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The investigation and development of bimetallic phosphosulphide electrocatalyst with low cost and abundant reserves is extremely significant for the improvement of the efficiency of hydrogen evolution reaction (HER), while it remains a challenge. Herein, we explored a feasible method to prepare three-dimensional (3D) self-supported FeNiP-S/NF-5 nanosheet arrays on Ni foil (NF) by hydrothermal method and in situ phosphorization and following sulfurization treatment. The as-obtained FeNiP-S/NF-5 only needs a potential of 183 mV vs. RHE to reach 20 mA cm−2, which is smaller than that of FeNiP/NF (187 mV vs. RHE) and FeNiS/NF-5 (239 mV vs. RHE), presenting excellent electrocatalytic stability. Such outstanding performance of the FeNiP-S/NF-5 can be attributed to following several reasons: (i) bi-metallic phosphide and sulphide have the high intrinsic activity because of its synergistic effect; (ii) the 3D nanosheet arrays structure of FeNiP-S/NF-5 is conducive to expose plentiful active sites and facilitate the electrolyte penetration along with electron transportation; (iii) the sulfurization process followed phosphorization treatment could further optimize their electronic structure and inhibited the surface oxidation of catalyst in the catalytic process. Image 1 • NiS modified FeNiP nanosheet electrocatalyst have been synthesized. • The best condition of sulfurization treatment has also been investigated. • The 3D structure and the introduction of NiS can boost activity. [ABSTRACT FROM AUTHOR]

The introduction of metal atom or heteroatom into transition metal phosphide is an effective strategy to enhance the electrochemical activity for hydrogen evolution reaction, while the controllable synthesis and purposeful design of efficient and stable transition metal phosphide based electrocatalyst with typical structural morphology is still a big challenge. Here, we investigated the relationship among the variety of the doped metal element (Fe and Mn), the corresponding morphology and electrocatalytic performance of the obtained sample for hydrogen evolution reaction. We found that with the doping of Fe and Mn, the cylinder-like CoP has transformed into microflower-like CoP-FeP and rambutan-like CoP-MnP, respectively. Meanwhile, the obtained CoP-FeP exhibits the excellent electrocatalytic activity hydrogen evolution reaction (HER) over a wide pH range (0–14), followed by CoP-MnP and CoP, resulting from the typical nanostructure and the moderately optimized electronic structure of P and Co center. Image 1 • CoP-MP (M = Fe, Mn) nanomaterials with different morphology have been controlled synthesized. • CoP-FeP shows excellent electrochemical performance for HER over a wide pH range (0–14). • The introduction of Fe or Mn element could optimized electronic structure of Co centers and P. [ABSTRACT FROM AUTHOR]

Molybdenum disulfide (MoS 2) exhibits the modest properties toward hydrogen evolution due to its poor electrical conductivity and a limited number of active sites. To make up for the defects in MoS 2 , we built hierarchical P-doped MoS 2 /NiS 2 @carbon hollow nanospheres (P–MoS/NiS@CHNS) electrocatalyst via one-step hydrothermal method owning to the priority of the reaction between Ni2+ and H 2 S. Motivated by high-efficient electron transfer at the interface of heterostructure and the activation of MoS 2 by P dopant, P–MoS/NiS@CHNS exhibits optimal Gibbs free energies (ΔG H∗) and superior HER performance with low overpotential (ƞ 10) of 110 ​mV ​at 10 ​mA ​cm−2 and small Tafel slope of 61 ​mV dec−1. The focus of this work is to optimize the HER performance of MoS 2 through P-doping and heterostructure construction, which can further provide a reference for the design of MoS 2 based catalysts. Image 1 • The P–MoS 2 /NiS 2 heterostructure is in favor of expeditious electrons transfer. • Thanks to the priority of the reaction between Ni2+ and H 2 S, the heterostructure was constructed. • The introduction of P optimizes the electron configuration of MoS 2. • The well-designed P–MoS/NiS@CHNS electrocatalyst has the optimal ΔG H∗ and E a value. [ABSTRACT FROM AUTHOR]

[Display omitted] Ultrafast (60 s) microwave quasi-solid approach is applied to design phosphorous-doped black TiO 2 supported Ru (Ru/P-TiO 2). The modulation d-band center of Ru endows the prepared catalyst with exceptional HER performance in alkaline freshwater/seawater electrolytes. • Ru/P-TiO 2 is constructed through ultrafast (60 s) quasi-solid microwave approach. • The strong metal-support electronic interaction optimize the reaction kinetics. • Optimal d-band center black Ru/P-TiO 2 exhibits efficient HER performance. Metal oxide has been considered as promising support to regulate the active microenvironment of noble metals to promote the catalytic performance, but they suffer from unsatisfactory electrical resistance and poor stability. Herein, ultrafast quasi-solid microwave (60 s) is employed to achieve phosphorous-doped black TiO 2 supported Ru (Ru/P-TiO 2) with d-band center modulation to optimize the reaction kinetics of hydrogen evolution reaction (HER). The as-synthesized Ru/P-TiO 2 exhibits extraordinary HER activities in alkaline fresehwater/seawater electrolytes with overpotential of 43 mV to reach 10 mA cm−2 coupled with satisfactory stability. Experiment and density functional theory (DFT) calculation clarify that the achieved Ru/P-TiO 2 owns optimal d-band center for H* adsorption. Moreover, the phosphorous doping enhanced the electronic interactions between Ru and oxygen vacancy-enriched TiO 2 to optimize the reaction kinetics and enhance the stability. This work provides promising strategy to modulate the metal oxide matrix for designing novel catalysts on energy conversion and storage applications. [ABSTRACT FROM AUTHOR]