State Key Laboratory of Pollution Control and Resource Reuse, Tongji University, Shanghai 200092, China.
State Key Laboratory of Pollution Control and Resource Reuse, Tongji University, Shanghai 200092, China.
J Colloid Interface Sci. 2016 Nov 1;481:144-57. doi: 10.1016/j.jcis.2016.07.051. Epub 2016 Jul 21.
In this work, a series of novel Zn-Al-Ce multi-metal oxide (Zn-Al-Ce-MMO) photocatalysts with different Ce doping contents were prepared by calcination of Ce-doped Zn-Al layered double hydroxide (Zn-Al-Ce-LDH) precursors at various temperatures in air atmosphere. The synthesized Zn-Al-Ce-MMO materials were characterized by XRD, FTIR, TGA, BET, SEM, TEM, XPS and UV-vis DRS. The photocatalytic activities of the Zn-Al-Ce-MMO materials were evaluated by the photodegradation of rhodamine B (RhB) dye and paracetamol in aqueous solution under simulated solar light irradiation. The result of photodegradation of RhB showed that the Zn-Al-Ce-MMO samples exhibit much higher photocatalytic activity than that of Zn-Al-MMO, and the optimal Ce doping content is 5% of mole ratio (nCe/n(Zn+Al+Ce)). The enhanced photocatalytic activity of the Zn-Al-Ce-MMO was mainly attributed to the increasing in the separation efficiency of electrons and holes. The effect of calcination temperature was also studied. The photocatalytic activity of Zn-Al-Ce-MMO increased with increasing calcination temperature up to 750°C, which can be ascribed to the formation of well-crystallized metal oxides during calcination. Under experimental conditions, 97.8% degradation efficiency of RhB and 98.9% degradation efficiency of paracetamol were achieved after 240min. Active species trapping and EPR experiments suggested that hole (h(+)), superoxide radical (O2(-)) and hydroxyl radical (OH) played important roles during the RhB photocatalytic process. Moreover, the results indicated that the synthesized Zn-Al-Ce-MMO materials had good stability and reusability.
在这项工作中,通过在空气气氛中于不同温度下煅烧 Ce 掺杂的 Zn-Al 层状双氢氧化物(Zn-Al-Ce-LDH)前体,制备了一系列具有不同 Ce 掺杂含量的新型 Zn-Al-Ce 多金属氧化物(Zn-Al-Ce-MMO)光催化剂。所合成的 Zn-Al-Ce-MMO 材料通过 XRD、FTIR、TGA、BET、SEM、TEM、XPS 和 UV-vis DRS 进行了表征。通过模拟太阳光照射下 RhB 染料和扑热息痛在水溶液中的光降解,评价了 Zn-Al-Ce-MMO 材料的光催化活性。RhB 光降解结果表明,Zn-Al-Ce-MMO 样品表现出比 Zn-Al-MMO 更高的光催化活性,最佳 Ce 掺杂含量为摩尔比(nCe/n(Zn+Al+Ce))的 5%。Zn-Al-Ce-MMO 增强的光催化活性主要归因于电子和空穴分离效率的提高。还研究了煅烧温度的影响。Zn-Al-Ce-MMO 的光催化活性随煅烧温度的升高而增加,在 750°C 时达到最高,这可以归因于煅烧过程中形成了结晶良好的金属氧化物。在实验条件下,RhB 的降解效率达到 97.8%,扑热息痛的降解效率达到 98.9%,反应 240min 后达到。活性物质捕获和 EPR 实验表明,空穴(h(+))、超氧自由基(O2(-))和羟基自由基(OH)在 RhB 光催化过程中起重要作用。此外,结果表明,所合成的 Zn-Al-Ce-MMO 材料具有良好的稳定性和可重复使用性。