MO_x電極的制備與改性及電催化氧化有機(jī)廢水的研究
發(fā)布時(shí)間:2019-06-17 12:51
【摘要】:本文利用靜電紡絲法制備了單組份金屬氧化物電極,用于電催化有機(jī)廢水,對(duì)其催化活性進(jìn)行篩選。對(duì)優(yōu)選的單組份金屬氧化物電極進(jìn)行雙組份混紡,制備出雙金屬?gòu)?fù)合電極和稀土金屬鈰改性的SnO2電極,電催化氧化有機(jī)廢水。通過掃描電子顯微鏡(SEM)、X射線衍射(XRD)、線性掃描伏安法(LSV)和循環(huán)伏安法(CV)等手段對(duì)制備所得的電極材料的形貌、結(jié)構(gòu)及其電化學(xué)性能進(jìn)行了表征。通過紫外分光光度法(UV)、化學(xué)需氧量(COD)和總有機(jī)碳分析(TOC)對(duì)電極的催化性能進(jìn)行評(píng)價(jià)。本文中以苯酚、亞甲基藍(lán)和剛果紅為模型污染物,初始濃度為200mg/L,0.25mol/L的NaN03為電解質(zhì),電流密度為30 mA/cm2,極板間的距離為2 cm,溶液初始pH為7的體系下電催化處理280 min。本研究主要分三個(gè)部分:單組份金屬的篩選;Co(Fe)-SnO2復(fù)合電極的制備與電催化性能研究;Ce改性SnO2電極的制備及電催化性能的研究。得到的主要結(jié)論如下:(1)用靜電紡絲法制備的單組份金屬氧化物電極(SnO2、Co3O4、Fe2O3、MnOx、CuO);通過SEM、XRD和電化學(xué)表征,可以得出SnO2電極,其纖維表面連續(xù),直徑較細(xì),且分布均勻,析氧電位高。通過紫外分光光度法(UV)、化學(xué)需氧量(COD)和總有機(jī)碳分析(TOC)對(duì)電極的催化性能進(jìn)行評(píng)價(jià);可以得出SnO2電極分別在電催化苯酚廢水、亞甲基藍(lán)廢水和剛果紅廢水中具有較高的電催化活性。綜上可以得出在單組份金屬氧化物電極催化活性的篩選中SnO2電極優(yōu)越。(2)對(duì)SnO2電極的制備條件和電催化條件進(jìn)行優(yōu)化。通過改變升溫速率、煅燒溫度、電流密度、環(huán)境溫度和溶液的初始pH值。實(shí)驗(yàn)結(jié)果表明:升溫速率為3 ℃/min,煅燒溫度為550℃時(shí),SnO2電極的催化效果最好,亞甲基藍(lán)廢水的脫除率、COD的去除率和TOC的去除率分別為93.2%、66.3%和75.2%。電流密度為40 mA/cm2,環(huán)境溫度為40℃和溶液初始pH值為5具有最好的催化效果。(3)通過在紡絲液中摻雜不同量的C10H14CoO4(C15H21FeO6)和SnCl4·5H2O制備出Co(Fe)-SnO2復(fù)合電極;在摻雜C10H14CoO4的量與SnCl4·5H2O的質(zhì)量之比為50%條件下,Co-SnO2電極的亞甲基藍(lán)脫除率、COD去除率和TOC去除率分別為94.5%、66.4%和77.4%;在摻雜C15H21Fe06的量與SnCl4·5H20的質(zhì)量之比為75%時(shí),Fe-Sn02電極的亞甲基藍(lán)脫除率、COD去除率和TOC去除率分別為93.9%、63.2%和74.2%。綜上可以得出,Co-SnO2復(fù)合電極和Fe-Sn02復(fù)合電極的電催化活性均比單組份金屬的SnO2、Co3O4和Fe2O3電極催化活性高。(4)摻雜Ce(N03)3·6H2O對(duì)SnO2電極進(jìn)行改性,制備了Ce改性的Sn02電極作為陽(yáng)極電催化處理亞甲基藍(lán)廢水;在摻雜硝酸鈰的量與五水四氯化錫的質(zhì)量比為3%條件下,Ce改性SnO2電極的電催化活性最高,亞甲基藍(lán)廢水脫除率、COD去除率和TOC去除率分別為95.2%、67.7%和79.2%。
[Abstract]:In this paper, one-component metal oxide electrode was prepared by electrospinning method, which was used to screen the catalytic activity of electrocatalytic organic wastewater. The bimetallic composite electrode and rare earth cerium modified SnO2 electrode were prepared by two-component blending of the optimized one-component metal oxide electrode to electrocatalytic oxidation of organic wastewater. The morphology, structure and electrochemical properties of the prepared electrode materials were characterized by scanning electron microscope (SEM),) X-ray diffraction (XRD), linear scanning Voltammetric method (LSV) and cyclic Voltammetric method (CV). The catalytic performance of the electrode was evaluated by UV spectrophotometry (UV), chemical oxygen demand (COD) and total organic carbon analysis (TOC). In this paper, phenol, methylene blue and Congo red were used as model pollutants, the initial concentration was 200 mg 路L, 0.25 mol 路L NaN03 was used as electrolyte, and the current density was 30 mA/cm2,. The distance between the plates was 2 cm,. The initial pH was 7. The electrocatalytic treatment of 280 min. was carried out. This study is divided into three parts: the preparation and electrocatalytic performance of; Co (Fe)-SnO2 composite electrode and the preparation and electrocatalytic performance of Ce modified SnO2 electrode. The main conclusions are as follows: (1) one-component metal oxide electrode (SnO2,Co3O4,Fe2O3,MnOx,CuO) prepared by electrospinning can be obtained by SEM,XRD and electrochemical characterization. The fiber surface of SnO2 electrode is continuous, the diameter is fine, and the distribution is uniform, and the oxygen evolution potential is high. The catalytic performance of (UV), chemical oxygen demand (COD) and total organic carbon analysis (TOC) was evaluated by UV spectrophotometry, and it was concluded that SnO2 electrode had high electrocatalytic activity in electrocatalytic phenol wastewater, methylene blue wastewater and Congo red wastewater, respectively. In summary, it can be concluded that SnO2 electrode is superior in the screening of catalytic activity of one-component metal oxide electrode. (2) the preparation and electrocatalytic conditions of SnO2 electrode are optimized. By changing the heating rate, calcination temperature, current density, ambient temperature and the initial pH value of the solution. The experimental results show that when the heating rate is 3 鈩,
本文編號(hào):2501000
[Abstract]:In this paper, one-component metal oxide electrode was prepared by electrospinning method, which was used to screen the catalytic activity of electrocatalytic organic wastewater. The bimetallic composite electrode and rare earth cerium modified SnO2 electrode were prepared by two-component blending of the optimized one-component metal oxide electrode to electrocatalytic oxidation of organic wastewater. The morphology, structure and electrochemical properties of the prepared electrode materials were characterized by scanning electron microscope (SEM),) X-ray diffraction (XRD), linear scanning Voltammetric method (LSV) and cyclic Voltammetric method (CV). The catalytic performance of the electrode was evaluated by UV spectrophotometry (UV), chemical oxygen demand (COD) and total organic carbon analysis (TOC). In this paper, phenol, methylene blue and Congo red were used as model pollutants, the initial concentration was 200 mg 路L, 0.25 mol 路L NaN03 was used as electrolyte, and the current density was 30 mA/cm2,. The distance between the plates was 2 cm,. The initial pH was 7. The electrocatalytic treatment of 280 min. was carried out. This study is divided into three parts: the preparation and electrocatalytic performance of; Co (Fe)-SnO2 composite electrode and the preparation and electrocatalytic performance of Ce modified SnO2 electrode. The main conclusions are as follows: (1) one-component metal oxide electrode (SnO2,Co3O4,Fe2O3,MnOx,CuO) prepared by electrospinning can be obtained by SEM,XRD and electrochemical characterization. The fiber surface of SnO2 electrode is continuous, the diameter is fine, and the distribution is uniform, and the oxygen evolution potential is high. The catalytic performance of (UV), chemical oxygen demand (COD) and total organic carbon analysis (TOC) was evaluated by UV spectrophotometry, and it was concluded that SnO2 electrode had high electrocatalytic activity in electrocatalytic phenol wastewater, methylene blue wastewater and Congo red wastewater, respectively. In summary, it can be concluded that SnO2 electrode is superior in the screening of catalytic activity of one-component metal oxide electrode. (2) the preparation and electrocatalytic conditions of SnO2 electrode are optimized. By changing the heating rate, calcination temperature, current density, ambient temperature and the initial pH value of the solution. The experimental results show that when the heating rate is 3 鈩,
本文編號(hào):2501000
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