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Adaptive and Reconfigurable Architected Materials Driven by Electrochemistry


Xia, Xiaoxing (2019) Adaptive and Reconfigurable Architected Materials Driven by Electrochemistry. Dissertation (Ph.D.), California Institute of Technology. doi:10.7907/Q092-P711.


Architected materials are a new class of engineered materials with carefully controlled internal structures that give rise to properties that differ from or surpass those of their constituent materials. Recent advances in additive manufacturing provide an extraordinary opportunity to rationally design the structure and the chemical composition of architected materials across multiple length scales to optimize properties and functionalities for a variety of applications. These functional architected materials are capable of decoupling critical trade-offs, such as strength vs. density, to reach new regions of the material property space, and enabling exotic properties that rarely exist in classical materials such as negative refraction and negative thermal expansion.

This thesis probes into the dynamic behaviors of architected materials undergoing electrochemical reactions and aims to provide an in-depth understanding of the underlying mechanisms as well as design principles generalizable for other functional architected material systems. We developed novel fabrication methods based on two-photon lithography and various physical and chemical post-processing techniques to create architected materials with multi-level design freedom including feature sizes, structural geometries, and material compositions, which resonates with the multi-faceted challenges in electrochemical systems. We demonstrated that architected materials provide a new platform to design battery electrodes that could accommodate the large volumetric changes associated with conversion-based electrode materials, while decoupling the longstanding trade-off between active material loading and transport kinetics in batteries. Furthermore, we presented a new class of electrochemically reconfigurable architected materials that could transform their structures in a programmable, reversible and non-volatile fashion, which provide new vistas for designing mechanical metamaterials with tunable phononic bandgaps and deployable micro-devices for biomedical applications.

The multi-scale and multi-physics nature of these electrochemically driven architected materials prompted us to develop a toolset of (1) in situ SEM and optical microscopy to visualize the dynamic responses, (2) coupled chemo-mechanical finite element analysis to reconstruct detailed mechanical evolution as electrochemical reactions proceed, and (3) a statistical mechanics framework to capture the transient interactions between coupled mechanical instabilities. Using these tools, we investigated lithiation-induced cooperative beam buckling in tetragonal Si microlattices: from the deformation mechanisms of individual beams and the cooperative coupling between buckling directions of neighboring beams to the lithiation rate-dependent distribution of ordered buckling domains separated by distorted domain boundaries. Results indicate that local defects and stochastic energy fluctuations play a critical role in the dynamic response of architected materials in a way analogous to that during phase transformations of classical materials. These connections have profound implications on how we could understand and design architected materials by drawing inspiration from established theories in materials science.

Item Type:Thesis (Dissertation (Ph.D.))
Subject Keywords:Architected Materials, Additive Manufacturing, Electrochemistry, Batteries
Degree Grantor:California Institute of Technology
Division:Engineering and Applied Science
Major Option:Materials Science
Thesis Availability:Public (worldwide access)
Research Advisor(s):
  • Greer, Julia R.
Group:Kavli Nanoscience Institute
Thesis Committee:
  • Faber, Katherine T. (chair)
  • Greer, Julia R.
  • Johnson, William L.
  • Daraio, Chiara
Defense Date:21 May 2019
Funding AgencyGrant Number
Caltech Innovation Initiative (CI2) Research GrantUNSPECIFIED
Samsung Global Research Outreach GrantUNSPECIFIED
Caltech EAS Discovery FundUNSPECIFIED
Record Number:CaltechTHESIS:06012019-140706232
Persistent URL:
Related URLs:
URLURL TypeDescription adapted for Chapter 3
Xia, Xiaoxing0000-0003-1255-3289
Default Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:11595
Deposited By: Xiaoxing Xia
Deposited On:03 Jun 2019 23:20
Last Modified:08 Nov 2023 00:27

Thesis Files

PDF (Thesis) - Final Version
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[img] Video (MPEG) (Supplementary Video 1: In situ SEM lithiation of a Cu-Si Nanolattice) - Supplemental Material
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[img] Video (MPEG) (Supplementary Video 2: In situ SEM delithiation of a Cu-Si Nanolattice) - Supplemental Material
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[img] Video (MPEG) (Supplementary Video 3: FEA simulation results for Cu-Si Nanolattices) - Supplemental Material
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[img] Video (MPEG) (Supplementary Video 4: In situ lithiation of a Si microlattice at a constant current) - Supplemental Material
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[img] Video (MPEG) (Supplementary Video 5: In situ delithiation of a Si microlattice at a constant current) - Supplemental Material
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[img] Video (MPEG) (Supplementary Video 6: In situ lithiation of a Si microlattice with a resistor load) - Supplemental Material
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[img] Video (MPEG) (Supplementary Video 7: In situ cycling of a Si microlattice at high rates) - Supplemental Material
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[img] Video (MPEG) (Supplementary Video 8: In situ lithiation of a Si microlattice with programed artificial defects) - Supplemental Material
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[img] Video (MPEG) (Supplementary Video 9: FEA simulation of a 3D beam that buckles upon lithiation) - Supplemental Material
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[img] Video (MPEG) (Supplementary Video 10: FEA simulation to compare different deformation mechanisms) - Supplemental Material
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[img] Video (MPEG) (Supplementary Video 11: FEA simulation to compare beams with different slenderness ratios) - Supplemental Material
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[img] Video (MPEG) (Supplementary Video 12: FEA simulation of cooperative buckling of 2D extended unit cells) - Supplemental Material
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