本文關(guān)鍵詞： 酚類有機(jī)廢水 Cu-MOFs GrO/HKUST-1復(fù)合組分 催化濕式過氧化氫氧化 羥基自由基　出處：《東南大學(xué)》2016年碩士論文　論文類型：學(xué)位論文

【摘要】：隨著化工行業(yè)的發(fā)展,酚類有機(jī)廢水的排放日益增多,導(dǎo)致嚴(yán)重的環(huán)境污染,使得酚類有機(jī)廢水的處理備受關(guān)注。催化濕式過氧化氫氧化技術(shù)因較溫和的操作條件和較好降解效果,成為酚類有機(jī)廢水處理的研究熱點。MOFs材料因具有較大的比表面積和規(guī)整可控的孔結(jié)構(gòu)使其在催化領(lǐng)域表現(xiàn)出較好的應(yīng)用前景。將Cu-MOFs作為非均相催化劑應(yīng)用于濕式催化氧化苯酚廢水,有著其它催化劑無法媲美的優(yōu)勢。本文采用溶劑熱法制備了HKUST-1和Cu(BDC)兩種不同的Cu-MOFs材料。HKUST-1和Cu(BDC)分別為八面體結(jié)構(gòu)和六面體結(jié)構(gòu)。且Cu在兩種MOFs中的含量分別為24.18%,15.21%。分別將兩種Cu-MOFs作為非均相催化劑,以H202為氧化劑,來催化降解苯酚廢水�？疾炝朔磻�(yīng)溫度、催化劑用量、H202用量、苯酚廢水的pH等條件對Cu-MOFs催化降解苯酚的影響。此外還研究了Cu-MOFs的重復(fù)利用性能和穩(wěn)定性,初步考查了其催化降解機(jī)理。結(jié)果表明：Cu(BDC)骨架表現(xiàn)出比HKUST-1骨架更好的催化活性,當(dāng)溫度為60℃,H2O2用量為1.0 mL, Cu(BDC)的用量為20 mg,苯酚溶液的初始pH為6.65時,Cu(BDC)催化降解苯酚達(dá)到最佳效果,此時,苯酚的轉(zhuǎn)化率為99%,COD的去除率為93%。重復(fù)利用兩次后,Cu(BDC)骨架仍然能保持較好的催化活性,苯酚的轉(zhuǎn)化率能達(dá)到99%,COD的去除率能達(dá)到85%以上。類似于其它催化劑,Cu(BDC)濕式催化氧化苯酚也是遵循羥基自由基機(jī)理。并且Cu(BDC)表現(xiàn)出較好的穩(wěn)定性,Cu2+的浸出量僅為7ppm。本文采用溶劑熱法合成了GrO含量分別為1wt%,3 wt%和5wt%的GrO/HKUST-1復(fù)合組分,并分別將其作為非均相催化劑進(jìn)行苯酚的催化降解。結(jié)果表明：加入GrO后沒有阻止HKUST-1骨架的形成,大部分的HKUST-1晶體仍然保持八面體結(jié)構(gòu),且GrO附著在HKUST-1晶體的表面。隨著GrO摻雜量的增加,所形成的GrO/HKUST-1復(fù)合組分催化劑對苯酚的催化降解活性先提高后降低。當(dāng)GrO的含量為3wt%時,GrO-3/HKUST-1復(fù)合組分催化劑的活性最高。較高的溫度有利于GrO-3/HKUST-1復(fù)合組分催化劑催化氧化苯酚。GrO-3/HKUST-1復(fù)合組分催化劑在pH=4-9內(nèi)都表現(xiàn)出較好的催化活性,表明GrO-3/HKUST-1復(fù)合組分催化劑具有較強(qiáng)的抗酸堿性能。摻雜GrO后,GrO-3/HKUST-1復(fù)合組分催化劑具有較好的重復(fù)利用性能,且GrO-3/HKUST-1催化降解苯酚依然依賴于羥基自由基。
[Abstract]:With the development of chemical industry, the discharge of phenolic organic wastewater is increasing day by day, resulting in serious environmental pollution. The treatment of phenolic organic wastewater has attracted much attention. Catalytic wet hydrogen peroxide oxidation technology is more effective because of mild operation conditions and better degradation effect. Because of its large specific surface area and regular and controllable pore structure, MOFs have a good application prospect in the field of catalysis. Homogeneous catalyst is used in wet catalytic oxidation of phenol wastewater. In this paper, two different kinds of Cu-MOFs materials, HKUST-1 and CuBDC, were prepared by solvothermal method. HKUST-1 and Cu( 2) were prepared by solvothermal method. BDC is octahedron and hexahedron respectively, and the content of Cu in the two kinds of MOFs is 24.18%. 15.21. two kinds of Cu-MOFs were used as heterogeneous catalysts and H202 as oxidant to catalyze the degradation of phenol wastewater. The reaction temperature and the amount of catalyst were investigated. The effect of pH of phenol wastewater on the degradation of phenol catalyzed by Cu-MOFs was studied. The reusability and stability of Cu-MOFs were also studied. The catalytic degradation mechanism of the catalyst was investigated. The results showed that the HKUST-1 skeleton exhibited better catalytic activity than the HKUST-1 skeleton, and the amount of H _ 2O _ 2 was 1.0 mL at 60 鈩，

本文編號：1457972