Nickel sulfide (Ni3S2) is a promising hydrogen evolution reaction (HER) catalyst by virtue of its metallic electrical conductivity and excellent stability in alkaline medium. However, the reported catalytic activities for Ni3S2are still relatively low. Herein, an effective strategy to boost the H adsorption capability and HER performance of Ni3S2through nitrogen (N) doping is demonstrated. N‐doped Ni3S2nanosheets achieve a fairly low overpotential of 155 mV at 10 mA cm−2and an excellent exchange current density of 0.42 mA cm−2in 1.0
Molybdenum sulfide (MoS2) has emerged as a promising electrocatalyst for hydrogen evolution reaction (HER) owing to its high activity and stability during the reaction. However, the efficiency of hydrogen production is limited by the number of active sites in MoS2. In this work, a simple method of fabricating polycrystalline multilayer MoS2on Mo foil for efficient hydrogen evolution is demonstrated by controlling the sulfur (S) vacancy concentration, which can introduce new bands and lower the hydrogen adsorption free energy (Δ
- NSF-PAR ID:
- 10030911
- Publisher / Repository:
- Wiley Blackwell (John Wiley & Sons)
- Date Published:
- Journal Name:
- Advanced Materials Interfaces
- Volume:
- 4
- Issue:
- 16
- ISSN:
- 2196-7350
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
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Abstract m KOH electrolyte. The mass activity of 16.9 mA mg−1and turnover frequency of 2.4 s−1obtained at 155 mV are significantly higher than the values reported for other Ni3S2‐based HER catalysts, and comparable to the performance of best HER catalysts in alkaline medium. These experimental data together with theoretical analysis suggest that the outstanding catalytic activity of N‐doped Ni3S2is due to the enriched active sites with favorable H adsorption free energy. The activity in the Ni3S2is highly correlated with the coordination number of the surface S atoms and the charge depletion of neighbor Ni atoms. These new findings provide important guidance for future experimental design and synthesis of optimal HER catalysts. -
Abstract Solid‐state electrocatalysis plays a crucial role in the development of renewable energy to reshape current and future energy needs. However, finding an inexpensive and highly active catalyst to replace precious metals remains a big challenge for this technology. Here, tri‐molybdenum phosphide (Mo3P) is found as a promising nonprecious metal and earth‐abundant candidate with outstanding catalytic properties that can be used for electrocatalytic processes. The catalytic performance of Mo3P nanoparticles is tested in the hydrogen evolution reaction (HER). The results indicate an onset potential of as low as 21 mV, H2formation rate, and exchange current density of 214.7 µmol s−1g−1cat(at only 100 mV overpotential) and 279.07 µA cm−2, respectively, which are among the closest values yet observed to platinum. Combined atomic‐scale characterizations and computational studies confirm that high density of molybdenum (Mo) active sites at the surface with superior intrinsic electronic properties are mainly responsible for the remarkable HER performance. The density functional theory calculation results also confirm that the exceptional performance of Mo3P is due to neutral Gibbs free energy (Δ
G H*) of the hydrogen (H) adsorption at above 1/2 monolayer (ML) coverage of the (110) surface, exceeding the performance of existing non‐noble metal catalysts for HER. -
Abstract The development of stable and efficient hydrogen evolution reaction (HER) catalysts is essential for the production of hydrogen as a clean energy resource. A combination of experiment and theory demonstrates that the normally inert basal planes of 2D layers of MoS2can be made highly catalytically active for the HER when alloyed with rhenium (Re). The presence of Re at the ≈50% level converts the material to a stable distorted tetragonal (DT) structure that shows enhanced HER activity as compared to most of the MoS2‐based catalysts reported in the literature. More importantly, this new alloy catalyst shows much better stability over time and cycling than lithiated 1T‐MoS2. Density functional theory calculations find that the role of Re is only to stabilize the DT structure, while catalysis occurs primarily in local Mo‐rich DT configurations, where the HER catalytic activity is very close to that in Pt. The study provides a new strategy to improve the overall HER performance of MoS2‐based materials via chemical doping.
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Abstract The development of non‐noble metal materials for efficient hydrogen evolution reaction (HER) in wide pH range is still a challenge at present. Herein, a predesigned polyoxometalate (POM)‐based metal–organic polymer {L3Co2 · 6H2O}[H3GeMo12O40] · 9H2O (L = 1,2,4‐triazole) is employed as bimetallic source together with thiourea converting to CoS2@MoS2on carbon cloth (CC) (abbreviated to CoS2@MoS2@CC) for the first time. Impressively, the CoS2@MoS2in the form of vertically interconnected nanoarrays with multiple interfaces are grown in situ on CC and act as electrodes directly for HER. The CoS2@MoS2@CC‐30h composite exhibits superb activity and long‐durability in both acidic and alkaline media. Low overpotential is achieved in 0.5
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