Optimizing band structure of CoP nanoparticles via rich-defect carbon shell toward bifunctional electrocatalysts for overall water splitting

Transition-metal phosphides(TMPs)with high catalytic activity are widely used in the design of electrodes for water splitting.However,a major challenge is how to achieve the trade-off between activity and stability of TMPs.Herein,a novel method for synthesizing CoP nanoparticles encapsu-lated in a rich-defect carbon shell(CoP/DCS)is developed through the self-assembly of modified polycyclic aromatic molecules.The graft and removal of high-activity C-N bonds of aromatic molecules render the controllable design of crystallite defects of carbon shell.The density functional theory calculation indicates that the carbon defects with unpaired electrons could effectively tailor the band structure of CoP.Benefiting from the improved activity and corrosion resistance,the CoP/DCS delivers outstanding difunctional hydrogen evolution reaction(88 mV)and oxygen evolution reaction(251 mV)performances at 10 mA cm^(−2)current density.Furthermore,the coupled water electrolyzer with CoP/DCS as both the cathode and anode presents ultralow cell voltages of 1.49 V to achieve 10 mA cm^(−2)with long-time stability.This strategy to improve TMPs electrocatalyst with rich-DCS and heterogeneous structure will inspire the design of other transition metal compound electrocatalysts for water splitting.

Defect-rich and highly porous carbon nanosheets derived from Ti_(3)AlC_(2) MAX with good lithium storage properties

Defect-rich,highly porous two-dimensional carbon nanosheets(CNS) have attracted tremendous research interests in catalysis and environmental purification and other fields,because of their unique micromorphology,chemical stability and high specific surface area.Herein,in this work,we report a new solution to synthesize an ultrathin two-dimensional CNS with rich defects and abundant pores via two-step etching the Ti_(3)AlC_(2)with the help of I2and NaOH.The CNS thickness,specific surface area and pore volume could be all tunable by adding the amount of I2.And the highest specific surface area and pore volume of the synthesized 2D CNS can be achieved 1134.4 m^(2)/g and 0.80 cm^(3)/g,with a thickness of only 0.64 nm and a yield of 35.9%.When employed as the anodes for lithium-ion batteries,the synthesized CNS anodes exhibit good cycling and rate capabilities.This work provides a novel and facile strategy for synthesizing highly porous and defective 2D carbon materials with good lithium storage properties.