Structurally Ordered Pt₃Co Nanoparticles Anchored on N-Doped Graphene for Highly Efficient Hydrogen Evolution Reaction

Abstract

Developing highly efficient catalysts for hydrogen evolution reaction (HER) play a significant role in the large-scale application of electrochemical water splitting. Here, we develop an ultrafine ordered Pt3Co NPs supported on N-doped graphene (NG), which achieves high HER activity with a small overpotential of 13 mV at 10 mA cm–2. More importantly, at the overpotential of 20 mV, the ordered Pt3Co catalyst (Pt3Co/NG-700) indicates 19.0 and 51.8 times mass activity than that of the disordered Pt3Co catalyst (Pt3Co/NG) and commercialized Pt/C catalyst, respectively. Additionally, the Pt3Co/NG-700 electrocatalyst displays outstanding long-term stability under harsh chronopotentiometry and cycling tests in the acidic media. The theory calculations reveal that the extraordinary HER performance on Pt3Co/NG-700 electrocatalyst originates from the charge redistribution of Pt induced by Co in the structurally ordered Pt3Co intermetallic. The charge redistribution of Pt facilitates the adsorption and dissociation of H* and provides a higher electron transfer and better conductivity, resulting in high HER. Our work opens new opportunities to design noble based alloy catalysts for highly efficient HER.

Synergistically coupling Pt with Ni towards accelerated water dissociation for enhanced alkaline hydrogen evolution

“…Alloying Pt with other earth-abundant transition metals has been widely demonstrated as an effective strategy to tune the electronic properties of Pt towards enhanced electrocatalysis, apart from reducing the dosage of Pt. [22][23][24][25][26] To rationalize the choice of alloying element, it is essential to take into account the fundamental HER mechanisms. 1 Normally, Pt has the optimal hydrogen adsorption free energy (DG H* ) among various transition metals; therefore it locates at the summit of the HER volcano under acidic conditions where dissociated hydrogen ions are readily available.…”

“…32,[38][39][40] But single alloy nanoparticles typically tend to aggregate, and thus conductive carbon materials are oen required as supports to load and disperse the target alloy nanoparticles. 24 Although it is a common approach to combine alloy nanoparticles and carbonaceous additives by mechanical mixing, it can hardly realize good dispersion of alloy species and strong interactions between the alloy and the carbon support. For this reason, it is highly desired to optimize the support effect by in situ anchoring nanostructured catalysts on carbonaceous substrates with uniform distribution, aiming to boost the activities and stability of the resulting hybrid catalysts.…”

Dual roles of sub-nanometer NiO in alkaline hydrogen evolution reaction: breaking the Volmer limitation and optimizing d-orbital electronic configuration

“…As is known to us, the activity of the A-HER is strongly associated with the electronic state of the catalyst surface. 57,58 As shown in Fig. 5a, the confined NiO nanocluster is logy for alkaline hydrogen evolution while other Pt/NiO, PtNi, pure Pt and benchmark catalysts show a relatively high HER activity.…”

Recent Progress on Structurally Ordered Materials for Electrocatalysis

“…introduced nitrogen‐doped graphene (NG) as a support to anchor ordered Pt 3 Co nanoparticles. [ 119 ] Moreover, the support can provide anchoring sites for modulating the particle size and uniform dispersion of the nanoparticles (Figure 13k). Meanwhile, the metal‐support interaction can further improve the electrocatalytic activity and stability.…”