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  Direct control of electron spin at an intrinsically chiral surface for highly efficient oxygen reduction reaction

Wang, X., Peralta, M., Li, X., Möllers, P. V., Zhou, D., Merz, P., et al. (2025). Direct control of electron spin at an intrinsically chiral surface for highly efficient oxygen reduction reaction. Proceedings of the National Academy of Sciences of the United States of America, 122(9): e2413609122. doi:10.1073/pnas.2413609122.

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 Creators:
Wang, Xia1, Author
Peralta, Mayra1, Author
Li, Xiaodong1, Author
Möllers, Paul V.1, Author
Zhou, Dong1, Author
Merz, Patrick1, Author
Burkhardt, Ulrich1, Author
Borrmann, Horst1, Author
Robredo, Iñigo1, Author
Shekhar, Chandra1, Author
Zacharias, Helmut1, Author
Feng, Xinliang2, Author                 
Felser, Claudia1, Author
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1External Organizations, ou_persistent22              
2Department of Synthetic Materials and Functional Devices (SMFD), Max Planck Institute of Microstructure Physics, Max Planck Society, ou_3316580              

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 Abstract: The oxygen reduction reaction (ORR) in acidic media suffers from sluggish kinetics, primarily due to the spin-dependent electron transfer involved. The direct generation of spin-polarized electrons at catalytic surfaces remains elusive, and the underlying mechanisms are still controversial due to the lack of intrinsically chiral catalysts. To address this challenge, we investigate topological homochiral PdGa (TH PdGa) crystals with intrinsically chiral catalytic surfaces for ORR. Through spin-resolved photoemission spectroscopy and theoretical simulations, we show that both structural chirality and spin–orbit coupling are critical for inducing spin polarization at the surface of TH PdGa. As a result, TH PdGa achieves a kinetic current density over 100 times higher than the achiral PdGa (AC PdGa) at 0.85 V versus the reversible hydrogen electrode. This work underscores the pivotal role of spin polarization in enhancing acidic ORR activity and lays the groundwork for the rational design of chiral catalysts for spin-dependent catalysis.

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 Dates: 2025-02-25
 Publication Status: Issued
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 Identifiers: DOI: 10.1073/pnas.2413609122
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Title: Proceedings of the National Academy of Sciences of the United States of America
  Other : PNAS
  Other : Proceedings of the National Academy of Sciences of the USA
  Abbreviation : Proc. Natl. Acad. Sci. U. S. A.
Source Genre: Journal
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Publ. Info: Washington, D.C. : National Academy of Sciences
Pages: - Volume / Issue: 122 (9) Sequence Number: e2413609122 Start / End Page: - Identifier: ISSN: 0027-8424
CoNE: https://pure.mpg.de/cone/journals/resource/954925427230