Search NASA⌕ Search
Home/Archive/DOE OSTI

DOE OSTI · 3365194

Revealing multiscale competing processes in the solid-state synthesis of single-crystalline layered oxide positive electrodes

Xue, Zhichen [SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States). Stanford Synchrotron Radiation Lightsource (SSRL)] (ORCID:0000000315111777)·Sun, Tianxiao [Univ. of Texas, Austin, TX (United States)] (ORCID:0000000219873915)·Oruganti, Sreevishnu [Univ. of Illinois at Urbana-Champaign, IL (United States); Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States). Advanced Light Source (ALS)]·Huang, Xiaojing [Brookhaven National Laboratory (BNL), Upton, NY (United States). National Synchrotron Light Source II (NSLS-II)] (ORCID:0000000160345893)·Parkinson, Dilworth Y. [Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States). Advanced Light Source (ALS)] (ORCID:0000000218170716)·Chu, Yong S. [Brookhaven National Laboratory (BNL), Upton, NY (United States). National Synchrotron Light Source II (NSLS-II)]·Pianetta, Piero [SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States). Stanford Synchrotron Radiation Lightsource (SSRL)] (ORCID:0000000248346014)·Ge, Mingyuan [Brookhaven National Laboratory (BNL), Upton, NY (United States). National Synchrotron Light Source II (NSLS-II)] (ORCID:0000000156827443)·Liu, Yijin [Univ. of Texas, Austin, TX (United States)] (ORCID:0000000284172488)
View original source ↗Read source document ↗Export metadata ↓

Abstract

Solid-state synthesis involves a web of coupled chemical reactions and physical changes that unfold across multiple scales. Efforts to fine-tune its parameters have historically followed heuristic, trial-driven workflows that demand significant time and resources. In this study, we aimed to open this black box by employing multiscale in situ synchrotron imaging and diffraction. Using LiNi 0.5 Mn 0.3 Co 0.2 O 2 battery positive electrode material as a model system and Ba-based sintering aids, we reveal dopant segregation, intergranular mass transport, and porosity evolution as key drivers of single-crystalline particle formation. Notably, we uncovered a dynamic competition between particle-level grain coalescence and atomic-scale cation disordering, both of which are thermally activated yet have opposing impacts on battery performance. These findings highlight the coupled, multiscale nature of structure development and offer a mechanistic basis for optimizing the solid-state synthesis process. This framework provides a path toward more controlled, efficient, and scalable production of high-performance battery positive electrode materials.

Explore related subjects

36 MATERIALS SCIENCE

Keep this discovery

Explore connections, maps & timelines

BibTeXRIS

Xue, Zhichen [SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States). Stanford Synchrotron Radiation Lightsource (SSRL)] (ORCID:0000000315111777), Sun, Tianxiao [Univ. of Texas, Austin, TX (United States)] (ORCID:0000000219873915), Oruganti, Sreevishnu [Univ. of Illinois at Urbana-Champaign, IL (United States); Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States). Advanced Light Source (ALS)], Huang, Xiaojing [Brookhaven National Laboratory (BNL), Upton, NY (United States). National Synchrotron Light Source II (NSLS-II)] (ORCID:0000000160345893), Parkinson, Dilworth Y. [Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States). Advanced Light Source (ALS)] (ORCID:0000000218170716), Chu, Yong S. [Brookhaven National Laboratory (BNL), Upton, NY (United States). National Synchrotron Light Source II (NSLS-II)], Pianetta, Piero [SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States). Stanford Synchrotron Radiation Lightsource (SSRL)] (ORCID:0000000248346014), Ge, Mingyuan [Brookhaven National Laboratory (BNL), Upton, NY (United States). National Synchrotron Light Source II (NSLS-II)] (ORCID:0000000156827443), Liu, Yijin [Univ. of Texas, Austin, TX (United States)] (ORCID:0000000284172488). 2026-03-15. Revealing multiscale competing processes in the solid-state synthesis of single-crystalline layered oxide positive electrodes. https://doi.org/10.1038/s41467-026-70607-9

Cite the original work for its findings. Save a collection to share your selection of sources.

KEEP EXPLORING

Related reports

DOE OSTI2026

Cyclic moisture reactivation of calcium sorbents for long duration thermochemical energy storage

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.

36 MATERIALS SCIENCE↗