Heteroaggregation behavior of graphene oxide on Zr-based metal-organic frameworks in aqueous solutions: a combined experimental and theoretical study

doi:10.1039/c7ta06462d

	Heteroaggregation behavior of graphene oxide on Zr-based metal-organic frameworks in aqueous solutions: a combined experimental and theoretical study
	Hayat, T; Hou, J; Wang, XX; Wu, QY; Shi WQ(石伟群); Chai ZF(柴之芳); Wu QY(吴群燕); Li, J; Shi, WQ; Chai, ZF
刊名	JOURNAL OF MATERIALS CHEMISTRY A
	2017
卷号	5 期号:38 页码:20398-20406
ISSN号	2050-7488
DOI	10.1039/c7ta06462d
文献子类	Article
英文摘要	A series of zirconium-based metal-organic frameworks (Zr-based MOFs) (UiO-66, UiO-66-NH2, UiO-66-OH, UiO-66-(OH)(2) and UiO-67) with different surface charge properties and geometric dimensions were tested to decrease the concentration of graphene oxide (GO) nanosheets in aqueous solutions. Based on the experimental results and density functional theory (DFT) calculations, UiO-67 showed the highest adsorption capacity of all Zr-based MOFs studied herein. The p-p interaction/stacking, hydrogen bonding and Lewis acid-base interactions were the main cause for the removal of GO by negatively charged UiO-66-OH and UiO-66-(OH)(2). Electrostatic attractions governed the association between GO and positively charged Zr-based MOFs (UiO-66, UiO-66-NH2 and UiO-67) via heteroaggregation. All adsorption and desorption isotherms of GO on UiO-66, UiO-66-NH2 or UiO-67 followed the linear model, and the obvious intercept (27-51 mg g(-1)) between adsorption-desorption isotherms disclosed that the GO adsorption over these MOFs was irreversible. This irreversible phenomenon was associated with a type of specific sheet-particle configuration, in which the particles of Zr-based MOFs were wrapped by GO nanosheets to form multilayered GO-MOF heteroaggregates with high geometric stability. The DFT calculations showed that the most stable adsorption structures were the geometries with the para-site of the linked ligand. Given the low-cost and simple preparation of Zr-based MOFs, it is clear that Zr-based MOFs could potentially act as coagulants for the efficient elimination of GO from aqueous solutions. This experimental evidence provides valuable information for the understanding of the interaction between GO and coagulants, and the potential fate, toxicity and migration of GO under natural conditions in aquatic environments, as well as in soils and sediments.
电子版国际标准刊号	2050-7496
WOS关键词	LAYERED DOUBLE HYDROXIDES ; AQUATIC ENVIRONMENT ; SURFACE-CHEMISTRY ; CARBON NANOTUBES ; ADSORPTION ; REMOVAL ; AGGREGATION ; WATER ; NANOMATERIALS ; NANOSHEETS
WOS研究方向	Chemistry ; Energy & Fuels ; Materials Science
语种	英语
WOS记录号	WOS:000412781700034
内容类型	期刊论文
源URL	[http://ir.ihep.ac.cn/handle/311005/285292]
专题	高能物理研究所_多学科研究中心中国科学院高能物理研究所_中国散裂中子源
作者单位	中国科学院高能物理研究所
推荐引用方式 GB/T 7714	Hayat, T,Hou, J,Wang, XX,et al. Heteroaggregation behavior of graphene oxide on Zr-based metal-organic frameworks in aqueous solutions: a combined experimental and theoretical study[J]. JOURNAL OF MATERIALS CHEMISTRY A,2017,5(38):20398-20406.
APA	Hayat, T.,Hou, J.,Wang, XX.,Wu, QY.,石伟群.,...&Alsaedi, A.(2017).Heteroaggregation behavior of graphene oxide on Zr-based metal-organic frameworks in aqueous solutions: a combined experimental and theoretical study.JOURNAL OF MATERIALS CHEMISTRY A,5(38),20398-20406.
MLA	Hayat, T,et al."Heteroaggregation behavior of graphene oxide on Zr-based metal-organic frameworks in aqueous solutions: a combined experimental and theoretical study".JOURNAL OF MATERIALS CHEMISTRY A 5.38(2017):20398-20406.