Fe-Ni共掺杂ZnO/凹凸棒光催化降解废水中抗生素性能研究

以水热法制备了Fe-Ni共掺杂的ZnO/凹凸棒(Fe-Ni-ZnO/ATP)光催化剂,通过XRD和FT-IR对其结构进行了表征,考察了催化剂用量、溶液pH值、光照条件、抗生素种类等因素对催化剂降解抗生素性能的影响.结果表明,Fe-Ni-ZnO/ATP中,ZnO为六方纤锌矿结构,Fe主要以Fe2O3的形式存在,Ni2+取代了ZnO晶格中的部分Zn2+并造成品格缺陷,部分Zn2+进入了 ATP层间生成了Zn-O-Si键,实现了与ATP的复合,并促使其层间距增大.Fe-Ni共掺杂拓宽了催化剂的光谱响应范围和提高了其催化活性,当催化剂投入量为2.5 g/L、溶液pH值为6时,在可见光下反应90 min后,该催化剂对30mg/L的诺氟沙星降解率可达90.63％,并且,在相同条件下,该催化剂对其他两种抗生素废水的降解率均在80％以上,表现出良好的普适性.此外,该催化剂还具有良好的再生性能.     

V/Ce共掺杂TiO2光催化降解甲醛的实验研究

采用溶胶-凝胶法制备了不掺杂、V掺杂、Ce掺杂、V/Ce共掺杂纳米TiO2光催化剂,并将其分别负载于瓷砖上,利用X射线衍射分析（XRD）和扫描电镜分析（SEM）技术对薄膜样品的结构和形貌进行了表征。通过对甲醛的降解实验评价光催化剂的光催化活性。实验结果表明,光催化剂的负载量、共掺杂离子的掺杂量、掺杂配比、煅烧温度影响纳米TiO2的光催化活性。V/Ce共掺杂TiO2光催化剂产生了协同效应,其光催化活性优于纯TiO2和单掺杂TiO2样品。     

Visible light induced photodegradation of organic pollutants on nitrogen and fluorine co-doped TiO2 photocatalyst

The nitrogen and fluorine co-doped TiO2 polycrystalline powder was synthesized by calcinations of the hydrolysis product of tetrabutyl titanate with ammonium fluoride. Nitrogen and fluorine co-doping causes the absorption edge of TiO2 to shift to a lower energy region.The photocatalytic activity of co-doped TiO2 with anatase phases was found to be 2.4 times higher than that of the commercial TiO2 photocatalyst Degussa P‘25 for phenol decomposition under visible light irradiation. The co-doped TiO2 powders only contain anatase phases even at 1000%. Apparently, ammonium fluoride added retarded phase transformation of the TiO2 powders from anatase to futile.The substitutional fluorine and interstitial nitrogen atoms in co-doped TiO2 polycrystalline powder were responsible for the vis light response and caused the absorption edge of TiO2 to shift to a lower energy region.     

Co/N/S共掺杂纳米TiO2的制备及其可见光催化活性

为提高纳米TiO2的可见光催化活性,采用溶胶-凝胶法制备了一种掺杂型纳米可见光催化剂Co/N/S/TiO2,并用正交试验法对其制备工艺进行了优化;用紫外-可见漫反射光谱(DRS)、X射线衍射(XRD)、透射电子显微镜(TEM)等方法对其吸光性能和结构进行了表征;以活性艳蓝X-BR溶液为光降解模型,对其可见光催化活性进行了评价,并与Degussa P25进行对比.结果表明,在Co:N:S:Ti物质的量比为0.15:0.2:0.2:1、煅烧温度为400℃、煅烧时间为1h的最佳制备条件下,所制得的Co/N/S/TiO2光催化剂为单一锐钛矿晶相,平均粒径为8～ 10 nm,比表面积约为192.19 m2/g.Co/N/S/TiO2光催化剂吸收边可红移至近900 nm,可见光催化活性突出,在纯粹可见光(λ＞400 nm)下光解活性艳蓝X-BR溶液120 min的降解率可达91.5％,与Degussa P25相比,其可见光催化活性提高了80.1％,且重复使用性能良好.     

Pr-N共掺杂TiO2光电催化降解孔雀石绿动力学

以溶胶-凝胶法制备的Pr-N共掺杂TiO2催化剂为电极,在光电催化反应器中,研究了光电催化降解孔雀石绿的动力学过程.结果表明,孔雀石绿氧化降解速率与溶液的初始浓度、pH、外加电压及反应的温度有关,在初始浓度为10～30 mg.L-1、pH为3～8、电压1～5 V、温度为298～338 K的实验范围内,反应的氧化降解符合一级反应动力学模型且模型值与实验值吻合良好.模型中反应的初始反应活化能Ea为11.99 kJ.mol-1,说明反应较易进行;pH的反应级数1.634 7,远远高于电压的级数0.850 2及初始浓度的级数0.123 8,表明通过控制pH可有效地提高光电催化的氧化降解速率.     

上流边光型反应器中负载型TiO_2光催化剂处理印染废水的研究

试验采用Fe3+-Ce4+双元素共掺杂改性的TiO2光催化剂在自制的边光上流型光催化反应器中处理人造丝织物印染废水。在成功地解决了催化剂与水分离的同时,达到了充分发挥双元素改性TiO2光催化剂性能的目的。试验结果表明,催化剂投加量、pH值、曝气量、反应时间等指标对光催化效果有影响。在上流型反应器中加入10 g/L双元素掺杂改性的TiO2光催化剂,曝气量0.5 m3/L,处理水样240 min后出水水质色度去除率为97.6%,COD去除率为73.9%,去除效果良好。     

B,N和Ce共掺杂TiO2催化剂光催化活性研究

采用溶胶-凝胶法制备出B,N和Ce共掺杂TiO2光催化剂,并用XRD、SEM等表征了其结构特征。以酸性大红染料溶液的光催化降解为探针反应,考察了制备条件对共掺杂TiO2催化剂活性的影响。结果表明,在400℃,当B,N和Ce的原子比为1∶2∶0.1,焙烧3 h时,光催化剂活性最大,大红染料的降解率达到98%。     

泡沫镍负载Pr-N共掺杂TiO2的制备及其光催化性能

以泡沫镍为载体,钛酸丁酯为原料,采用溶胶-凝胶法制备Pr-N共掺杂TiO2光催化剂。利用X射线衍射(XRD)、紫外-可见漫反射光谱(DRS)、扫描电镜(SEM)对催化剂进行表征,结果表明,Pr和N的掺杂抑制了TiO2从锐钛矿晶型向金红石晶型的转变,提高了催化剂在可见光区的吸收能力。以孔雀石绿为目标模型化合物,利用正交实验得出当n(Pr)∶n(N)∶n(Ti)为0.0020∶0.2∶1、焙烧温度为400℃时制得的催化剂活性最高。同时,考察了Pr-N共掺杂、Pr掺杂、N掺杂及TiO2对孔雀石绿降解并利用傅立叶红外光谱对降解产物进行分析,实验表明,Pr-N共掺杂之后催化剂对孔雀石绿的降解率较改性之前提高了1.6倍。     

Peroxymonosulfate activation by Fe-N-S co-doped tremella-like carbocatalyst for degradation of bisphenol A: Synergistic effect of pyridine N, Fe-Nx, thiophene S

Bisphenol A (BPA) has received increasing attention due to its long-term industrial application and persistence in environmental pollution. Iron-based carbon catalyst activation of peroxymonosulfate (PMS) shows a good prospect for effective elimination of recalcitrant contaminants in water. Herein, considering the problem about the leaching of iron ions and the optimization of heteroatoms doping, the iron, nitrogen and sulfur co-doped tremella-like carbon catalyst (Fe-NS@C) was rationally designed using very little iron, S-C₃N₄ and low-cost chitosan (CS) via the impregnation-calcination method. The as-prepared Fe-NS@C exhibited excellent performance for complete removal of BPA (20 mg/L) by activating PMS with the high kinetic constant (1.492 min⁻¹) in 15 min. Besides, the Fe-NS@C/PMS system not only possessed wide pH adaptation and high resistance to environmental interference, but also maintained an excellent degradation efficiency on different pollutants. Impressively, increased S-C₃N₄ doping amount modulated the contents of different N species in Fe-NS@C, and the catalytic activity of Fe-NS@C-1-x was visibly enhanced with increasing S-C₃N₄ contents, verifying pyridine N and Fe-N_x as main active sites in the system. Meanwhile, thiophene sulfur (C-S-C) as active sites played an auxiliary role. Furthermore, quenching experiment, EPR analysis and electrochemical test proved that surface-bound radicals (^·OH and SO₄^⋅−) and non-radical pathways worked in the BPA degradation (the former played a dominant role). Finally, possible BPA degradation route were proposed. This work provided a promising way to synthesize the novel Fe, N and S co-doping carbon catalyst for degrading organic pollutants with low metal leaching and high catalytic ability.     

La~(3+)和Fe~(3+)共掺杂TiO_2/浮石的制备及光催化矿化二级出水的效果

采用溶胶-凝胶法和浸涂法制备了以浮石为载体、La~(3+)和Fe~(3+)为共掺杂离子的TiO_2光催化剂,并用其光催化矿化城市污水处理厂二级出水.La~(3+)、Fe~(3+)改性TiO_2/浮石催化剂用X射线衍射、电镜扫描进行了表征和分析,探讨了La~(3+)、Fe~(3+)掺杂量对TiO_2光催化性能的影响,以及浮石粒径、涂膜层数、催化剂投加量对TiO_2/浮石光催化矿化二级出水效果的影响.结果显示,所制备的TiO_2以混晶形式存在,锐钛矿的含量为78.1%,平均粒径为36nm;TiO_2薄膜在浮石上负载良好,当La~(3+)、Fe~(3+)掺杂量分别为0.5%和0.05%、浮石粒径为20-40目、涂膜层数为4层、催化剂投加量为15 g·L~(-1),光催化反应时间为200min时,二级出水中TOC的去除率为51.6%,La~(3+)、Fe~(3+)改性TiO_2/浮石光催化是一种有效的污水深度处理方法.