High vacancy formation energy boosts the stability of structurally ordered PtMg in hydrogen fuel cells

Caleb Gyan-Barimah, Jagannath Sai Pavan Mantha, Ha-Young Lee, Yi Wei, Cheol-Hwan Shin, Muhammad Irfansyah Maulana, Junki Kim, Graeme Henkelman () and Jong-Sung Yu ()
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Caleb Gyan-Barimah: Daegu Gyeongbuk Institute of Science & Technology (DGIST)
Jagannath Sai Pavan Mantha: The University of Texas at Austin
Ha-Young Lee: DGIST
Yi Wei: Daegu Gyeongbuk Institute of Science & Technology (DGIST)
Cheol-Hwan Shin: Daegu Gyeongbuk Institute of Science & Technology (DGIST)
Muhammad Irfansyah Maulana: Daegu Gyeongbuk Institute of Science & Technology (DGIST)
Junki Kim: Daegu Gyeongbuk Institute of Science & Technology (DGIST)
Graeme Henkelman: The University of Texas at Austin
Jong-Sung Yu: Daegu Gyeongbuk Institute of Science & Technology (DGIST)

Nature Communications, 2024, vol. 15, issue 1, 1-13

Abstract: Abstract 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.

Date: 2024
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DOI: 10.1038/s41467-024-51280-2

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