Molecular-scale modulation of interfaces between different unilamellar nanosheets in superlattices is promising for efficient catalytic activities. Here, three kinds of superlattices from alternate restacking of any two of the three unilamellar nanosheets of MoS 2 , NiFe-layered double hydroxide (NiFe-LDH), and graphene are systematically investigated for electrocatalytic water splitting. The MoS 2 /NiFe-LDH superlattice exhibits a low overpotential of 210 and 110 mV at 10 mA cm −2 for oxygen evolution reaction (OER) and alkaline hydrogen evolution reaction (HER), respectively, superior than MoS 2 / graphene and NiFe-LDH/graphene superlattices. High activity and stability toward the overall water splitting are also demonstrated on the MoS 2 /NiFe-LDH superlattice bifunctional electrocatalyst, outperforming the commercial Pt/C-RuO 2 couple. This outstanding performance can be attributed to optimal adsorption energies of both HER and OER intermediates on the MoS 2 /NiFe-LDH superlattice, which originates from a strong electronic coupling effect at the heterointerfaces. These results herald the interface modulation of superlattices providing a promising approach for designing advanced electrocatalysts.

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Two-dimensional transition metal dichalcogenides have been regarded as cheap and abundant catalysts for driving electrolysis of water. Using density functional theory methods, we systematically investigate the hydrogen evolution reduction of metal dichalcogenides/ graphene heterostructures (MX 2 /Gs, M = Mo, W; X = S, Se) with various defects, MX 2 /G_V X , MX 2 /G_V M , and MX 2 /G_V (M+X) . We find that such defected MX 2 /Gs show better hydrogen evolution reactive activities than pure MX 2 /Gs as well as freestanding MX 2 monolayers, due to the metallic states induced by the defects. Particularly, MX 2 / G_V X s with a S(Se) vacancy display catalytic performance comparable to that of Pt. Moreover, the catalytic performance for the hydrogen evolution reaction of most defected MX 2 /G_V M s and MX 2 /G_V (M+X) s varies with H coverage and the M vacancy concentration. Our results provide a feasible way to apply MX 2 /graphene heterostructures to water electrolysis for hydrogen production.

Catalytic mechanisms and activity trend of Ni-based heterostructures were revealed by combining experimental data and theoretical calculation results.