As an efficient water treatment method for treating dilute solution systems, electrosorption is promising for the separation and recovery of organic compounds, wastewater treatment, and deep purification of water. Here, two types of UiO-66 samples were prepared using the solvothermal synthesis method, and the effects of different regulators on the microstructure of materials were compared using the various characterization methods. The electrochemical properties of the activated carbon and two types of materials were tested by cyclic voltammetry and AC impedance spectroscopy, and the desalination effect of the materials on phosphate was investigated. The UiO-66 material with uniform-size particles, smaller-size particles, and more surface adsorption sites exhibited better phosphate removal and adsorption capacity. It was found that the desalination process of the UiO-66 material is reversible, and the adsorbent material can be reused, which is advantageous for engineering applications.