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DOE OSTI · 1968162

A single-Pt-atom-on-Ru-nanoparticle electrocatalyst for CO-resilient methanol oxidation

Poerwoprajitno, Agus R.·Gloag, Lucy·Watt, John Daniel·Cheong, Soshan·Tan, Xin·Lei, Han·Tahini, Hassan A.·Henson, Aaron·Subhash, Bijil·Bedford, Nicholas M.·Miller, Benjamin K.·O’Mara, Peter B.·Benedetti, Tania M.·Huber, Dale L.·Zhang, Wenhua·Smith, Sean C.·Gooding, J. Justin·Schuhmann, Wolfgang·Tilley, Richard D.
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Abstract

Single Pt atom catalysts are key targets because a high exposure of Pt substantially enhances electrocatalytic activity. In addition, PtRu alloy nanoparticles are the most active catalysts for the methanol oxidation reaction. To combine the exceptional activity of single Pt atom catalysts with an active Ru support we must overcome the synthetic challenge of forming single Pt atoms on noble metal nanoparticles. In this report we demonstrate a process that grows and spreads Pt islands on Ru branched nanoparticles to create single-Pt-atom-on-Ru catalysts. By following the spreading process by in situ TEM, we found that the formation of a stable single atom structure is thermodynamically driven by the formation of strong Pt–Ru bonds and the lowering of the surface energy of the Pt islands. The stability of the single-Pt-atom-on-Ru structure and its resilience to CO poisoning result in a high current density and mass activity for the methanol oxidation reaction over time.

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36 MATERIALS SCIENCE

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Poerwoprajitno, Agus R., Gloag, Lucy, Watt, John Daniel, Cheong, Soshan, Tan, Xin, Lei, Han, Tahini, Hassan A., Henson, Aaron, Subhash, Bijil, Bedford, Nicholas M., Miller, Benjamin K., O’Mara, Peter B., Benedetti, Tania M., Huber, Dale L., Zhang, Wenhua, Smith, Sean C., Gooding, J. Justin, Schuhmann, Wolfgang, Tilley, Richard D.. 2022-03-25. A single-Pt-atom-on-Ru-nanoparticle electrocatalyst for CO-resilient methanol oxidation. https://doi.org/10.1038/s41929-022-00756-9

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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↗