Tailoring the Interfacial Interactions of van der Waals 1T-MoS₂/C₆₀ Heterostructures for High-Performance Hydrogen Evolution Reaction Electrocatalysis

Abstract

Fullerene-based low-dimensional (LD) heterostructures have emerged as excellent energy conversion materials. We constructed van der Waals 1T-MoS2/C60 0D-2D heterostructures via a one-pot synthetic approach for catalytic hydrogen generation. The interfacial 1T-MoS2–C60 and C60–C60 interactions as well as their electrocatalytic properties were finely controlled by varying the weight percentages of the fullerenes. 1T-MoS2 platforms provided a novel template for the formation of C60 nanosheets (NSs) within a very narrow fullerene concentration range. The heterostructure domains of 1T-MoS2 and C60 NSs exhibited excellent hydrogen evolution reaction (HER) performances, with one of the lowest onset potentials and ΔG H* values for LD non-precious nanomaterials reported to date.

Van der Waals Heterostructures—Recent Progress in Electrode Materials for Clean Energy Applications

“…van der Waals heterostructures have shown their capability as possible electrode materials and electrocatalysts. van der Waals heterostructures have been shown to catalyze HER, ORR, and OER much better than their 2D counterparts owing to their unique electrochemical properties, and in some cases, rivaling precious metal catalysts, such as platinum and iridium [7,33,41,42,[48][49][50]. Graphene and MoS 2 based van der Waals heterostructures have shown particular promise as a trifunctional catalyst of all three reactions [41].…”

“…Molybdenum disulfide, graphene heterostructures (MoS 2 /Gr), have shown particular promise as HER catalysts [40,48,49]. MoS 2 is a highly abundant metal and a fair catalyst by itself, exhibiting thermoneutral hydrogen absorption free energy and stability in acidic solutions [48]. It usually exists as a 2D layered material, in which sheets of covalently bound S-Mo-S are stacked on top of one another.…”

“…The catalytic ability of pure MoS 2 is limited by two major drawbacks, both of which conduce poor atom utilization. The first being poor conversion efficiency since the catalyst is saturated when approximately only 25% of active sites are covered in H 2 [48]. Second, the vast majority of atoms are contained within an inert basal plane that contains no active sites to contribute towards catalysis [50].…”

“…Second, the vast majority of atoms are contained within an inert basal plane that contains no active sites to contribute towards catalysis [50]. van der Waals heterostructures with graphene enhance catalytic performance compared to pure MoS 2 by increasing the interlayer spacing, thereby exposing more active sites and improving electrical conductivity [40,48,49,51]. Yu et al was able to synthesize a MoS 2 /Gr heterostructure via a three-step process and tracked its performance in 0.5 M H 2 SO 4 and 0.5 M KOH [48].…”

“…van der Waals heterostructures with graphene enhance catalytic performance compared to pure MoS 2 by increasing the interlayer spacing, thereby exposing more active sites and improving electrical conductivity [40,48,49,51]. Yu et al was able to synthesize a MoS 2 /Gr heterostructure via a three-step process and tracked its performance in 0.5 M H 2 SO 4 and 0.5 M KOH [48]. Although the heterostructure was unable to outperform the standard Pt/C HER catalyst, it did show significant improvement over MoS 2 , boasting overpotentials of 180 mV and 263 mV at electric current densities of 10 mA cm −2 and 100 mA cm −2 , plus a Tafel slope of 79 mV dec −1 in the acidic solution and in basic solution, an overpotential of 183 mV at an electric current density of 10 mA cm −2 and Tafel slope of 127 mV dec −1 .…”