AgI/NH2-UiO-66(Zr)异质结制备及其可见光催化性能

Preparation and photocatalytic performance of AgI/NH2-UiO-66(Zr) heterojunction

  • 摘要: 开发可见光响应型金属有机框架材料(MOFs)异质结,有望高效利用太阳能进行催化降解/减毒环境污染物。以氯化锆(ZrCl4)和2-氨基对苯二甲酸(2-ATA)为原料,用溶剂热法制备了NH2-UiO-66(Zr)作为基底MOFs,采用对离子沉淀法在其表面负载AgI,制备一系列AgI/NH2-UiO-66(Zr)异质结复合光催化剂。通过XRD、BET、TEM、UV-Vis DRS、FT-IR、TGA及光电化学测试等手段对材料进行结构和光电响应性质表征。以Cr(VI)为模型污染物,探究复合材料在可见光照射下的光催化性能,以及影响其性能的各种因素:pH、初始Cr(VI)浓度、催化剂投加量、捕获剂种类及浓度。实验结果显示:当AgI负载量为20%时,优选得到的AgI/NH2-UiO-66(Zr)具有最佳的光催化性能,可见光照射120 min后,Cr(VI)还原率为97.8%,远高于纯AgI和NH2-UiO-66(Zr),拟合的一级动力学常数k分别是AgI和NH2-UiO-66(Zr)体系的7.9倍和7.4倍。此外,异质结催化剂循环使用稳定性良好,循环5次后对Cr(VI)还原率仍保持在90%左右。

     

    Abstract: The development of visible-light-responsive metal organic framework materials (MOFs) heterojunctions is expected to make efficient use of solar energy for catalytic degradation/detoxification of environmental pollutants. Using zircomiun tetrachloride (ZrCl4) and 2-aminoterephthalic acid (2-ATA) as raw materials, NH2-UiO-66(Zr) was prepared as MOFs substrate by solvothermal method. A series of AgI/NH2-UiO-66(Zr) heterojunction composites were prepared by counter ion deposition method. The materials were characterized by XRD, BET, TEM, UV-Vis DRS, FT-IR, TGA and photoelectrochemical tests. Taking Cr(VI) as a model pollutant, the photocatalytic performance of the composite was studied under visible light and various factors were also investigated, including pH, initial Cr(VI) concentration, catalyst loading amount, type and concentration of trapping agent. It is found that 20% AgI/NH2-UiO-66(Zr) displays optimal photocatalytic performance. After 120 min of visible light irradiation, the Cr(VI) reduction efficiency is 97.8%, which is much higher than that of naked AgI and NH2-UiO-66(Zr). The fitted first-order kinetic constant k is 7.9 and 7.4 times that in the AgI and NH2-UiO-66(Zr) systems, respectively. In addition, the catalyst has good cyclic stability. After 5 cycles, the reduction rate of Cr(VI) still remain at about 90%.

     

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