A Scalable Interfacial Engineering Strategy for a Finely Tunable, Homogeneous MoS2/rGO-Based HER Catalytic Structure

The electronic structures and catalytic efficacies of molybdenum disulfide (MoS2)-based catalysts are sensitive to embedding environment. In order to develop a finely tunable strategy, a "layer-by-layer and Nafion capping" strategy for the scalable preparation of interfacial (MoS2)-based catalytic structures is developed. The study shows that the assembly partner influences the electronic structures of the Zn&N co-doped (MoS2) (Zn-N-(MoS2)) catalysts. Poly(allylamine hydrochloride) (PAH) decreases the catalytic efficacy, whereas when PAH-rGO (rGO [reduced graphene oxide]) is the assembly partner, effective interfacial catalysts are prepared. The superior catalytic efficacy of (PAH-rGO/Zn-N-(MoS2))(n) can be attributed to the fact that rGO effectively activates the basal plane S2- as the active sites. The catalytic efficacy of the multilayers at 16 assembly cycles due to a balance between the number of active sites and low resistance. After capping with Nafion layer, the interfacial catalysts exhibit high stability. Compared with the widely used drop-casting methods, the layer-by-layer strategy possesses unique benefits, including fine-tune the structures, free choice of the partner, and planar homogeneity. It is expected that this layer-by-layer catalyst immobilization strategy will benefit fundamental understandings regarding the finely controlled scalable interfacial immobilization of catalysts with superior efficacy, and assist in promoting the practical utilization of various catalysts.