We developed a method to engineer well-distributed dicobalt phosphide (Co2P) nanoparticles encapsulated in N,P-doped graphene (Co2P@NPG) as electrocatalysts for hydrogen evolution reaction (HER). We fabricated such nanostructure by the absorption of initiator and functional monomers, including acrylamide and phytic acid on graphene oxides, followed by UV-initiated polymerization, then by adsorption of cobalt ions and finally calcination to form N,P-doped graphene structures. Our experimental results show significantly enhanced performance for such engineered nanostructures due to the synergistic effect from nanoparticles encapsulation and nitrogen and phosphorus doping on graphene structures. The obtained Co2P@NPG modified cathode exhibits small overpotentials of only -45 mV at 1 mA cm(-2), respectively, with a low Tafel slope of 58 mV dec(-1) and high exchange current density of 0.21 mA cm(-2) in 0.5 M H2SO4. In addition, encapsulation by N,P-doped graphene effectively prevent nanoparticle from corrosion, exhibiting nearly unfading catalytic performance after 30 h testing. This versatile method also opens a door for unprecedented design and fabrication of novel low-cost metal phosphide electrocatalysts encapsulated by graphene.

Potassium‐based energy storage devices (PESDs) are promising candidates for large‐scale energy storage applications owing to potassiums abundant in nature, the low standard redox potential (−2.93 V for K/K+ vs the standard hydrogen electrode) of potassium (K), and high ionic conductivity of K‐ion based electrolytes. However, lack of proper cathode and anode materials hinder practical applications of PESDs. In this work, carbon nanosheets doped with an ultrahigh content of nitrogen (22.7 at%) are successfully synthesized as an anode material for a K‐ion battery, which delivers a high capacity of 410 mAh g−1 at a current density of 500 mA g−1, which is the best result among the carbon based anodes for PESDs. Moreover, the battery exhibits an excellent cycling performance with a capacity retention of 70% after 3000 cycles at a high current density of 5 A g−1. In situ Raman, galvanostatic intermittent titration, and density functional theory calculations reveal that the ultrahigh N‐doped carbon nanosheet (UNCN) simultaneously combines the diffusion and pseudocapacitive mechanisms together, which remarkably improves its electrochemical performances in K‐ion storage. These results demonstrate the good potential of UNCNs as a high‐performance anode for PESDs.

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