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Theoretical Physics Letters
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Hydrogen Evolution Reaction (HER) has always gained wide attention as one of the eco-friendly and sustainable pathways for efficient hydrogen generation and storage; also, two-dimensional molybdenum dichalcogenide (MoX2, where X stands for S, Se, Te) layers have emerged as a class of quasi-ideal electrocatalysts because of their large surface area, rich reserves and outstanding conductivity. However, besides greater HER activity, the maturity and diversity of modification strategies result in a more puzzling relationship between electrocatalytic mechanisms and the corresponding practical performance. In this article, based on a comprehensive review of fundamentals, principles and interconnected similarities of the MoX2 family, we focus on the structure-activity correlation of layered MoX2 for HER enhancement via hydrothermal synthesis. This method is summarized from different experimental systems to efficiently modulate the crystal structure and surface for boosted HER activity. Here, with the adjustment of three key experimental parameters: the categories of MoX2, reaction temperature and the molar amount of added reactants, the optimum HER performance can be obtained at the best conditions (MoSe2 species, 180℃ and a vast ratio of the reductant or metal precursor), and more microscopically, a controlled structure-activity relationship can be inducted. This summary may pave a new path for the controllable synthesis and modification of MoX2-based catalyst materials.
As the environmental pollution and energy crisis become increasingly severe, hydrogen, owing to its tiptop energy density, renewability, high purity and zero-polluting combustion byproduct (water), has received greater attention as an ideal energy carrier to reduce the dependence on traditional fossil energy [1-3]. Over various hydrogen generation pathways (in Fig. 1), water splitting via electrochemical approaches has been regarded as a low-cost, eco-friendly and sustainable industrial pathway for high-efficiency hydrogen conversion and storage[4,5]. So far, numerous experimental studies about high-speed and efficient hydrogen evolution have been gradually categorized into two classes: 1) identifying HER mechanisms in pursuit of more strategies for accelerating HER reaction rates, especially at a wide range of pH containing neutral and alkaline electrolyte environments (theoretically) [6-12]; 2) the discovery and design of new kinds of durable and high-activity HER electrocatalysts (experimentally) [13-18]. Considering the class 1), the key to understanding the HER mechanism is to explore the inherent relationship between the microscopic viewpoint of intermediate adsorbed states (including intermediate species and the triggered activation and adsorption energy change) and the macroscopic reaction rates [19]. Although the perplexing principle of the HER process in different pH conditions (mainly referring to acidic, neutral and alkaline conditions) is still under heated debate, especially considering which factor plays a predominant role including the source of proton donors[6,7], the interfacial H*-M (hydrogen-metal) band intensity with the changed activation barriers[8,9], the availability of surface sites and electron trapping states[10], Hupd[11], pzfc (the potential of zero free charge) with the changed reorganizational energy[12], there is a common consensus based on the competing relationship between the extra water dissociation and activation step and the hydrogen adsorption/desorption step. Specifically, from the perspective of catalyst design, several feasible strategies should be implemented to accomplish two goals (as Fig.2 depicts[20]): improving the reaction thermodynamics by lessening the activation barrier from dissociated water molecules (e.g. creating more oxophilic sites); promoting the reaction kinetics by tuning the H*-M interactions (e.g. modulating the electronic structures)[20,21]. Accordingly, no matter what the respective value of two goals are in HER, more micro-to-macro relationship can be established between the HER-related principles and the apparent HER activity by taking theoretically well-defined surface structures and electronic band levels of a certain electrocatalyst into account. Another class of research entails the real-world design of a certain kind of high-activity electrocatalysts. Although noble metals with their compounds, especially platinum (Pt), exhibit the optimum HER activity according to the Sabatier principles[22], their rare reserves and exorbitant prices largely restricts the large-scale hydrogen production. With a comparably low overpotential, a low Tafel slope and a moderate ΔGH* (not too big or too small) to Pt, various materials have adequate potentialities to replace the Pt-based HER catalysts, including chalcogenides[13,14], oxides[15], phosphides[16], nitrides[17] and carbides[18] ranging from bulk to nanoscale. Fully considering important structural or physical properties like surface area, crystallinity, porosity, thickness, electron conductivity and layered assemblies, molybdenum dichalcogenides (MoX2) have superior activity and long-term durability to defeat other structured catalyst materials[23-26]. Accordingly, the suitable choice of MoX2 help govern and regulate the apparent reactivity and kinetics of HER by designing a practically high-performance electrocatalyst with controlled surfaces and morphologies from a theoretically well-defined catalyst surface based on the HER principles. Consequently, our work aims to provide a comprehensive structure-activity analysis of MoX2-based electrocatalysts to present a clear mapping between the sluggish-rate-related HER energetics of two intermediate thermodynamic states (produced by two competing steps: the extra water dissociation step and hydrogen adsorption with interfacial H*-M interactions, as shown in Fig. 3 (b)[27,28]) and the practical design of a high-activity electrocatalyst. Based on the aforementioned correlations among hydrogen generation and two classes of viewpoints (simplified in ........... Purchase to read more.
The low concentration of proton donors in alkaline HER, subsequently leading to the extra water adsorption and dissociation steps, identifies the value of active sites (edge and basal sites) and crystal phases in lowering the extra activation barrier and/or optimizing the H* adsorption kinetics; in addition, the outstanding morphology-based features (surface area, thickness, defects, disorders and crystallinity) of layered molybdenum dichalcogenide families pinpoint the roles of active sites and phases for more interpretable and feasible structure-activity analysis. In this context, hydrothermal synthetic method is used to exhibit a clear mapping between the nanostructure/nanosurface design and the practical HER performance by adjusting key experimental parameters. In this article, MoX2 nanostructures in different species (X = S, Se, Te), the molar ratio of added reactants (the Se metal precursor and the NaBH4 reducing agency) and hydrothermal temperature are considered for the modulated structure and the optimized HER performance. The tunability of the hydrothermal method can be well confirmed with regard to its structure-activity relationship and the underlying mechanism. A system of MoX2-based samples delivery their excellent HER activity, stability and kinetics, with the optimal value of overpotential η, exchange current density j0, Tafel slope b and charge transfer resistance Rct, which are well tuned by these parameters above. For better comprehensions of the parameter-tunable structure-activity correlations, the role of active sites and phases are crucially highlighted. In detail, different chalcogenide species are indicative of different exposure of surface defects as active sites on nanoscale; the concentration of the added precursor/reductant determines the specific content of metallic 1T/1T’ phase by inducing a 2H-to-1T(1T’) conversion; hydrothermal temperatures regulates the phase and defect structure simultaneously by generating a controlled core/shell-like structure with mixed phases. Furthermore, the tunable procedures contribute to more revelation in the weigh of the roles of structural factors (edge sites, bulk conductivity for in-plane activation and phases). The crystal phase plays the predominant role as the phase transition also results in the altered densities of active sites and intrinsic activity of basal plane. To conclude, with higher tunability and scalability, the hydrothermal method can pave a novel path for the oriented, rational design of higher-activity transition-metal-based electrocatalysts and better understandings of the underlying design rules and mechanisms.
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