Differential uranyl(v) oxo-group bonding between the uranium and metal cations from groups 1, 2, 4, and 12; a high energy resolution X-ray absorption, computational, and synthetic study
Zegke, Markus; Zhang, Xiaobin; Pidchenko, Ivan; Hlina, Johann A.; Lord, Rianne M.; Purkis, Jamie; Nichol, Gary S.; Magnani, Nicola; Schreckenbach, Georg; Vitova, Tonya; Love, Jason B.; Arnold, Polly L.; Chemical Science 10 (2019) 9740–; doi:10.1039/C8SC05717F

data_1554609
_publ_section_title
;
 Differential uranyl(v) oxo-group bonding between the uranium and metal
 cations from groups 1, 2, 4, and 12; a high energy resolution X-ray
 absorption, computational, and synthetic study
;
_journal_issue                   42
_journal_name_full               'Chemical Science'
_journal_page_first              9740
_journal_paper_doi               10.1039/C8SC05717F
_journal_volume                  10
_journal_year                    2019
_chemical_formula_moiety         'C282 H282 Cs6 N54 O12 U6, 6(C5 H5 N)'
_chemical_formula_sum            'C312 H312 Cs6 N60 O12 U6'
_chemical_formula_weight         7319.84
_space_group_crystal_system      trigonal
_space_group_IT_number           148
_space_group_name_Hall           '-R 3'
_space_group_name_H-M_alt        'R -3 :H'
_atom_sites_solution_hydrogens   geom
_atom_sites_solution_primary     heavy
_audit_creation_date             2015-03-18
_audit_creation_method
;
Olex2 1.2
(compiled 2015.01.26 svn.r3150 for OlexSys, GUI svn.r4998)
;
_audit_update_record
;
2018-12-07 deposited with the CCDC.	2019-08-27 downloaded from the CCDC.
;
_cell_angle_alpha                90
_cell_angle_beta                 90
_cell_angle_gamma                120
_cell_formula_units_Z            3
_cell_length_a                   27.7671(4)
_cell_length_b                   27.7671(4)
_cell_length_c                   35.7644(5)
_cell_measurement_reflns_used    21727
_cell_measurement_temperature    120.00(10)
_cell_measurement_theta_max      75.7770
_cell_measurement_theta_min      3.0797
_cell_volume                     23880.5(6)
_computing_cell_refinement
;
CrysAlisPro, Agilent Technologies,
Version 1.171.37.35e (release 07-10-2014 CrysAlis171 .NET)
(compiled Oct  7 2014,17:20:27)
;
_computing_data_collection
;
CrysAlisPro, Agilent Technologies,
Version 1.171.37.35e (release 07-10-2014 CrysAlis171 .NET)
(compiled Oct  7 2014,17:20:27)
;
_computing_data_reduction
;
CrysAlisPro, Agilent Technologies,
Version 1.171.37.35e (release 07-10-2014 CrysAlis171 .NET)
(compiled Oct  7 2014,17:20:27)
;
_computing_molecular_graphics    'Olex2 (Dolomanov et al., 2009)'
_computing_publication_material  'Olex2 (Dolomanov et al., 2009)'
_computing_structure_refinement  'ShelXL (Sheldrick, 2008)'
_computing_structure_solution    'ShelXS (Sheldrick, 2008)'
_diffrn_ambient_environment      N~2~
_diffrn_ambient_temperature      120.00(10)
_diffrn_detector                 'CCD plate'
_diffrn_detector_area_resol_mean 5.1574
_diffrn_detector_type            Atlas
_diffrn_measured_fraction_theta_full 1.000
_diffrn_measured_fraction_theta_max 0.995
_diffrn_measurement_details
;
  1 omega -122.00   -7.00   1.0000   15.0000
omega____ theta____ kappa____ phi______ frames
    -      -43.4186  -19.0000  -30.0000 115

  2 omega  -75.00   30.00   1.0000   15.0000
omega____ theta____ kappa____ phi______ frames
    -      -43.4186   77.0000 -120.0000 105

  3 omega  -50.00   29.00   1.0000   15.0000
omega____ theta____ kappa____ phi______ frames
    -      -43.4186   38.0000  150.0000 79

  4 omega  -95.00   -2.00   1.0000   15.0000
omega____ theta____ kappa____ phi______ frames
    -      -43.4186  125.0000 -120.0000 93

  5 omega   23.00   98.00   1.0000   15.0000
omega____ theta____ kappa____ phi______ frames
    -       43.4186 -125.0000   30.0000 75

  6 omega   23.00   98.00   1.0000   15.0000
omega____ theta____ kappa____ phi______ frames
    -       43.4186 -125.0000  -90.0000 75

  7 omega   37.00  142.00   1.0000   30.0000
omega____ theta____ kappa____ phi______ frames
    -      111.0000  -77.0000  120.0000 105

  8 omega   66.00  178.00   1.0000   30.0000
omega____ theta____ kappa____ phi______ frames
    -      111.0000   15.0000 -150.0000 112

  9 omega   39.00  121.00   1.0000   30.0000
omega____ theta____ kappa____ phi______ frames
    -      111.0000 -125.0000 -120.0000 82

 10 omega   30.00  109.00   1.0000   30.0000
omega____ theta____ kappa____ phi______ frames
    -      111.0000  -94.0000  -60.0000 79

 11 omega   40.00   98.00   1.0000   30.0000
omega____ theta____ kappa____ phi______ frames
    -      111.0000  -45.0000   90.0000 58

 12 omega   36.00   91.00   1.0000   30.0000
omega____ theta____ kappa____ phi______ frames
    -      111.0000  -30.0000    0.0000 55

 13 omega   36.00   91.00   1.0000   30.0000
omega____ theta____ kappa____ phi______ frames
    -      111.0000  -30.0000 -120.0000 55

 14 omega   40.00   98.00   1.0000   30.0000
omega____ theta____ kappa____ phi______ frames
    -      111.0000  -45.0000  -60.0000 58

 15 omega   30.00  109.00   1.0000   30.0000
omega____ theta____ kappa____ phi______ frames
    -      111.0000  -94.0000 -120.0000 79

 16 omega   39.00  121.00   1.0000   30.0000
omega____ theta____ kappa____ phi______ frames
    -      111.0000 -125.0000   60.0000 82

 17 omega   87.00  178.00   1.0000   30.0000
omega____ theta____ kappa____ phi______ frames
    -      111.0000   30.0000  -90.0000 91

 18 omega   40.00   98.00   1.0000   30.0000
omega____ theta____ kappa____ phi______ frames
    -      111.0000  -45.0000   30.0000 58

 19 omega   30.00  109.00   1.0000   30.0000
omega____ theta____ kappa____ phi______ frames
    -      111.0000  -94.0000   60.0000 79

 20 omega   36.00   91.00   1.0000   30.0000
omega____ theta____ kappa____ phi______ frames
    -      111.0000  -30.0000  -60.0000 55

 21 omega   40.00   98.00   1.0000   30.0000
omega____ theta____ kappa____ phi______ frames
    -      111.0000  -45.0000 -150.0000 58

 22 omega -114.00  -17.00   1.0000   15.0000
omega____ theta____ kappa____ phi______ frames
    -      -43.4186  -57.0000 -120.0000 97

 23 omega -117.00  -12.00   1.0000   15.0000
omega____ theta____ kappa____ phi______ frames
    -      -43.4186  -77.0000  -30.0000 105

 24 omega -117.00  -12.00   1.0000   15.0000
omega____ theta____ kappa____ phi______ frames
    -      -43.4186  -77.0000  150.0000 105

 25 omega -117.00  -12.00   1.0000   15.0000
omega____ theta____ kappa____ phi______ frames
    -      -43.4186  -77.0000 -150.0000 105

 26 omega  -50.00   29.00   1.0000   15.0000
omega____ theta____ kappa____ phi______ frames
    -      -43.4186   38.0000   60.0000 79

 27 omega -117.00  -12.00   1.0000   15.0000
omega____ theta____ kappa____ phi______ frames
    -      -43.4186  -77.0000   60.0000 105

 28 omega   66.00  178.00   1.0000   30.0000
omega____ theta____ kappa____ phi______ frames
    -      111.0000   15.0000   60.0000 112

 29 omega   87.00  137.00   1.0000   30.0000
omega____ theta____ kappa____ phi______ frames
    -      111.0000   30.0000  120.0000 50

 30 omega   87.00  178.00   1.0000   30.0000
omega____ theta____ kappa____ phi______ frames
    -      111.0000   30.0000  -30.0000 91
;
_diffrn_measurement_device       'four-circle diffractometer'
_diffrn_measurement_device_type  'SuperNova, Dual, Cu at zero, Atlas'
_diffrn_measurement_method       '\w scans'
_diffrn_orient_matrix_UB_11      -0.0023395000
_diffrn_orient_matrix_UB_12      -0.0541677000
_diffrn_orient_matrix_UB_13      -0.0126432000
_diffrn_orient_matrix_UB_21      -0.0412007000
_diffrn_orient_matrix_UB_22      -0.0068761000
_diffrn_orient_matrix_UB_23      -0.0312236000
_diffrn_orient_matrix_UB_31      0.0490105000
_diffrn_orient_matrix_UB_32      0.0335224000
_diffrn_orient_matrix_UB_33      -0.0268371000
_diffrn_radiation_monochromator  mirror
_diffrn_radiation_probe          x-ray
_diffrn_radiation_type           CuK\a
_diffrn_radiation_wavelength     1.54184
_diffrn_reflns_av_R_equivalents  0.0962
_diffrn_reflns_av_unetI/netI     0.0451
_diffrn_reflns_Laue_measured_fraction_full 1.000
_diffrn_reflns_Laue_measured_fraction_max 0.995
_diffrn_reflns_limit_h_max       34
_diffrn_reflns_limit_h_min       -33
_diffrn_reflns_limit_k_max       34
_diffrn_reflns_limit_k_min       -34
_diffrn_reflns_limit_l_max       43
_diffrn_reflns_limit_l_min       -44
_diffrn_reflns_number            123779
_diffrn_reflns_point_group_measured_fraction_full 1.000
_diffrn_reflns_point_group_measured_fraction_max 0.995
_diffrn_reflns_theta_full        67.684
_diffrn_reflns_theta_max         76.240
_diffrn_reflns_theta_min         3.080
_diffrn_source                   'sealed X-ray tube'
_diffrn_source_type              'SuperNova (Cu) X-ray Source'
_exptl_absorpt_coefficient_mu    14.249
_exptl_absorpt_correction_T_max  0.995
_exptl_absorpt_correction_T_min  0.992
_exptl_absorpt_correction_type   gaussian
_exptl_absorpt_process_details
;
CrysAlisPro, Agilent Technologies,
Version 1.171.37.35e (release 07-10-2014 CrysAlis171 .NET)
(compiled Oct  7 2014,17:20:27)
Numerical absorption correction based on gaussian integration over
			a multifaceted crystal model
Empirical absorption correction using spherical harmonics,
 implemented in SCALE3 ABSPACK scaling algorithm.
;
_exptl_crystal_colour            red
_exptl_crystal_colour_primary    red
_exptl_crystal_density_diffrn    1.527
_exptl_crystal_description       block
_exptl_crystal_F_000             10746
_exptl_crystal_size_max          0.0466
_exptl_crystal_size_mid          0.0416
_exptl_crystal_size_min          0.0293
_refine_diff_density_max         12.923
_refine_diff_density_min         -1.915
_refine_diff_density_rms         0.228
_refine_ls_extinction_method     none
_refine_ls_goodness_of_fit_ref   1.027
_refine_ls_hydrogen_treatment    constr
_refine_ls_matrix_type           full
_refine_ls_number_parameters     579
_refine_ls_number_reflns         11060
_refine_ls_number_restraints     21
_refine_ls_restrained_S_all      1.026
_refine_ls_R_factor_all          0.0808
_refine_ls_R_factor_gt           0.0658
_refine_ls_shift/su_max          0.001
_refine_ls_shift/su_mean         0.000
_refine_ls_structure_factor_coef Fsqd
_refine_ls_weighting_details
'w=1/[\s^2^(Fo^2^)+(0.0917P)^2^+1001.9244P] where P=(Fo^2^+2Fc^2^)/3'
_refine_ls_weighting_scheme      calc
_refine_ls_wR_factor_gt          0.1669
_refine_ls_wR_factor_ref         0.1764
_reflns_Friedel_coverage         0.000
_reflns_number_gt                9096
_reflns_number_total             11060
_reflns_threshold_expression     'I > 2\s(I)'
_cod_data_source_file            c8sc05717f2.cif
_cod_data_source_block           po15003_refinalized
_cod_original_cell_volume        23880.5(8)
_cod_original_sg_symbol_H-M      'R -3'
_cod_database_code               1554609
_chemical_oxdiff_formula         'C54 H54 Cs N12 O2 U'
_chemical_oxdiff_usercomment     '@ 120 K RML126'
_reflns_odcompleteness_completeness 99.99
_reflns_odcompleteness_iscentric 1
_reflns_odcompleteness_theta     66.97
_olex2_refinement_description
;
1. Fixed Uiso
 At 1.2 times of:
  All C(H) groups, All N(H) groups
 At 1.5 times of:
  All C(H,H,H) groups
2. Uiso/Uaniso restraints and constraints
Uanis(C45) = Uanis(C47)
Uanis(C44) = Uanis(C43)
3. Rigid body (RIGU) restrains
 C43, C44, C45, C46, C47
 with sigma for 1-2 distances of 0.004 and sigma for 1-3 distances of 0.004
4.a Aromatic/amide H refined with riding coordinates:
 N5(H5), N6(H6), C43(H43), C44(H44), C45(H45), C46(H46), C47(H47), C2(H2),
 C3(H3), C5(H5A), C7(H7), C12(H12), C14(H14), C16(H16), C17(H17), C23(H23),
 C24(H24), C26(H26), C28(H28), C33(H33), C35(H35), C37(H37), C38(H38), C48(H48),
  C49(H49), C50(H50), C51(H51), C52(H52)
4.b Fitted hexagon refined as free rotating group:
 N9(C43,C44,C45,C46,C47)
4.c Idealised Me refined as rotating group:
 C9(H9A,H9B,H9C), C11(H11A,H11B,H11C), C20(H20A,H20B,H20C), C21(H21A,H21B,
 H21C), C30(H30A,H30B,H30C), C32(H32A,H32B,H32C), C41(H41A,H41B,H41C), C42(H42A,
 H42B,H42C)
;
_shelx_res_checksum              82720
_shelx_shelxl_version_number     2014/7
_olex2_submission_special_instructions 'No special instructions were received'