Spin Polarization by Magnetic Proximity Enhances Electron Transport in Catalysts

The interfacial coupling between metals and graphene-like carbon has demonstrated great potential in tuning electronic structures and spin behavior, emerging as a frontier in the development of high-performance catalytic systems and spintronic materials. Most studies on spin catalysis target open-shell molecules, in which spin-state matching can accelerate reaction kinetics. In contrast, closed-shell molecules have fully occupied orbitals, which restrict direct spin-mediated effects. Here, we introduce a strategy that bypasses direct spin manipulation of reactants. By selectively tuning the catalyst's electronic structure via spin polarization, this approach indirectly optimizes adsorption and activation. Based on this strategy, we constructed a Pd-C-FeOx architecture featuring synergistic charge-spin regulation. Pd nanoparticles (NPs) are encapsulated by graphene-like layers and interfaced with magnetic FeOx species. This design couples with the magnetic substrate to induce spin splitting in graphene-like carbon. As a result, spin-dependent electron transport is enhanced, enabling more effective control over closed-shell molecular transformations and improving both the hydrogenation activity and sulfur tolerance. The graphene-like layer simultaneously protects Pd cores from sulfur poisoning and facilitates H₂ activation, ensuring high catalytic performance under harsh conditions. Experimental and theoretical results reveal that ferromagnetic driving induces asymmetric spin polarization, which strengthens d-p coupling between Pd and carbon; additionally, it enriches the surface electron density, collectively delivering a pronounced synergistic catalytic enhancement. This approach broadens the scope of spin-related regulation in closed-shell molecular catalysis and provides a design paradigm for developing hydrogenation catalysts that combine high activity with robust sulfur resistance.