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

Abstract

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.

Selective Area Growth and Transfer of High Optical Quality MoS2 Layers

“…[ 4–13 ] With the rapid advancement of 2D materials research, it is recognized that the rational growth of such layered materials with the desired phase, thickness, and chemical composition represents one of the bottlenecks for their integration into a wide range of applications. [ 1–3,14–16 ] One of the most promising methodologies for the large‐scale synthesis with high crystal quality would be chemical vapor deposition (CVD). The vast majority of CVD‐derived TMDCs is based on the use of metal oxide (MO) precursors as the feedstock for the desired metal (Mo, W, etc.).…”

Graphene Oxide Layer-by-Layer Films for Sensors and Devices

“…As the number of bilayers increases, the surface becomes more heterogeneous, as can be clearly seen from the (PAH/GO) 20 LbL film images presented in Figure 3 (3a-3c). The surface of the film, besides exhibiting PAH/GO aggregate formation, also showed GO and/or PAH/GO stacks.…”

“…The band centered at 149.2 nm is a π-π* transition of the carbonyl group associated with aldehydes and ketones [23]. Parameters for fitting to the low intensity peak at 178 nm could not be found, but can be identified as being associated with n N -3pa type electronic transitions of pairs from solitary nitrogen electrons to orbitals of the same type (amine) [20] and n-σ* transitions from the carbonyl group (aldehydes and ketones) [23]. The band at 196.1 nm corresponds to n N -3sa transitions [21] and π-π* transitions in the aromatic ring (phenol) [23] and/or to the n-π transitions of the carboxylic group.…”

“…Moreover, the LbL film deposition method is carried out using aqueous solutions, which from an environmental point of view makes this technique lower risk. In recent years, several LbL films based on GO have been prepared and characterized, having the development of devices and sensors in mind [17][18][19][20][21][22][23].…”

FeV3O8/MoS2 nanostructure heterojunctions as a highly effective electrocatalyst for hydrogen evolution

“…[18][19][20] A lot of reported theoretical and experimental research in the related fields has indicated that the most active sites in 2H-MoS 2 are located at the edges, while the poor electrical conductivity of MoS 2 basal planes is generally bad for catalysis of the HER. 15,21,22 Therefore, in order to solve the above obstacles, many modified methods have been conducted to enhance the catalytic capacity of MoS 2 in HER, involving doping, 23,24 building up of hybrid structures, 2,25,26 crystalline phase and band-gap engineering 27,28 and so on. Compared with doping or phase transition engineering, the process of constructing composite nanostructure heterojunctions is simple and cost-effective.…”