Abstract
In lithium-ion batteries, the critical need for high-energy-density, low-cost storage for applications ranging from wearable computing to megawatt-scale stationary storage has created an unmet need for facile methods to produce high-density, low-tortuosity, kinetically accessible storage electrodes. Here we show that magnetic control of sacrificial features enables the creation of directional pore arrays in lithium-ion electrodes. The directional pores result in faster charge transport kinetics and enable electrodes with more than threefold higher area capacity (for example, >12 mAh cm−2 versus <4 mAh cm−2 in conventional electrodes) at practical charge–discharge rates. We demonstrate these capabilities in laboratory cells under various test conditions, including an electric vehicle model drive cycle.
Access options
Subscribe to Journal
Get full journal access for 1 year
$62.00
only $5.17 per issue
All prices are NET prices.
VAT will be added later in the checkout.
Rent or Buy article
Get time limited or full article access on ReadCube.
from$8.99
All prices are NET prices.
References
- 1.
Gaudillere, C., Garcia-Fayos, J. & Serra, J. M. Enhancing oxygen permeation through hierarchically-structured perovskite membranes elaborated by freeze-casting. J. Mater. Chem. A 2, 3828–3833 (2014).
- 2.
Deville, S., Saiz, E. & Tomsia, A. P. Freeze casting of hydroxyapatite scaffolds for bone tissue engineering. Biomaterials 27, 5480–5489 (2006).
- 3.
Wicklein, B. et al. Thermally insulating and fire-retardant lightweight anisotropic foams based on nanocellulose and graphene oxide. Nature Nanotech. 10, 277–283 (2015).
- 4.
Dong, X., Jin, W., Xu, N. & Li, K. Dense ceramic catalytic membranes and membrane reactors for energy and environmental applications. Chem. Commun. 47, 10886–10902 (2011).
- 5.
Lai, W. et al. Ultrahigh-energy-density microbatteries enabled by new electrode architecture and micropackaging design. Adv. Mater. 22, E139–E144 (2010).
- 6.
Nemani, V. P., Harris, S. J. & Smith, K. C. Design of bi-tortuous, anisotropic graphite anodes for fast ion-transport in Li-ion batteries. J. Electrochem. Soc. 162, A1415–A1423 (2015).
- 7.
Gallagher, K. G. & Nelson, P. A. in Lithium-Ion Batteries (ed. Pistoia, G.) 97–126 (Elsevier, 2014).
- 8.
Patry, G., Romagny, A., Martinet, S. & Froelich, D. Cost modeling of lithium-ion battery cells for automotive applications. Energy Sci. Eng. 3, 71–82 (2015).
- 9.
Doyle, M. & Newman, J. Analysis of capacity-rate data for lithium batteries using simplified models of the discharge process. J. Appl. Electrochem. 27, 846–856 (1997).
- 10.
Johns, P. A., Roberts, M. R., Wakizaka, Y., Sanders, J. H. & Owen, J. R. How the electrolyte limits fast discharge in nanostructured batteries and supercapacitors. Electrochem. Commun. 11, 2089–2092 (2009).
- 11.
Ebner, M., Chung, D.-W., Garcia, R. E. & Wood, V. Tortuosity anisotropy in lithium-ion battery electrodes. Adv. Energy Mater. 4, 1301278 (2014).
- 12.
Kehrwald, D., Shearing, P. R., Brandon, N. P., Sinha, P. K. & Harris, S. J. Local tortuosity inhomogeneities in a lithium battery composite electrode. J. Electrochem. Soc. 158, A1393–A1399 (2011).
- 13.
Chung, D.-W., Ebner, M., Ely, D. R., Wood, V. & Garcia, R. E. Validity of the Bruggeman relation for porous electrodes. Modelling Simul. Mater. Sci. Eng. 21, 074009 (2013).
- 14.
Ebner, M. & Wood, V. Tool for tortuosity estimation in lithium ion battery porous electrodes. J. Electrochem. Soc. 162, A3064–A3070 (2015).
- 15.
Thorat, I. V. et al. Quantifying tortuosity in porous Li-ion battery materials. J. Power Sources 188, 592–600 (2009).
- 16.
Zacharias, N. A. et al. Direct measurements of effective ionic transport in porous Li-ion electrodes. J. Electrochem. Soc. 160, A306–A311 (2013).
- 17.
Bae, C.-J., Erdonmez, C. K., Halloran, J. W. & Chiang, Y.-M. Design of battery electrodes with dual-scale porosity to minimize tortuosity and maximize performance. Adv. Mater. 25, 1254–1258 (2012).
- 18.
Behr, S., Amin, R., Chiang, Y. M. & Tomsia, A. P. Highly structured, additive free lithium-ion cathodes by freeze-casting technology. Ceram. Forum Int. 92, E39–E43 (2015).
- 19.
Erb, R. M., Libanori, R., Rothfuchs, N. & Studart, A. R. Composites reinforced in three dimensions by using low magnetic fields. Science 335, 199–204 (2012).
- 20.
Dreyfus, R., Lacoste, D., Bibette, J. & Baudry, J. Measuring colloidal forces with the magnetic chaining technique. Eur. Phys. J. E 28, 113–123 (2009).
- 21.
Sander, J. S., Erb, R. M., Denier, C. & Studart, A. R. Magnetic transport, mixing and release of cargo with tailored nanoliter droplets. Adv. Mater. 24, 2582–2587 (2012).
- 22.
Sommer, M. R., Erb, R. M. & Studart, A. R. Injectable materials with magnetically controlled anisotropic porosity. ACS Appl. Mater. Interfaces 4, 5086–5091 (2012).
- 23.
Erb, R. M., Segmehl, J., Schaffner, M. & Studart, A. R. Temporal response of magnetically labeled platelets under dynamic magnetic fields. Soft Matter 9, 498–505 (2013).
- 24.
Chiang, Y. M. & Hellweg, B. Reticulated and controlled porosity battery structures. US Patent 7,781,098 (2010) and 8,277,975 B2 (2012).
Acknowledgements
This work was supported by the Assistant Secretary for Energy Efficiency and Renewable Energy, Office of Vehicle Technologies of the US Department of Energy under Contract no. DE-AC02-05CH11231, Subcontract no. 7056592 under the Batteries for Advanced Transportation Technologies (BATT) Program. J.S.S. thanks the Swiss National Science Foundation for financial Support (Grant Numbers P300P2_154584 and P2EZP2_148768).
Author information
Affiliations
Department of Materials Science and Engineering, MIT, Cambridge, Massachusetts 02139, USA
- J. S. Sander
- , L. Li
- & Y.-M. Chiang
Department of Mechanical and Industrial Engineering, Northeastern University, Boston, Massachusetts 02115, USA
- R. M. Erb
- & A. Gurijala
Authors
Search for J. S. Sander in:
Search for R. M. Erb in:
Search for L. Li in:
Search for A. Gurijala in:
Search for Y.-M. Chiang in:
Contributions
J.S.S., R.M.E. and Y.-M.C. conceived the research, designed the experiments, and wrote the manuscript. J.S.S., L.L. and A.G. carried out the experiments and analysed the data.
Competing interests
The authors declare no competing financial interests.
Corresponding author
Correspondence to Y.-M. Chiang.
Supplementary information
PDF files
- 1.
Supplementary Information
Supplementary Figures 1–5
Videos
- 1.
Supplementary Video 1
Out-of-plane alignment of magnetic emulsion droplets in water. The movie shows chaining and alignment of magnetic emulsion droplets in a dc magnetic field.
- 2.
Supplementary Video 2
Out-of-plane alignment of magnetic emulsion droplets in water. The movie shows chaining and alignment of magnetic emulsion droplets in a dc magnetic field.
Rights and permissions
To obtain permission to re-use content from this article visit RightsLink.
