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DOE OSTI · 3020813

Valence-free open nanoparticle superlattices

Nayak, Binay P. [Ames Laboratory, and Iowa State Univ., Ames, IA (United States)] (ORCID:0000000239954114)·Wang, Wenjie [Ames Laboratory (AMES), Ames, IA (United States)]·Kakkar, Prapti [Ames Laboratory, and Iowa State Univ., Ames, IA (United States)] (ORCID:0000000273834642)·Zhang, Honghu [Brookhaven National Laboratory (BNL), Upton, NY (United States). National Synchrotron Light Source II (NSLS-II)] (ORCID:0000000317847825)·Mallick, Zinnia [South Dakota School of Mines and Technology, Rapid City, SD (United States)] (ORCID:0009000013185401)·Zhou, Shan [South Dakota School of Mines and Technology, Rapid City, SD (United States)] (ORCID:0000000264763280)·Nykypanchuk, Dmytro [Brookhaven National Laboratory (BNL), Upton, NY (United States). Center for Functional Nanomaterials (CFN)]·Mallapragada, Surya K. [Ames Laboratory, and Iowa State Univ., Ames, IA (United States)] (ORCID:0000000294827273)·Travesset, Alex [Ames Laboratory, and Iowa State Univ., Ames, IA (United States)]·Vaknin, David [Ames Laboratory, and Iowa State Univ., Ames, IA (United States)] (ORCID:0000000208999248)
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Abstract

A cornerstone of advanced materials design is establishing a framework for assembling nanoparticle superstructures with tailored symmetries. A longstanding challenge has been assembling diamond-like superstructures for photonic devices. Traditionally, such open superstructures require functionalized nanoparticles with directional or anisotropic interactions, reminiscent of valence bonding in a diamond. Here, we present a robust strategy for assembling valence-free nanoparticles into a broad array of cubic superstructures. By grafting nanoparticles with oppositely charged, end-functionalized water-soluble polymers of adjustable molecular weight, we gain control over electrostatic interactions and conformational constraints. This unified approach yields lattices analogous to rock salt, CsCl, zinc-blende, diamond, and the rare simple cubic phase, with tunable lattice constants. Theoretical models and simulations elucidate the underlying interactions, providing a framework for engineering valence-free nanoparticle superlattices.

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36 MATERIALS SCIENCEmetamaterialsmolecular self-assembly

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Nayak, Binay P. [Ames Laboratory, and Iowa State Univ., Ames, IA (United States)] (ORCID:0000000239954114), Wang, Wenjie [Ames Laboratory (AMES), Ames, IA (United States)], Kakkar, Prapti [Ames Laboratory, and Iowa State Univ., Ames, IA (United States)] (ORCID:0000000273834642), Zhang, Honghu [Brookhaven National Laboratory (BNL), Upton, NY (United States). National Synchrotron Light Source II (NSLS-II)] (ORCID:0000000317847825), Mallick, Zinnia [South Dakota School of Mines and Technology, Rapid City, SD (United States)] (ORCID:0009000013185401), Zhou, Shan [South Dakota School of Mines and Technology, Rapid City, SD (United States)] (ORCID:0000000264763280), Nykypanchuk, Dmytro [Brookhaven National Laboratory (BNL), Upton, NY (United States). Center for Functional Nanomaterials (CFN)], Mallapragada, Surya K. [Ames Laboratory, and Iowa State Univ., Ames, IA (United States)] (ORCID:0000000294827273), Travesset, Alex [Ames Laboratory, and Iowa State Univ., Ames, IA (United States)], Vaknin, David [Ames Laboratory, and Iowa State Univ., Ames, IA (United States)] (ORCID:0000000208999248). 2026-01-17. Valence-free open nanoparticle superlattices. https://doi.org/10.1038/s41467-026-68316-4

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DOE OSTI2026

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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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