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DOE OSTI · 3375886

Ion transport through reconfigurable nanoparticle-surfactant stabilized droplet interface bilayers

Wu, Xuefei [Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)]·Xue, Han [Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States); Chinese Academy of Sciences (CAS), Beijing (China)] (ORCID:0009000699423696)·Fink, Zachary [Univ. of Massachusetts, Amherst, MA (United States); Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States). Advanced Light Source (ALS)]·Xia, Zhiqin [Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)]·Sarma, Nivedina A. [Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States); University of California, Berkeley, CA (United States)] (ORCID:0000000185690562)·Gan, Xuchen [Univ. of Massachusetts, Amherst, MA (United States)]·Katsaras, John [Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States). Shull-Wollan Center] (ORCID:0000000289374177)·Ercius, Peter [Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States). Molecular Foundry] (ORCID:0000000267629976)·Rad, Behzad [Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States). Molecular Foundry] (ORCID:0000000165319168)·Helms, Brett A. [Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States). Molecular Foundry] (ORCID:0000000339254174)·Ashby, Paul D. [Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States). Molecular Foundry] (ORCID:000000034195310X)·Omar, Ahmad K. [Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States); University of California, Berkeley, CA (United States)] (ORCID:0000000264047612)·Collier, C. Patrick [Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Sciences (CNMS)] (ORCID:000000028198793X)·Russell, Thomas P. [Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States); Univ. of Massachusetts, Amherst, MA (United States); Tohoku Univ., Sendai (Japan)] (ORCID:0000000163845826)
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Abstract

Despite their adaptability and mechanical stability, Pickering emulsions based on the interfacial assembly of colloidal particles have not found use in iontronics, since the dense interfacial packing of micron-sized particles precludes functional connectivity between two droplets. In this work, we introduce a chemically reconfigurable droplet interface bilayer (DIB) platform based on the interfacial assembly of nanoparticle-surfactants (NPSs) that enables spontaneous or field-induced formation of ion-conducting nanochannels, eliminating the need of ionophores or nanochannel-forming proteins. These nanoscopic channels emerge from packing defects in the jammed interfacial assemblies of the charged NPSs and support size and charge selective, hysteretic ion transport governed by interfacial electrostatics and dimensional constraints. The NPS-DIBs show short-term and long-term plasticity, hallmarks of neuromorphic behavior, that are mediated by the structural and chemical design of the bilayer. These assemblies establish a versatile, chemically tunable platform that couples soft-matter mechanics with interfacial ionic functionality, offering a robust foundation for soft iontronic systems.

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36 MATERIALS SCIENCEdroplet interface bilayernanochannelsnanoparticle-surfactantsneuromorphic behaviorself-assembly

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Wu, Xuefei [Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)], Xue, Han [Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States); Chinese Academy of Sciences (CAS), Beijing (China)] (ORCID:0009000699423696), Fink, Zachary [Univ. of Massachusetts, Amherst, MA (United States); Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States). Advanced Light Source (ALS)], Xia, Zhiqin [Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)], Sarma, Nivedina A. [Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States); University of California, Berkeley, CA (United States)] (ORCID:0000000185690562), Gan, Xuchen [Univ. of Massachusetts, Amherst, MA (United States)], Katsaras, John [Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States). Shull-Wollan Center] (ORCID:0000000289374177), Ercius, Peter [Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States). Molecular Foundry] (ORCID:0000000267629976), Rad, Behzad [Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States). Molecular Foundry] (ORCID:0000000165319168), Helms, Brett A. [Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States). Molecular Foundry] (ORCID:0000000339254174), Ashby, Paul D. [Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States). Molecular Foundry] (ORCID:000000034195310X), Omar, Ahmad K. [Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States); University of California, Berkeley, CA (United States)] (ORCID:0000000264047612), Collier, C. Patrick [Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Sciences (CNMS)] (ORCID:000000028198793X), Russell, Thomas P. [Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States); Univ. of Massachusetts, Amherst, MA (United States); Tohoku Univ., Sendai (Japan)] (ORCID:0000000163845826). 2026-02-17. Ion transport through reconfigurable nanoparticle-surfactant stabilized droplet interface bilayers. https://doi.org/10.1073/pnas.2522349123

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The transition to a flexible and reliable energy infrastructure, using electro-thermal energy generation technologies such as geothermal, concentrated solar power, and nuclear, usually demands simultaneous advancement of thermal energy storage (TES) to support on-demand electricity generation and industrial applications while mitigating the inherent intermittency of renewable energy sources and power outages from direct energy generation. Among TES technologies, thermochemical energy storage (TCES) based on calcium looping emerges as a compelling high-power energy storage candidate due to its high reaction enthalpy, compatibility with elevated operating temperatures, and abundance of low-cost materials. However, the long-term durability of calcium-based sorbents for TCES is hindered by surface sintering and particle aggregation, leading to performance degradation over repeated thermal cycles. This study explores a moisture hydration-based strategy to regenerate a degraded calcium sorbent and mitigate performance degradation for long duration TCES. The addition of moisture transforms calcium oxide into calcium hydroxide and produces intercalation water layers, associated with a regenerated surface area and reduced calcium oxide crystallite size. Both these effects are beneficial in restoring the sorbents' reactivity for carbonization. Additionally, an optimized hydration-assisted reactivation protocol balances the recovered energy storage capacity with heating penalty required for moisture removal from hydrated samples, resulting in an enhanced energy storage capacity up to 176% compared to benchmark sorbents that undergo cycling without reactivation after 60 cycles. In conclusion, these results highlight the potential of hydration-assisted reactivation to enhance the long-term performance of TCES, providing an effective pathway to advancing electro-thermal storage technologies.

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