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1 Supporting Information Adsorption of Small Molecules in the Porous Zirconium-Based Metal Organic Framework MIL-140A (Zr): A Joint Computational-Experimental Approach X-Ray Powder Diffraction Data was collected on a Bruker D8 Advance diffractometer (CuKα1 radiation (λ = Å) with a Debye-Scherrer geometry. Topas software 1 was used for indexing and pattern matching. Figure S1: Pattern matching for MIL-140A(Zr), a = (2) Å, b = (5) Å, c = 7.807(5) Å, β = (6), V = (1) Å 3, space group: C2/c (Rwp = 8.545). Thermogravimetric Analysis (TGA) Thermogravimetric analysis was performed with a PerkinElmer STA 6000 apparatus. The measurement was performed under O 2 with a heating rate of 2 C.min -1. The weigh losses are in good agreement with the expected range i.e., 55% ligand loss (theoretical) and 54% ligand loss (experimental). The linker starts to degrade at temperatures higher than 773K followed by oxide formation above this temperature. S1
2 Figure S2: Thermogravimetric analysis for MIL-140A(Zr). Nitrogen Sorption N 2 sorption analysis was performed on a BelsorpII max BEL apparatus. The sample was -1 degassed at 423 K for 4 hours. Surface area was evaluated using the BET model: ~ 500 m 2 g Figure S3: N 2 sorption for MIL-140A(Zr). S2
3 NMR Figure S4: 13 C CPMAS NMR spectrum of MIL140-A, on which the resonances are assigned. S3
4 Table S1: Experimental and theoretical 13 C and 1 H NMR parameters of reference systems of known structure. Compound Site δ iso experimental (ppm) δ iso simulated (ppm) σ iso simulated Adamantane C(1) Adamantane C(2) α glycine C(1) α glycine C(2) Benzene C(1) Diamond C(1) Adamantane H(1) Brucite H(1) Pyrophyllite H(1) Bohemite H(1) Talc H(1) (Taylor, 2004), 3 (Taylor, 2004), 4 (Hoffmann, 2012), 5 (Panich, 2006), 6 (Marchetti et al., 2012), 7 (Cadars et al., 2012) S4
5 Figure S5: Correlation between experimental isotropic chemical shift δ iso and calculated isotropic chemical shielding for 13 C and 1 H nuclei. Infra-red Figure S6: Simulated Infrared spectrum for MIL-140A(Zr) S5
6 Figure S7: Experimental Infrared spectrum for MIL-140A(Zr) S6
7 Simulations Figure S8: Preferential adsorption sites for H 2, CH 4, CO, CO 2 and N 2 in MIL-140A(Zr) obtained by MC simulations at low coverage. S7
8 Table S2: Some relevant geometrical parameters for isolated and adsorbed molecule. The distance and angle values are in Å and respectively. DFT D2 Molecule Distance or angle Isolated Adsorbed CO 2 C-O O-C-O CH 4 C-H H-C-H H 2 S H-S H-S-H H 2 O H-O H-O-H CO C-O H 2 H-H N 2 N-N S8
9 Table S3: Mean-value of the torsion angle for the phenyl rings of MIL-14A(Zr) in the presence of the guest molecules obtained for the DFT-optimized structure compared with the MIL-140A before the adsorption MIL- 140A Vertical Diagonal1 Diagonal2 Torsion Angle Torsion Angle Torsion Angle Ref CO CH CO N H H 2 S References (1) TOPAS V4.2: General Profile and Structure Analysis Software for Powder Diffraction Data, Bruker AXS Ltd, (2) Taylor, R. E. Setting Up 13C CP/MAS Experiments. Concepts in Magnetic Resonance Part A 2004a, 22, S9
10 (3)Taylor, R. E. 13C CP/MAS: Application to Glycine Experiments. Concepts in Magnetic Resonance Part A 2004b, 22, (4) Hoffmann, H. C.; Debowski, M.; Müller, P.; Paasch, S.; Senkovska, I.; Kaskel, S.; Brunner, E. Solid-state NMR Spectroscopy of Metal-Organic Framework Compounds (MOFs). Materials 2012, 5, (5) Panich, A.M.; Shames, A.I.; Vieth, H.-M.; Osawa, E.; Takahashi, M.; Vul, A.Y. Nuclear Magnetic Resonance Study of Ultrananocrystalline Diamonds. Eur. Phys. J. B 2006, 52, (6) Marchetti, A.; Jehle, S.; Felletti, M.; Knight, M. J.; Wang, Y.; Xu, Z.-Q.; Park, A. Y.; Otting, G.; Lesage, A.; et al. Backbone Assignment of Fully Protonated Solid Proteins by 1 H Detection and Ultrafast Magic-Angle-Spinning NMR Spectroscopy. Angew. Chem. Int. Ed. 2012, 51, (7) Cadars, S.; Guégan, R.; Garaga, M. N.; Bourrat, X.; Forestier, L. L.; Fayon, F.; Huynh, T. V.; Allier, T.; Nour, Z.; Massiot, D. New Insights Into the Molecular Structures, Compositions, and Cation Distributions in Synthetic and Natural Montmorillonite Clays. Chem. Mat. 2012, 24, The full citation of References (3) and (6) of the main text are listed below: (3) Nugent, P.; Belmabkhout, Y.; Burd, S. D.; Cairns, A. J.; Luebke, R.; Forrest, K.; Pham, T.; Ma, S.; Space, B.; Wojtas, L.; Eddaoudi, M.; Zaworotko, M.J. Porous Materials with Optimal Adsorption Thermodynamics and Kinetics for CO2 Separation. Nature 2013, 495, (6) Llewellyn, P. L.; Garcia-Rates, M.; Gaberová, L.; Miller, S. R.; Devic, T.; Lavalley, J. C.; Bourrelly, S.; Bloch, E.; Filinchuk, Y.; Wright, P.A.; Serre, C.; Vimont, A.; Maurin, G., Structural Origin of Unusual CO 2 Adsorption Behavior of a Small-Pore Aluminum Bisphosphonate MOF. J. Phys. Chem. C 2015, 119, S10
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