Highly active platinum single-atom catalyst grafted onto 3D carbon cloth support for the electrocatalytic hydrogen evolution reaction

Platinum single-atom catalysts (PtSACs) on 3D support are emerging as the new frontier in catalysis due to their atom-economy, outstanding performance, and the advantage to bridge the gap between homogeneous and heterogeneous catalysis. This work reports on a simple, single-step electrochemical grafting attachment of a metal-selective ligand onto 3D carbon cloth and the synthesis of platinum single-atom electrocatalyst via metal uptake from aqueous salt solution. At an ultra-low loading of 0.26 ± 0.02 μg cm−2 of platinum, the single-atom catalysts supported on porous 3D carbon cloth electrode via chemical bonding revealed higher mass activity ratios, up to 83.0 at η = 50 mV/RHE, compared to the commercial catalyst 20 % Pt/C. Using hydrogen binding energy as the descriptor for efficiency, density functional theory calculations show that promoting hydrogen evolution using terpyridine-Pt proceeds when the catalyst is in a 2+ charge state and with a single hydroxy co-ligand attached to Pt catalytic center.