| The chlor-alkali industry is the most basic chemical industrial process,and it has similarities with the current frontiers of electrolysis of seawater to produce hydrogen.Electrolytic water evolution reaction is carried out in a weak acid or weakly alkaline electrolyte.The electrolysis process in the chlor-alkali industry is carried out in a high concentration lye.Therefore,it is necessary to find a material which can perform well in high-concentration electrolyte.In recent years,nickel phosphide has become a research hotspot as a semiconductor electrode material.This thesis studies the preparation of nickel phosphide,especially high index surface phosphide nickel electrode materials.Based on the self-supporting electrode,a high-index surface phosphide was prepared by a simple phosphating,and the structure-activity relationship of the electrolyzed water process was systematically investigated.(1)Self-supporting nickel phosphide electrode materials were synthesized by vapor deposition method,and the effects of synthesis conditions on the synthesized products were investigated in detail.The experimental results show that the high-index surface Ni5P4electrode material can be prepared by using red phosphorus as phosphorus source at 500°C,which has high specific surface area and unique morphology.Compared with the Ni2P electrode material prepared by using sodium hypophosphite as the phosphorus source,the high index surface Ni5P4exhibits superior electrolysis hydrogen evolution performance due to its high index surface,and its initial overpotential in 1mol?dm-3alkali solution is only 30m V.The use of red phosphorus as a phosphorus source can produce a high-index surface Ni5P4electrode material with stable performance,which has high application value.(2)The high-index surface sulfur phosphide electrode material was synthesized by combining vapor deposition method and hydrothermal method,and the influence of sulfur dosage was investigated.The experimental results show that the high-index surface Ni5P4|S electrode material has improved hydrogen evolution performance after being doped into the sulfur atom,and has high activity in both acid and lye,and has high stability.Theoretical calculations show that the high-index crystal plane has high surface energy;after doping the sulfur atom,the adsorption Gibbs free energy(?GH*)of the hydrogen ion on the surface of Ni5P4|S is higher,so that the adsorption and desorption ability of hydrogen atoms on the electrode surface is balanced.(3)A cationically modified nickel phosphide electrode material was prepared by using a vapor deposition method to incorporate a second metal element into the metal source.The hydrogen evolution performance of the electrolyzed water in a high concentration lye was investigated in detail.The experimental results show that the introduction of a small amount of iron can significantly improve the hydrogen evolution performance of electrolytic water. |