Hydrogen is a clean energy source with high energy density and is considered the most promising alternative to traditional energy sources.Electrocatalytic hydrogen evolution(HER)is an ideal hydrogen production process,but Pt-type precious metal catalysts are expensive,so it is necessary to develop low-cost new HER catalysts.Molybdenum carbide(Mo2C),which has a unique electronic structure similar to the electronic construction of Pt,is considered the material with great potential to replace Pt as catalysts for HER.We use RF magnetron sputtering to prepare Mo2C films.The influences of differential process parameters on the optical properties and electrocatalytic hydrogen evolution properties of Mo2C films were studied.The films were modified by Ni doping to analyze the influence of Ni doping on the catalytic activity of Mo2C films.(1)Mo2C films with different structures were prepared by changing the CH4 flow rate and were annealed at 850℃to study the structure and optical properties of Mo2C films.The results indicate that the prepared Mo2C thin films exhibit semiconductor properties,and the optical bandgap decreases with the increase of the CH4 flow rate.After annealing at 850℃,the Mo2C recrystallization of the(002)crystal surface and the crystallinity of the film was significantly increased.At the same time,the PL emission intensity of Mo2C film decreases with the increase in the CH4 flow rate because the ratio of sp2/sp3 is regulated by the CH4 flow rate.(2)Mo2C thin films with different Mo/C ratios were prepared by adjusting the RF power of Mo and C targets.Study the structure and electrocatalytic hydrogen evolution performance of thin films.These Mo2C films show good catalytic activity in alkaline and acidic media.For Mo and C(power:200 W and 150 W)in an alkaline medium,the overpotential of 10 m A·cm-2current density is 190 m V,the slope of Tafel is only 86m V·dec-1,and the highest electrochemically active surface area is 80 F·cm-1.The enhanced catalytic activity was attributed to the improved charge transfer ability of the more rational Mo/C atom structure.(3)Mo2C thin films were prepared by changing the RF power of Mo2C targets.Study the effects of different power levels on the electrocatalytic hydrogen evolution performance.The results indicate that these thin film catalysts exhibit excellent electrocatalytic performance in acidic and alkaline media.Among them,Mo2C film with 250 W has 190 m V overpotential with a current density of 10 m A·cm-2and a Tafel slope of 111 m V·dec-1 in an alkaline medium.The higher Mo/C atom ratio of the Mo2C crystal structure was obtained by high-power sputtering,which enhanced the electron transport and charge transfer ability.(4)Mo2C films were modified by 0.5,1,and 2Ni doping to study the effect of Ni doping on electrocatalytic hydrogen evolution performance of Mo2C films.The results indicate that the appropriate amount of Ni-doped Mo2C thin films showed significantly enhanced HER activity in both acidic and alkaline media.The current density is 10m A·cm-2 of the 1 Ni-Mo2C film in an acidic medium,the overpotential is 201 m V,and the slope of Tafel is as low as 96 m V·dec-1.In alkaline,the corresponding overpotential is as low as 163 m V,and the Tafel slope is 107 m V·dec-1.The corresponding overpotential of 2 Ni-Mo2C in alkaline medium is as low as 155 m V.The Ni-doped Mo2C film has excellent electrochemistry stability.The strength of the Mo-H bond is optimized by Ni-doped adjustment of the electronic structure of Mo2C and the synergistic effect of vacancy in Mo2C,thus enhancing HER kinetics. |