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DOE OSTI · 2569474

Fermi Level Equilibration and Charge Transfer at the Exsolved Metal-Oxide Interface

Wang, Jiayue [Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States); Stanford Univ., CA (United States); SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)] (ORCID:0000000220273634)·Yang, Jing [Max Planck Institute for Sustainable Materials, Düsseldorf (Germany)] (ORCID:0000000318550708)·Wardini, Jenna L. [Univ. of California, Irvine, CA (United States)]·Waluyo, Iradwikanari [Brookhaven National Laboratory (BNL), Upton, NY (United States)] (ORCID:0000000240469722)·Hunt, Adrian [Brookhaven National Laboratory (BNL), Upton, NY (United States)] (ORCID:0000000252839647)·Crumlin, Ethan J. [Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)] (ORCID:000000033132190X)·Fairley, Neal [Casa Software Ltd, Teignmouth, Devon (United Kingdom)]·Bowman, William J. [Univ. of California, Irvine, CA (United States)] (ORCID:0000000243461144)·Hwang, Harold Y. [Stanford Univ., CA (United States); SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)]·Yildiz, Bilge [Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States)] (ORCID:0000000226885666)
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Abstract

Exsolution is a promising approach for fabricating oxide-supported metal nanocatalysts through redox-driven metal precipitation. A defining feature of exsolved nanocatalysts is their anchored metal-oxide interface, which exhibits exceptional structural stability in (electro)catalysis. However, the electronic interactions at this unique interface remain unclear, despite their known impact on catalytic performance. In this study, we confirm charge transfer between the host oxide and the exsolved metal by demonstrating a two-stage Fermi level ( E F ) evolution on SrTi 0.65 Fe 0.35 O 3−δ (STF) during metallic iron (Fe 0 ) exsolution. Combining ambient pressure X-ray photoelectron spectroscopy with theoretical analysis, we show that E F initially rises due to electron doping from oxygen vacancy formation in STF. Subsequently, upon Fe 0 precipitation, E F stabilizes and becomes insensitive to further oxygen release in STF, driven by E F equilibration and charge transfer between STF and the exsolved Fe 0 . In conclusion, these findings highlight the importance of considering electronic metal–support interactions when optimizing exsolved nanocatalysts.

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36 MATERIALS SCIENCECharge transferDefectsInterfacesOxygenPrecipitation

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Wang, Jiayue [Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States); Stanford Univ., CA (United States); SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)] (ORCID:0000000220273634), Yang, Jing [Max Planck Institute for Sustainable Materials, Düsseldorf (Germany)] (ORCID:0000000318550708), Wardini, Jenna L. [Univ. of California, Irvine, CA (United States)], Waluyo, Iradwikanari [Brookhaven National Laboratory (BNL), Upton, NY (United States)] (ORCID:0000000240469722), Hunt, Adrian [Brookhaven National Laboratory (BNL), Upton, NY (United States)] (ORCID:0000000252839647), Crumlin, Ethan J. [Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)] (ORCID:000000033132190X), Fairley, Neal [Casa Software Ltd, Teignmouth, Devon (United Kingdom)], Bowman, William J. [Univ. of California, Irvine, CA (United States)] (ORCID:0000000243461144), Hwang, Harold Y. [Stanford Univ., CA (United States); SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)], Yildiz, Bilge [Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States)] (ORCID:0000000226885666). 2025-01-16. Fermi Level Equilibration and Charge Transfer at the Exsolved Metal-Oxide Interface. https://doi.org/10.1021/jacs.4c14695

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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.

36 MATERIALS SCIENCE↗