Kinetic molecular sieving, thermodynamic and structural aspects of gas/vapor sorption on metal organic framework [Ni-1.5(4,4 '-bipyridine)(1.5)(H3L)(H2O)(3)][H2O](7) where H6L=2,4,6-trimethylbenzene-1,3,5-triyl tris(methylene)triphosphonic acid

doi:10.1039/c5ta08261g

QIBEBT-IR > 多相催化转化研究组

	Kinetic molecular sieving, thermodynamic and structural aspects of gas/vapor sorption on metal organic framework [Ni-1.5(4,4 '-bipyridine)(1.5)(H3L)(H2O)(3)][H2O](7) where H6L=2,4,6-trimethylbenzene-1,3,5-triyl tris(methylene)triphosphonic acid
	Zhao, Xuebo 1; Bell, Jon G.2; Tang, Si -Fu 3; Li, Liangjun1 ; Thomas, K. Mark 2,3
	2016
发表期刊	JOURNAL OF MATERIALS CHEMISTRY A
卷号	4 期号:4 页码:1353-1365
摘要	A metal organic framework [Ni-1.5(4,4'-bipy)(1.5)(H3L)(H2O)(3)center dot[H2O](7) where H6L = 2,4,6-trimethyLbenzene-1,3,5-triyl tris(methylene)triphosphonic acid and 4,4'-bipy = 4,4'-bipyridine has been prepared. The structures of [Ni-1.5(4,4'-bipy)(1.5)(H3L)(H2O)(3)center dot[H2O](7) and the desoLvated form [Ni-1.5(4,4'-bipy)(1.5)(H3L)(H2O)(3) have been determined by single crystal X-ray diffraction and the framework structures are virtually identical with the former having disordered water moLecuLes in the pores. The framework structure comprises of two-dimensional Ni-1.5(H3L) Layers and 4,4'-bipy Linkers acting as pillars with an unusual framework topology of a (3, 3, 6) net that can be denoted as: {4.62}2{63}2{68.85.102}. The framework has one-dimensional channels decorated with acidic O -H groups with irregular shape varying from narrow windows (cross section: 4.2 x 4.2 A) to pore cavities (diameter: -12 A). Thermogravimetric studies showed that both coordinated and Lattice water moLecuLes adsorbed in pores were removed in Ora high vacuum to give [Ni-1.5(4,4'-bipy)(1.5)(H3L)]. The water vapor adsorption isotherm for [Ni-1.5(4,4'bipy)(1.5)(H3L)] showed that 3 coordinated and -7 pore Lattice water moLecuLes were adsorbed and the framework structure was reformed. The desorption isotherm showed that the Lattice water was easily desorbed in vacuum at 20 degrees C to form [Ni-1.5(4,4'-bipy)(1.5)(H3L)(H2O)(3). The ethanoL adsorption isotherms for [Ni-1.5(4,4'-bipyh.5(H3L)] for temperature range 20-50 degrees C were markedly hysteretic. The stoichiometry was [Ni-1.5(4,4'-bipy)(1.5)(H3L)1[1.11C(2)H(5)OH] at p/p = 0.97 and 20 degrees C gave a total pore volume approximately half that of [Ni-1.5(4,41-bipy)15(H3L)(H2O)(3)]. The desorption isotherms show that ethanoL is strongly retained with decreasing pressure indicating a stable framework structure. The kinetic profiles for oxygen, nitrogen, carbon dioxide, and water and ethanoL vapors, can be described by Fickian, combined barrier resistance/diffusion (CBRD), and stretched exponential models for both adsorption and desorption. Gas adsorption studies for [Nit5(4,4'-bipy)(1.5)(H3L)] reveal kinetic moLecuLar sieving occurs with very high kinetic seLectivity for O-2/N-2 at O degrees C. Carbon dioxide adsorption has intermediate rates of adsorption between oxygen and nitrogen. The isosteric enthalpy for CO2 adsorption at zero surface coverage was 30.7 2.4 kJ moL(-1). The corresponding activation energy for diffusion of CO2 into the framework was -48 kJ moL(-1). Narrow constrictions in the porous structure of [Ni-1.5(4,4'-bipy)(1.5)(H3L)] give rise to kinetic moLecuLar sieving effects and do not allow adsorption of moLecuLes such as methane, which has a Larger cross-section. The seLectivity for CO2/CH4 was very high (x1000) at 30 degrees C. The adsorption results are discussed in terms of diffusion, thermodynamics and surface interactions in pores.
文章类型	Article
WOS标题词	Science & Technology ; Physical Sciences ; Technology
DOI	10.1039/c5ta08261g
关键词[WOS]	URANYL PHENYLPHOSPHONATE ; UNIDIMENSIONAL CHANNELS ; ACTIVATED CARBON ; ALUMINUM METHYLPHOSPHONATE ; ADSORPTION-KINETICS ; PROTON CONDUCTIVITY ; PHOSPHONATE LIGANDS ; AIR SEPARATION ; GASES ; VAPORS
收录类别	SCI
语种	英语
WOS研究方向	Chemistry ; Energy & Fuels ; Materials Science
项目资助者	Special Project Fund of "Taishan Scholars" of Shandong Province ; Natural Science Foundation of China(21473254 ; 'Hemilabile and Switchable Metal-Organic Frameworks' EPSRC(EP/K005499/1) ; 21173246 ; 21171173)
WOS类目	Chemistry, Physical ; Energy & Fuels ; Materials Science, Multidisciplinary
WOS记录号	WOS:000368837800025
引用统计
文献类型	期刊论文
条目标识符	http://ir.qibebt.ac.cn/handle/337004/7961
专题	多相催化转化研究组
作者单位	1.China Univ Petr East China, Res Inst Unconvent Petr & Renewable Energy, Qingdao 266580, Peoples R China 2.Newcastle Univ, Sch Chem Engn & Adv Mat, Wolfson Northern Carbon Reduct Labs, Newcastle Upon Tyne NE1 7RU, Tyne & Wear, England 3.Chinese Acad Sci, Qingdao Inst Bioenergy & Bioproc Technol, Key Lab Biofuel, Qingdao 266101, Shandong, Peoples R China
推荐引用方式 GB/T 7714	Zhao, Xuebo,Bell, Jon G.,Tang, Si -Fu,et al. Kinetic molecular sieving, thermodynamic and structural aspects of gas/vapor sorption on metal organic framework [Ni-1.5(4,4 '-bipyridine)(1.5)(H3L)(H2O)(3)][H2O](7) where H6L=2,4,6-trimethylbenzene-1,3,5-triyl tris(methylene)triphosphonic acid[J]. JOURNAL OF MATERIALS CHEMISTRY A,2016,4(4):1353-1365.
APA	Zhao, Xuebo,Bell, Jon G.,Tang, Si -Fu,Li, Liangjun,&Thomas, K. Mark.(2016).Kinetic molecular sieving, thermodynamic and structural aspects of gas/vapor sorption on metal organic framework [Ni-1.5(4,4 '-bipyridine)(1.5)(H3L)(H2O)(3)][H2O](7) where H6L=2,4,6-trimethylbenzene-1,3,5-triyl tris(methylene)triphosphonic acid.JOURNAL OF MATERIALS CHEMISTRY A,4(4),1353-1365.
MLA	Zhao, Xuebo,et al."Kinetic molecular sieving, thermodynamic and structural aspects of gas/vapor sorption on metal organic framework [Ni-1.5(4,4 '-bipyridine)(1.5)(H3L)(H2O)(3)][H2O](7) where H6L=2,4,6-trimethylbenzene-1,3,5-triyl tris(methylene)triphosphonic acid".JOURNAL OF MATERIALS CHEMISTRY A 4.4(2016):1353-1365.