| Nitrate(NO3-)is found in almost all bodies of water and has the potential to harm the ecosystem,plants,animals,and people.As a result,it is critical to work on creating NO3-removal technology that is both safe and effective while also being ecologically friendly.In recent years,NO3-pollution in water has been addressed using biological procedures,physicochemical methods,chemical processes,electrochemical methods,and other technologies.Because of their simplicity,high denitrification efficiency,and low operation cost,zero-valent iron(ZVI)denitrification in chemical processes and electrochemical denitrification have gotten a lot of attention.Both tactics,on the other hand,have their own set of drawbacks.In ZVI denitrification,for example,nanometer-scale ZVI is often used,with ammonia nitrogen(NH4+-N)as the major product.Cathode materials are limiting the advancement of electrochemical denitrification technology.The composition of real wastewater is complex,resulting in an unsatisfactory electrochemical reduction efficiency.In order to increase denitrification efficiency and alleviate NO3-pollution,in this paper,the ZVI denitrification process was perfected,cathode materials with high reducing activity were developed,and the influence of common components in real wastewater on NO3-reduction were investigated.The specific research contents of the research are as follows:(1)150μm ZVI(ZVI150)was used as a reductant to remove NO3-and NH4+-N was removed by folding point chlorination in order to develop a suitable denitrification technology for large-scale application.The effects of the operating parameters of ZVI150 denitrification process on the NO3-reduction were systematically studied.And the corresponding kinetic models were established to describe the NO3-reduction process.The results were shown that when the p H=3.5 and n(ZVI150:NO3--N)=12.50,the efficiency of NO3--N reduction reached 97.8%.In the overdose of ZVI150,the reaction conformed to the nth-order kinetics.In the moderate amount of ZVI150,the reaction followed the pseudo-first-order reaction.In both cases,the pseudo-second-order adsorption kinetics had good applicability.Then,the optimum condition of folding point chlorination was studied.When n(Cl2:NH4+-N)=1.8 and p H=7.5,the concentration of NH4+-N was 3.7 mg/L in water.(2)A new type of Co3O4/Cu electrode was prepared by electrodeposition and calcination at high temperature.The preparation conditions of the electrode were optimized and the electrodes were characterized by SEM,EDS and XRD.In addition,the effects of operating conditions on NO3-reduction were studied.The results were shown that the Co3O4/Cu electrode which was prepared by electrodeposition of cobalt on a substrate for 10 min and then calcined at 500°C had large specific surface area,good crystallinity and high catalytic activity.Its reduction efficiency was 2.2,1.3 and 5.5 times that of Cu,Cu/Zn and Ti,respectively.After optimizing,the optimal electrolytic parameters were determined as follows:the initial concentration of NO3--N was 50 mg/L,the concentration of Cl-was 500 mg/L,the current density was 10 m A/cm2 and p H=7.0.After 60 min of electrolysis,the efficiencies of NO3--N reduction,NH4+-N generation and total nitrogen removal were 87.6%,34.7%and52.8%,respectively.(3)The real wastewater has complex components and different properties.Experiments without background interference are difficult to simulate the real situations.Therefore,the effects of operating parameters and common pollutants(e.g.PO43-,CO32-,Ca2+and organic matter)on the efficiency of NO3-reduction were investigated in water.After optimizing,the efficiency of NO3--N reduction reached 80.2%.In the existence of PO43-(more than 50 mg/L),NO3--N reduction was inhibited.This can be attributed to the competing adsorption of interference ions and NO3-in the surface of the electrode,and the density functional theory calculations proved this.The interference of PO43-can be alleviated by adding Ca2+to the solution,which was harmless to NO3-reduction.When studying the influence of organic compounds on NO3-reduction,glucose was selected as the target pollutant and chemical oxygen demand content was taken as the evaluation index.Because organic matter can be degraded by cathodic reduction or anodic oxidation in long-term electrolysis,the existence of organic matter also had a negative impact on NO3-reduction.Finally,2.5 L real wastewater was treated by electrochemical method.The feasibility and practical application of this method were illustrated from the aspects of reduction efficiency,operation cost,electrode stability and recycling efficiency.This work can lay a foundation for real wastewater treatment... |