硝基酚生物電化學(xué)還原性能與其結(jié)構(gòu)的關(guān)系探究
發(fā)布時(shí)間：2018-10-16 17:57
【摘要】：本研究通過搭建生物電化學(xué)體系(BES),考察了不同陰極電位、pH值等參數(shù)條件下4-硝基酚(PNP)、2,4-二硝基酚(DNP)、2,4,6-三硝基酚(TNP)的還原情況,探究了其可能產(chǎn)生的還原產(chǎn)物,并對(duì)還原規(guī)律進(jìn)行了對(duì)比分析。當(dāng)采用不同電極材料對(duì)PNP進(jìn)行還原時(shí),采用石墨顆粒作為電極的BES無論是PNP去除效果還是PAP生成效果,均優(yōu)于采用石墨氈作為電極的BES。硝基酚的還原效果受電極材料的比表面積、內(nèi)阻等因素影響巨大,比表面積越大,內(nèi)阻越小,則硝基酚的還原效果越好。在本研究所采用的生物電化學(xué)體系中,PNP.DNP.TNP等三種硝基酚均發(fā)生了還原。其中PNP的還原產(chǎn)物是PAP,且PAP相對(duì)穩(wěn)定,在BES陰極未發(fā)生進(jìn)一步轉(zhuǎn)化；DNP的最終還原產(chǎn)物DAP極不穩(wěn)定,無法檢出,出水中僅檢測到中間還原產(chǎn)物2-A-4-NP;TNP在該體系中首先被還原為中間還原產(chǎn)物2-A-4,6-DNP,其中絕大部分又被進(jìn)一步還原為未知還原產(chǎn)物。PNP.DNP的急性毒性經(jīng)還原處理后可以得到一定程度的改善,而TNP經(jīng)還原后急性毒性有所上升,表明TNP的還原產(chǎn)物急性毒性比TNP更強(qiáng)。硝基酚的去除效率及去除速率隨陰極電位的降低而逐漸增大,說明較低的陰極電位更有利于硝基酚的還原；硝基酚的去除效率及去除速率隨pH值的升高而降低,表明硝基酚的還原情況與溶液中H+的多少密切相關(guān),pH越低越有利于硝基酚的還原。酸性條件下,NPs去除效率大小關(guān)系依次為：PNPDNPTNP;堿性條件下,NPs去除效率大小關(guān)系依次為：DNPTNPPNP。實(shí)驗(yàn)表明,NPs生物電化學(xué)還原性能的強(qiáng)弱與其結(jié)構(gòu)上氮原子的電子云密度、其在水溶液中的離子化程度以及硝基數(shù)量等多種因素有關(guān)。
[Abstract]:In this study, the reduction of 4-nitrophenol (PNP), _ 2N _ 2H _ 2N _ 2N _ 2N _ 2N _ 2N _ 2N _ 4N _ 4N _ 6 _ 3-trinitrophenol (TNP) under different cathodic potential and pH values was investigated by means of a bioelectrochemical system (BES), and the possible reduction products were investigated. The law of reduction was compared and analyzed. When different electrode materials are used to reduce PNP, BES with graphite particles as electrode is better than BES. with graphite felt as electrode, regardless of PNP removal effect or PAP formation effect. The reduction effect of nitrophenol is greatly affected by the specific surface area and internal resistance of the electrode material. The larger the specific surface area is, the smaller the internal resistance is, the better the reduction effect of nitrophenol is. In the bioelectrochemical system, three kinds of nitrophenol, such as PNP.DNP.TNP, were reduced. The reduction product of PNP is PAP, and PAP is relatively stable, and no further transformation occurs in the BES cathode, DAP, the final reduction product of DNP, is very unstable and can not be detected. Only the intermediate reduction product 2-A-4-NPNP-TNP was first reduced to the intermediate product 2-A-4-NP6-DNPs in the effluent, and most of them were further reduced to unknown reductive products. The acute toxicity of PNP.DNP could be improved to some extent after reduction. However, the acute toxicity of TNP increased after reduction, indicating that the acute toxicity of TNP was stronger than that of TNP. The removal efficiency and removal rate of nitrophenol gradually increased with the decrease of cathode potential, which indicated that the lower cathode potential was more favorable to the reduction of nitrophenol, and the removal efficiency and removal rate of nitrophenol decreased with the increase of pH value. It is shown that the reduction of nitrophenol is closely related to the amount of H in the solution, and the lower the pH is, the more favorable the reduction of nitrophenol is. Under acidic conditions, the relation of removal efficiency of NPs is as follows: under the condition of PNPDNPTNP; alkalinity, the relation of removal efficiency of NPs is DNPTNPPNP.. The experimental results show that the bioelectrochemical reduction performance of NPs is related to the electron cloud density of nitrogen atoms in the structure, the degree of ionization in aqueous solution and the amount of nitro.
【學(xué)位授予單位】：南京理工大學(xué)
【學(xué)位級(jí)別】：碩士
【學(xué)位授予年份】：2015
【分類號(hào)】：O657.1;X703
本文編號(hào)：2275182
[Abstract]:In this study, the reduction of 4-nitrophenol (PNP), _ 2N _ 2H _ 2N _ 2N _ 2N _ 2N _ 2N _ 2N _ 4N _ 4N _ 6 _ 3-trinitrophenol (TNP) under different cathodic potential and pH values was investigated by means of a bioelectrochemical system (BES), and the possible reduction products were investigated. The law of reduction was compared and analyzed. When different electrode materials are used to reduce PNP, BES with graphite particles as electrode is better than BES. with graphite felt as electrode, regardless of PNP removal effect or PAP formation effect. The reduction effect of nitrophenol is greatly affected by the specific surface area and internal resistance of the electrode material. The larger the specific surface area is, the smaller the internal resistance is, the better the reduction effect of nitrophenol is. In the bioelectrochemical system, three kinds of nitrophenol, such as PNP.DNP.TNP, were reduced. The reduction product of PNP is PAP, and PAP is relatively stable, and no further transformation occurs in the BES cathode, DAP, the final reduction product of DNP, is very unstable and can not be detected. Only the intermediate reduction product 2-A-4-NPNP-TNP was first reduced to the intermediate product 2-A-4-NP6-DNPs in the effluent, and most of them were further reduced to unknown reductive products. The acute toxicity of PNP.DNP could be improved to some extent after reduction. However, the acute toxicity of TNP increased after reduction, indicating that the acute toxicity of TNP was stronger than that of TNP. The removal efficiency and removal rate of nitrophenol gradually increased with the decrease of cathode potential, which indicated that the lower cathode potential was more favorable to the reduction of nitrophenol, and the removal efficiency and removal rate of nitrophenol decreased with the increase of pH value. It is shown that the reduction of nitrophenol is closely related to the amount of H in the solution, and the lower the pH is, the more favorable the reduction of nitrophenol is. Under acidic conditions, the relation of removal efficiency of NPs is as follows: under the condition of PNPDNPTNP; alkalinity, the relation of removal efficiency of NPs is DNPTNPPNP.. The experimental results show that the bioelectrochemical reduction performance of NPs is related to the electron cloud density of nitrogen atoms in the structure, the degree of ionization in aqueous solution and the amount of nitro.
【學(xué)位授予單位】：南京理工大學(xué)
【學(xué)位級(jí)別】：碩士
【學(xué)位授予年份】：2015
【分類號(hào)】：O657.1;X703
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