Symmetry-broken atomic ensemble induced by mandated charge for efficient water dissociation in hydrogen generation

Abstract

Efficient water dissociation catalysts are important for reducing the activation energy barrier of water molecules in the field of energy conversion. Herein, symmetry-broken Rh ensemble induced by mandated charge was established to boost the catalytic activity toward water dissociation. As an experimental verification, the turnover frequency of 1.0-RTO_V4 in hydrogen generation from ammonia borane hydrolysis reaches up to 2838 min⁻¹ (24828 min⁻¹ depend on Rh dispersion), exceeding the benchmark set up by state-of-the-art catalysts. The transfer of mandated charge from O_V to Rh near O_V breaks the local symmetry of Rh nanoparticle and forms Rh^γ− (electron-aggregation Rh)-Rh interfacial atomic ensemble. This symmetry-broken Rh ensemble is the reason for the high activity of the catalyst. This work provides an effective electronic regulation strategy based on symmetry-broken atomic ensemble induced by mandated charge, designed to stimulate the limiting activity of metal catalyst in the field of next generation energy chemistry.