by varying these parameters systematically. Results showed that the magnitude of surface charge density decreased with increasing EDL overlap and decreasing connectivity effects. We formulized this behavior and developed an extended model to predict mesoporous silica’s internal charge as a function of porosity, pore size, and pore to throat size ratio.
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Abbreviations
- EDL:
-
Electric double layer
- BD:
-
Boltzmann distribution
- PNP:
-
Poisson-Nernst-Planck
- CR:
-
Charge regulation
- REV:
-
Representative elementary volume
- H :
-
Pore size
- R pt :
-
Pore to throat size ratio
- c10 :
-
Bulk concentration of H+
- c20 :
-
Bulk concentration of K+
- c30 :
-
Bulk concentration of Cl−
- c40 :
-
Bulk concentration of OH−
- ε :
-
Porosity
- λ :
-
Debye length
- κ :
-
Debye-Hückel parameter
- ε 0 :
-
Permitivity of vacuum
- ε r :
-
Dielectric constant
- k B :
-
Boltzmann constant
- T :
-
Temperature
- N A :
-
Avagadro constant
- e:
-
Elementary charge
- ci :
-
Local concentration of the ith ion
- z i :
-
Valance of the ith ion
- Ψ :
-
Electric potential
- N i :
-
Flux density
- D:
-
Diffusivity
- F:
-
Faraday constant
- R:
-
Universal gas constant
- Γ:
-
Site density
- KA, KB :
-
Equilibrium constants
- σ:
-
Surface charge density
- AR:
-
Aspect ratio of the solid parts
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Acknowledgments
This work was supported by the Scientific and Technological Research Council of Turkey (TÜBİTAK) under the Grant Number 118M710. Authors also would like to thank the Center for Scientific Computation at Southern Methodist University.
Funding
This work was supported by the Scientific and Technological Research Council of Turkey (TÜBİTAK) under the Grant Number 118M710
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Sen, T., Barisik, M. Pore connectivity effects on the internal surface electric charge of mesoporous silica. Colloid Polym Sci 297, 1365–1373 (2019). https://doi.org/10.1007/s00396-019-04555-w
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DOI: https://doi.org/10.1007/s00396-019-04555-w