Synthesis and characterization of uranyl(VI) complex with 2,6-pyridine-bis(methylaminophenolato) and its ligand-centred aerobic oxidation mechanism to diimino derivative
Takeyama, Tomoyuki; Iwatsuki, Satoshi; Tsushima, Satoru; Takao, Koichiro; Dalton Transactions  (2022) –; doi:10.1039/D2DT00325B

data_7709934
_publ_section_title
;
 Synthesis and characterization of uranyl(VI) complex with
 2,6-pyridine-bis(methylaminophenolato) and its ligand-centred aerobic
 oxidation mechanism to diimino derivative
;
_journal_name_full               'Dalton Transactions'
_journal_paper_doi               10.1039/D2DT00325B
_journal_year                    2022
_chemical_formula_moiety         'C35 H45 N3 O4 U, C5 H5 N'
_chemical_formula_sum            'C40 H50 N4 O4 U'
_chemical_formula_weight         888.87
_space_group_crystal_system      triclinic
_space_group_IT_number           2
_space_group_name_Hall           '-P 1'
_space_group_name_H-M_alt        'P -1'
_atom_sites_solution_hydrogens   geom
_atom_sites_solution_primary     dual
_audit_creation_date             2021-04-08
_audit_creation_method
;
Olex2 1.3
(compiled 2020.07.31 svn.rc2a77460 for OlexSys, GUI svn.r6145)
;
_audit_update_record
;
2022-04-05 deposited with the CCDC.	2022-04-06 downloaded from the CCDC.
;
_cell_angle_alpha                68.939(4)
_cell_angle_beta                 68.074(5)
_cell_angle_gamma                81.267(3)
_cell_formula_units_Z            2
_cell_length_a                   11.4156(5)
_cell_length_b                   13.2468(5)
_cell_length_c                   14.4323(8)
_cell_measurement_reflns_used    8389
_cell_measurement_temperature    113
_cell_measurement_theta_max      24.1730
_cell_measurement_theta_min      1.8880
_cell_volume                     1888.95(17)
_computing_cell_refinement       'CrysAlisPro 1.171.40.60a (Rigaku OD, 2019)'
_computing_data_collection       'CrysAlisPro 1.171.40.60a (Rigaku OD, 2019)'
_computing_data_reduction        'CrysAlisPro 1.171.40.60a (Rigaku OD, 2019)'
_computing_molecular_graphics    'Olex2 1.3 (Dolomanov et al., 2009)'
_computing_publication_material  'Olex2 1.3 (Dolomanov et al., 2009)'
_computing_structure_refinement  'SHELXL 2018/3 (Sheldrick, 2015)'
_computing_structure_solution    'SHELXT 2018/2 (Sheldrick, 2018)'
_diffrn_ambient_temperature      113
_diffrn_detector                 'Hybrid Pixel Array Detector'
_diffrn_detector_area_resol_mean 10.0000
_diffrn_measured_fraction_theta_full 0.990
_diffrn_measured_fraction_theta_max 0.942
_diffrn_measurement_details
;
List of Runs (angles in degrees, time in seconds):

  # Type    Start    End  Width  t~exp~   \w     \q     \k     \f   Frames
  1  \w    -73.00  75.00   0.50  100.00    --   20.00  54.00 -95.53  296
  2  \w     82.00 109.00   0.50  100.00    --   20.00  54.00 -95.53   54
  3  \w    -73.00 -35.00   0.50  100.00    --   20.00  54.00  30.00   76
  4  \w     20.00  47.00   0.50  100.00    --   20.00  54.00  30.00   54
  5  \w     67.00 107.00   0.50  100.00    --   20.00  54.00  30.00   80
  6  \w    -72.00  44.50   0.50  100.00    --   20.00  54.00 -30.00  233
  7  \w    -74.00 -24.00   0.50  100.00    --   20.00  54.00-150.00  100
  8  \w     35.00  74.00   0.50  100.00    --   20.00  54.00-150.00   78
  9  \w    -62.00 -21.00   0.50  100.00    --   20.00  54.00  90.00   82
 10  \w     -8.00  45.00   0.50  100.00    --   20.00  54.00  90.00  106
 11  \w     85.00 110.00   0.50  100.00    --   20.00  54.00  90.00   50
 12  \w    -16.00  96.00   0.50  100.00    --   20.00  54.00-167.52  224
 13  \w    -68.00 -29.00   0.50  100.00    --   20.00  54.00  60.00   78
 14  \w    -74.00 107.00   0.50  100.00    --   20.00  54.00-180.00  362
 15  \w    -60.00 -35.00   0.50  100.00    --   20.00  54.00 -90.00   50
 16  \w     -1.00  44.00   0.50  100.00    --   20.00  54.00 -60.00   90
 17  \w    -35.00 -10.00   0.50  100.00    --   20.00  54.00   0.00   50
 18  \w     77.00 102.00   0.50  100.00    --   20.00  54.00   0.00   50
 19  \w    -73.00  62.00   0.50  100.00    --   20.00  54.00 150.00  270
;
_diffrn_measurement_device       'two-circle diffractometer'
_diffrn_measurement_device_type  'XtaLAB Mini II'
_diffrn_measurement_method       '\w scans'
_diffrn_orient_matrix_type
'CrysAlisPro convention (1999,Acta A55,543-557)'
_diffrn_orient_matrix_UB_11      -0.0040682000
_diffrn_orient_matrix_UB_12      -0.0006667000
_diffrn_orient_matrix_UB_13      -0.0476303000
_diffrn_orient_matrix_UB_21      0.0611415000
_diffrn_orient_matrix_UB_22      0.0221245000
_diffrn_orient_matrix_UB_23      -0.0283413000
_diffrn_orient_matrix_UB_31      0.0270783000
_diffrn_orient_matrix_UB_32      -0.0529495000
_diffrn_orient_matrix_UB_33      0.0088379000
_diffrn_radiation_monochromator  graphite
_diffrn_radiation_probe          x-ray
_diffrn_radiation_type           'Mo K\a'
_diffrn_radiation_wavelength     0.71073
_diffrn_reflns_av_R_equivalents  0.0970
_diffrn_reflns_av_unetI/netI     0.1272
_diffrn_reflns_Laue_measured_fraction_full 0.990
_diffrn_reflns_Laue_measured_fraction_max 0.942
_diffrn_reflns_limit_h_max       16
_diffrn_reflns_limit_h_min       -16
_diffrn_reflns_limit_k_max       19
_diffrn_reflns_limit_k_min       -19
_diffrn_reflns_limit_l_max       20
_diffrn_reflns_limit_l_min       -20
_diffrn_reflns_number            41195
_diffrn_reflns_point_group_measured_fraction_full 0.990
_diffrn_reflns_point_group_measured_fraction_max 0.942
_diffrn_reflns_theta_full        25.242
_diffrn_reflns_theta_max         30.992
_diffrn_reflns_theta_min         1.886
_diffrn_source                   'fine-focus sealed X-ray tube'
_diffrn_source_type              'Rigaku (Mo) X-ray Source'
_exptl_absorpt_coefficient_mu    4.341
_exptl_absorpt_correction_T_max  1.00000
_exptl_absorpt_correction_T_min  0.71415
_exptl_absorpt_correction_type   multi-scan
_exptl_absorpt_process_details
;
CrysAlisPro 1.171.40.60a (Rigaku Oxford Diffraction, 2019)
Empirical absorption correction using spherical harmonics,
 implemented in SCALE3 ABSPACK scaling algorithm.
;
_exptl_crystal_colour            violet
_exptl_crystal_colour_primary    violet
_exptl_crystal_density_diffrn    1.563
_exptl_crystal_description       plate
_exptl_crystal_F_000             884
_exptl_crystal_size_max          0.273
_exptl_crystal_size_mid          0.073
_exptl_crystal_size_min          0.048
_refine_diff_density_max         6.541
_refine_diff_density_min         -4.709
_refine_diff_density_rms         0.296
_refine_ls_extinction_method     none
_refine_ls_goodness_of_fit_ref   1.015
_refine_ls_hydrogen_treatment    constr
_refine_ls_matrix_type           full
_refine_ls_number_parameters     400
_refine_ls_number_reflns         11337
_refine_ls_number_restraints     0
_refine_ls_restrained_S_all      1.015
_refine_ls_R_factor_all          0.1165
_refine_ls_R_factor_gt           0.0722
_refine_ls_shift/su_max          0.000
_refine_ls_shift/su_mean         0.000
_refine_ls_structure_factor_coef Fsqd
_refine_ls_weighting_details
'w=1/[\s^2^(Fo^2^)+(0.1027P)^2^] where P=(Fo^2^+2Fc^2^)/3'
_refine_ls_weighting_scheme      calc
_refine_ls_wR_factor_gt          0.1622
_refine_ls_wR_factor_ref         0.1817
_reflns_Friedel_coverage         0.000
_reflns_number_gt                7834
_reflns_number_total             11337
_reflns_threshold_expression     'I > 2\s(I)'
_cod_data_source_file            d2dt00325b2.cif
_cod_data_source_block           201116_uo2_tbupdiop_red2
_cod_database_code               7709934
_shelx_shelxl_version_number     2018/3
_chemical_oxdiff_formula         C35H47N3O4U1
_chemical_oxdiff_usercomment     201116_UO2_tBupdiop_red
_reflns_odcompleteness_completeness 98.94
_reflns_odcompleteness_iscentric 1
_reflns_odcompleteness_theta     27.42
_olex2_refinement_description
;
1. Fixed Uiso
 At 1.2 times of:
  All C(H) groups
 At 1.5 times of:
  All C(H,H,H) groups
2. Uiso/Uaniso restraints and constraints
Uanis(C14) = Uanis(C19) = Uanis(C18) = Uanis(C17) = Uanis(C16) = Uanis(C15)
Uanis(O3) = Uanis(O4) = Uanis(N3) = Uanis(N2) = Uanis(N1)
3.a Aromatic/amide H refined with riding coordinates:
 C9(H9), C7(H7), C11(H11), C13(H13), C10(H10), C15(H15), C17(H17), C5(H5),
 C3(H3), C36(H36), C37(H37), C40(H40), C38(H38), C39(H39)
3.b Idealised Me refined as rotating group:
 C31(H31A,H31B,H31C), C23(H23A,H23B,H23C), C21(H21A,H21B,H21C), C34(H34A,H34B,
 H34C), C27(H27A,H27B,H27C), C33(H33A,H33B,H33C), C29(H29A,H29B,H29C), C30(H30A,
 H30B,H30C), C26(H26A,H26B,H26C), C25(H25A,H25B,H25C), C35(H35A,H35B,H35C),
 C22(H22A,H22B,H22C)
;
_shelx_res_checksum              15590
_shelx_hkl_checksum              47727
_olex2_submission_special_instructions 'No special instructions were received'
_oxdiff_exptl_absorpt_empirical_details
;
Empirical correction (ABSPACK) includes:
- Absorption correction using spherical harmonics
- Frame scaling
;
_oxdiff_exptl_absorpt_empirical_full_max 1.301
_oxdiff_exptl_absorpt_empirical_full_min 0.805