Nitride Protonation and NH3 Binding versus N‒H Bond Cleavage in Uranium Nitrides
Keener, Megan; Scopelliti, Rosario; Mazzanti, Marinella; Chemical Science  (2021) –; doi:10.1039/D1SC03957A

data_1564377
_publ_section_title
;
 Nitride Protonation and NH3 Binding versus N--H Bond Cleavage in Uranium
 Nitrides
;
_journal_name_full               'Chemical Science'
_journal_paper_doi               10.1039/D1SC03957A
_journal_year                    2021
_chemical_formula_moiety
'C44 H100 N O14 Si3 U, C24 H20 B, 0.5(C4 H10 O)'
_chemical_formula_sum            'C70 H125 B N O14.5 Si3 U'
_chemical_formula_weight         1545.81
_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   mixed
_atom_sites_solution_primary     dual
_atom_sites_solution_secondary   difmap
_audit_creation_date             2021-06-11
_audit_creation_method
;
Olex2 1.3
(compiled 2020.11.12 svn.r5f609507 for OlexSys, GUI svn.r6272)
;
_audit_update_record
;
2021-07-16 deposited with the CCDC.	2021-08-13 downloaded from the CCDC.
;
_cell_angle_alpha                78.867(3)
_cell_angle_beta                 72.917(3)
_cell_angle_gamma                73.341(3)
_cell_formula_units_Z            2
_cell_length_a                   13.6571(5)
_cell_length_b                   14.5356(5)
_cell_length_c                   22.7110(8)
_cell_measurement_reflns_used    18656
_cell_measurement_temperature    140.00(10)
_cell_measurement_theta_max      71.6240
_cell_measurement_theta_min      3.1260
_cell_volume                     4099.4(3)
_computing_cell_refinement       'CrysAlisPro 1.171.41.99a (Rigaku OD, 2021)'
_computing_data_collection       'CrysAlisPro 1.171.41.99a (Rigaku OD, 2021)'
_computing_data_reduction        'CrysAlisPro 1.171.41.99a (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, 2015)'
_diffrn_ambient_environment      N~2~
_diffrn_ambient_temperature      140.00(10)
_diffrn_detector                 'CCD plate'
_diffrn_detector_area_resol_mean 10.2665
_diffrn_detector_type            Atlas
_diffrn_measured_fraction_theta_full 0.998
_diffrn_measured_fraction_theta_max 0.973
_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    -82.00   2.00   1.00    4.00    --  -42.88 110.00  50.00   84
  2  \w     21.00  79.00   1.00    4.00    --   42.88-110.00 -44.00   58
  3  \w     70.00 108.00   1.00   16.00    --  102.23-110.00 -44.00   38
  4  \w    124.00 159.00   1.00   16.00    --  102.23 110.00  50.00   35
  5  \w    -47.00 -19.00   1.00    4.00    --  -42.88 -37.00  90.00   28
  6  \w   -114.00 -19.00   1.00    4.00    --  -42.88 -37.00-180.00   95
  7  \w   -105.00 -74.00   1.00    4.00    --  -42.88 -37.00  90.00   31
  8  \w   -116.00 -15.00   1.00    4.00    --  -42.88 -57.00 -60.00  101
  9  \w     27.00  66.00   1.00   16.00    --  102.23 -77.00 -60.00   39
 10  \w     27.00 103.00   1.00   16.00    --  102.23 -94.00   0.00   76
 11  \w     35.00 106.00   1.00   16.00    --  102.23 -94.00  90.00   71
 12  \w     32.00  75.00   1.00   16.00    --  102.23 -77.00 150.00   43
 13  \w    103.00 163.00   1.00   16.00    --  102.23 125.00 -30.00   60
 14  \w    103.00 135.00   1.00   16.00    --  102.23 -77.00 150.00   32
 15  \w     75.00 163.00   1.00   16.00    --  102.23  61.00-120.00   88
 16  \w    103.00 130.00   1.00   16.00    --  102.23 -77.00 -60.00   27
 17  \w    104.00 177.00   1.00   16.00    --  102.23  77.00 150.00   73
 18  \w     81.00 112.00   1.00   16.00    --  102.23-125.00-120.00   31
 19  \w     73.00 158.00   1.00   16.00    --  102.23  61.00 120.00   85
 20  \w    105.00 148.00   1.00   16.00    --  102.23  45.00  30.00   43
 21  \w     80.00 112.00   1.00   16.00    --  102.23  30.00  90.00   32
 22  \w    136.00 168.00   1.00   16.00    --  102.23  30.00  90.00   32
 23  \w     76.00 112.00   1.00   16.00    --  102.23-125.00 150.00   36
 24  \w     81.00 106.00   1.00   16.00    --  102.23 -94.00-180.00   25
 25  \w    103.00 162.00   1.00   16.00    --  102.23  77.00 -60.00   59
;
_diffrn_measurement_device       'four-circle diffractometer'
_diffrn_measurement_device_type  'SuperNova, Dual, Cu at home/near, Atlas'
_diffrn_measurement_method       '\w scans'
_diffrn_orient_matrix_type
'CrysAlisPro convention (1999,Acta A55,543-557)'
_diffrn_orient_matrix_UB_11      -0.0363109000
_diffrn_orient_matrix_UB_12      -0.0333140000
_diffrn_orient_matrix_UB_13      0.0698097000
_diffrn_orient_matrix_UB_21      -0.1066812000
_diffrn_orient_matrix_UB_22      0.0750118000
_diffrn_orient_matrix_UB_23      0.0033688000
_diffrn_orient_matrix_UB_31      -0.0460172000
_diffrn_orient_matrix_UB_32      -0.0753498000
_diffrn_orient_matrix_UB_33      -0.0149463000
_diffrn_radiation_monochromator  mirror
_diffrn_radiation_probe          x-ray
_diffrn_radiation_type           'Cu K\a'
_diffrn_radiation_wavelength     1.54184
_diffrn_reflns_av_R_equivalents  0.0516
_diffrn_reflns_av_unetI/netI     0.0616
_diffrn_reflns_Laue_measured_fraction_full 0.998
_diffrn_reflns_Laue_measured_fraction_max 0.973
_diffrn_reflns_limit_h_max       16
_diffrn_reflns_limit_h_min       -16
_diffrn_reflns_limit_k_max       14
_diffrn_reflns_limit_k_min       -17
_diffrn_reflns_limit_l_max       27
_diffrn_reflns_limit_l_min       -27
_diffrn_reflns_number            34513
_diffrn_reflns_point_group_measured_fraction_full 0.998
_diffrn_reflns_point_group_measured_fraction_max 0.973
_diffrn_reflns_theta_full        67.684
_diffrn_reflns_theta_max         71.750
_diffrn_reflns_theta_min         3.196
_diffrn_source                   'micro-focus sealed X-ray tube'
_diffrn_source_type              'SuperNova (Cu) X-ray Source'
_exptl_absorpt_coefficient_mu    6.435
_exptl_absorpt_correction_T_max  0.955
_exptl_absorpt_correction_T_min  0.507
_exptl_absorpt_correction_type   gaussian
_exptl_absorpt_process_details
;
CrysAlisPro 1.171.41.99a (Rigaku Oxford Diffraction, 2021)
Numerical absorption correction based on Gaussian integration over
a multifaceted crystal model.
Empirical absorption correction using spherical harmonics
as implemented in SCALE3 ABSPACK scaling algorithm
;
_exptl_crystal_colour            colourless
_exptl_crystal_colour_primary    colourless
_exptl_crystal_density_diffrn    1.252
_exptl_crystal_description       prism
_exptl_crystal_F_000             1614
_exptl_crystal_size_max          0.17
_exptl_crystal_size_mid          0.1
_exptl_crystal_size_min          0.04
_refine_diff_density_max         2.749
_refine_diff_density_min         -2.248
_refine_diff_density_rms         0.116
_refine_ls_extinction_method     none
_refine_ls_goodness_of_fit_ref   1.030
_refine_ls_hydrogen_treatment    mixed
_refine_ls_matrix_type           full
_refine_ls_number_parameters     876
_refine_ls_number_reflns         15595
_refine_ls_number_restraints     33
_refine_ls_restrained_S_all      1.029
_refine_ls_R_factor_all          0.0524
_refine_ls_R_factor_gt           0.0432
_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^)+(0.0652P)^2^] where P=(Fo^2^+2Fc^2^)/3'
_refine_ls_weighting_scheme      calc
_refine_ls_wR_factor_gt          0.1045
_refine_ls_wR_factor_ref         0.1117
_reflns_Friedel_coverage         0.000
_reflns_number_gt                13556
_reflns_number_total             15595
_reflns_threshold_expression     'I > 2\s(I)'
_cod_data_source_file            d1sc03957a2.cif
_cod_data_source_block           mk-164
_cod_depositor_comments
;
The following automatic conversions were performed:

data item '_exptl_absorpt_correction_type' value 'Gaussian' was
changed to 'gaussian' in accordance with the
/home/data/users/saulius/crontab/automatic-downloads/rss-feeds/RSC/lib/dictionaries/cif_core.dic
dictionary named 'cif_core.dic' version 2.4.2 last updated on
2011-04-26.

Automatic conversion script
Id: cif_fix_values 7556 2019-12-06 15:28:31Z antanas 
;
_cod_original_formula_sum        'C70 H125 B N O14.50 Si3 U'
_cod_database_code               1564377
_shelx_shelxl_version_number     2018/3
_audit_contact_author            'Farzaneh Fadaei Tirani'
_chemical_oxdiff_formula         'C70 H125 B N O14.50 Si3 U'
_shelx_estimated_absorpt_t_max   0.783
_shelx_estimated_absorpt_t_min   0.408
_reflns_odcompleteness_completeness 99.90
_reflns_odcompleteness_iscentric 1
_reflns_odcompleteness_theta     66.49
_olex2_refinement_description
;
1. Fixed Uiso
 At 1.2 times of:
  All C(H) groups, {H1A,H1B,H1C} of C84, All C(H,H) groups
 At 1.5 times of:
  {H84A,H84B,H84C} of C84, {H82A,H82B,H82C} of C82, {H32A,H32B,H32C} of C32,
  {H47A,H47B,H47C} of C47, {H28A,H28B,H28C} of C28, {H30A,H30B,H30C} of C30,
  {H43A,H43B,H43C} of C43, {H52A,H52B,H52C} of C52, {H26A,H26B,H26C} of C26,
  {H46A,H46B,H46C} of C46, {H31A,H31B,H31C} of C31, {H48A,H48B,H48C} of C48,
  {H50A,H50B,H50C} of C50, {H51A,H51B,H51C} of C51, {H42A,H42B,H42C} of C42,
  {H27A,H27B,H27C} of C27, {H44A,H44B,H44C} of C44, {H24A,H24B,H24C} of C24,
  {H2A,H2B,H2C} of C2, {H12A,H12B,H12C} of C12, {H22A,H22B,H22C} of C22, {H11A,
  H11B,H11C} of C11, {H23A,H23B,H23C} of C23, {H7A,H7B,H7C} of C7, {H8A,H8B,
  H8C} of C8, {H4A,H4B,H4C} of C4, {H3A,H3B,H3C} of C3, {H6A,H6B,H6C} of C6,
  {H10A,H10B,H10C} of C10
2. Restrained distances
 O81-C81
 1.41 with sigma of 0.02
 C83-C84
 1.5 with sigma of 0.02
 O81-C83
 1.42 with sigma of 0.02
 C82-C81
 1.48 with sigma of 0.02
 N1-H1A = N1-H1B = N1-H1C
 1 with sigma of 0.02
 O81-C82 = O81-C84
 2.37 with sigma of 0.04
3. Uiso/Uaniso restraints and constraints
O81 \\sim C81 \\sim C82 \\sim C83 \\sim C84: within 2A with sigma of 0.01 and
sigma for terminal atoms of 0.02 within 2A
4. Others
 Fixed Sof: O81(0.5) C81(0.5) H81A(0.5) H81B(0.5) C82(0.5) H82A(0.5) H82B(0.5)
 H82C(0.5) C83(0.5) H83A(0.5) H83B(0.5) C84(0.5) H84A(0.5) H84B(0.5) H84C(0.5)
5.a Secondary CH2 refined with riding coordinates:
 C61(H61A,H61B), C62(H62A,H62B), C63(H63A,H63B), C64(H64A,H64B), C71(H71A,
 H71B), C72(H72A,H72B), C73(H73A,H73B), C74(H74A,H74B), C81(H81A,H81B),
 C83(H83A,H83B)
5.b Aromatic/amide H refined with riding coordinates:
 C102(H102), C103(H103), C104(H104), C105(H105), C106(H106), C108(H108),
 C109(H109), C110(H110), C111(H111), C112(H112), C114(H114), C115(H115),
 C116(H116), C117(H117), C118(H118), C120(H120), C121(H121), C122(H122),
 C123(H123), C124(H124)
5.c Idealised Me refined as rotating group:
 C2(H2A,H2B,H2C), C3(H3A,H3B,H3C), C4(H4A,H4B,H4C), C6(H6A,H6B,H6C), C7(H7A,
 H7B,H7C), C8(H8A,H8B,H8C), C10(H10A,H10B,H10C), C11(H11A,H11B,H11C), C12(H12A,
 H12B,H12C), C22(H22A,H22B,H22C), C23(H23A,H23B,H23C), C24(H24A,H24B,H24C),
 C26(H26A,H26B,H26C), C27(H27A,H27B,H27C), C28(H28A,H28B,H28C), C30(H30A,H30B,
 H30C), C31(H31A,H31B,H31C), C32(H32A,H32B,H32C), C42(H42A,H42B,H42C), C43(H43A,
 H43B,H43C), C44(H44A,H44B,H44C), C46(H46A,H46B,H46C), C47(H47A,H47B,H47C),
 C48(H48A,H48B,H48C), C50(H50A,H50B,H50C), C51(H51A,H51B,H51C), C52(H52A,H52B,
 H52C), C82(H82A,H82B,H82C), C84(H84A,H84B,H84C)
;
_shelx_res_checksum              35625
_shelx_hkl_checksum              42702
_olex2_date_sample_data_collection 2021-02-26
_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
- Detector area scaling
- B-factor correction
;
_oxdiff_exptl_absorpt_empirical_full_max 1.528
_oxdiff_exptl_absorpt_empirical_full_min 0.610