Chen Yang, Yao Zhixiao, Miras Haralampos N, Song Yu-Fei
State Key Laboratory of Chemical Resource Engineering, Beijing University of Chemical Technology, Beijing, 100029 (P. R. China).
WestCHEM, School of Chemistry, University of Glasgow, Glasgow, G12 8QQ (UK).
Chemistry. 2015 Jul 20;21(30):10812-20. doi: 10.1002/chem.201501214. Epub 2015 Jun 17.
The exploitation of intercalation techniques in the field of two-dimensional layered materials offers unique opportunities for controlling chemical reactions in confined spaces and developing nanocomposites with desired functionality. In this study, the exploitation of the novel and facile "one-pot" anion-exchange method for the functionalization of layered double hydroxides (LDHs) is demonstrated. As a proof-of-concept, we demonstrate the intercalation of a series of polyoxometalate (POM) clusters, Na3[PW12O40]⋅15 H2O (Na3PW12), K6[P2W18O62]⋅14 H2O (K6P2W18), and Na9LaW10O36⋅32 H2O (Na9LaW10) into tris(hydroxymethyl)aminomethane (Tris)-modified layered double hydroxides (LDHs) under ambient conditions without the necessity of degassing CO2. Investigation of the resultant intercalated materials of Tris-LDHs-PW12 (1), Tris-LDH-P2W18 (2), and Tris-LDH-LaW10 (3) for the degradation of methylene blue (MB), rhodamine B (RB) and crystal violet (CV) has been carried out, where Tris-LDH-PW12 reveals the best performance in the presence of H2O2. Additionally, degradation of a mixture of RB, MB and CV by Tris-LDH-PW12 follows the order of CV>MB>RB, which is directly related to the designed accessible area of the interlayer space. Also, the composite can be readily recycled and reused at least ten cycles without measurable decrease of activity.
在二维层状材料领域中利用插层技术为在受限空间中控制化学反应以及开发具有所需功能的纳米复合材料提供了独特的机会。在本研究中,展示了利用新颖且简便的“一锅法”阴离子交换方法对层状双氢氧化物(LDHs)进行功能化。作为概念验证,我们展示了在环境条件下,一系列多金属氧酸盐(POM)簇,即Na3[PW12O40]⋅15 H2O(Na3PW12)、K6[P2W18O62]⋅14 H2O(K6P2W18)和Na9LaW10O36⋅32 H2O(Na9LaW10)插入到三(羟甲基)氨基甲烷(Tris)改性的层状双氢氧化物(LDHs)中,而无需对二氧化碳进行脱气。对所得的Tris-LDHs-PW12(1)、Tris-LDH-P2W18(2)和Tris-LDH-LaW10(3)插层材料降解亚甲基蓝(MB)、罗丹明B(RB)和结晶紫(CV)进行了研究,其中Tris-LDH-PW12在过氧化氢存在下表现出最佳性能。此外,Tris-LDH-PW12对RB、MB和CV混合物的降解遵循CV>MB>RB的顺序,这与层间空间设计的可及面积直接相关。而且,该复合材料可以很容易地回收再利用至少十个循环,而活性没有可测量的下降。