Spin Polarization by Magnetic Proximity Enhances Electron Transport in Catalysts

Area of Science:

• Catalysis
• Materials Science
• Spintronics

Background:

• Interfacial coupling in graphene-like carbon and metals is key for tuning electronic and spin properties in catalysis and spintronics.
• Spin catalysis typically targets open-shell molecules, limiting direct spin effects on closed-shell molecules due to fully occupied orbitals.

Purpose of the Study:

• To develop a strategy for spin-related regulation in closed-shell molecular catalysis by indirectly optimizing adsorption and activation.
• To design a high-performance hydrogenation catalyst with enhanced activity and sulfur tolerance using synergistic charge-spin regulation.

Main Methods:

• Constructed a Palladium-Carbon-Iron Oxide (Pd-C-FeOx) architecture with Pd nanoparticles encapsulated by graphene-like layers and interfaced with magnetic FeOx.
• Utilized spin polarization of the catalyst's electronic structure to induce spin splitting in the graphene-like carbon via coupling with a magnetic substrate.
• Employed experimental and theoretical analyses to investigate the effects of ferromagnetic driving on spin polarization, d-p coupling, and surface electron density.

Main Results:

• The Pd-C-FeOx architecture demonstrated enhanced spin-dependent electron transport, enabling effective control over closed-shell molecular transformations.
• Achieved improved hydrogenation activity and significant sulfur tolerance due to the protective graphene-like layer and synergistic charge-spin effects.
• Ferromagnetic driving induced asymmetric spin polarization, strengthening Pd-carbon coupling and enriching surface electron density, leading to pronounced catalytic enhancement.

Conclusions:

• The developed strategy successfully bypasses direct spin manipulation of reactants, broadening the application of spin regulation in closed-shell catalysis.
• The Pd-C-FeOx catalyst provides a design paradigm for hydrogenation catalysts that exhibit high activity and robust sulfur resistance under harsh conditions.
• This work highlights the potential of synergistic charge-spin regulation in designing advanced catalytic materials.