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Electrochemically Reconfigurable Architected Materials

Xia, Xiaoxing and Afshar, Arman and Yang, Heng and Portela, Carlos M. and Kochmann, Dennis M. and Di Leo, Claudio V. and Greer, Julia R. (2019) Electrochemically Reconfigurable Architected Materials. Nature, 573 (7773). pp. 205-213. ISSN 0028-0836. doi:10.1038/s41586-019-1538-z.

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[img] Video (MPEG) (Supplementary Video 1. In situ lithiation of a Si microlattice at a constant current) - Supplemental Material
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[img] Video (MPEG) (Supplementary Video 2. In situ delithiation of a Si microlattice at a constant current) - Supplemental Material
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[img] Video (MPEG) (Supplementary Video 3. In situ lithiation of a Si microlattice with a resistor load) - Supplemental Material
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[img] Video (MPEG) (Supplementary Video 4. In situ cycling of a Si microlattice at high rates) - Supplemental Material
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[img] Video (MPEG) (Supplementary Video 5. In situ lithiation of a Si microlattice with programed artificial defects) - Supplemental Material
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[img] Video (MPEG) (Supplementary Video 6. FEA simulation of a 3D beam that buckles upon lithiation) - Supplemental Material
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[img] Video (MPEG) (Supplementary Video 7. FEA simulation to compare different deformation mechanisms) - Supplemental Material
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[img] Video (MPEG) (Supplementary Video 8. FEA simulation to compare beams with different slenderness ratios) - Supplemental Material
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[img] Video (MPEG) (Supplementary Video 9. FEA simulation of cooperative buckling of 2D extended unit cells) - Supplemental Material
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[img] Image (JPEG) (Extended Data Fig. 1: Sn microlattices before and after lithiation-induced cooperative beam buckling) - Supplemental Material
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[img] Image (JPEG) (Extended Data Fig. 2: Custom electrochemical testing set-up) - Supplemental Material
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[img] Image (JPEG) (Extended Data Fig. 4: Tracing of domain boundaries to generate digital domain maps) - Supplemental Material
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[img] Image (JPEG) (Extended Data Fig. 5: Domain maps and correlation functions for various lithiation rates at room temperature) - Supplemental Material
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[img] Image (JPEG) (Extended Data Fig. 6: Influence of defect distributions and energy fluctuations in Monte Carlo simulations of domain formation dynamics) - Supplemental Material
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[img] Image (JPEG) (Extended Data Fig. 7: Simulation of phononic dispersion relation for Si microlattices) - Supplemental Material
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[img] Image (JPEG) (Extended Data Table 1 Comparison of reported reconfiguration mechanisms) - Supplemental Material
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Architected materials can actively respond to external stimuli—such as mechanical forces, hydration and magnetic fields—by changing their geometries and thereby achieve novel functionalities. Such transformations are usually binary and volatile because they toggle between ‘on’ and ‘off’ states and require persistent external stimuli. Here we develop three-dimensional silicon-coated tetragonal microlattices that transform into sinusoidal patterns via cooperative beam buckling in response to an electrochemically driven silicon-lithium alloying reaction. In situ microscopy reveals a controllable, non-volatile and reversible structural transformation that forms multiple ordered buckling domains separated by distorted domain boundaries. We investigate the mechanical dynamics of individual buckling beams, cooperative coupling among neighbouring beams, and lithiation-rate-dependent distributions of domain sizes through chemo-mechanical modelling and statistical mechanics analysis. Our results highlight the critical role of defects and energy fluctuations in the dynamic response of architected materials. We further demonstrate that domain boundaries can be programmed to form particular patterns by pre-designing artificial defects, and that a variety of reconfigurational degrees of freedom can be achieved through micro-architecture design. This framework enables the design, fabrication, modelling, behaviour prediction and programming of electrochemically reconfigurable architected materials, and could open the way to beyond-intercalation battery electrodes, tunable phononic crystals and bio-implantable devices.

Item Type:Article
Related URLs:
URLURL TypeDescription ReadCube access
Xia, Xiaoxing0000-0003-1255-3289
Yang, Heng0000-0001-7431-932X
Portela, Carlos M.0000-0002-2649-4235
Kochmann, Dennis M.0000-0002-9112-6615
Di Leo, Claudio V.0000-0002-3410-6677
Greer, Julia R.0000-0002-9675-1508
Additional Information:© 2019 Springer Nature Limited. Received 20 November 2018; Accepted 02 August 2019; Published 11 September 2019. Data availability: The data that support the findings of this study are available from the corresponding author upon reasonable request. We thank D. Tozier, O. A. Tertuliano, W. L. Johnson, J. Y. Chen, K. Bhattacharya, P. W. Voorhees and D. J. Srolovitz for helpful discussions, and N. S. Lee, M. S. Hunt, A. R. Wertheim, G. A. DeRose, H. A. Atwater, N. S. Lewis, B. S. Brunschwig, J. Shi and A.H. Shih for support and assistance with experiments and instruments. We gratefully acknowledge the facilities and infrastructure provided by the Kavli Nanoscience Institute and the Molecular Materials Research Center at Caltech. J.R.G. acknowledges financial support from the Department of Defense through a Vannevar-Bush Faculty Fellowship, a Caltech Innovation Initiative Grant (CI2), and a Samsung Global Research Outreach Grant. C.V.D.L. acknowledges support from the National Science Foundation Division of Civil, Mechanical, and Manufacturing Innovation (CMMI-1825132). D.M.K. acknowledges financial support from the Office of Naval Research (N00014-16-1-2431). Author Contributions: X.X., C.V.D.L. and J.R.G. designed the study and interpreted the results. X.X. and J.R.G. conceived the idea of electrochemically driven cooperative buckling in architected materials. X.X. developed the fabrication process, fabricated all samples, and designed the experimental set-ups. X.X. and H.Y. conducted electrochemical testing and analysed the electrochemical data. A.A. and C.V.D.L. designed and conducted the coupled chemo-mechanical finite element simulations and the reduced-order simulations. X.X. analysed the domain maps and conducted the Monte Carlo simulations. C.M.P. and D.M.K. conducted the phononic dispersion relation simulations. X.X., C.V.D.L. and J.R.G. wrote the manuscript with input from all authors. The authors declare no competing interests. Peer review information: Nature thanks Sung Hoon Kang, Michael Zaiser and the other, anonymous, reviewer(s) for their contribution to the peer review of this work.
Group:Kavli Nanoscience Institute
Funding AgencyGrant Number
Kavli Nanoscience InstituteUNSPECIFIED
Caltech Molecular Materials Research CenterUNSPECIFIED
National Security Science and Engineering Faculty FellowshipUNSPECIFIED
Vannevar Bush FellowshipUNSPECIFIED
Caltech Innovation Initiative (CI2)UNSPECIFIED
Samsung Global ResearchUNSPECIFIED
Office of Naval Research (ONR)N00014-16-1-2431
Subject Keywords:Electrochemistry; Materials science; Mechanical engineering; Statistical physics, thermodynamics and nonlinear dynamics
Issue or Number:7773
Record Number:CaltechAUTHORS:20190701-140145897
Persistent URL:
Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:96869
Deposited By: Katherine Johnson
Deposited On:11 Sep 2019 18:11
Last Modified:16 Nov 2021 17:24

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