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

Journal Article · 19 September 2024 · Materials Science and Engineering. R, Reports

DOI: https://doi.org/10.1016/j.mser.2024.100856 · OSTI ID:2472678

Li, Yang ^[1]; Wang, Yan ^[1]; May, Andrew F.  ^[2]; Fianchini, Mauro ^[3]; Biz, Chiara ^[4]; Oh, Saeyoung ^[5]; Zhu, Yiru ^[1]; Jeong, Hu Young ^[5]; Yang, Jieun ^[6]; Gracia, Jose ^[4]; Chhowalla, Manish ^[1]

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1. Univ. of Cambridge (United Kingdom)
2. Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)
3. MagnetoCat SL (Spain); University of Alicante (Spain)
4. MagnetoCat SL (Spain)
5. Ulsan National Institute of Science and Technology (UNIST) (Korea, Republic of)
6. Kyung Hee Univ., Seoul (Korea, Republic of)

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.

• Research Organization: Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)
• Sponsoring Organization: USDOE Office of Science (SC), Basic Energy Sciences (BES). Materials Sciences & Engineering Division (MSE)
• Grant/Contract Number: AC05-00OR22725
• OSTI ID: 2472678
• Journal Information: Materials Science and Engineering. R, Reports, Journal Name: Materials Science and Engineering. R, Reports Vol. 161; ISSN 0927-796X
• Publisher: ElsevierCopyright Statement
• Country of Publication: United States
• Language: English