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DOE OSTI · 3375230

Metal Identity and Coordination Environment Modulate Single-Atom Catalyst Stability During Electrocatalysis

Rigby, Kali [Yale Univ., New Haven, CT (United States); Nanosystems Engineering Research Center for Nanotechnology Enabled Water Treatment (NEWT), Houston, TX (United States)] (ORCID:0000000245822388)·Yu, Saerom [Univ. of Texas, Austin, TX (United States)]·Arrazolo, Leslie [Yale Univ., New Haven, CT (United States)]·Leshchev, Denis [Brookhaven National Laboratory (BNL), Upton, NY (United States). National Synchrotron Light Source II (NSLS-II)] (ORCID:0000000280493671)·Meese, Aidan [Yale Univ., New Haven, CT (United States)]·Stavitski, Eli [Brookhaven National Laboratory (BNL), Upton, NY (United States). National Synchrotron Light Source II (NSLS-II)] (ORCID:0000000233372930)·Liu, Yuanyue [Univ. of Texas, Austin, TX (United States)]·Kim, Jae-Hong [Yale Univ., New Haven, CT (United States); Nanosystems Engineering Research Center for Nanotechnology Enabled Water Treatment (NEWT), Houston, TX (United States)] (ORCID:0000000322243516)
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Abstract

A major hurdle to the implementation of single-atom catalysts (SACs) in real-world systems is a poor understanding of their stability under operating conditions, which is particularly relevant due to the high surface free energy of SACs. Here, we evaluated the aggregation behavior of a suite of SACs varied by metal identity (Fe, Co, Ni, and Cu) during electrocatalytic nitrate reduction using in situ X-ray absorption spectroscopy. The metal center had significant influence on reconstruction, where under identical applied reductive potentials, SACs underwent varying levels of reconstruction, ranging from no discernible change to complete reduction into metallic nanoparticles. Such in situ experiments revealed Cu SACs to be the most susceptible to aggregation, prompting a deeper investigation into how coordination environment (O-, B-, and N-graphene) affected Cu SAC aggregation. We further conducted density functional theory calculations to elucidate the relationship between Cu SAC structure and stability. This work deconvolutes the relationship between SAC architecture and stability, which is essential to evaluate and explain for the realization of SACs for electrocatalysis.

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36 MATERIALS SCIENCEdensity functional theory calculationselectrocatalysismetallic nanoparticlessingle-atom catalysts

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Rigby, Kali [Yale Univ., New Haven, CT (United States); Nanosystems Engineering Research Center for Nanotechnology Enabled Water Treatment (NEWT), Houston, TX (United States)] (ORCID:0000000245822388), Yu, Saerom [Univ. of Texas, Austin, TX (United States)], Arrazolo, Leslie [Yale Univ., New Haven, CT (United States)], Leshchev, Denis [Brookhaven National Laboratory (BNL), Upton, NY (United States). National Synchrotron Light Source II (NSLS-II)] (ORCID:0000000280493671), Meese, Aidan [Yale Univ., New Haven, CT (United States)], Stavitski, Eli [Brookhaven National Laboratory (BNL), Upton, NY (United States). National Synchrotron Light Source II (NSLS-II)] (ORCID:0000000233372930), Liu, Yuanyue [Univ. of Texas, Austin, TX (United States)], Kim, Jae-Hong [Yale Univ., New Haven, CT (United States); Nanosystems Engineering Research Center for Nanotechnology Enabled Water Treatment (NEWT), Houston, TX (United States)] (ORCID:0000000322243516). 2026-06-19. Metal Identity and Coordination Environment Modulate Single-Atom Catalyst Stability During Electrocatalysis. https://doi.org/10.1021/acscatal.6c02142

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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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