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Ce 掺杂 Zn-Al 多金属氧化物复合材料的层状双氢氧化物前驱体制备及其光催化性能增强。

Enhanced photocatalytic activity of Ce-doped Zn-Al multi-metal oxide composites derived from layered double hydroxide precursors.

机构信息

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.

出版信息

J Colloid Interface Sci. 2016 Nov 1;481:144-57. doi: 10.1016/j.jcis.2016.07.051. Epub 2016 Jul 21.

Abstract

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.

摘要

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。

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