改性生物質(zhì)材料制備及對(duì)水中砷吸附性能與處理工藝研究
[Abstract]:In order to cope with the arsenic pollution incidents in the water environment, it has become a practical demand to develop high flow rate, low flow resistance and low cost emergency adsorption materials. Adsorption properties and adsorption mechanism were discussed. Modified wood chips were used as adsorption materials to establish adsorption fixed bed process and adsorption-ultrafiltration combined process, respectively, to provide technical support for the removal of arsenic in water. The optimized preparation conditions were as follows: the ratio of sawdust to epichlorohydrin was 1:3 (that is, 3 L epichlorohydrin per kg of sawdust), the ratio of sawdust to diethylenetriamine was 1:1 (that is, 1 L diethylenetriamine per kg of sawdust), the etherification temperature was 90 C, the etherification reaction was 60 min, and the cross-linking reaction was trans-linked. The results showed that the etherification reaction temperature and the dosage of etherifying agent were the key factors in the preparation of the adsorbent. The optimum pH range of the modified wood chip adsorbent was 5-6, and the maximum adsorption capacity of As (III) and As (V) was 13.2 and 46.1 mg/g, respectively, which were better than those reported in literature. Result: The modified coffee cellulose adsorbent material was prepared by using coffee residue as matrix, pretreated with sodium hydroxide solution, rinsed and extracted repeatedly with 5% sodium hypochlorite solution, polyethylenimine (PEI) as ammoniating agent, glutaraldehyde as crosslinking agent, and complexed with Fe (III). The reaction time was 120 min, the concentration of glutaraldehyde was 0.1%, the crosslinking reaction time was 240 min, and the concentration of Fe (NO3) 3 solution was 500 mg/L. Unlike the modified sawdust adsorption material, the modified coffee cellulose complex with Fe (III) did not use alkali aging method to load iron oxide, because the complex Fe (III) could significantly increase the content of Caffee. The Zeta potential on the surface of enkephalin cellulose can better realize the adsorption of As (V). Weak acidity conditions are favorable for the adsorption of As (V). The maximum adsorption capacity of modified coffee cellulose for As (V) is 91 mg/g. After adsorbing As (V), the modified coffee cellulose can also achieve the continuous adsorption of Cu (II) in water, and the maximum adsorption capacity of Cu (II) can reach the maximum. To 200 mg/L, the adsorption processes of the two modified biomass materials were modeled and the adsorption mechanism of arsenic in water was discussed according to the characteristics of the two modified biomass materials. The Langmuir model showed that the adsorption of arsenic on the surface of the two modified biomass materials was a chemical adsorption process. The Langmuir model showed that the adsorption of arsenic on the surface of the two modified biomass materials was monolayer chemical adsorption. The larger proportion of internal mass transfer coefficient [kLa] D in total mass transfer coefficient [kLa] g indicates that the main mass transfer resistance comes from the physicochemical reaction between arsenic and the surface active adsorption sites of modified sawdust, as well as the diffusion of arsenic into the pores of adsorption materials; for modified coffee cellulose, the main mass transfer resistance comes from As (V) and modified coffee. The adsorption mechanism of arsenic in water was discussed based on the characteristics of two modified biomass materials. The results showed that the adsorption of As (III) by iron oxides loaded on wood chips played a major role, while the adsorption of As (V) by grafted amino groups played a major role. The Zeta potential on the surface of the adsorbent material was significantly increased by grafting amino group and complexing ferric ion, and the adsorption effect of As (V) and Cu (II) on the modified coffee cellulose surface was greatly improved. The continuous adsorption of As (V) and Cu (II) on the modified coffee cellulose surface was the result of the interaction of electrostatic attraction and surface complexation reaction. The adsorption process was fitted and analyzed by dynamic adsorption model. The results of Thomas model showed that when the initial concentration of total arsenic was 10 mg/L and the flow rate was 4.8 mL/min, the modified sawdust filter bed was saturated. The adsorption capacity reached 15.6 mg/g; BDST model fitting results showed that the maximum dynamic adsorption rate constant of modified sawdust reached 3.13 *10-4 L/min.mg, and the difference between model fitting value and measured value of fixed bed penetration time was very small, indicating that BDST model can better predict the filter bed penetration time to saturation under different column heights. A combined process of adsorption and ultrafiltration was designed to remove arsenic pollutants effectively and separate adsorbents saturated by adsorption. The experimental results show that aeration stirring can not only make the mixture of adsorbents more uniform in the reactor, but also increase the dissolution of adsorbents in water. The removal efficiency of total arsenic in simulated arsenic-containing surface water was studied. When the initial concentration of total arsenic was 0.1 mg/L, the concentration of arsenic in effluent treated by the combined process was better than that of the environmental quality standard of class I surface water. Material adsorption materials and adsorption process are suitable for emergency treatment of arsenic contamination in water environment.
【學(xué)位授予單位】:哈爾濱工業(yè)大學(xué)
【學(xué)位級(jí)別】:博士
【學(xué)位授予年份】:2017
【分類號(hào)】:X52
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