Pt3Co nanoparticles anchored on Co@NCNT via one-step high-temperature pyrolysis boosting methanol oxidation and high-efficiency pH-universal hydrogen evolution

Hydrogen production via electrocatalytic water splitting is hampered by the slow kinetics of the anodic oxygen evolution reaction (OER). Herein, Pt 3 Co nano-alloy embedded in cobalt-based N-doped carbon nanotubes (Pt 3 Co@Co@NCNTs) was prepared by one-step high temperature thermal method, achieving energy-saving efficient hydrogen (H 2 ) fabrication by hydrogen evolution reaction (HER) coupled with the methanol oxidation reaction (MOR). Due to the optimal electronic structure of the Pt 3 Co NPs and asymmetric electron transfer in the NCNTs, the Pt 3 Co@Co@NCNTs presents the overpotential of as low as 17 mV at 10 mA cm −2 for the HER, and a mass activity of as high as 1170 mA mg Pt −1 for the MOR in alkaline conditions, which are better than that of commercial Pt/C (η 10  = 35 mV, 692 mA mg Pt −1 ). This dual-electrode cell boasts impressive long-life cycling stability and operates with a cell voltage of only 1.49 V at the current density of 10 mA cm −2 . This performance even exceeds that of the commercial Pt/C||RuO 2 electrode pairs. Density functional theory (DFT) simulations have confirmed that the exceptional activity and CO poisoning resistance originate from Co-doping, which leads to a reconfiguration of charge and a reduction in reaction energy barriers for between the rate-determining step of a Volmer procedure in the HER and the formation of *CO to*COOH in the MOR. This study presents a novel approach to achieving efficient HER through overall water splitting.