The effect of ancillary ligands on hydrocarbon C-H bond functionalization by uranyl photocatalysts.
Rutkauskaite, Ryte; Zhang, Xiaobin; Woodward, Adam W.; Liu, Yanlin; Herrera, Gabriel; Purkis, Jamie; Woodall, Sean D.; Sarsfield, Mark; Schreckenbach, Georg; Natrajan, Louise S.; Arnold, Polly L.; Chemical science 15 (2024) 6965–6978; doi:10.1039/d4sc01310g

data_1571454
_publ_section_title
;
 The effect of ancillary ligands on hydrocarbon C-H bond functionalization
 by uranyl photocatalysts.
;
_journal_issue                   18
_journal_name_full               'Chemical science'
_journal_page_first              6965
_journal_page_last               6978
_journal_paper_doi               10.1039/d4sc01310g
_journal_volume                  15
_journal_year                    2024
_chemical_formula_moiety         'C48 H32 Cl2 N4 O2 U'
_chemical_formula_sum            'C48 H32 Cl2 N4 O2 U'
_chemical_formula_weight         1005.70
_space_group_crystal_system      orthorhombic
_space_group_IT_number           19
_space_group_name_Hall           'P 2ac 2ab'
_space_group_name_H-M_alt        'P 21 21 21'
_atom_sites_solution_hydrogens   geom
_atom_sites_solution_primary     dual
_audit_creation_date             2023-02-02
_audit_creation_method
;
Olex2 1.5
(compiled 2022.04.07 svn.rca3783a0 for OlexSys, GUI svn.r6498)
;
_audit_update_record
;
2023-02-03 deposited with the CCDC.	2024-03-22 downloaded from the CCDC.
;
_cell_angle_alpha                90
_cell_angle_beta                 90
_cell_angle_gamma                90
_cell_formula_units_Z            4
_cell_length_a                   12.2797(2)
_cell_length_b                   12.7824(2)
_cell_length_c                   24.6681(3)
_cell_measurement_reflns_used    36651
_cell_measurement_temperature    99.99(13)
_cell_measurement_theta_max      31.1980
_cell_measurement_theta_min      2.2600
_cell_volume                     3872.00(10)
_computing_cell_refinement       'CrysAlisPro 1.171.41.104a (Rigaku OD, 2021)'
_computing_data_collection       'CrysAlisPro 1.171.41.104a (Rigaku OD, 2021)'
_computing_data_reduction        'CrysAlisPro 1.171.41.104a (Rigaku OD, 2021)'
_computing_molecular_graphics    'Olex2 1.5 (Dolomanov et al., 2009)'
_computing_publication_material  'Olex2 1.5 (Dolomanov et al., 2009)'
_computing_structure_refinement  'SHELXL 2018/3 (Sheldrick, 2015)'
_computing_structure_solution    'SHELXT 2018/2 (Sheldrick, 2018)'
_diffrn_ambient_environment      N~2~
_diffrn_ambient_temperature      99.99(13)
_diffrn_detector                 'Hybrid Pixel Array Detector'
_diffrn_detector_area_resol_mean 10.0000
_diffrn_detector_type            HyPix
_diffrn_measured_fraction_theta_full 1.000
_diffrn_measured_fraction_theta_max 0.910
_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     32.00  59.00   0.50   27.27    --    4.95  57.00  60.00   54
  2  \w     -7.00  78.00   0.50   27.27    --    4.95  37.00 150.00  170
  3  \w    -11.00  24.00   0.50   27.27    --    4.95  77.00 120.00   70
  4  \w    -20.00   7.00   0.50   27.27    --    4.95  94.00 173.78   54
  5  \w    -10.00  17.00   0.50   27.27    --    4.95  57.00  60.00   54
  6  \w    -61.00  -1.00   0.50   27.27    --    4.95 -19.00 -90.00  120
  7  \w    -25.00  23.00   0.50   27.27    --    4.95 -77.00-120.00   96
  8  \w    -14.00  40.00   0.50   27.27    --    4.95-102.00 -46.00  108
  9  \w    -25.00   0.00   0.50   27.27    --    4.95 -77.00  90.00   50
 10  \w     -7.00  27.00   0.50   27.27    --   -5.34 -99.00  60.00   68
 11  \w      0.00  28.00   0.50   27.27    --   -5.34 -99.00  30.00   56
 12  \w     -7.00  18.00   0.50   27.27    --   -5.34 -99.00 -30.00   50
 13  \w    -19.00  16.00   0.50   27.27    --   -5.34 -77.00 -30.00   70
 14  \w    -25.00  25.00   0.50   27.27    --    4.95 -77.00-180.00  100
 15  \w    -32.00  -1.00   0.50   27.27    --    4.95 -19.00-180.00   62
 16  \w    -68.00 -42.00   0.50   27.27    --    4.95 -19.00-180.00   52
 17  \w    -20.00  17.00   0.50   27.27    --   -5.34 -77.00 120.00   74
 18  \w     -6.00  20.00   0.50   27.27    --   -5.34 -99.00 150.00   52
;
_diffrn_measurement_device       'four-circle diffractometer'
_diffrn_measurement_device_type  'XtaLAB Synergy, Dualflex, HyPix'
_diffrn_measurement_method       '\w scans'
_diffrn_orient_matrix_type
'CrysAlisPro convention (1999,Acta A55,543-557)'
_diffrn_orient_matrix_UB_11      -0.0112874000
_diffrn_orient_matrix_UB_12      0.0127421000
_diffrn_orient_matrix_UB_13      0.0274178000
_diffrn_orient_matrix_UB_21      0.0522875000
_diffrn_orient_matrix_UB_22      0.0231379000
_diffrn_orient_matrix_UB_23      0.0024500000
_diffrn_orient_matrix_UB_31      -0.0218192000
_diffrn_orient_matrix_UB_32      0.0487911000
_diffrn_orient_matrix_UB_33      -0.0083089000
_diffrn_radiation_monochromator  mirror
_diffrn_radiation_probe          x-ray
_diffrn_radiation_type           'Mo K\a'
_diffrn_radiation_wavelength     0.71073
_diffrn_reflns_av_R_equivalents  0.0600
_diffrn_reflns_av_unetI/netI     0.0402
_diffrn_reflns_Laue_measured_fraction_full 1.000
_diffrn_reflns_Laue_measured_fraction_max 0.910
_diffrn_reflns_limit_h_max       17
_diffrn_reflns_limit_h_min       -17
_diffrn_reflns_limit_k_max       16
_diffrn_reflns_limit_k_min       -17
_diffrn_reflns_limit_l_max       35
_diffrn_reflns_limit_l_min       -35
_diffrn_reflns_number            90543
_diffrn_reflns_point_group_measured_fraction_full 1.000
_diffrn_reflns_point_group_measured_fraction_max 0.878
_diffrn_reflns_theta_full        25.242
_diffrn_reflns_theta_max         31.027
_diffrn_reflns_theta_min         1.794
_diffrn_source                   'micro-focus sealed X-ray tube'
_diffrn_source_type              'PhotonJet (Mo) X-ray Source'
_exptl_absorpt_coefficient_mu    4.377
_exptl_absorpt_correction_T_max  1.000
_exptl_absorpt_correction_T_min  0.335
_exptl_absorpt_correction_type   gaussian
_exptl_absorpt_process_details
;
CrysAlisPro 1.171.41.104a (Rigaku Oxford Diffraction, 2021)
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            'clear yellow'
_exptl_crystal_colour_lustre     clear
_exptl_crystal_colour_primary    yellow
_exptl_crystal_density_diffrn    1.725
_exptl_crystal_description       prism
_exptl_crystal_F_000             1960
_exptl_crystal_preparation       Luminescent
_exptl_crystal_recrystallization_method
'Crystallized by layering a dichloromethane solution with hexanes'
_exptl_crystal_size_max          0.201
_exptl_crystal_size_mid          0.058
_exptl_crystal_size_min          0.025
_refine_diff_density_max         1.088
_refine_diff_density_min         -0.710
_refine_diff_density_rms         0.112
_refine_ls_abs_structure_details
;
 Flack x determined using 4040 quotients [(I+)-(I-)]/[(I+)+(I-)]
 (Parsons, Flack and Wagner, Acta Cryst. B69 (2013) 249-259).
;
_refine_ls_abs_structure_Flack   -0.012(2)
_refine_ls_extinction_method     none
_refine_ls_goodness_of_fit_ref   1.021
_refine_ls_hydrogen_treatment    constr
_refine_ls_matrix_type           full
_refine_ls_number_parameters     514
_refine_ls_number_reflns         10857
_refine_ls_number_restraints     0
_refine_ls_restrained_S_all      1.021
_refine_ls_R_factor_all          0.0316
_refine_ls_R_factor_gt           0.0246
_refine_ls_shift/su_max          0.004
_refine_ls_shift/su_mean         0.000
_refine_ls_structure_factor_coef Fsqd
_refine_ls_weighting_details
'w=1/[\s^2^(Fo^2^)+(0.0170P)^2^+2.1349P] where P=(Fo^2^+2Fc^2^)/3'
_refine_ls_weighting_scheme      calc
_refine_ls_wR_factor_gt          0.0430
_refine_ls_wR_factor_ref         0.0443
_reflns_Friedel_coverage         0.753
_reflns_Friedel_fraction_full    1.000
_reflns_Friedel_fraction_max     0.838
_reflns_number_gt                9968
_reflns_number_total             10857
_reflns_threshold_expression     'I > 2\s(I)'
_cod_data_source_file            d4sc01310g2.cif
_cod_data_source_block           pla21015refinalised
_cod_depositor_comments
'Adding full bibliography for 1571453--1571456.cif.'
_cod_database_code               1571454
_shelx_shelxl_version_number     2018/3
_chemical_oxdiff_formula         UO2Cl2N4C20H30
_shelx_estimated_absorpt_t_max   0.898
_shelx_estimated_absorpt_t_min   0.473
_olex2_refinement_description
;
1. Fixed Uiso
 At 1.2 times of:
  All C(H) groups
2.a Aromatic/amide H refined with riding coordinates:
 C10(H10), C18(H18), C5(H5), C38(H38), C39(H39), C2(H2), C24(H24), C6(H6),
 C14(H14), C25(H25), C26(H26), C21(H21), C30(H30), C41(H41), C17(H17), C45(H45),
  C34(H34), C1(H1), C20(H20), C29(H29), C16(H16), C40(H40), C33(H33), C42(H42),
 C46(H46), C15(H15), C9(H9), C22(H22), C23(H23), C44(H44), C47(H47), C48(H48)
;
_shelx_res_checksum              82204
_olex2_exptl_crystal_mounting_method
'Mounted on a gioniometer loop with fomblin'
_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 1.357
_oxdiff_exptl_absorpt_empirical_full_min 0.727