Spin-dependent electron transfer in electrochemically transparent van der Waals heterostructures for oxygen evolution reaction

Yang Li, Yan Wang, Andrew F. May, Mauro Fianchini, Chiara Biz, Saeyoung Oh, Yiru Zhu, Hu Young Jeong, Jieun Yang, Jose Gracia, Manish Chhowalla

Research output: Contribution to journalArticlepeer-review

Abstract

Spin selective catalysis is an emerging approach for improving the thermodynamics and kinetics of reactions. The role of electron spins has been scarcely studied in catalytic reactions. One exception is the oxygen evolution reaction (OER) where strongly correlated metals and oxides are used as catalysts. In OER, spin alignment facilitates the transition of singlet state of the reactant to the triplet state of O2. However, the influence of strong correlations on spin exchange mechanism and spin selective thermodynamics of most catalytic reactions remain unclear. Here we decouple the strongly correlated catalyst from the electrolyte to study spin exchange in two-dimensional (2D) magnetic iron germanium telluride (FGT) heterostructure. We demonstrate that transmission of spin and electrochemical information between the catalyst and the reactant can occur through quantum exchange interaction despite the catalyst of FGT being completely encapsulated by graphene or hexagonal boron nitride (hBN). The strong correlations in FGT that lead to enhanced spin exchange in OER are observed in graphene or hBN layers with thicknesses of up to 6 nm. We demonstrate that spin alignment in FGT leads to a lowering of thermodynamic barrier for adsorption of hydroxide ion and electron transfer to the catalyst. This results in up to fivefold enhancement in OER performance and improved kinetics. Our results provide clear evidence that transmission of both quantum mechanical and electrochemical information through quantum spin exchange interaction in FGT leads to an enhancement in catalytic performance.

Original languageEnglish
Article number100856
JournalMaterials Science and Engineering R: Reports
Volume161
DOIs
StatePublished - Dec 2024

Funding

The work was supported by the EU Graphene Flagship, EPSRC H2CAT (EP/V012932/1) and the European Research Council through the ERC 2D-LOTTO (101019828). H.Y.J. acknowledges support from the National R&D Program through the National Research Foundation of Korea funded by the Ministry of Science and ICT (2022M3H4A1A01013228). Synthesis and characterization of Fe 2.9 GeTe2 crystals (AFM) was supported by the U. S. Department of Energy, Office of Science, Basic Energy Sciences, Materials Sciences and Engineering Division. MagnetoCat SL acknowledges support from the European Union\u2019s Horizon 2020 research and innovation program (964972). The work was supported by the EU Graphene Flagship, EPSRC H2CAT (EP/V012932/1) and the European Research Council through the ERC 2D-LOTTO (101019828). H.Y.J. acknowledges support from the National R&D Program through the National Research Foundation of Korea funded by the Ministry of Science and ICT (2022M3H4A1A01013228). Synthesis and characterization of Fe2.9GeTe2 crystals (A.F.M.) was supported by the U.S. Department of Energy, Office of Science, Basic Energy Sciences, Materials Sciences and Engineering Division. MagnetoCat SL acknowledges support from the European Union's Horizon 2020 research and innovation program (964972).

FundersFunder number
National Research Foundation of Korea
Basic Energy Sciences
Division of Materials Sciences and Engineering
European Commission
U.S. Department of Energy
Office of Science
European Research Council
Horizon 2020
Engineering and Physical Sciences Research CouncilEP/V012932/1
Engineering and Physical Sciences Research Council
ERC 2D-LOTTO101019828
Ministry of Science and ICT2022M3H4A1A01013228
Horizon 2020 Framework Programme964972
Horizon 2020 Framework Programme

    Keywords

    • 2D materials
    • Electrochemical reaction
    • Magnetic materials
    • Quantum spin exchange interaction
    • Spin polarization
    • Van der Waals heterostructure

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