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_7709935
_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 H49 N3 O4 U, C H2 Cl2'
_chemical_formula_sum            'C36 H51 Cl2 N3 O4 U'
_chemical_formula_weight         898.72
_chemical_properties_physical    Air-sensitive
_space_group_crystal_system      monoclinic
_space_group_IT_number           14
_space_group_name_Hall           '-P 2yn'
_space_group_name_H-M_alt        'P 1 21/n 1'
_atom_sites_solution_hydrogens   geom
_atom_sites_solution_primary     dual
_audit_creation_date             2021-03-18
_audit_creation_method
;
Olex2 1.3
(compiled 2020.11.12 svn.r5f609507 for OlexSys, GUI svn.r6272)
;
_audit_update_record
;
2022-04-05 deposited with the CCDC.	2022-04-06 downloaded from the CCDC.
;
_cell_angle_alpha                90
_cell_angle_beta                 91.234(4)
_cell_angle_gamma                90
_cell_formula_units_Z            4
_cell_length_a                   13.9394(7)
_cell_length_b                   13.7474(11)
_cell_length_c                   21.7612(11)
_cell_measurement_reflns_used    3838
_cell_measurement_temperature    123
_cell_measurement_theta_max      74.4720
_cell_measurement_theta_min      3.7790
_cell_volume                     4169.1(4)
_computing_cell_refinement       'CrysAlisPro 1.171.39.20a (Rigaku OD, 2015)'
_computing_data_collection       'CrysAlisPro 1.171.39.20a (Rigaku OD, 2015)'
_computing_data_reduction        'CrysAlisPro 1.171.39.20a (Rigaku OD, 2015)'
_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      123
_diffrn_detector                 'CCD plate'
_diffrn_measured_fraction_theta_full 0.988
_diffrn_measured_fraction_theta_max 0.952
_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    -27.00  23.00   0.50   40.00    --    0.00  77.00 -90.00  100
  2  \w     18.00  86.00   0.50   40.00    --    0.00  82.00 -60.00  136
  3  \w    -22.00   6.00   0.50   40.00    --    0.00 -37.00-120.00   56
  4  \w     45.00  78.00   0.50   40.00    --    0.00  77.00 -90.00   66
  5  \w    -72.00 -47.00   0.50   40.00    --    0.00 -37.00-120.00   50
  6  \w    -29.00   4.00   0.50   40.00    --    0.00  82.00 -60.00   66
  7  \w     93.00 118.00   0.50  120.00    --   96.10 -82.00 -60.00   50
  8  \w      8.00 107.00   0.50  120.00    --   96.10 -30.00 150.00  198
  9  \w      8.00  33.00   0.50  120.00    --   96.10   0.00-180.00   50
 10  \w     10.00 119.00   0.50  120.00    --   96.10 -15.00-150.00  218
 11  \w     27.00 111.00   0.50  120.00    --   96.10 -30.00  60.00  168
 12  \w     16.00 118.00   0.50  120.00    --   96.10 -61.00-180.00  204
 13  \w     83.00 108.00   0.50  120.00    --   96.10 -82.00 -30.00   50
 14  \w     77.00 104.00   0.50  120.00    --   96.10 -82.00   0.00   54
 15  \w     73.00 119.00   0.50  120.00    --   96.10 -82.00 -90.00   92
 16  \w    134.00 159.00   0.50  120.00    --   96.10   0.00-180.00   50
 17  \w     82.00 126.00   0.50  120.00    --   96.10 -82.00  52.39   88
 18  \w     49.00 114.00   0.50  120.00    --   96.10 -82.00  22.85  130
;
_diffrn_measurement_device       'four-circle diffractometer'
_diffrn_measurement_device_type  'XtaLAB Pro: Kappa dual home/near'
_diffrn_measurement_method       '\w scans'
_diffrn_orient_matrix_type
'CrysAlisPro convention (1999,Acta A55,543-557)'
_diffrn_orient_matrix_UB_11      -0.0627822000
_diffrn_orient_matrix_UB_12      -0.0029918000
_diffrn_orient_matrix_UB_13      -0.0591262000
_diffrn_orient_matrix_UB_21      0.0910069000
_diffrn_orient_matrix_UB_22      -0.0017810000
_diffrn_orient_matrix_UB_23      -0.0388745000
_diffrn_orient_matrix_UB_31      0.0002089000
_diffrn_orient_matrix_UB_32      -0.1120126000
_diffrn_orient_matrix_UB_33      0.0022736000
_diffrn_radiation_monochromator  graphite
_diffrn_radiation_probe          x-ray
_diffrn_radiation_type           'Cu K\a'
_diffrn_radiation_wavelength     1.54184
_diffrn_reflns_av_R_equivalents  0.1993
_diffrn_reflns_av_unetI/netI     0.1915
_diffrn_reflns_Laue_measured_fraction_full 0.988
_diffrn_reflns_Laue_measured_fraction_max 0.952
_diffrn_reflns_limit_h_max       16
_diffrn_reflns_limit_h_min       -17
_diffrn_reflns_limit_k_max       9
_diffrn_reflns_limit_k_min       -16
_diffrn_reflns_limit_l_max       27
_diffrn_reflns_limit_l_min       -23
_diffrn_reflns_number            25037
_diffrn_reflns_point_group_measured_fraction_full 0.988
_diffrn_reflns_point_group_measured_fraction_max 0.952
_diffrn_reflns_theta_full        67.684
_diffrn_reflns_theta_max         75.013
_diffrn_reflns_theta_min         3.803
_diffrn_source                   'fine-focus sealed X-ray tube'
_diffrn_source_type              'Enhance (Cu) X-ray Source'
_exptl_absorpt_coefficient_mu    12.423
_exptl_absorpt_correction_T_max  1.00000
_exptl_absorpt_correction_T_min  0.39853
_exptl_absorpt_correction_type   multi-scan
_exptl_absorpt_process_details
;
CrysAlisPro 1.171.39.20a (Rigaku Oxford Diffraction, 2015)
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    1.432
_exptl_crystal_description       needle
_exptl_crystal_F_000             1784
_exptl_crystal_size_max          0.257
_exptl_crystal_size_mid          0.022
_exptl_crystal_size_min          0.013
_refine_diff_density_max         3.182
_refine_diff_density_min         -6.316
_refine_diff_density_rms         0.301
_refine_ls_extinction_coef       0.00029(8)
_refine_ls_extinction_expression Fc^*^=kFc[1+0.001xFc^2^\l^3^/sin(2\q)]^-1/4^
_refine_ls_extinction_method     'SHELXL-2018/3 (Sheldrick 2018)'
_refine_ls_goodness_of_fit_ref   1.016
_refine_ls_hydrogen_treatment    constr
_refine_ls_matrix_type           full
_refine_ls_number_parameters     212
_refine_ls_number_reflns         8183
_refine_ls_number_restraints     0
_refine_ls_restrained_S_all      1.016
_refine_ls_R_factor_all          0.1934
_refine_ls_R_factor_gt           0.1061
_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^)+(0.1876P)^2^] where P=(Fo^2^+2Fc^2^)/3'
_refine_ls_weighting_scheme      calc
_refine_ls_wR_factor_gt          0.2765
_refine_ls_wR_factor_ref         0.3447
_reflns_Friedel_coverage         0.000
_reflns_number_gt                3745
_reflns_number_total             8183
_reflns_threshold_expression     'I > 2\s(I)'
_cod_data_source_file            d2dt00325b2.cif
_cod_data_source_block           UO2tBupdaop
_cod_database_code               7709935
_shelx_shelxl_version_number     2018/3
_chemical_oxdiff_formula         C35H49N3O4U1Cl2
_reflns_odcompleteness_completeness 99.29
_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 C(H,H) groups, All N(H) groups
 At 1.5 times of:
  All C(H,H,H) groups
2. Uiso/Uaniso restraints and constraints
Uanis(C3) = Uanis(C4) = Uanis(C5) = Uanis(C6) = Uanis(C1) = Uanis(C2)
Uanis(C19) = Uanis(C14) = Uanis(C15) = Uanis(C16) = Uanis(C17) = Uanis(C18)
Uanis(O3) = Uanis(O4) = Uanis(N3) = Uanis(N2) = Uanis(N1)
Uanis(C7) = Uanis(C8) = Uanis(C9) = Uanis(C10) = Uanis(C11) = Uanis(C12) =
Uanis(C13)
Uanis(C23) = Uanis(C21) = Uanis(C20) = Uanis(C22)
Uanis(C25) = Uanis(C26) = Uanis(C24) = Uanis(C27)
Uanis(C32) = Uanis(C33) = Uanis(C34) = Uanis(C35)
Uanis(C30) = Uanis(C29) = Uanis(C31) = Uanis(C28)
Uanis(O1) = Uanis(O2)
Uanis(O3) = Uanis(N1) = Uanis(N2) = Uanis(O1) = Uanis(O2) = Uanis(O4) =
Uanis(N3)
Uanis(C36) = Uanis(Cl2) = Uanis(Cl1)
3.a Ternary CH refined with riding coordinates:
 N1(H1), N3(H3)
3.b Secondary CH2 refined with riding coordinates:
 C7(H7A,H7B), C13(H13A,H13B), C36(H36A,H36B)
3.c Aromatic/amide H refined with riding coordinates:
 C9(H9), C17(H17), C11(H11), C5(H5), C3(H3A), C10(H10), C15(H15)
3.d Idealised Me refined as rotating group:
 C23(H23A,H23B,H23C), C35(H35A,H35B,H35C), C31(H31A,H31B,H31C), C22(H22A,H22B,
 H22C), C33(H33A,H33B,H33C), C29(H29A,H29B,H29C), C30(H30A,H30B,H30C), C34(H34A,
 H34B,H34C), C21(H21A,H21B,H21C), C26(H26A,H26B,H26C), C25(H25A,H25B,H25C),
 C27(H27A,H27B,H27C)
;
_smtbx_masks_void_probe_radius   1.2
_smtbx_masks_void_truncation_radius 1.2
_shelx_res_checksum              10424
_shelx_hkl_checksum              24958
_shelx_fab_checksum              4571
_platon_squeeze_void_probe_radius 1.20
_olex2_submission_original_sample_id 210317UO2-tBupdaop
_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 3.827
_oxdiff_exptl_absorpt_empirical_full_min 0.340