Magnetic Field Driven Dynamic Reorganization of Electrocatalytic Interface for Sustainable Enhancement in Oxygen Evolution

Abstract

Hydrogen with high calorific content (150 MJ/kg) and environment-friendly combustion product (H2O) becomes the alternative fossil fuel. Catalytic electrolysis of water is one of the attractive routes for generating H2. Energy-efficient and cost-effective electrolytic production of H2 has predominantly focused on lowering the overpotential for water splitting process by developing newer non-Pt group-based catalysts.This work demonstrates a new direction towards sustainable oxygen evolution reaction (OER) by exploiting the fundamental interplay of electromagnetic forces. Introducing an external magnetic field (Hext = 100 mT) perpendicular to the heterogeneous electrocatalytic interface produces an unprecedented increase in rate of electrocatalytic OER in phosphate buffer with pH=7. Such electromagnetic catalysis is achieved with metal phosphides (NiCoP and NiCoFeP) with different morphology, leading 2.5 fold increase in the OER current density and concomitant lowering of overpotential by 10% (Hext = 100 mT). Thereby, 50% lowering of charge transfer resistance (Rct) is achieved. This is substantiated by the lowering of the Tafel slope (by 5%) in the presence of Hext. Thus, we report two important observations influenced by the magnetic field: (a) direct effect of magnetic field on the catalyst surface to reduce the charge-transfer resistance, (b) spin-dependant OER process to get influenced under magnetic field and (c) indirect effect of magnetic field to sustain the magneto-electrocatalytic enhancement even after removing the magnetic field. The time-scale of magnetic relaxation is million times higher than conventional spin-lattice relaxation events in para/ferromagnetic systems. Such long-term stability of magnetized states is predominantly proposed to be originating from the NiCoP and NiCoFeP interface. So, we attribute the long-lived states to be additionally contributed from the volumetric expansion and active site expansion of the catalyst upon magnetization. Catalyst interface is arising due to the dendritic structure of catalyst. Such synergism of magnetization, is expected to increase the applicability of magneto-electrocatalysis as a more sustainable electrocatalytic approach towards a hydrogen-driven economy. Figure 1