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Hydrogel-Based Additive Manufacturing of Lithium Cobalt Oxide

Yee, Daryl W. and Citrin, Michael A. and Taylor, Zane W. and Saccone, Max A. and Tovmasyan, Victoria L. and Greer, Julia R. (2021) Hydrogel-Based Additive Manufacturing of Lithium Cobalt Oxide. Advanced Materials Technologies, 6 (2). Art. No. 2000791. ISSN 2365-709X.

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3D multicomponent metal oxides with complex architectures can enable previously impossible energy storage devices, particularly lithium‐ion battery (LIB) electrodes with fully controllable form factors. Existing additive manufacturing approaches for fabricating 3D multicomponent metal oxides rely on particle‐based or organic–inorganic binders, which are limited in their resolution and chemical composition, respectively. In this work, aqueous metal salt solutions are used as metal precursors to circumvent these limitations, and provide a platform for 3D printing multicomponent metal oxides. As a proof‐of‐concept, architected lithium cobalt oxide (LCO) structures are fabricated by first synthesizing a homogenous lithium and cobalt nitrate aqueous photoresin, and then using it with digital light processing printing to obtain lithium and cobalt ion containing hydrogels. The 3D hydrogels are calcined to obtain micro‐porous self‐similar LCO architectures with a resolution of ≈100 µm. These free‐standing, binder‐ and conductive additive‐free LCO structures are integrated as cathodes into LIBs, and exhibit electrochemical capacity retention of 76% over 100 cycles at C/10. This facile approach to fabricating 3D LCO structures can be extended to other materials by tailoring the identity and stoichiometry of the metal salt solutions used, providing a versatile method for the fabrication of multicomponent metal oxides with complex 3D architectures.

Item Type:Article
Related URLs:
URLURL TypeDescription
Yee, Daryl W.0000-0002-4114-6167
Citrin, Michael A.0000-0001-8183-5437
Saccone, Max A.0000-0003-3846-2908
Tovmasyan, Victoria L.0000-0001-8202-5057
Greer, Julia R.0000-0002-9675-1508
Additional Information:© 2020 Wiley‐VCH GmbH. Issue Online: 08 February 2021; Version of Record online: 11 November 2020; Manuscript revised: 24 September 2020; Manuscript received: 10 August 2020. The authors would like to acknowledge the following people: K. Narita and A. Vyatskikh for assistance with the vacuum furnace setup. A. Kwong for assistance with the FIB experiments. C. Ma for assistance with the EDS experiments. J.R.G. acknowledges the financial support from the National Institutes of Health (Grant No. 1R01CA194533), the Caltech SURF office, and the Vannevar‐Bush Faculty Fellowship from the US Department of Defense. Conflict of Interest: A patent has been filed on this work. Author Contributions: D.W.Y. and M.A.C. contributed equally to the work. D.W.Y., M.A.C., and J.R.G. conceived and designed the experiments. D.W.Y., Z.W.T., and V.L.T. developed the polymer chemistry and fabricated the structures. D.W.Y. and M.A.C. developed the heating profile and performed SEM/FIB analyses. D.W.Y. performed the XRD and EDS data collection. M.A.C. and M.A.S. performed the electrochemical experiments. D.W.Y., M.A.C., and J.R.G. wrote the manuscript.
Funding AgencyGrant Number
Caltech Summer Undergraduate Research Fellowship (SURF)UNSPECIFIED
Vannevar Bush FellowshipUNSPECIFIED
Subject Keywords:additive manufacturing; hydrogels; lithium cobalt oxide; lithium ion batteries; multicomponent metal oxides
Issue or Number:2
Record Number:CaltechAUTHORS:20201111-131428787
Persistent URL:
Official Citation:Yee, D. W., Citrin, M. A., Taylor, Z. W., Saccone, M. A., Tovmasyan, V. L., Greer, J. R., Hydrogel‐Based Additive Manufacturing of Lithium Cobalt Oxide. Adv. Mater. Technol. 2021, 6, 2000791.
Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:106622
Deposited By: Tony Diaz
Deposited On:12 Nov 2020 17:06
Last Modified:09 Feb 2021 17:06

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