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• W4229035087 endingPage "136797" @default.
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• W4229035087 abstract "• The polyoxometalate-based metal–organic framework with host–guest-structure is employed as self-template. • FeS 2 /MoS 2 nanoflower particles are uniformly dispersed on reduced graphene oxide matrix. • The interconnected and staggered nanosheets in FeS 2 /MoS 2 would be beneficial N 2 fixation and ammonia synthesis. • FeS 2 /MoS 2 @RGO exhibits an excellent NRR performance and stability in acidic and alkaline media. The electrocatalytic nitrogen reduction reaction (NRR) provides a promising way for storage and sustainable utilization of ammonia. In order to reduce the cost of ammonia synthesis and promote large-scale production, it is very important to develop stable and highly active electrocatalysts. In this work, we demonstrate an iron-based metal–organic framework (MIL-100) and molybdenum-based polyoxometalate (PMo 12 ) host–guest-assisted strategy for synthesizing nanostructured bimetallic sulfides through a one-pot hydrothermal synthesis process. FeS 2 /MoS 2 particles are evenly distributed on reduced graphene oxide (RGO) with high conductivity, forming a well-defined nanoflower structure. Benefiting from the synergistic effect of FeS 2 , MoS 2 (with inherent rich catalytically active sites and uniform nanoflower structure) and RGO, the as-synthesized FeS 2 /MoS 2 @RGO achieves electrocatalytic activity and stability towards NRR in both basic and acidic solutions. The electrochemical results show a high Faradaic efficiency (FE) of 38.6 % and NH 3 yield rate of 41.1 μg h −1 mg cat -1 at −0.2 V with respect to a reversible hydrogen electrode (RHE) in acidic potassium sulfate, and FE of 9.62 % and NH 3 yield rate of 10.35 μg h −1 mg cat –1 at −0.4 V vs . RHE in alkaline potassium hydroxide solution at room temperature. Density functional theory (DFT) calculation indicates that NRR on FeS 2 /MoS 2 has optimized nitrogen binding and ammonia release which promotes the fast kinetics process through the distal mechanism, and the protonation of N 2 to form *N 2 H species is the rate-determining step (RDS) with the maximum ΔG values (+0.43 eV). This work develop a general and promising method for the design of efficient and low cost pH-universal NRR electrocatalysts." @default.
• W4229035087 created "2022-05-08" @default.
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• W4229035087 date "2022-10-01" @default.
• W4229035087 modified "2023-10-17" @default.
• W4229035087 title "FeS2/MoS2@RGO hybrid materials derived from polyoxomolybdate-based metal–organic frameworks as high-performance electrocatalyst for ammonia synthesis under ambient conditions" @default.
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• W4229035087 doi "https://doi.org/10.1016/j.cej.2022.136797" @default.
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