Syntheses, Structures, Photoluminescence, and Gas Adsorption of

ARTICLE pubs.acs.org/crystal

Syntheses, Structures, Photoluminescence, and Gas Adsorption of Rare Earth Organic Frameworks Based on a Flexible Tricarboxylate Jin Yang,† Shu-Yan Song,§ Jian-Fang Ma,*,† Ying-Ying Liu,† and Zhen-Tao Yu*,‡ †

Key Lab of Polyoxometalate Science, Department of Chemistry, Northeast Normal University, Changchun 130024, People’s Republic of China ‡ Eco-Materials and Renewable Energy Research Center, National Laboratory of Solid State Microstructures, Nanjing University, Nanjing 210093, People's Republic of China § State Key Laboratory of Rare Earth Resources Utilization, Changchun Institute of Applied Chemistry, Changchun 130022, People's Republic of China

bS Supporting Information ABSTRACT: Three new organic-lanthanide frameworks based on a flexible H3L acid, namely, [Er3(L)3(H2O)4] 3 5.64H2O (1), [Dy3(L)3(H2O)4] 3 2H2O (2), and [Tb3(L)3(H2O)4] 3 2H2O (3), where H3L = 5-(benzonic-4-ylmethoxy)isophthalic acid, have been synthesized under mild solvothermal conditions. Compounds 1 3 are isostructural, in which L ligands linked the lanthanide(III) ions (M) to generate two kinds of cages, [M2L]6 and [M2L2]12. These cages are further connected through sharing the M(III) atoms to yield a 3D framework with 1D channels. Topologically, the 3D framework belongs to a binodal (3,6)-connected net with the point symbol of (42.6)(44.62.86.103). Furthermore, compounds 1 and 2 display interesting emissions in the near-IR regions. Compound 3 exhibited strong green luminescence upon 249 nm excitation. The adsorption property of 1 has also been investigated.

’ INTRODUCTION In the past two decades, porous metal organic frameworks (MOFs) have attracted great attention because of their fascinating structural diversities and potential applications in gas storage, catalysis, drug delivery, and chemical sensing.1 So far, much effort has been focused on the design and controlled synthesis of porous MOFs.2 Generally, the topological architectures of the porous MOFs can be controlled by the deliberate design and judicious choice of the organic ligands and coordination geometries of the metals.3 In this aspect, the structural features of the organic ligands, such as shape, functionality, flexibility, symmetry, length, and substituent group, can influence the structure types of the MOFs directly.4 Among various organic ligands, the polycarboxylate ligands, as good candidates for the construction of porous MOFs, have aroused a good deal of interest from chemists. So far, a number of functional porous MOFs based on rigid tricarboxylates and d-block metals have been widely reported.4 Nevertheless, the ones constructed by flexible tricarboxylates and lanthanide metals have received less attention.5 Usually, the flexible tricarboxylates can adopt versatile conformations according to the geometric requirements of different metal ions and may afford unpredictable and interesting framework topologies.5 Recently, organic lanthanide frameworks have attracted increasing attention because of their interesting properties such as r 2011 American Chemical Society

magnetism, photoluminescence, and photovoltaic conversion.6 The optical properties of lanthanide ions are different from those of other metal ions and molecular species because they absorb and emit light over narrow wavelength ranges with high quantum yields.6 In addition, the organic lanthanide frameworks can yield versatile motifs because of the high coordination number and flexible coordination geometry of lanthanides. On the basis of the above consideration, we synthesized a flexible tricarboxylate ligand 5-(benzonic-4-ylmethoxy)isophthalic acid (H3L). The H3L possesses the rigid isophthalic acid and benzoic acid moieties, which can exhibit a great variety of coordination modes. On the other hand, it holds flexibility because of the presence of the O spacer that can bend to meet the requirement of the coordination conformation. In this paper, three isostructural organic lanthanide frameworks based on a flexible H3L acid have been successfully synthesized under mild solvothermal conditions, namely, [Er3(L)3(H2O)4] 3 5.64H2O (1), [Dy3(L)3(H2O)4] 3 2H2O (2), and [Tb3(L)3(H2O)4] 3 2H2O (3). The variable-temperature PXRD patterns, thermal stability, adsorption, and photoluminescence properties have been investigated for 1 3. Received: August 10, 2011 Revised: October 1, 2011 Published: October 24, 2011 5469

dx.doi.org/10.1021/cg2010425 | Cryst. Growth Des. 2011, 11, 5469–5474

Crystal Growth & Design

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Table 1. Crystal Data and Structure Refinements for Compounds 1 3 1

2

3

empirical formula

C48H33.33Er3O30.50

C48H31Dy3O27

C48H31Tb3O27

Fw crystal system

1599.86 trigonal

1527.23 trigonal

1516.49 trigonal

space group

R3

R3

R3

a (Å)

19.641(17)

19.7921(9)

19.8558(7)

b (Å)

19.641(17)

19.7921(9)

19.8558(7)

c (Å)

45.07(3)

45.3830(17)

45.5011(14)

α (°)

90

90

90

β (°)

90

90

90

γ (°) V (Å3)

120 15058(20)

120 15396.0(11)

120 15535.6(9)

Z

6

6

6

Rint

0.0363

0.0775

0.0438

R1 [I > 2σ(I)]

0.0409

0.0437

0.0499

wR2 (all data)

0.1634

0.1514

0.1868

’ EXPERIMENTAL SECTION Materials and Methods. The tricarboxylate H3 L was prepared by the procedures reported in the literatures. 7 All other reagents were purchased from commercial sources and used without further purification. Synthesis of [Er3(L)3(H2O)4] 3 5.64H2O (1). ErCl3 3 6H2O (0.127 g, 0.33 mmol) and H3L (0.108 g, 0.5 mmol) were dissolved in a solution of DMF (10 mL) and ethanol (2 mL). The resulting mixture was stirred for about 30 min at room temperature, sealed in a 15 mL Teflon-lined stainless steel autoclave, and heated at 78 °C for 2 days under autogenous pressure. Afterward, the reaction system was gradually cooled to room temperature at a rate of 10 °C h 1. Colorless crystals of 1 suitable for single-crystal X-ray diffraction analysis were collected from the final reaction system by filtration, washed several times with DMF, and dried in air at ambient temperature. Yield, 41% based on Er(III). IR (cm 1): 3442 (m), 3080 (w), 2932 (w), 1664 (s), 1592 (m), 1541 (w), 1454 (w), 1388 (s), 1320 (w), 1255 (w), 1099 (m), 1039 (w), 1018 (w), 959 (w), 780 (m), 709 (w). Synthesis of [Dy3(L)3(H2O)4] 3 2H2O (2). Compound 2 was prepared in the same way as that for 1 but using DyCl3 3 6H2O (0.126 g, 0.33 mmol) and H3L (0.108 g, 0.5 mmol) as the reactants. Crystals of 2 were collected in 37% yield. IR (cm 1): 3414 (m), 3080 (w), 2932 (w), 1663 (s), 1591 (m), 1548 (m), 1454 (w), 1384 (s), 1321 (w), 1267 (w), 1133 (w), 1056 (w), 1019 (w), 960 (w), 782 (m), 719 (w), 678 (w). Synthesis of [Tb3(L)3(H2O)4] 3 2H2O (3). Compound 3 was prepared in the same way as that for 1 but using TbCl3 3 6H2O (0.124 g, 0.33 mmol) and H3L (0.108 g, 0.5 mmol) as the reactants. Crystals of 3 were obtained in 32% yield. IR (cm 1): 3417 (m), 3067 (w), 2932 (w), 1665 (s), 1590 (m), 1548 (m), 1455 (w), 1384 (s), 1320 (w), 1267 (w), 1250 (w), 1134 (w), 1106 (w), 1056 (w), 960 (w), 783 (m), 719 (w), 678 (w). Physical Measurements. The FT-IR spectra were recorded from KBr pellets in the range of 4000 400 cm 1 on a Mattson AlphaCentauri spectrometer. TGA was performed on a Perkin-Elmer TG-7 analyzer heated from room temperature to 800 °C under nitrogen gas. The photoluminescent properties and lifetime of 3 were measured on a FLSP920 Edinburgh Fluorescence Spectrometer. XRD patterns of the samples were collected on a Rigaku Dmax 2000 X-ray diffractometer with graphite monochromatized Cu Kα radiation (λ = 0.154 nm) and 2θ ranging from 5 to 40°. N2 and CO2 adsorption desorption isotherms were collected on a micromeritics Tristar-3000 analyzer.

Figure 1. (a) View of the asymmetric unit of 1 (all H atoms are omitted for clarity) and (b) view of the distorted monocapped square antiprism coordination of the Er(III) atom in 1.

X-ray Crystallography. Single-crystal X-ray diffraction data for 1 3 were recorded on an Oxford Diffraction Gemini R Ultra diffractometer with graphite-monochromated Mo Kα radiation (λ = 0.71073 Å) at 293 K. Absorption corrections were applied using a multiscan technique. All of the structures were solved by Direct Method of SHELXS-978 and refined by full-matrix least-squares techniques using the SHELXL-97 program.9 Nonhydrogen atoms of the compounds were refined with anisotropic temperature parameters. All hydrogen atoms on carbon atoms were generated geometrically and refined using a riding model with d(C H) = 0.93 Å, Uiso = 1.2Ueq(C) for aromatic and d(C H) = 0.97 Å, Uiso = 1.2Ueq(C) for CH2 atoms. The hydrogen atoms of water molecules for 1 3 were not located from difference Fourier maps. The detailed crystallographic data and structure refinement parameters for these compounds are summarized in Table 1.

’ RESULTS AND DISCUSSION Synthesis and Characterization. Compounds 1 3 were obtained under the same conditions by the mild solvothermal 5470

dx.doi.org/10.1021/cg2010425 |Cryst. Growth Des. 2011, 11, 5469–5474


Figure 2. (a) View of the [Er2L]6 cage. (b) View of the [Er2L2]12 cage. (c) Two kinds of cages are connected through sharing the Er(III) atoms. (d) View of the 3D framework of 1 with 1D channels.

reactions of lanthanide hydrochlorides with H3L in a solution of DMF and ethanol at 78 °C. Single-crystal X-ray crystallographic studies revealed that compounds 1 3 are isostructural and are insoluble in water and common organic solvents, such as chloroform, toluene, acetonitrile, DMF, methanol, and ethanol. The IR spectra of 1 3 are similar. The absorption bands in the range of 3414 3442 cm 1 in 1 3 can be attributed to the characteristic peaks of water O H vibrations. The vibrations at around 1665 and 1455 cm 1 correspond to the asymmetric and symmetric stretching vibrations of the carboxylate groups of L anions, respectively. The absence of strong absorption bands varying from 1680 to 1730 cm 1 shows that H3L ligand is completely deproponated. Crystal Structures of Compounds 1 3. Selected bond distances and angles for compounds 1 3 are listed in Table S1 in the Supporting Information. Compounds 2 and 3 are isostructural with compound 1; therefore, only the structure of 1 will be described in detail. An ORTEP view of compound 1 is shown in Figure 1a. The asymmetric unit of 1 contains one

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unique Er(III) atom and one L ligand. Each Er(III) atom is ninecoordinated by nine oxygen atoms from five L ligands (O1, O2A, O3A, O4A, O5A, O6A, and O6B) and two water molecules (O1W and O2W). The Er O(carboxylate) bond distances vary from 2.239(5) to 2.843(6) Å, and the Er O(water) bond distances are 2.421(12) and 2.435(18) Å. It is well established that the two possible ground-state geometries for a nine-coordination polyhedron are the monocapped square antiprism with C4v symmetry and the symmetrical tricapped trigonal prism with D3h symmetry. Obviously, the polyhedron of the Er(III) coordination sphere for 1 is best described as a distorted monocapped square antiprism (Figure 1b).6c Notably, the three carboxylates of the L ligand show three different coordination modes: one carboxylate group chelates one Er(III) atom, while the rest two carboxylate groups bridges two adjacent Er(III) ions, respectively. In this way, six pairs of Er(II) dimers are linked by six L ligands to form one [Er2L]6 cage (Figures 2a and S1 in the Supporting Information). Interestingly, 12 pairs of Er(III) dimers are bridged by 24 L ligands to generate another [Er2L2]12 cage (Figures 2b and S2 and S3 in the Supporting Information). Two kinds of cages are connected through sharing the Er(III) atoms to yield a 3D framework with 1D channels (Figures 2c,d and S4 in the Supporting Information). The guest water molecules occupy the void interspace region and interact with the coordinated water molecules of frameworks. PLATON calculated suggested a solvent-accessible volume of 7024.5 Å 3 (approximately 46.7% of unit cell) by excluding the guest water molecules.10 Network topological approach has been proven to be an important and essential tool for the design and analysis of MOFs. A better insight into the nature of this intricate 3D framework can be achieved by the application of topological approach.3 From the topological point of view, the L ligand can be viewed as a 3-connected node (Figure 3a), and the Er(III) dimer functions as a 6-connected node (Figure 3b). Thus, the 3D framework of 1 can be reduced to a binodal (3,6)-connected net with the point symbol of (42.6)(44.62.86.103) (Figure 3c). So far, a variety of uninodal network topologies with nodes of 3-, 4-, and 6-connectivity have been achieved. However, there is a disappointing lack of systematic investigations on higher-dimensional networks with mixed connectivity, such as (3,6)-, (4,6)-, and (4,8)-connected frameworks, which are considered more difficult to achieve.11 PXRD Patterns and Thermal Properties. Compounds 1 3 show similar steps of weight loss (Figures 4 and S5 in the Supporting Information); therefore, only the TGA and variable-temperature PXRD patterns of 1 will be described. TG curves of 1 3 in N2 atmosphere with a heating rate of 10 °C/min were performed on polycrystalline samples to determine their thermal stability from 50 to 800 °C. From Figure 4, we can see that compound 1 undergoes two steps of weight loss. A sharp weight loss in the temperature range 50 160 °C was attributed to the loss of the free and coordinated water molecules. The removal of the organic components occurred in the temperature range of 200 600 °C. As shown in Figure 5, the experimental PXRD pattern of 1 is still in good agreement with the simulated PXRD pattern of 1, indicating that the crystal lattice of 1 remains intact at 160 °C. When the sample of 1 was heated at 170 °C, the structure of 1 begin to change and form amorphous phase. Powder X-ray diffraction studies under different temperatures show that the orders of the framework structure of the complex was retained upon complete removal of the free water molecules and partial removal of the coordinated water molecules. 5471



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Figure 4. TGA curve of compound 1.

Figure 5. Variable-temperature PXRD patterns of 1 at the temperature range of 50 160 °C.

Figure 3. (a) View of the 3-connected L ligand. (b) View of the 6-connected Er(III) dimer. (c) Schematic representation of (3,6)connected net with the point symbol of (42.6)(44.62.86.103).

Luminescent Properties. The solid state photoluminescent spectra of compounds 1 3 were recorded at room temperature. As shown in Figure 6a, the H3L ligand exhibits a fluorescent emission band at 408 nm (λex = 345 nm). The emission for the free H3L ligand is attributable to the π* f n transitions.6a Compounds 2 and 3 show distinct emissions in the near-IR regions. Recently, near-IR-emitting (NIR) materials based on rare earth compounds have attracted considerable attention because they are promising candidates for active components in near-IR luminescent optical devices.12 The NIR emission spectrum of 1 was obtained by direct excitation at 333 nm (Figure 6b). The broad emission band extended from 1466 to 1625 nm and centered at 1535 nm and is attributed to the transition from the first excited state (4I13/2) to the ground state (4I15/2) of the partically filled 4f shell of Er3+ ion. The observed

peak, centered at 1536 nm, is typical for Er3+ luminescence and is attributed to the 4I13/2 f 4I15/2 transition.13 Upon excitation at 333 nm, 2 shows the characteristic NIR luminescence of the Dy3+ ion (Figure 6c). The emission spectrum consists of several bands at λ = 839, 941, 1001, 1176, 1284, 1385, 1525, and 1675 nm, which are attributed to the f f transitions 4F9/2 f 6 H7/2 + 6F9/2, 6H5/2, 6F7/2, 6F5/2, 6F11/2 + 6H9/2 f 6H15/2, 4F9/2 f 6 F1/2, 6F5/2 f 6H11/2, and 6H11/2 f 6H15/2, respectively.14 When the Tb3+ complex 3 is excited at 249 nm, its emission spectrum exhibits the characteristic emission bands for Tb3+ ion centered at 490, 545, 585, and 620 nm (Figure 6d), which result from deactivation of the 5D4 excited state to the corresponding ground state 7FJ (J = 6, 5, 4, 3) of the Tb3+ ion. The most intense emission is centered at 545 nm and corresponds to the hypersensitive transition 5D4 f 7F5.15 It should be pointed out that the photoluminescent spectra of compounds 1 3 exhibit emission bands characteristic of the corresponding luminescent lanthanide ions, whereas the emissions arising from the free ligands are not observable for these three compounds. The absence of ligandbased emission suggests energy transfer from the ligands to the lanthanide center during photoluminescence.6a The luminescence decay curve of 3 was conducted at room temperature. As shown in Figure S6 in the Supporting Information, the luminescence lifetime of 3 is about 1.5 ms. The decay curve is well fitted into a single-exponential function as I = I0 exp( t/τ), where I 5472



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Figure 7. Gas sorption isotherms of 1 for N2 at 77 K and CO2 at 273 K.

and I0 are the luminescent intensities at times t and 0 and τ is defined as the luminescent lifetime. The result indicates that all of the Tb(III) atoms occupy the same average local environment.6a Gas Adsorption. To assess the porosity of 1, gas sorption measurements were carried out. The gas physisorption experiments toward N2 at 77 K and CO2 at 273 K were carried out to determine the permanent porosity of framework 1. The freshly prepared sample was soaked in methanol to exchange the less volatile H2O solvent, which was then followed by evacuation under a dynamic vacuum at 120 °C for 7 h. As shown in Figure 7, The N2 (kinetic diameter: 3.64 Å) sorption of dehydrated sample at 77 K is reversible and shows no hysteresis behavior upon desorption of gases from the pores. Nitrogen sorption capacity increased slowly at the lowpressure region and increases rapidly from P/P0 = 0.8, ended with the value of 4.16 cm3 g 1 at the final pressure without saturation being reached, which corresponds to apparent Brunauer Emmett Teller (BET) areas of 3.64 m2/g and Langmuir surface areas of 6.85 m2/g, respectively. The nitrogen adsorption and desorption are reversible. On the other hand, the activated sample adsorbs CO2 gas only up to 2.60 cm3 g 1 at 273 K and 1 atm. The CO2 adsorption and desorption are not reversible. The very low adsorption results indicate that there exists the possibility of strong interactions of N2 and CO2 with the narrow pore windows, which make it more difficult for the access of other molecules to the pores.16

’ CONCLUSIONS We have successfully synthesized three isostructural organic lanthanide frameworks by using a flexible H3L acid under mild solvothermal conditions. The three compounds show 3D frameworks with 1D channels composed of two kinds of fascinating cages. Topologically, the 3D frameworks belong to binodal (3,6)connected nets with the point symbol of (42.6)(44.62.86.103). The solid-state luminescent spectra demonstrate that compounds 1 and 2 are good candidates for near-IR-emitting applications, and compound 3 is green luminescent material potentially useful for optical devices. Furthermore, compound 1 shows N2 and CO2 adsorption property. ’ ASSOCIATED CONTENT Figure 6. Solid-state emission spectra for the free H3L ligand excited at 345 nm (a), for 1 excited at 333 nm (b), for 2 excited at 333 nm (c), and for 3 excited at 249 nm (d). All of the spectra were recorded at room temperature.

bS

Supporting Information. Three X-ray crystallographic files (CIF) and figures for compounds 1 3. This material is available free of charge via the Internet at http://pubs.acs.org. 5473



’ AUTHOR INFORMATION Corresponding Author

*Fax: +86-431-85098620. E-mail: [email protected] (J.-F.M.). E-mail: [email protected] (Z.-T.Y.).

’ ACKNOWLEDGMENT We thank the National Natural Science Foundation of China (Grant Nos. 21071028 and 21001023), the Science Foundation of Jilin Province (20090137 and 20100109), the Fundamental Research Funds for the Central Universities, the Specialized Research Fund for the Doctoral Program of Higher Education, the Training Fund of NENU's Scientific Innovation Project, and the State Key Laboratory of Rare Earth Resources Utilization of Changchun Institute of Applied Chemistry (RERU2011017) for support. ’ REFERENCES (1) (a) Ockwig, N. W.; Delgado-Friederichs, O.; O'Keeffe, M.; Yaghi, O. M. Acc. Chem. Res. 2005, 38, 176. (b) Perry, J. J., IV; Kravtsov, V. C.; McManus, G. J.; Zaworotko, M. J. J. Am. Chem. Soc. 2007, 129, 10076. (c) Kitagawa, S.; Kitaura, R.; Noro, S. I. Angew. Chem., Int. Ed. 2004, 43, 2334. (d) Batten, S. R.; Robson, R. Angew. Chem., Int. Ed. 1998, 37, 1460. (e) Ma, L.-Q.; Jin, A.; Xie, Z.-G.; Lin, W.-B. Angew. Chem., Int. Ed. 2009, 48, 9905. (f) Ferey, G. Chem. Soc. Rev. 2008, 37, 191. (g) Li, Z. Y.; Zhu, G. S.; Lu, G. Q.; Qiu, S. L.; Yao, X. D. J. Am. Chem. Soc. 2010, 132, 1490. (h) Jiang, J. J.; Li, L.; Lan, M. H.; Pan, M.; Eichhofer, A.; Fenske, D.; Su, C. Y. Chem.—Eur. J. 2010, 16, 1841. (i) Li, J. R.; Tao, Y.; Yu, Q.; Bu, X. H.; Sakamoto, H.; Kitagawa, S. Chem.—Eur. J. 2008, 14, 2771. (2) (a) Wong-Foy, A. G.; Matzger, A. J.; Yaghi, O. M. J. Am. Chem. Soc. 2006, 128, 3494. (b) Ferey, G.; Latroche, M.; Serre, C.; Millange, F.; Loiseau, T.; Guegan, A. P. Chem. Commun. 2003, 2976. (c) Zhang, Y.-B.; Zhang, W.-X.; Feng, F.-Y.; Zhang, J.-P.; Chen, X.-M. Angew. Chem., Int. Ed. 2009, 48, 5287. (d) Xue, M.; Liu, Y.; Schaffino, R. M.; Xiang, S.-C.; Zhao, X.-J.; Zhu, G.-S.; Qiu, S.-L.; Chen, B.-L. Inorg. Chem. 2009, 48, 4649. (3) (a) Wu, H.; Yang, J.; Su, Z.-M.; Batten, S. R.; Ma, J.-F. J. Am. Chem. Soc. 2011, 133, 11406. (b) Yang, J.; Ma, J.-F.; Batten, S. R.; Su, Z.-M. Chem. Commun. 2008, 2233. (c) Carlucci, L.; Ciani, G.; Proserpio, D. M. CrystEngComm 2003, 5, 269. (d) Kim, K. Chem. Soc. Rev. 2002, 31, 96. (e) Proserpio, D. M. Nat. Chem. 2010, 2, 435. (f) Batten, S. R. CrystEngComm 2001, 3, 67. (g) Li, Z.-X.; Xu, Y.; Zuo, Y.; Li, L.; Pan, Q.; Hu, T.-L.; Bu, X.-H. Cryst. Growth Des. 2009, 9, 3904. (h) Yang, J.; Ma, J.-F.; Liu, Y.-Y.; Ma, J.-C.; Batten, S. R. Cryst. Growth Des. 2008, 8, 4383. (i) Zhang, L.-P.; Ma, J.-F.; Yang, J.; Pang, Y.-Y.; Ma, J.-C. Inorg. Chem. 2010, 49, 1535. (j) Wu, H.; Liu, H.-Y.; Liu, Y.-Y.; Yang, J.; Liu, B.; Ma, J.-F. Chem. Commun. 2011, 47, 1818. (4) (a) Yang, J.; Li, B.; Ma, J.-F.; Liu, Y.-Y.; Zhang, J.-P. Chem. Commun. 2010, 46, 8383. (b) Yang, J.; Li, G. D.; Cao, J. J.; Yue, Q.; Li, G. H.; Chen, J. S. Chem.—Eur. J. 2007, 13, 3248. (c) Carlucci, L.; Ciani, G.; Proserpio, D. M. Coord. Chem. Rev. 2003, 246, 247. (d) Bourne, S. A.; Lu, J.; Moulton, B.; Zaworotko, M. J. Chem. Commun. 2001, 861. (e) Moulton, B.; Zaworotko, M. J. Chem. Rev. 2001, 101, 1629. (f) Millward, A. R.; Yaghi, O. M. J. Am. Chem. Soc. 2005, 127, 17998. (5) (a) Zheng, B.; Bai, J.; Duan, J.; Wojtas, L.; Zaworotko, M. J. J. Am. Chem. Soc. 2011, 133, 748. (b) Long, J. R.; Yaghi, O. M. Chem. Soc. Rev. 2009, 38, 1213. (c) Li, J.-R.; Kuppler, R. J.; Zhou, H.-C. Chem. Soc. Rev. 2009, 38, 1477. (d) Murray, L. J.; Dinca, M.; Long, J. R. Chem. Soc. Rev. 2009, 38, 1294. (e) Eddaoudi, M.; Moler, D. B.; Li, H.; Chen, B.; Reineke, T. M.; O’Keefee, M.; Yaghi, O. M. Acc. Chem. Res. 2001, 34, 319. (f) Lama, P.; Aijaz, A.; Neogi, S.; Barbour, L. J.; Bharadwaj, P. K. Cryst. Growth Des. 2011, 10, 3410. (6) (a) Yang, J.; Yue, Q.; Li, G. D.; Cao, J. J.; Li, G. H.; Chen, J. S. Inorg. Chem. 2006, 45, 2857. (b) Yue, Q.; Yang, J.; Li, G. H.; Li, G. D.;

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Syntheses, Structures, Photoluminescence, and Gas Adsorption of

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