Controlling mixed-valence states of pyridyldiimino-bis(<i>o</i>-phenolato) ligand radical in uranyl(VI) complexes.
Takeyama, Tomoyuki; Tsushima, Satoru; Takao, Koichiro; Dalton transactions (Cambridge, England : 2003) 53 (2024) 16671–16684; doi:10.1039/d4dt01821d

data_7717091
_publ_section_title
;
 Controlling mixed-valence states of
 pyridyldiimino-bis(<i>o</i>-phenolato) ligand radical in uranyl(VI)
 complexes.
;
_journal_issue                   40
_journal_name_full
'Dalton transactions (Cambridge, England : 2003)'
_journal_page_first              16671
_journal_page_last               16684
_journal_paper_doi               10.1039/d4dt01821d
_journal_volume                  53
_journal_year                    2024
_chemical_formula_moiety         'C27 H28 N4 O6 U'
_chemical_formula_sum            'C27 H28 N4 O6 U'
_chemical_formula_weight         742.56
_space_group_crystal_system      monoclinic
_space_group_IT_number           14
_space_group_name_Hall           '-P 2ybc'
_space_group_name_H-M_alt        'P 1 21/c 1'
_atom_sites_solution_hydrogens   geom
_audit_creation_date             2024-04-22
_audit_creation_method
;
Olex2 1.3
(compiled 2020.11.12 svn.r5f609507 for OlexSys, GUI svn.r6408)
;
_audit_update_record
;
2024-08-20 deposited with the CCDC.	2024-09-25 downloaded from the CCDC.
;
_cell_angle_alpha                90
_cell_angle_beta                 95.980(2)
_cell_angle_gamma                90
_cell_formula_units_Z            16
_cell_length_a                   11.5790(3)
_cell_length_b                   20.8632(6)
_cell_length_c                   43.8957(10)
_cell_measurement_reflns_used    9020
_cell_measurement_temperature    93
_cell_measurement_theta_max      74.8300
_cell_measurement_theta_min      4.0410
_cell_volume                     10546.4(5)
_computing_cell_refinement       'CrysAlisPro 1.171.41.106a (Rigaku OD, 2021)'
_computing_data_collection       'CrysAlisPro 1.171.41.106a (Rigaku OD, 2021)'
_computing_data_reduction        'CrysAlisPro 1.171.41.106a (Rigaku OD, 2021)'
_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      93
_diffrn_detector_area_resol_mean 10.0000
_diffrn_detector_type            HyPix
_diffrn_measured_fraction_theta_full 0.993
_diffrn_measured_fraction_theta_max 0.940
_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    -21.00   5.00   0.25    2.00    --  -46.31  21.00 -85.00  104
  2  \w   -106.00 -46.00   0.25    2.00    --  -46.31 -21.00 108.00  240
  3  \w     35.00 113.00   0.25    2.00    --   46.31  21.00 -85.00  312
  4  \w    -26.00  23.00   0.25    2.00    --   46.31 -21.00 108.00  196
  5  \w   -174.00 -92.00   0.25    8.00    -- -102.00 -21.00 108.00  328
  6  \w    102.00 128.00   0.25    8.00    --  104.62  21.00 -85.00  104
  7  \w    -24.00  20.00   0.25    2.00    --   46.31 -19.00 -30.00  176
  8  \w     26.00  92.00   0.25    2.00    --   46.31-125.00 -90.00  264
  9  \w    -67.00 -30.00   0.25    8.00    -- -102.00  61.00 -60.00  148
 10  \w    -70.00 -30.00   0.25    8.00    -- -102.00  61.00   0.00  160
 11  \w   -173.00-112.00   0.25    8.00    -- -102.00 -45.00  30.00  244
 12  \w    -65.00 -30.00   0.25    8.00    -- -102.00  61.00 120.00  140
 13  \w   -168.00-138.00   0.25    8.00    -- -102.00-125.00 -90.00  120
 14  \w    -69.00 -34.00   0.25    8.00    -- -102.00  61.00-180.00  140
 15  \w   -106.00 -76.00   0.25    8.00    -- -102.00-125.00 -90.00  120
 16  \w    -55.00 -30.00   0.25    8.00    -- -102.00  61.00-150.00  100
 17  \w    -68.00 -35.00   0.25    8.00    -- -102.00  61.00  30.00  132
 18  \w   -108.00 -30.00   0.25    8.00    -- -102.00 125.00-180.00  312
 19  \w     85.00 175.00   0.25    8.00    --  104.62 125.00-180.00  360
 20  \w     50.00  97.00   0.25    8.00    --  104.62 -94.00 -30.00  188
 21  \w     33.00  73.00   0.25    8.00    --  104.62 -61.00  90.00  160
 22  \w     36.00  64.00   0.25    8.00    --  104.62 -61.00 150.00  112
;
_diffrn_measurement_device       'four-circle diffractometer'
_diffrn_measurement_device_type  'XtaLAB Synergy R, DW system, HyPix'
_diffrn_measurement_method       '\w scans'
_diffrn_radiation_type           CuK\a
_diffrn_radiation_wavelength     1.54184
_diffrn_reflns_av_R_equivalents  0.1519
_diffrn_reflns_av_unetI/netI     0.1565
_diffrn_reflns_Laue_measured_fraction_full 0.993
_diffrn_reflns_Laue_measured_fraction_max 0.940
_diffrn_reflns_limit_h_max       14
_diffrn_reflns_limit_h_min       -14
_diffrn_reflns_limit_k_max       18
_diffrn_reflns_limit_k_min       -25
_diffrn_reflns_limit_l_max       54
_diffrn_reflns_limit_l_min       -53
_diffrn_reflns_number            72147
_diffrn_reflns_point_group_measured_fraction_full 0.993
_diffrn_reflns_point_group_measured_fraction_max 0.940
_diffrn_reflns_theta_full        67.684
_diffrn_reflns_theta_max         76.481
_diffrn_reflns_theta_min         2.347
_exptl_absorpt_coefficient_mu    17.744
_exptl_absorpt_correction_T_max  1.00000
_exptl_absorpt_correction_T_min  0.71854
_exptl_absorpt_correction_type   multi-scan
_exptl_absorpt_process_details
;
CrysAlisPro 1.171.41.106a (Rigaku Oxford Diffraction, 2021)
Empirical absorption correction using spherical harmonics,
implemented in SCALE3 ABSPACK scaling algorithm.
;
_exptl_crystal_colour            orange
_exptl_crystal_colour_primary    orange
_exptl_crystal_density_diffrn    1.871
_exptl_crystal_description       needle
_exptl_crystal_F_000             5728
_exptl_crystal_size_max          0.23
_exptl_crystal_size_mid          0.02
_exptl_crystal_size_min          0.01
_refine_diff_density_max         6.212
_refine_diff_density_min         -5.154
_refine_diff_density_rms         0.307
_refine_ls_extinction_method     none
_refine_ls_goodness_of_fit_ref   0.960
_refine_ls_hydrogen_treatment    constr
_refine_ls_matrix_type           full
_refine_ls_number_parameters     733
_refine_ls_number_reflns         20847
_refine_ls_number_restraints     0
_refine_ls_restrained_S_all      0.960
_refine_ls_R_factor_all          0.1839
_refine_ls_R_factor_gt           0.0809
_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^)+(0.1131P)^2^] where P=(Fo^2^+2Fc^2^)/3'
_refine_ls_weighting_scheme      calc
_refine_ls_wR_factor_gt          0.1947
_refine_ls_wR_factor_ref         0.2489
_reflns_Friedel_coverage         0.000
_reflns_number_gt                8970
_reflns_number_total             20847
_reflns_threshold_expression     'I > 2\s(I)'
_cod_data_source_file            d4dt01821d2.cif
_cod_data_source_block           210628_uo2tbuno2pdiop3
_cod_depositor_comments
'Adding full bibliography for 7717089--7717091.cif.'
_cod_database_code               7717091
_shelx_shelxl_version_number     2018/3
_shelx_estimated_absorpt_t_max   0.843
_shelx_estimated_absorpt_t_min   0.106
_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(C26C) = Uanis(C24C) = Uanis(C25C) = Uanis(C27C)
Uanis(C14B) = Uanis(C15B) = Uanis(C16B) = Uanis(C17B) = Uanis(C18B)
Uanis(C25A) = Uanis(C24A) = Uanis(C27A) = Uanis(C26A)
Uanis(C18C) = Uanis(C17C) = Uanis(C16C) = Uanis(C15C) = Uanis(C14C) =
Uanis(C19C)
Uanis(C7A) = Uanis(C8A) = Uanis(C9A) = Uanis(C10A) = Uanis(C11A) = Uanis(C12A)
= Uanis(C13A)
Uanis(C13C) = Uanis(C12C) = Uanis(C11C) = Uanis(C9C) = Uanis(C10C) = Uanis(C8C)
= Uanis(C7C)
Uanis(C3B) = Uanis(C4B) = Uanis(C5B) = Uanis(C6B) = Uanis(C1B) = Uanis(C2B)
Uanis(C6C) = Uanis(C1C) = Uanis(C2C) = Uanis(C3C) = Uanis(C4C) = Uanis(C5C)
Uanis(C21B) = Uanis(C20B) = Uanis(C23B) = Uanis(C22B)
Uanis(C20D) = Uanis(C21D) = Uanis(C23D) = Uanis(C22D)
Uanis(C14A) = Uanis(C19A) = Uanis(C18A) = Uanis(C17A) = Uanis(C16A) =
Uanis(C15A)
Uanis(C16D) = Uanis(C15D) = Uanis(C14D) = Uanis(C19D) = Uanis(C18D) =
Uanis(C17D)
Uanis(C22A) = Uanis(C20A) = Uanis(C21A) = Uanis(C23A)
Uanis(C24D) = Uanis(C25D) = Uanis(C26D) = Uanis(C27D)
Uanis(C7B) = Uanis(C8B) = Uanis(C9B) = Uanis(C10B) = Uanis(C11B) = Uanis(C12B)
= Uanis(C13B)
Uanis(C12D) = Uanis(C13D) = Uanis(C11D) = Uanis(C10D) = Uanis(C9D) = Uanis(C8D)
= Uanis(C7D)
Uanis(C26B) = Uanis(C24B) = Uanis(C25B) = Uanis(C27B)
Uanis(C6D) = Uanis(C5D) = Uanis(C4D) = Uanis(C3D) = Uanis(C2D) = Uanis(C1D)
Uanis(C1A) = Uanis(C2A) = Uanis(C3A) = Uanis(C4A) = Uanis(C5A) = Uanis(C6A)
Uanis(O1D) = Uanis(O2D) = Uanis(O4D) = Uanis(O3D)
Uanis(O1B) = Uanis(O2B)
Uanis(N1A) = Uanis(N2A) = Uanis(N3A)
Uanis(O1B) = Uanis(O3B) = Uanis(O4B)
Uanis(N1B) = Uanis(N2B) = Uanis(N3B)
Uanis(O2C) = Uanis(O1C) = Uanis(O4C) = Uanis(O3C)
Uanis(N3C) = Uanis(N2C) = Uanis(N1C)
Uanis(C25B) = Uanis(O1A) = Uanis(O3A) = Uanis(O4A)
Uanis(N3D) = Uanis(N2D) = Uanis(N1D)
Uanis(O5D) = Uanis(N4D) = Uanis(O6D)
Uanis(O5B) = Uanis(N4B) = Uanis(O6B)
Uanis(O1A) = Uanis(O2A) = Uanis(O4A) = Uanis(O3A)
Uanis(O3B) = Uanis(O2B) = Uanis(O4B) = Uanis(O1B) = Uanis(N3B) = Uanis(N2B) =
Uanis(N1B)
3.a Aromatic/amide H refined with riding coordinates:
 C7A(H7A), C7C(H7C), C5D(H5D), C5B(H5B), C3A(H3A), C9A(H9A), C2A(H2A),
 C11A(H11A), C11C(H11C), C13A(H13A), C15B(H15B), C10B(H10B), C11B(H11B),
 C10A(H10A), C13D(H13D), C17D(H17D), C13C(H13C), C15D(H15D), C15C(H15C),
 C9C(H9C), C3B(H3B), C5A(H5A), C10C(H10C), C2C(H2C), C9B(H9B), C15A(H15A),
 C7D(H7D), C3D(H3D), C2D(H2D), C5C(H5C), C17B(H17B), C9D(H9D), C17C(H17C),
 C10D(H10D), C3C(H3C), C17A(H17A), C7B(H7B), C13B(H13B), C2B(H2B), C11D(H11D)
3.b Idealised Me refined as rotating group:
 C25A(H25D,H25E,H25F), C25D(H25A,H25B,H25C), C27B(H27J,H27K,H27L), C23A(H23D,
 H23E,H23F), C27C(H27G,H27H,H27I), C21B(H21J,H21K,H21L), C27A(H27D,H27E,H27F),
 C22D(H22A,H22B,H22C), C21C(H21G,H21H,H21I), C26D(H26A,H26B,H26C), C26B(H26J,
 H26K,H26L), C23C(H23G,H23H,H23I), C25B(H25J,H25K,H25L), C26A(H26D,H26E,H26F),
 C21A(H21D,H21E,H21F), C23B(H23J,H23K,H23L), C25C(H25G,H25H,H25I), C26C(H26G,
 H26H,H26I), C22B(H22J,H22K,H22L), C23D(H23A,H23B,H23C), C27D(H27A,H27B,H27C),
 C21D(H21A,H21B,H21C), C22C(H22G,H22H,H22I), C22A(H22D,H22E,H22F)
;
_shelx_res_checksum              7350
_shelx_hkl_checksum              47681
_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
;