Au Nanoparticle Modification Induces Charge-Transfer Channels to Enhance the Electrocatalytic Hydrogen Evolution Reaction of InSe Nanosheets

Abstract

Electrocatalytic water splitting for hydrogen production is an efficient, clean, and sustainable strategy to solve energy and environmental problems. As the important alternative materials for noble metals (Pt, Ir, etc.), two-dimensional (2D) materials have been widely applied for electrocatalysis, although the practical performance is restricted by low carrier mobility and slow reaction kinetics. Here, we adopt the strategy of Au nanoparticle modification to achieve the enhanced hydrogen evolution reaction (HER) performance of InSe nanosheets. Experimental results prove that the HER performance of InSe nanosheets is significantly enhanced under the modification of Au nanoparticles, and the overpotential (392 mV) and Tafel slope (59 mV/dec) are significantly reduced compared to sole InSe nanosheets (580 mV and 148.2 mV/dec). First-principles calculations have found that the InSe/Au system exhibits metallicity because the free electrons provided by the Au particles are injected into the InSe, thereby improving its conductivity. The difference charge density and localized charge density of InSe/Au show that Au nanoparticle loading can induce the formation of Au–Se electron-transfer channels with electrovalent bond characteristics, which effectively promotes the charge transfer. Meanwhile, the standard free-energy calculation of the HER process shows that the InSe/Au heterojunction has a H* adsorption/desorption Gibbs free energy [(|ΔG H*|) = 0.59 eV] closer to the optimal value. This study reveals the theoretical mechanism of metal modification to improve the performance of electrocatalytic HER and is expected to motivate the development of a new strategy for enhancing the catalytic activity of 2D semiconductor materials.

Pd nanoparticles-decorated borophene nanosheets for intrinsic polarization-induced visible light photocatalysis

“…To simplify the calculations, a feasible periodic single-atom model was employed as adopted previously by several other researchers. [43][44][45][46] The atomic ratio of Pd and B was considered to be 1 : 20, which corroborated the experimentally obtained composition of 1 : 19.1 (from EDX analysis). To capture the location/site for Pd nucleation on the borophene sheets, the structure of Pd-B was optimized.…”

Sulfur-Modified Nickel-Based Hybrid Nanosheet as a Robust Bifunctional Electrode for Hydrogen Generation via Formaldehyde Reforming

“…In recent years, precious metal catalysts have been widely utilized and show excellent activity for HER or formaldehyde (FOR), but large-scale application is greatly limited due to their high cost and low reserves. − With the in-depth development of low-cost electrode materials, a range of non-noble materials are exploited as efficient electrocatalysts for HER or FOR, such as transition metal-based oxides/hydroxides, sulfides, phosphides, alloys, and so on. − Among them, nickel (Ni)-based materials present promising catalytic activity and high durability, thus achieving widespread attention.…”

Ni(II)-Pyrazolate Framework Bearing a Metalated Schiff-Base Moiety for Electrocatalytic Hydrogen Evolution

“…Hydrogen (H 2 ) fuel, with high energy density, is an alternative to nonrenewable energy resources and relieves global warming based on greenhouse gas coming from burning carbon-based fuel. − The electrocatalytic hydrogen evolution reaction (HER) represents one of the key technologies to produce H 2 as clean energy to achieve sustainable development. − So far, materials based on noble metals (e.g., Ru, Ir, Pt, etc.) are still the dominant electrocatalysts for HER owing to their favorable hydrogen/oxygen adsorption free energies. − However, sky-high cost and low abundance of noble metal limit the wide application of these electrocatalysts for HER. Therefore, researchers have been exploiting highly active and economical electrocatalysts based on abundant transition metals.…”