Green Preparation Of Carbon-supported Manganese Oxides And Catalytic Enhancement Of ECWAO Reaction

Wet air oxidation technology is an advanced oxidation technology,but its application is limited because of its harsh conditions.The addition of catalyst greatly reduced the reaction conditions,so catalytic wet air oxidation（CWAO）came into being.However,the temperature and pressure of CWAO reaction are still higher than normal temperature and pressure.In order to reduce energy consumption and look for milder conditions,our research group applied the anode electric field to the CWAO process and proposed electro-assisted catalytic wet air oxidation（ECWAO）,which can further reduce the temperature and pressure required by CWAO.This activates O₂molecules at room temperature,thereby oxidizing organic pollutants.This paper mainly studies the green preparation and catalytic strengthening of carbon manganese oxide anode material carrier under the ECWAO system.The main work of this paper is as follows:Biomass is an important resource of functional carbon materials,and it is cheap and easy to obtain,so it has a broad application prospect.In this paper,self-supporting three-dimensional activated carbon felt（LSCF）was prepared from sponge sponge biomass,and then manganese oxide（Mn Ox）nanoparticles were loaded on the surface of LSCF by solution impregnation method and heat treatment process to prepare Mn Ox@LSCF composite material.The results show that the specific surface area of Mn Ox@LSCF composite is 120 m2 g-1,which contains a large number of mesopores,which is conducive to the adsorption of oxygen molecules and organic pollutants on the surface of the composite.In addition,the electrochemical oxidation of chemisorbed oxygen on Mn Ox surface showed effective activation of oxygen molecules.The prepared Mn Ox@LSCF composite material was used as the anode of ECWAO reaction to catalyze oxidation degradation of organic pollutants at room temperature.The material showed excellent catalytic activity.The mineralization efficiency of Bisphenol A（BPA）and Methylene blue（MB）can reach 92.3±1.2%and 304.0±7.3%in 120 min at+1.0 V（vs.SCE）potential.The mineralization efficiency of Ciprofloxacin（CIP）and Tetracycline（TC）reached 35.1±1.9%and 45.6±3.1%after 300 min,respectively.LSCF is a kind of energy saving and green carrier,which can replace industrial graphite felt（GF）as electrode carrier of ECWAO process metal catalyst.On the basis of the above studies,in order to further improve the catalytic performance of carbon manganese oxide,this paper took GF as the substrate,used CO ions to compound manganese oxidation,and prepared Mn O-Co O@Co/GF composite material,which was used as the anode of ECWAO reaction system.The catalytic performance of its degradation of organic pollutants at room temperature was investigated.The results show that Mn O-Co O@Co/GF composite anode has excellent catalytic performance in degrading sulfamethoxazole（SMX）.SMX was rapidly degraded within 150 min,and the total TOC removal rate was 78.1±3%.In the process of ECWAO,the composite catalyst of Mn O and Co O@Co has obvious synergistic effect on O₂activation and SMX degradation.Moreover,it has good catalytic activity,stability and durability as ECWAO electrode.