【摘要】：生化法對(duì)實(shí)際煤化工廢水中的難降解有機(jī)污染物降解效果差,使得生化出水水質(zhì)很難達(dá)標(biāo)。因而,一種可靠的深度處理方法對(duì)煤化工生化二級(jí)出水進(jìn)行再處理是十分必要的。濕式H2O2催化氧化技術(shù)(Catalytic Wet Peroxide Oxidation,CWPO)作為一種深度處理方法,微波技術(shù)作為一項(xiàng)成熟的高效低成本能量供給技術(shù),二者結(jié)合所形成的微波輔助催化濕式雙氧水氧化工藝(MWCWPO),給深度處理難降解工業(yè)廢水提供了新思路。本研究以銅鎳為活性組分,顆粒活性炭為載體,分別以浸漬法和沉淀法制備了CuOx-NiO/AC負(fù)載型催化劑,通過(guò)MWCWPO體系對(duì)喹啉的降解實(shí)驗(yàn)優(yōu)化和比較了兩種方法制備負(fù)載型催化劑的催化性能,并通過(guò)一系列表征手段進(jìn)一步研究了催化劑制備方法對(duì)催化劑結(jié)構(gòu)的影響。實(shí)驗(yàn)結(jié)果顯示,沉淀法制備的催化劑對(duì)污染物降解效果更好,并確定了沉淀法制備負(fù)載型催化劑的最佳條件為:浸漬液硝酸銅和硝酸鎳的混合濃度為0.2 mol/L,沉淀劑氨水的濃度為0.25 mol/L,硝酸銅和硝酸鎳活性組分配比為4:1,沉淀劑投加方式為逆加法,焙燒溫度為300℃,焙燒時(shí)間為4 h。對(duì)負(fù)載型催化劑進(jìn)行表征分析后,發(fā)現(xiàn)由沉淀法制備的負(fù)載型催化劑活性組分晶粒更小,晶粒在顆粒活性炭中分布更加均勻,催化劑比表面積更大,表面化學(xué)吸附氧更多,是導(dǎo)致沉淀法制備負(fù)載型催化劑催化性能更好的主要原因。通過(guò)HFSS電磁模擬仿真軟件對(duì)不同的微波腔體結(jié)構(gòu)形式進(jìn)行了微波分布均勻性分析,并對(duì)微波反應(yīng)器腔體進(jìn)行結(jié)構(gòu)優(yōu)化。研究表明負(fù)載水中微波均勻性大小的腔體結(jié)構(gòu)為圓柱形微波腔體八面體微波腔體矩形微波腔體,優(yōu)化后微波裝置對(duì)污染物的去除效果更優(yōu)。研究證明了MWCWPO工藝的優(yōu)越性,發(fā)現(xiàn)反應(yīng)溫度和有效水力停留時(shí)間為MWCWPO工藝的主要控制條件,得到最佳反應(yīng)溫度和有效水力停留時(shí)間分別為60℃和1.12 min,微波功率(200~600 W)和催化劑投加量(50~200 g)在一定范圍內(nèi)對(duì)MWCWPO體系影響不大,處理后出水COD值為34 mg/L,滿足《污水綜合排放標(biāo)準(zhǔn)》(GB8978-1996)一級(jí)標(biāo)準(zhǔn)。催化劑在連續(xù)流實(shí)驗(yàn)中銅鎳離子溶出量遠(yuǎn)低于排放標(biāo)準(zhǔn),連續(xù)使用7次后,體系對(duì)TOC的去除率下降5%,催化劑穩(wěn)定性高。為了提高M(jìn)WCWPO反應(yīng)器對(duì)廢水的處理量,設(shè)計(jì)處理量為10 t/d的微波反應(yīng)器,并對(duì)微波反應(yīng)器的直徑、高度、微波源的數(shù)目、微波腔體尺寸進(jìn)行了模擬優(yōu)化,構(gòu)建出了微波反應(yīng)器系統(tǒng),為工業(yè)微波催化氧化中試裝置提供參考。
[Abstract]:The biochemistry method has a poor effect on the degradation of organic pollutants in actual coal chemical wastewater, which makes the quality of biochemical effluent difficult to reach the standard. Therefore, it is necessary to retreat the secondary effluent from coal chemical industry by a reliable advanced treatment method. Wet H2O2 catalytic oxidation technology (Catalytic Wet Peroxide Oxidation,CWPO) as an advanced treatment method, microwave technology as a mature high efficiency and low cost energy supply technology, The microwave-assisted catalytic wet hydrogen peroxide oxidation process (MWCWPO),) formed by the combination of the two provides a new idea for advanced treatment of refractory industrial wastewater. In this study, CuOx-NiO/AC supported catalysts were prepared by impregnation method and precipitation method using copper and nickel as active component and granular activated carbon as carrier, respectively. The catalytic properties of the supported catalysts prepared by MWCWPO system were optimized and compared by the degradation experiments of quinoline. The influence of the preparation methods on the structure of the catalysts was further studied by a series of characterization methods. The results showed that the catalyst prepared by precipitation method had better degradation effect on pollutants. The optimum conditions for the preparation of supported catalyst by precipitation method were determined as follows: the mixed concentration of copper nitrate and nickel nitrate was 0. 2 mol/L, the concentration of ammonia water was 0. 25 mol/L, the distribution ratio of copper nitrate and nickel nitrate was 4: 1, and the precipitation agent was added. The way of addition is inverse addition, The calcination temperature is 300 鈩，

本文編號(hào)：2223572