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石墨烯基尖晶石型金属氧化物复合物的制备及其催化过硫酸盐降解双酚A的研究
论文作者:童鞋论文网  论文来源:www.txlunwenw.com  发布时间:2019/9/4 7:57:57  

摘要:作为一种典型的内分泌干扰物,废水中的双酚A(BPA)对人类和自然环境危害极大。近年来,基于硫酸根自由基(SO4–·)的高级氧化技术因其独特优势备受关注,该技术利用固体催化剂活化过硫酸盐(PS)来实现BPA的有效降解,从而降低其对人类和环境的危害。目前,石墨烯基尖晶石型金属氧化物复合物在催化领域得到了广泛研究,石墨烯和尖晶石型金属氧化物颗粒间的协同作用赋予复合物优异的催化性能。本研究采用石墨烯基尖晶石金属氧化物复合物活化PS产生SO4–·,来氧化降解BPA,并用液相色谱法对氧化反应进行跟踪。主要研究内容如下:

(1) 通过水热法成功制备了锡酸镍(Ni2SnO4)、锡酸镍/还原氧化石墨烯(Ni2SnO4-RGO5)复合物,并将其用作非均相活化过硫酸盐的催化剂。通过X-射线衍射(XRD)、红外吸收光谱(FTIR)、场发射扫描电子显微镜(SEM)和透射电子显微镜(TEM)等表征证明了RGO抑制了Ni2SnO4纳米颗粒的团聚,提高了复合物催化性能。同时,Cl–、NO3–、HCO3–的存在均促进了Ni2SnO4对BPA的催化降解,而Cl–和HCO3–抑制了Ni2SnO4-RGO5对BPA的催化降解;NO3–对Ni2SnO4-RGO5催化降解BPA没有产生影响,而H2PO4–极大地抑制了Ni2SnO4和Ni2SnO4-RGO5对BPA的催化降解。相较于Ni2SnO4,pH对Ni2SnO4-RGO5催化降解BPA的影响较小。与Ni2SnO4相比,Ni2SnO4-RGO5复合物四次循环后仍保持较高的催化活性,Ni2SnO4-RGO5复合物具有更加优异的稳定性。此外,自由基捕获实验显示,羟基自由基·OH和SO4–·在Ni2SnO4/PS、NiSn2O4-RGO5/PS两个体系中均参与了BPA的氧化过程,且SO4–·在氧化过程中起主导作用。

(2) 采用水热法成功制备了钴酸锌/还原氧化石墨烯(ZnCo2O4-RGO5)复合物,通过XRD、FTIR、SEM和TEM等手段对复合物的形貌结构进行了分析,结果表明RGO为ZnCo2O4纳米颗粒的生长提供了成核位点,并抑制了纳米颗粒的团聚。同时,探究了不同反应条件如RGO含量、反应温度、BPA初始浓度、反应液的pH和阴离子等对ZnCo2O4-RGO5催化氧化BPA的影响。实验结果表明,0.02 g的ZnCo2O4-RGO5复合物在25 °C、pH = 7的条件下,20 min可将50 mL的0.10 mM的BPA溶液完全降解。Cl–、NO3–的存在对ZnCo2O4-RGO5催化降解BPA的影响很小,而H2PO4–和HCO3–均抑制了ZnCo2O4-RGO5对BPA的催化降解。此外,ZnCo2O4-RGO5在外加磁场下即可分离,经5次循环使用后仍保持95%的BPA降解率。根据自由基捕获实验确定了在BPA的氧化过程中,伴随着自由基氧化过程还存在非自由基氧化机制,且非自由基氧化机制起主导作用。

(3) 采用溶剂热法制备NiFe0.7Co1.3O4-RGO1复合物,通过XRD、FTIR、SEM、TEM、XPS、BET和TGA等对复合物的微观形貌和组成结构进行了表征和分析,结果表明直径约为14 nm的NiFe0.7Co1.3O4纳米粒子均匀生长在RGO片层上,RGO的引入增大了复合物的比表面积,抑制了纳米颗粒的团聚,提高了催化性能。与NiFe2O4、NiCo2O4和NiFe0.7Co1.3O4相比,NiFe0.7Co1.3O4-RGO1对BPA的降解具有最高的催化活性。同时,NiFe0.7Co1.3O4-RGO1对BPA的催化降解效率比最近报道的催化剂快约5倍。此外,NiFe0.7Co1.3O4-RGO1在宽泛的pH范围内具有优异催化性能。与HCO3–和H2PO4–不同,Cl–或NO3–的存在对NiFe0.7Co1.3O4-RGO1的催化性能没有影响。四次循环后,NiFe0.7Co1.3O4-RGO1对BPA矿化率仍高达86%,且在矿化过程中金属离子的浸出浓度低于工业废水的排放标准。此外,根据自由基捕获和EPR实验,NiFe0.7Co1.3O4-RGO1/PS体系对BPA的降解可能是通过由自由基、表面自由基和非自由基三种途径实现的,其中表面自由基途径更为主要。

As a typical endocrine disruptor, bisphenol A (BPA) in wastewater is extremely harmful to humans and the natural environment. In recent years, advanced oxidation technology based on sulfate radicals (SO4–·) has attracted much attention due to its unique advantages. Degradation of BPA is achieved by this technology using solid catalysts to activate potassium persulfate (PS), which reduces its harm to humans and the environment. At present, graphene-based spinel metal oxide composite has been extensively studied in the field of catalysis. The synergistic effect between graphene and spinel metal oxide nanoparticles endows the composite excellent catalytic performance. Therefore, in this study, the method of activating PS by graphene-based spinel metal oxide composite was used to produce SO4–· for the oxidative degradation of BPA, and the oxidation reaction was followed by liquid chromatography. The main contents are as follows:

(1) Nickel stannate (Ni2SnO4) and nickel stannate/reduced graphene oxide (Ni2SnO4-RGO5) composite were successfully prepared by the hydrothermal method and used as catalysts for heterogeneous activation of PS. It was confirmed by X-ray diffraction (XRD), Fourier transform infrared spectroscopy (FTIR), field emission scanning electron microscopy (SEM), and transmission electron microscopy (TEM) that RGO inhibited the agglomeration of Ni2SnO4 nanoparticles and improved the catalytic performance of the composite. Simultaneously, the presence of Cl–, NO3– and HCO3– promoted the catalytic degradation of BPA by Ni2SnO4, while Cl– and HCO3– inhibited the catalytic degradation of BPA by Ni2SnO4-RGO5. NO3– did not affect the degradation of BPA by Ni2SnO4-RGO5. But H2PO4– greatly inhibited the catalytic degradation of BPA by Ni2SnO4 and Ni2SnO4-RGO5. Compared with Ni2SnO4, pH has little effect on the catalytic degradation of BPA by Ni2SnO4-RGO5. In Comparsion with Ni2SnO4, the Ni2SnO4-RGO5 maintains high catalytic activity after four cycles, which indicates Ni2SnO4-RGO5 composite has more excellent stability. In addition, free radical experiments show that hydroxyl radical ·OH and SO4–· participate in the oxidation process of BPA in both Ni2SnO4/PS and NiSn2O4-RGO5/PS systems, and SO4–· plays a leading role in the oxidation process.

(2) Zinc cobaltate/reduced graphene oxide (ZnCo2O4-RGO5) composite was successfully prepared by the hydrothermal method. The structure and morphology of the composite were analyzed by XRD, FTIR, SEM and TEM. The results show that graphene provides nucleation sites for the growth of ZnCo2O4 nanoparticles and inhibits the agglomeration of nanoparticles. Simultaneously, the effect of different reaction conditions on catalytic oxidation of BPA such as graphene content, reaction temperature, initial concentration of BPA, pH of reaction solution and anions were also systematically explored. The experimental results show that 50 mL of 0.10 mM BPA could be completely degraded by 0.02 g of ZnCo2O4-RGO5 composite and 0.02 g of PS as oxidant in 20 min at 25 °C, pH = 7. The presence of Cl– and NO3– has little effect on the catalytic degradation of BPA by ZnCo2O4-RGO5, while H2PO4– and HCO3– inhibit the catalytic degradation of BPA. In addition, ZnCo2O4-RGO5 can be separated under an external magnetic field, and the degradation rate of BPA maintaines 95% after 5 cycles. According to the free radical experiment, in the oxidation process of BPA, there is a non-radical oxidation mechanism accompanied by the free radical oxidation process, and the non-radical oxidation mechanism plays a leading role in the process of degrading BPA.

(3) The NiFe0.7Co1.3O4-RGO1 composite was prepared by the solvothermal method. Through XRD, FTIR, SEM, TEM, XPS, BET and TGA, the structure and morphology of the composite were characterized and analyzed. The results show that NiFe2-xCoxO4 nanoparticles with a size around 14 nm are uniformly anchored on RGO sheets.

关键词:尖晶石型金属氧化物;石墨烯;过硫酸盐;双酚A

Spinel metal oxide; Graphene; Persulfate; Bisphenol A

上一篇:铁基材料/过氧化物协同降解水环境中的PAEs研究     下一篇:甲壳素及其衍生物材料对水中重金属的去除及活性形态测定的研究
 
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