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1.
Nat Commun ; 15(1): 7034, 2024 Aug 15.
Artículo en Inglés | MEDLINE | ID: mdl-39147744

RESUMEN

Alloys of platinum with alkaline earth metals promise to be active and highly stable for fuel cell applications, yet their synthesis in nanoparticles remains a challenge due to their high negative reduction potentials. Herein, we report a strategy that overcomes this challenge by preparing platinum-magnesium (PtMg) alloy nanoparticles in the solution phase. The PtMg nanoparticles exhibit a distinctive structure with a structurally ordered intermetallic core and a Pt-rich shell. The PtMg/C as a cathode catalyst in a hydrogen-oxygen fuel cell exhibits a mass activity of 0.50 A mgPt-1 at 0.9 V with a marginal decrease to 0.48 A mgPt-1 after 30,000 cycles, exceeding the US Department of Energy 2025 beginning-of-life and end-of-life mass activity targets, respectively. Theoretical studies show that the activity stems from a combination of ligand and strain effects between the intermetallic core and the Pt-rich shell, while the stability originates from the high vacancy formation energy of Mg in the alloy.

2.
Chem Soc Rev ; 52(6): 2145-2192, 2023 Mar 20.
Artículo en Inglés | MEDLINE | ID: mdl-36799134

RESUMEN

Magnesium (Mg) has many unique properties suitable for applications in the fields of energy conversion and storage. These fields presently rely on noble metals for efficient performance. However, among other challenges, noble metals have low natural abundance, which undermines their sustainability. Mg has a high negative standard reduction potential and a unique crystal structure, and its low melting point at 650 °C makes it a good candidate to replace or supplement numerous other metals in various energy applications. These attractive features are particularly helpful for improving the properties and limits of materials in energy systems. However, knowledge of Mg and its practical uses is still limited, despite recent studies which have reported Mg's key roles in synthesizing new structures and modifying the chemical properties of materials. At present, information about Mg chemistry has been rather scattered without any organized report. The present review highlights the chemistry of Mg and its uses in energy applications such as electrocatalysis, photocatalysis, and secondary batteries, among others. Future perspectives on the development of Mg-based materials are further discussed to identify the challenges that need to be addressed.

3.
ACS Appl Mater Interfaces ; 14(22): 25246-25256, 2022 Jun 08.
Artículo en Inglés | MEDLINE | ID: mdl-35609281

RESUMEN

Over the last years, the development of highly active and durable Pt-based electrocatalysts has been identified as the main target for a large-scale industrial application of fuel cells. In this work, we make a significant step ahead in this direction by preparing a high-performance electrocatalyst and suggesting new structure-activity design concepts which could shape the future of oxygen reduction reaction (ORR) catalyst design. For this, we present a new one-dimensional nanowire catalyst consisting of a L10 ordered intermetallic PtCo alloy core and compressively strained high-index facets in the Pt-rich shell. We find the nanoscale PtCo catalyst to provide an excellent turnover for the ORR and hydrogen evolution reaction (HER), which we explain from high-resolution transmission electron microscopy and density functional theory calculations to be due to the high ratio of Pt(221) facets. These facets include highly active ORR and HER sites surprisingly on the terraces which are activated by a combination of sub-surface Co-induced high Miller index-related strain and oxygen coverage on the step sites. The low dimensionality of the catalyst provides a cost-efficient use of Pt. In addition, the high catalytic activity and durability are found during both half-cell and proton exchange membrane fuel cell (PEMFC) operations for both ORR and HER. We believe the revealed design concepts for generating active sites on the Pt-based catalyst can open up a new pathway toward the development of high-performance cathode catalysts for PEMFCs and other catalytic systems.

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