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

DOI: 10.1016/j.mser.2024.100856

Authors: Yang Li (University of Cambridge) , Yan Wang (University of Cambridge) , Andrew F. May (Oak Ridge National Laboratory) , Mauro Fianchini (MagnetoCat SL; Universidad de Alicante) , Chiara Biz (MagnetoCat SL) , Saeyoung Oh (Ulsan National Institute of Science and Technology) , Yiru Zhu (University of Cambridge) , Hu Young Jeong (Ulsan National Institute of Science and Technology) , Jieun Yang (Kyung Hee University) , Jose Gracia (MagnetoCat SL) , Manish Chhowalla (University of Cambridge)
Co-authored by industrial partner: No

Type: Journal Paper
Journal: Materials Science And Engineering: R: Reports , VOL 161

State: Published (Approved)
Published: December 2024
Diamond Proposal Number(s): 33245

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.

Journal Keywords: 2D materials; Van der Waals heterostructure; Magnetic materials; Spin polarization; Electrochemical reaction; Quantum spin exchange interaction

Subject Areas: Materials, Chemistry, Physics


Instruments: I06-Nanoscience (XPEEM)

Added On: 23/09/2024 10:14

Documents:
1-s2.0-S0927796X2400086X-main.pdf

Discipline Tags:

Quantum Materials Physics Physical Chemistry Catalysis Chemistry Magnetism Materials Science

Technical Tags:

Spectroscopy Circular Dichroism (CD) X-ray Magnetic Circular Dichroism (XMCD)