High-power lithium batteries from functionalized carbon-nanotube electrodes


Energy storage devices that can deliver high powers have many applications, including hybrid vehicles and renewable energy. Much research has focused on increasing the power output of lithium batteries by reducing lithium-ion diffusion distances, but outputs remain far below those of electrochemical capacitors and below the levels required for many applications. Here, we report an alternative approach based on the redox reactions of functional groups on the surfaces of carbon nanotubes. Layer-by-layer techniques are used to assemble an electrode that consists of additive-free, densely packed and functionalized multiwalled carbon nanotubes. The electrode, which is several micrometres thick, can store lithium up to a reversible gravimetric capacity of 200 mA h g−1electrode while also delivering 100 kW kgelectrode−1 of power and providing lifetimes in excess of thousands of cycles, both of which are comparable to electrochemical capacitor electrodes. A device using the nanotube electrode as the positive electrode and lithium titanium oxide as a negative electrode had a gravimetric energy 5 times higher than conventional electrochemical capacitors and power delivery 10 times higher than conventional lithium-ion batteries.

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Figure 1: Physical characteristics of LBL-MWNT electrodes.
Figure 2: Potential-dependent electrochemical behaviour of LBL-MWNT and functionalized MWNT composite electrodes measured in two-electrode lithium cells.
Figure 3: Electrochemical characteristics of LBL-MWNT electrodes in two-electrode lithium cells with 1 M LiPF6 in a mixture of ethylene carbonate and dimethyl carbonate (volume ratio 3:7).
Figure 4: Gravimetric energy and power densities, and cycle life of LBL-MWNT electrodes obtained from measurements of two-electrode cells.
Figure 5: Schematic of the energy storage mechanism of LBL-MWNT electrodes.


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The authors acknowledge partial support from the Dupont–MIT Alliance for this project. Y.S.H. acknowledges support from the Office of Naval Research (N000140410400) and the MRSEC Program of the National Science Foundation (award no. DMR – 0819762). The assistance of E.L. Shaw in collecting XPS data, Y.T. Kim in carrying out surface functionalization of MWNTs, and Y.C. Lu in electrochemical measurements and XPS analysis is greatly appreciated. T. Kawaguchi is thanked for assistance with Li4Ti5O12 and LiNi0.5Mn1.5O4 synthesis and measurements. S.W.L. acknowledges a Samsung Scholarship from the Samsung Foundation of Culture, and B.M.G. acknowledges a graduate research fellowship from the National Science Foundation.

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Y.S.H., S.W.L., N.Y. and B.M.G. conceived and designed the experiments. S.W.L., B.S.K. and P.T.H. were involved with the methods of film assembly. S.C. carried out microscopy analysis. Y.S.H., S.W.L., N.Y. and B.M.G. co-wrote the manuscript, and P.T.H. edited the manuscript.

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Correspondence to Byeong-Su Kim or Yang Shao-Horn.

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The authors declare no competing financial interests.

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Lee, S., Yabuuchi, N., Gallant, B. et al. High-power lithium batteries from functionalized carbon-nanotube electrodes. Nature Nanotech 5, 531–537 (2010). https://doi.org/10.1038/nnano.2010.116

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