Revealing the effect of electrocatalytic performance boost during hydrogen evolution reaction on free-standing SWCNT...

Large-scale sustainable hydrogen production by water electrolysis requires a highly active yet low-cost hydrogen evolution reaction (HER) electrocatalyst. Conductive carbon nanomaterials with high surface areas are promising candidates for this purpose. In this contribution, single-walled carbon nanotubes (SWCNTs) are assembled into free-standing films and directly used as HER electrodes. During the initial 20 h of electrocatalytic performance in galvanostatic conditions, the films undergo activation, which results in a gradual overpotential decrease to the value of 225 mV. Transient physicochemical properties of the films at various activation stages are characterized to reveal the material features responsible for the activity boost. Results indicate that partial oxidation of iron nanoparticles encapsulated in SWCNTs is the major contributor to the activity enhancement. Furthermore, besides high activity, the material, composed of only earth-abundant elements, possesses exceptional performance stability, with no activity loss for 200 h of galvanostatic performance at - 10 mA cm^-2. In conclusion, the work presents the strategy of engineering a highly active HER electrode composed of widely available elements and provides new insights into the origins of electrocatalytic performance of SWCNT-based materials in alkaline HER.