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• The special microstructure of urchin-like nanoflowers and nanowires was synthesized, which had superhydrophilicity. • Different sodium borohydride treatment time affects the morphology and activity of the product. • The elements B and P exhibit a synergistic effect, resulting in the attainment of favorable catalytic activity. This study presents a proposed three-step synthetic route for the efficient synthesis of B-NiCoP/NF, aiming to produce a highly active catalyst for the hydrogen evolution reaction (HER). The B-NiCoP/NF catalyst demonstrates a remarkable performance, requiring only 42.1 mV in 1 M KOH solution to achieve a current density of 10 mA·cm−2. Moreover, the catalyst demonstrates exceptional long-term stability, enduring 2000 CV cycles or 55 h of chronopotentiometry tests, at a current density of 50 mA·cm−2. The exceptional performance of the catalyst can be ascribed to the superhydrophilic properties of the unique microstructure of urchin-like nanoflowers and nanowires, as well as the synergistic effect of elements P and B. This effect promotes water dissociation, reduces surface hydrogen absorption, and hinders the oxidation of phosphide active sites. In conclusion, this research has successfully developed and produced an efficient catalyst for the HER, along with a versatile pretreatment technique. The application of this method holds significant importance in enhancing the phosphating process in various catalytic systems. [ABSTRACT FROM AUTHOR]

• NiCoP/NF with nanowire morphology was prepared by hydrothermal method and in-situ phosphating as a precatalyst. • The real active material NiCo 2 O 4 was obtained by spontaneous surface reconstruction of NiCoP/NF nanowires. • After surface reconstruction, the catalyst has a larger specific surface area and better conductivity, thus showing excellent catalytic performance. The investigation of transition metal phosphides (TMPs) as efficient electrocatalysts for water splitting has garnered significant attention in academic research. Nevertheless, limited research has been conducted on the alteration of the structural and morphological properties of TMPs resulting from the unavoidable surface reconstruction during the oxygen evolution reaction (OER). This study introduces a newly developed catalyst, namely nickel–cobalt phosphide nanowires (NiCoP), which facilitates the in-situ growth of nickel–cobalt oxide (NiCo 2 O 4) through surface reconstruction during anodic potential cycling in alkaline electrolytes. The catalyst's extensive modification can be observed through ex-situ characterization techniques. The catalyst undergoes a significant transformation that ultimately yields a phosphide scaffold, leading to the formation of a spinel oxide surface. This transformation enhances the catalytic environment for the OER, making it highly efficient and potent. The transformed catalyst demonstrates comparable catalytic performance to the precious RuO 2 catalyst across various current densities. Importantly, it exhibits remarkable long-term stability, as demonstrated by its ability to sustain continuous operation for 72 h at a current density of 50 mA while maintaining stable catalytic performance. [ABSTRACT FROM AUTHOR]

The electrolytes for lithium metal batteries (LMBs) are plagued by a low Li+ transference number (T+) of conventional lithium salts and inability to form a stable solid electrolyte interphase (SEI). Here, we synthesized a self‐folded lithium salt, lithium 2‐[2‐(2‐methoxy ethoxy)ethoxy]ethanesulfonyl(trifluoromethanesulfonyl) imide (LiETFSI), and comparatively studied with its structure analogue, lithium 1,1,1‐trifluoro‐N‐[2‐[2‐(2‐methoxyethoxy)ethoxy)]ethyl]methanesulfonamide (LiFEA). The special anion chemistry imparts the following new characteristics: i) In both LiFEA and LiETFSI, the ethylene oxide moiety efficiently captures Li+, resulting in a self‐folded structure and high T+ around 0.8. ii) For LiFEA, a Li−N bond (2.069 Å) is revealed by single crystal X‐ray diffraction, indicating that the FEA anion possesses a high donor number (DN) and thus an intensive interphase "self‐cleaning" function for an ultra‐thin and compact SEI. iii) Starting from LiFEA, an electron‐withdrawing sulfone group is introduced near the N atom. The distance of Li−N is tuned from 2.069 Å in LiFEA to 4.367 Å in LiETFSI. This alteration enhances ionic separation, achieves a more balanced DN, and tunes the self‐cleaning intensity for a reinforced SEI. Consequently, the fast charging/discharging capability of LMBs is progressively improved. This rationally tuned anion chemistry reshapes the interactions among Li+, anions, and solvents, presenting new prospects for advanced LMBs. [ABSTRACT FROM AUTHOR]

The electrolytes for lithium metal batteries (LMBs) are plagued by a low Li+ transference number (T+) of conventional lithium salts and inability to form a stable solid electrolyte interphase (SEI). Here, we synthesized a self‐folded lithium salt, lithium 2‐[2‐(2‐methoxy ethoxy)ethoxy]ethanesulfonyl(trifluoromethanesulfonyl) imide (LiETFSI), and comparatively studied with its structure analogue, lithium 1,1,1‐trifluoro‐N‐[2‐[2‐(2‐methoxyethoxy)ethoxy)]ethyl]methanesulfonamide (LiFEA). The special anion chemistry imparts the following new characteristics: i) In both LiFEA and LiETFSI, the ethylene oxide moiety efficiently captures Li+, resulting in a self‐folded structure and high T+ around 0.8. ii) For LiFEA, a Li−N bond (2.069 Å) is revealed by single crystal X‐ray diffraction, indicating that the FEA anion possesses a high donor number (DN) and thus an intensive interphase "self‐cleaning" function for an ultra‐thin and compact SEI. iii) Starting from LiFEA, an electron‐withdrawing sulfone group is introduced near the N atom. The distance of Li−N is tuned from 2.069 Å in LiFEA to 4.367 Å in LiETFSI. This alteration enhances ionic separation, achieves a more balanced DN, and tunes the self‐cleaning intensity for a reinforced SEI. Consequently, the fast charging/discharging capability of LMBs is progressively improved. This rationally tuned anion chemistry reshapes the interactions among Li+, anions, and solvents, presenting new prospects for advanced LMBs. [ABSTRACT FROM AUTHOR]