research communications
accessCrystal structures of products from the BBr3-promoted demethylation of 3-(methoxymethyl)-6-phenyl-1,2,4,5-tetrazine
aBielefeld University, Department of Chemistry, Universitätsstr. 25, 33615 Bielefeld, Germany
*Correspondence e-mail: [email protected]
The BBr3-promoted demethylation of 3-(methoxymethyl)-6-phenyl-1,2,4,5-tetrazine, C10H10N4O, resulted in the alcohol (6-phenyl-1,2,4,5-tetrazin-3-yl)methanol, C9H8N4O, and the bromide 3-(bromomethyl)-6-phenyl-1,2,4,5-tetrazine, C9H7BrN4. All three compounds were analysed by nuclear magnetic resonance (NMR) spectroscopy in solution and by single-crystal X-ray diffraction using non-spherical scattering factors for structure refinement. The substrate as well as the corresponding bromide form π–π interactions between antiparallel stacks of molecules. In contrast, due to the intermolecular hydrogen bonds present, which lead to the formation of a bent dimer, the alcohol forms only very weak parallel π–π stacks. Corresponding O—H⋯N hydrogen bonds are established between the hydroxy group and an N atom of a neighbouring tetrazine molecule, an only rarely explored structural feature of 1,2,4,5-tetrazines.
Keywords: 1,2,4,5-tetrazine; hydrogen bonds; crystal structure; synthesis.
1. Chemical context
1,2,4,5-Tetrazines, first described by Pinner (1893
), are electron-deficient heterocycles of particular relevance in fast and chemoselective cycloaddition reactions (Zhao et al., 2022
). While structurally simple 1,2,4,5-tetrazines (herein further abbreviated as tetrazines) are well-known in the literature, for many modern applications, tetrazines substituted at the 3- and 6-positions are needed (Yim et al., 2026
). In particular, tetrazines modified with a hydroxymethyl group at the 3-position and derivatives thereof are frequently used as marker molecules in biochemical applications (Baalmann et al., 2019
; Tu et al., 2020
; Wang et al., 2022
). Early reports on the synthesis and derivatization of such tetrazines were provided by Lang et al. (1975
) through the synthesis of a panel of 3,6-disubstituted tetrazines. Out of this library, 3-(methoxymethyl)-6-phenyl-1,2,4,5-tetrazine (1) was synthesized (Tu et al., 2019
), and the BBr3-promoted demethylation re-investigated to obtain the deprotected alcohol (2) and the bromide (3) as a side product (Fig. 1
). In the scope of the present investigations, tetrazines (1)–(3) were characterised by NMR spectroscopy in solution and by single-crystal X-ray diffraction.
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Figure 1
Treatment of tetrazine (1) with BBr3 afforded both alcohol (2) and bromide (3). |
2. Structural commentary
While the structures of tetrazine (1) and alcohol (2) were clearly confirmed by NMR spectroscopy in solution with 13C{1H} NMR shifts of the methylene groups at 72.3 and 63.0 ppm, respectively, the strong upfield shift of the bromomethyl group of bromide (3) to 27.8 ppm hints to the introduction of a strongly deshielding substituent. However, unambiguous structural proof was given by the results of single-crystal X-ray diffraction.
Both the substrate (1) and the bromide (3) crystallize in the triclinic space group P with one molecule in the asymmetric unit each (Fig. 2
). In contrast, alcohol (2) crystallizes in the monoclinic space group P21/n with a hydrogen-bonded dimer in the asymmetric unit (Fig. 3
). The two crystallographically independent molecules (2A/2B) show close conformational similarity with a root-mean-square deviation of 0.169 Å (Fig. 3
, right). The phenyl units of all tetrazines (1)–(3) show similar bond lengths for all C—C bonds [1.391 (2)–1.401 (2) Å] and all C—N and N—N bonds of the tetrazine units [1.308 (1)–1.353 (1) Å], indicative of their aromaticity with an extended co-planar arrangement of the biaryl moieties. The dihedral angles between the phenyl and tetrazine rings are 3.63 (4)° (1), 2.29 (4)° (2A), 8.47 (5)° (2B), and 2.72 (1)° (3). All bond angles agree with values obtained from structurally similar disubstituted tetrazines containing a phenyl and substituted methyl substituents (for details see Section 4). The methoxymethyl group of tetrazine (1) and the bromomethyl group of bromide (3) accommodate the largest atoms (O and Br), resulting in the smallest torsion angles with 73.17 (8)° for the N1—C2—C1—O1 connection and −74.63 (17)° for the N4—C2—C1—Br1 connection, likely due to repulsion with the N-centered lone pairs of the tetrazine units. Interestingly, the N1—C2—C1—O1 torsion angles of alcohol (2) are different from those of (1) and (3) with −162.92 (7)° for (2A) and 16.06 (9)° for (2B), an observation that may be explained by the intermolecular hydrogen-bonding interactions between hydroxy groups and tetrazine-N atoms (see Section 3).
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Figure 2
Molecular structures of tetrazine (1) and bromide (3) with displacement ellipsoids represented at the 50% probability level and H atoms as spheres of arbitrary radius. |
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Figure 3
(Left) Molecular structure of alcohol (2) with displacement ellipsoids represented at the 50% probability level and H atoms as spheres of arbitrary radius; for the sake of clarity only molecule A is shown. (Right) Overlay-plot (generated using the ‘match' option within OLEX2) of molecules (2A/2B) showing their close conformational similarity. |
3. Supramolecular features
All of the tetrazines investigated here show π–π interactions, the strongest between antiparallel stacked molecules of tetrazine (1) and bromide (3) with centroid-to-centroid distances of 3.724 (1) Å [slippage of 1.676 (1) Å] between the phenyl/tetrazine rings for (1) and of 3.716 (1) Å [slippage of 1.643 (3) Å] for (3)], respectively (Fig. 4
).
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Figure 4
Supramolecular π–π interactions of molecules of tetrazine (1) (top) and bromide (3) (bottom) with centroid-to-centroid distances indicated. Displacement ellipsoids are represented at the 50% probability level; symmetry code to obtain the second molecule: (1 − x, 1 − y, 1 − z). |
Two hydrogen bonds between hydroxy groups and tetrazine N atoms of molecules (2A) and (2B) form a bent dimer of alcohol (2), as shown in Fig. 5
, bottom. The drastic reduction in the N1—C2—C1—O1 torsion angle compared with tetrazine (1) may be explained by the reduced electron density at the neighbouring N atom, which is attributable to its role as a hydrogen-bond acceptor (Table 1
). Similar hydrogen-bonding interactions were described previously for hydroxymethyl substituted tetrazines (Voss et al., 2025
).
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Figure 5
(Top) Supramolecular π–π interactions of molecules of alcohol (2) with the centroid-to-centroid distances indicated; (bottom) formation of a dimer through hydrogen bonds (dashed lines). Displacement ellipsoids are represented at the 50% probability level; symmetry code to obtain the second molecule: ( |
Interestingly, the intermolecular hydrogen bonds of alcohol (2) cause the formation of weakly interacting parallel stacks of molecules without contacts between phenyl/tetrazine ring centroids but with comparably elongated phenyl/phenyl and tetrazine/tetrazine centroid-to-centroid distances of 4.557 (1) Å [slippage of 3.245 (1) Å] and 4.622 (1) Å [slippage of 3.311 (1) Å], respectively (Fig. 5
, top). The observation of stronger interactions between antiparallel stacks of tetrazine (1) and the bromide (3) as compared to parallel stacks of alcohol (2) might be favoured by the increased dipole moment between phenyl and tetrazine rings in antiparallel stacks (Huber et al., 2014
; Voss et al., 2025
).
4. Database survey
A search of the Cambridge Structural Database (CSD version 6.01, November 2025; Groom et al., 2016
) using ConQuest (version 2026.1.0) revealed eight reports for 3-aryl-6-alkyl-1,2,4,5-tetrazines, including CSD refcodes VEMZUM (Voss et al., 2025
), CICPOU (Hu & Xu, 2008
) and REWDUT (Xu & Hu, 2007
). Out of these, the lengths of all aromatic C—C, C—N and N—N bonds are identical within a 3σ margin of error. With dihedral angles between the phenyl and tetrazine rings of tetrazines (1)–(3) in the range 2.29 (4) to 8.47 (5)°, similar values between the two rings are also reported for these structurally similar tetrazines.
5. Synthesis and crystallisation
5.1. Materials and methods
Solvents and starting materials were used without further purification, unless noted otherwise. Dichloromethane for reactions was dried by distillation over CaH2. The solvents used for extraction and chromatography were of technical grade and were distilled prior to use. Column chromatography was performed with silica gel 60 M (Acros, 0.04–0.063 mm). Reactions were monitored by thin-layer chromatography (TLC) carried out on silica gel plates (Merck, F254) using UV light (254 nm) for visualization. 3-(Methoxymethyl)-6-phenyl-1,2,4,5-tetrazine (1) was used as starting material and synthesised following a literature protocol (Tu et al., 2019
).
5.2. Analytical devices
Nuclear magnetic resonance spectra were recorded on an Avance 500 spectrometer (Bruker) at 298 K using the residual protonated solvent signal [δ(1H of CHCl3) = 7.26 ppm, δ(13C of CDCl3) = 77.36 ppm] (Fulmer et al., 2010
) as internal standard. Electrospray ionisation (ESI) mass spectra (MS) were acquired with an Esquire 3000 ion trap mass spectrometer (Bruker Daltonik) equipped with a nano-ESI source.
5.3. Demethylation of 3-(methoxymethyl)-6-phenyl-1,2,4,5-tetrazine (1)
This reaction was performed under an argon atmosphere. Tetrazine (1) (593 mg, 2.93 mmol) was dissolved in dry CH2Cl2 (8 ml) and the resulting pink solution cooled to 258 K. A solution of BBr3 (0.70 ml, 7.38 mmol) in dry CH2Cl2 (15 ml) was added dropwise to this solution over the course of 10 min while maintaining the temperature. The resulting orange solution was stirred at 258 K for 105 min after which a small part of the solution (50 µl) was withdrawn, added to H2O (0.3 ml), and the organic layer analysed by TLC (CH2Cl2), which indicated full consumption of tetrazine (1). After a total of 155 min, the reaction mixture was poured onto ice (50 g) and CH2Cl2 (100 ml) was added consecutively. After the ice had melted, the layers were separated and the aqueous layer extracted with CH2Cl2 (1×80 ml). The combined pink organic layers were washed with brine (40 ml), dried over MgSO4, filtered and evaporated to obtain a pink solid (481 mg). Purification by column chromatography (diameter = 4.5 cm, length = 23 cm) using CH2Cl2/MeOH (95:5, v/v) to firstly obtain bromide (3) (90.0 mg, 358 µmol, 12%) as a pink solid. Secondly, tetrazine (1) (42.3 mg, 209 µmol, 7%) was re-isolated as a pink solid. Note that since analysis by TLC indicated complete consumption of tetrazine (1) a small amount of it must have been formed during the work-up, likely by methylation of alcohol (2) through in situ formed bromomethane. Thirdly, a mixture of different compounds and alcohol (2) (333 mg, Rf (CH2Cl2/MeOH, 95:5, v/v) = 0.22–0.07) was obtained. Purification of the third fraction by column chromatography (diameter = 4.5 cm, length = 33 cm) using CH2Cl2/MeOH (97.5:2.5, v/v) obtained alcohol (2) (291 mg, 1.55 mmol, 53%) as a pink solid. In Lang's pioneering work (Lang et al., 1975
), alcohol (2) was described as ‘relatively unstable', a finding which we are unable to confirm – all the compounds isolated here remained stable in solid form at room temperature for over a year.
Analytical data of tetrazine (1): 1H NMR (500 MHz, CDCl3) δ [ppm]: 8.63 (m, 2H, o-CarylH), 7.67–7.57 (m, 3H, m-/p-CarylH), 5.10 (s, 2H, CH2), 3.64 (s, 3H, CH3). 13C{1H}NMR (125 MHz{500 MHz}, CDCl3) δ [ppm]: 166.3 (CarylCH2), 165.2 (CarylPh), 133.1 (p-Caryl), 131.7 (Caryl attached to tetrazine), 129.5 (m-Caryl), 128.4 (o-Caryl), 72.3 (CH2), 59.8 (CH3). MS (ESI, positive): m/z = 225.0 [C10H10N4O+Na]+, 427.1 [2·(C10H10N4O)+Na]+. Rf (CH2Cl2/MeOH, 95:5, v/v) = 0.25). Tetrazine (1) was crystallized by slow evaporation from a CH2Cl2/MeOH solution at room temperature.
Analytical data of alcohol (2): 1H NMR (500 MHz, CDCl3) δ [ppm]: 8.62 (m, 2H, o-CarylH), 7.66 (m, 1H, p-CarylH), 7.61 (m, 2H, m-CarylH), 5.34 (d, 3J = 6.2 Hz, 2H, CH2), 3.12 (t, 3J = 6.3 Hz, 1H, OH). 13C{1H}NMR (125 MHz{500 MHz}, CDCl3) δ [ppm]: 167.4 (CarylCH2), 165.6 (CarylPh), 133.2 (p-Caryl), 131.6 (Caryl attached to tetrazine), 129.5 (m-Caryl), 128.4 (o-Caryl), 63.0 (CH2). MS (ESI, negative): m/z = 186.9 [C9H8N4O–H]−. Rf (CH2Cl2/MeOH, 97.5:2.5, v/v) = 0.20). Alcohol (2) was crystallized by slow evaporation from a CH2Cl2/cyclohexane solution at room temperature.
Analytical data of bromide (3): 1H NMR (500 MHz, CDCl3) δ [ppm]: 8.63 (m, 2H, o-CarylH), 7.66 (m, 1H, p-CarylH), 7.61 (m, 2H, m-CarylH), 5.00 (s, 2H, CH2). 13C{1H}NMR (125 MHz{500 MHz}, CDCl3) δ [ppm]: 167.4 (CarylCH2), 164.3 (CarylPh), 133.4 (p-Caryl), 131.4 (Caryl attached to tetrazine), 129.6 (m-Caryl), 128.6 (o-Caryl), 27.8 (CH2). MS (ESI): the compound was not ionisable. Rf (CH2Cl2/MeOH, 95:5, v/v) = 0.79. Bromide (3) was crystallized by slow evaporation from a CH2Cl2/MeOH solution at room temperature.
6. Refinement
Crystal data, data collection and structure refinement details are summarised in Table 2
. All structures were refined using NoSpherA2 (Kleemiss et al., 2021
), an implementation of non-spherical atom-form-factors in OLEX2 (Dolomanov et al., 2009
). All non-hydrogen atoms were refined anisotropically; hydrogen atoms were refined isotropically. ORCA 5.0 (Neese, 2022
) was used for quantum mechanical calculations. The olex2_refinement_description section of the CIF gives further details.
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Supporting information
Crystal structure: contains datablocks global, 1, 2, 3. DOI: https://doi.org/10.1107/S2056989026009527/wm5811sup1.cif
Structure factors: contains datablock 1. DOI: https://doi.org/10.1107/S2056989026009527/wm58111sup2.hkl
Structure factors: contains datablock 2. DOI: https://doi.org/10.1107/S2056989026009527/wm58112sup3.hkl
Structure factors: contains datablock 3. DOI: https://doi.org/10.1107/S2056989026009527/wm58113sup4.hkl
Supporting information file. DOI: https://doi.org/10.1107/S2056989026009527/wm58111sup5.cml
Supporting information file. DOI: https://doi.org/10.1107/S2056989026009527/wm58112sup6.cml
| C10H10N4O | Z = 2 |
| Mr = 202.22 | F(000) = 212.144 |
| Triclinic, P1 | Dx = 1.443 Mg m−3 |
| a = 5.3147 (4) Å | Mo Kα radiation, λ = 0.71073 Å |
| b = 7.4164 (8) Å | Cell parameters from 3153 reflections |
| c = 12.2277 (8) Å | θ = 2.8–32.2° |
| α = 86.710 (7)° | µ = 0.10 mm−1 |
| β = 79.913 (6)° | T = 100 K |
| γ = 78.920 (8)° | Block, clear light red |
| V = 465.53 (7) Å3 | 0.52 × 0.24 × 0.18 mm |
| SuperNova, Single source at offset/far, Eos diffractometer | 3058 independent reflections |
| Radiation source: micro-focus sealed X-ray tube, SuperNova (Mo) X-ray Source | 2256 reflections with I ≥ 2u(I) |
| Mirror monochromator | Rint = 0.035 |
| Detector resolution: 8.0951 pixels mm-1 | θmax = 32.5°, θmin = 1.7° |
| ω scans | h = −7→7 |
| Absorption correction: gaussian (CrysAlisPro; Rigaku OD, 2025) | k = −10→10 |
| Tmin = 0.571, Tmax = 1.000 | l = −18→18 |
| 8849 measured reflections |
| Refinement on F2 | 10 constraints |
| Least-squares matrix: full | Primary atom site location: dual |
| R[F2 > 2σ(F2)] = 0.038 | H-atom parameters constrained |
| wR(F2) = 0.061 | w = 1/[σ2(Fo2) + (0.0081P)2 + 0.0348P] where P = (Fo2 + 2Fc2)/3 |
| S = 1.09 | (Δ/σ)max = −0.0002 |
| 3058 reflections | Δρmax = 0.34 e Å−3 |
| 166 parameters | Δρmin = −0.33 e Å−3 |
| 0 restraints |
Refinement. Refinement using NoSpherA2, an implementation of NOn-SPHERical Atom-form-factors in Olex2. The following options were used: SOFTWARE: ORCA 6.1 PARTITIONING: NoSpherA2 INT ACCURACY: Normal METHOD: r2SCAN BASIS SET: def2-TZVPP CHARGE: 0 MULTIPLICITY: 1 SOLVATION: Water DATE: 2026-09-01_14-23-46. Hydrogen atoms were refined isotropically. |
| x | y | z | Uiso*/Ueq | ||
| O1 | 0.92532 (11) | 0.72986 (10) | 0.04592 (5) | 0.01998 (16) | |
| N1 | 0.90879 (13) | 0.72470 (11) | 0.29459 (5) | 0.01504 (16) | |
| N2 | 0.80917 (13) | 0.68850 (11) | 0.39730 (5) | 0.01471 (16) | |
| N3 | 0.40354 (13) | 0.86997 (11) | 0.37086 (5) | 0.01404 (16) | |
| N4 | 0.50426 (13) | 0.90517 (11) | 0.26685 (5) | 0.01454 (16) | |
| C1 | 0.88144 (18) | 0.88087 (14) | 0.11730 (7) | 0.01780 (19) | |
| H1A | 1.0746 (17) | 0.9105 (14) | 0.1216 (7) | 0.0214 (2)* | |
| H1B | 0.7597 (17) | 0.9979 (14) | 0.0836 (7) | 0.0214 (2)* | |
| C2 | 0.75552 (15) | 0.83623 (13) | 0.23290 (6) | 0.01368 (17) | |
| C3 | 0.55900 (15) | 0.76548 (12) | 0.43439 (6) | 0.01153 (17) | |
| C4 | 0.45400 (15) | 0.73006 (12) | 0.55162 (6) | 0.01131 (17) | |
| C5 | 0.61259 (15) | 0.61944 (13) | 0.61873 (6) | 0.01317 (18) | |
| H5 | 0.8094 (16) | 0.5550 (13) | 0.5846 (7) | 0.0158 (2)* | |
| C6 | 0.51547 (16) | 0.58844 (13) | 0.73007 (7) | 0.01524 (18) | |
| H6 | 0.6404 (16) | 0.5014 (14) | 0.7800 (7) | 0.0183 (2)* | |
| C7 | 0.26109 (16) | 0.66712 (13) | 0.77537 (7) | 0.01518 (18) | |
| H7 | 0.1901 (16) | 0.6439 (13) | 0.8630 (7) | 0.0182 (2)* | |
| C8 | 0.10211 (16) | 0.77628 (13) | 0.70835 (7) | 0.01495 (18) | |
| H8 | −0.0982 (17) | 0.8388 (14) | 0.7428 (7) | 0.0179 (2)* | |
| C9 | 0.19769 (15) | 0.80708 (13) | 0.59684 (7) | 0.01359 (18) | |
| H9 | 0.0751 (16) | 0.8899 (13) | 0.5440 (7) | 0.0163 (2)* | |
| C10 | 0.6980 (2) | 0.70573 (16) | 0.00716 (8) | 0.0244 (2) | |
| H10A | 0.7482 (19) | 0.5807 (16) | −0.0412 (8) | 0.0366 (3)* | |
| H10B | 0.5439 (19) | 0.7009 (15) | 0.0746 (8) | 0.0366 (3)* | |
| H10C | 0.6313 (19) | 0.8196 (16) | −0.0467 (8) | 0.0366 (3)* |
| U11 | U22 | U33 | U12 | U13 | U23 | |
| O1 | 0.0209 (3) | 0.0204 (4) | 0.0158 (3) | 0.0008 (3) | 0.0004 (2) | −0.0028 (3) |
| N1 | 0.0115 (3) | 0.0168 (4) | 0.0148 (3) | 0.0001 (3) | 0.0004 (3) | −0.0006 (3) |
| N2 | 0.0115 (3) | 0.0165 (4) | 0.0143 (3) | 0.0009 (3) | −0.0012 (3) | 0.0004 (3) |
| N3 | 0.0111 (3) | 0.0158 (4) | 0.0140 (3) | −0.0007 (3) | −0.0011 (3) | 0.0007 (3) |
| N4 | 0.0132 (3) | 0.0153 (4) | 0.0137 (3) | −0.0005 (3) | −0.0014 (3) | 0.0009 (3) |
| C1 | 0.0188 (4) | 0.0172 (5) | 0.0158 (4) | −0.0032 (4) | 0.0011 (3) | 0.0005 (4) |
| C2 | 0.0138 (4) | 0.0131 (5) | 0.0134 (4) | −0.0025 (3) | 0.0000 (3) | −0.0005 (3) |
| C3 | 0.0103 (4) | 0.0112 (4) | 0.0130 (4) | −0.0019 (3) | −0.0018 (3) | −0.0007 (3) |
| C4 | 0.0102 (4) | 0.0114 (4) | 0.0123 (4) | −0.0019 (3) | −0.0015 (3) | −0.0007 (3) |
| C5 | 0.0114 (4) | 0.0141 (5) | 0.0134 (4) | −0.0010 (3) | −0.0018 (3) | −0.0006 (3) |
| C6 | 0.0142 (4) | 0.0175 (5) | 0.0135 (4) | −0.0018 (4) | −0.0025 (3) | 0.0006 (3) |
| C7 | 0.0152 (4) | 0.0167 (5) | 0.0129 (4) | −0.0029 (4) | −0.0003 (3) | −0.0011 (3) |
| C8 | 0.0124 (4) | 0.0167 (5) | 0.0146 (4) | −0.0023 (4) | 0.0008 (3) | −0.0014 (3) |
| C9 | 0.0108 (4) | 0.0152 (5) | 0.0140 (4) | −0.0011 (3) | −0.0017 (3) | −0.0001 (3) |
| C10 | 0.0280 (5) | 0.0250 (6) | 0.0199 (5) | −0.0030 (5) | −0.0043 (4) | −0.0032 (4) |
| O1—C1 | 1.4181 (11) | C4—C9 | 1.4003 (11) |
| O1—C10 | 1.4176 (11) | C5—H5 | 1.084 (8) |
| N1—N2 | 1.3087 (9) | C5—C6 | 1.3915 (11) |
| N1—C2 | 1.3422 (10) | C6—H6 | 1.078 (8) |
| N2—C3 | 1.3514 (10) | C6—C7 | 1.3952 (11) |
| N3—N4 | 1.3226 (9) | C7—H7 | 1.087 (9) |
| N3—C3 | 1.3403 (10) | C7—C8 | 1.3944 (11) |
| N4—C2 | 1.3359 (10) | C8—H8 | 1.096 (8) |
| C1—H1A | 1.101 (9) | C8—C9 | 1.3912 (11) |
| C1—H1B | 1.086 (9) | C9—H9 | 1.081 (8) |
| C1—C2 | 1.5019 (12) | C10—H10A | 1.092 (11) |
| C3—C4 | 1.4724 (11) | C10—H10B | 1.060 (10) |
| C4—C5 | 1.3986 (11) | C10—H10C | 1.084 (11) |
| C10—O1—C1 | 113.11 (7) | C6—C5—C4 | 119.78 (7) |
| C2—N1—N2 | 117.77 (7) | C6—C5—H5 | 119.5 (4) |
| C3—N2—N1 | 118.01 (7) | H6—C6—C5 | 118.5 (5) |
| C3—N3—N4 | 117.89 (6) | C7—C6—C5 | 120.50 (8) |
| C2—N4—N3 | 117.60 (7) | C7—C6—H6 | 121.0 (5) |
| H1A—C1—O1 | 106.1 (5) | H7—C7—C6 | 119.4 (4) |
| H1B—C1—O1 | 109.8 (5) | C8—C7—C6 | 119.77 (8) |
| H1B—C1—H1A | 111.3 (7) | C8—C7—H7 | 120.8 (4) |
| C2—C1—O1 | 112.18 (8) | H8—C8—C7 | 120.5 (5) |
| C2—C1—H1A | 108.1 (5) | C9—C8—C7 | 119.99 (8) |
| C2—C1—H1B | 109.4 (5) | C9—C8—H8 | 119.5 (5) |
| N4—C2—N1 | 124.67 (8) | C8—C9—C4 | 120.29 (8) |
| C1—C2—N1 | 115.93 (7) | H9—C9—C4 | 119.2 (5) |
| C1—C2—N4 | 119.39 (7) | H9—C9—C8 | 120.5 (5) |
| N3—C3—N2 | 123.89 (7) | H10A—C10—O1 | 107.4 (5) |
| C4—C3—N2 | 117.22 (7) | H10B—C10—O1 | 110.6 (5) |
| C4—C3—N3 | 118.89 (7) | H10B—C10—H10A | 112.8 (9) |
| C5—C4—C3 | 119.64 (7) | H10C—C10—O1 | 111.3 (6) |
| C9—C4—C3 | 120.71 (7) | H10C—C10—H10A | 108.2 (7) |
| C9—C4—C5 | 119.65 (7) | H10C—C10—H10B | 106.6 (8) |
| H5—C5—C4 | 120.7 (4) | ||
| O1—C1—C2—N1 | 73.17 (8) | N4—N3—C3—C4 | 177.76 (7) |
| O1—C1—C2—N4 | −105.80 (8) | C2—N1—N2—C3 | 0.06 (9) |
| N1—N2—C3—N3 | 3.10 (9) | C2—N4—N3—C3 | −1.00 (9) |
| N1—N2—C3—C4 | −177.26 (7) | C2—C1—O1—C10 | 78.41 (9) |
| N1—C2—N4—N3 | 4.28 (11) | C3—C4—C5—C6 | 178.83 (8) |
| N2—N1—C2—N4 | −3.79 (9) | C3—C4—C9—C8 | −178.51 (8) |
| N2—N1—C2—C1 | 177.30 (8) | C4—C5—C6—C7 | −0.10 (10) |
| N2—C3—N3—N4 | −2.60 (10) | C4—C9—C8—C7 | −0.51 (10) |
| N2—C3—C4—C5 | −0.45 (9) | C5—C4—C9—C8 | 1.00 (10) |
| N2—C3—C4—C9 | 179.06 (8) | C5—C6—C7—C8 | 0.59 (11) |
| N3—N4—C2—C1 | −176.84 (8) | C6—C5—C4—C9 | −0.69 (10) |
| N3—C3—C4—C5 | 179.21 (8) | C6—C7—C8—C9 | −0.29 (11) |
| N3—C3—C4—C9 | −1.28 (10) |
| C9H8N4O | F(000) = 784.550 |
| Mr = 188.19 | Dx = 1.439 Mg m−3 |
| Monoclinic, P21/n | Mo Kα radiation, λ = 0.71073 Å |
| a = 11.8719 (3) Å | Cell parameters from 9457 reflections |
| b = 8.4682 (2) Å | θ = 2.1–30.8° |
| c = 17.2987 (5) Å | µ = 0.10 mm−1 |
| β = 92.709 (2)° | T = 100 K |
| V = 1737.16 (8) Å3 | Needle, clear red |
| Z = 8 | 0.35 × 0.09 × 0.06 mm |
| SuperNova, Single source at offset/far, Eos diffractometer | 4666 independent reflections |
| Radiation source: micro-focus sealed X-ray tube, SuperNova (Mo) X-ray Source | 3774 reflections with I ≥ 2u(I) |
| Mirror monochromator | Rint = 0.045 |
| Detector resolution: 8.0951 pixels mm-1 | θmax = 29.1°, θmin = 2.0° |
| ω scans | h = −16→17 |
| Absorption correction: gaussian (CrysAlisPro; Rigaku OD, 2025) | k = −12→11 |
| Tmin = 0.744, Tmax = 1.000 | l = −24→24 |
| 32315 measured reflections |
| Refinement on F2 | 0 constraints |
| Least-squares matrix: full | Primary atom site location: dual |
| R[F2 > 2σ(F2)] = 0.030 | All H-atom parameters refined |
| wR(F2) = 0.066 | w = 1/[σ2(Fo2) + (0.0179P)2 + 0.2291P] where P = (Fo2 + 2Fc2)/3 |
| S = 1.07 | (Δ/σ)max = −0.0000 |
| 4666 reflections | Δρmax = 0.21 e Å−3 |
| 317 parameters | Δρmin = −0.21 e Å−3 |
| 0 restraints |
Refinement. Refinement using NoSpherA2, an implementation of NOn-SPHERical Atom-form-factors in Olex2. The following options were used: SOFTWARE: ORCA 6.1 PARTITIONING: NoSpherA2 INT ACCURACY: Normal METHOD: r2SCAN BASIS SET: def2-TZVPP CHARGE: 0 MULTIPLICITY: 1 SOLVATION: Water DATE: 2026-09-01_16-19-35. Hydrogen atoms were refined isotropically. |
| x | y | z | Uiso*/Ueq | ||
| O1A | 0.59801 (5) | 1.02413 (7) | 0.28063 (4) | 0.01965 (14) | |
| H1A | 0.6607 (10) | 0.9789 (14) | 0.3110 (7) | 0.029 (3)* | |
| O1B | 0.86881 (5) | 1.01966 (7) | 0.25962 (4) | 0.02058 (14) | |
| H1B | 0.8062 (11) | 0.9790 (15) | 0.2273 (7) | 0.035 (3)* | |
| N1A | 0.52904 (6) | 0.74303 (8) | 0.12699 (4) | 0.01679 (15) | |
| N1B | 0.76371 (6) | 0.82834 (8) | 0.36380 (4) | 0.01715 (15) | |
| N2A | 0.57676 (5) | 0.67508 (8) | 0.06899 (4) | 0.01688 (15) | |
| N2B | 0.71656 (6) | 0.75248 (8) | 0.42088 (4) | 0.01752 (15) | |
| N3A | 0.75136 (6) | 0.79518 (8) | 0.10707 (4) | 0.01599 (15) | |
| N3B | 0.89047 (6) | 0.62307 (9) | 0.45041 (4) | 0.01907 (16) | |
| N4A | 0.70263 (6) | 0.86196 (8) | 0.16591 (4) | 0.01601 (15) | |
| N4B | 0.93624 (6) | 0.69768 (9) | 0.39344 (4) | 0.01918 (16) | |
| C1A | 0.53859 (7) | 0.89889 (11) | 0.24476 (5) | 0.01957 (18) | |
| H1Aa | 0.5285 (9) | 0.8000 (13) | 0.2849 (6) | 0.039 (3)* | |
| H1Ab | 0.4555 (9) | 0.9394 (13) | 0.2265 (6) | 0.043 (3)* | |
| C1B | 0.92960 (7) | 0.88877 (11) | 0.28883 (5) | 0.01941 (18) | |
| H1Ba | 0.9452 (9) | 0.8015 (13) | 0.2444 (6) | 0.042 (3)* | |
| H1Bb | 1.0106 (9) | 0.9282 (12) | 0.3117 (6) | 0.034 (3)* | |
| C2A | 0.59403 (6) | 0.83232 (9) | 0.17545 (5) | 0.01452 (16) | |
| C2B | 0.87263 (7) | 0.80304 (10) | 0.35268 (5) | 0.01583 (17) | |
| C3A | 0.68812 (6) | 0.70005 (9) | 0.06061 (5) | 0.01377 (16) | |
| C3B | 0.78189 (7) | 0.65559 (10) | 0.46492 (5) | 0.01512 (17) | |
| C4A | 0.74238 (6) | 0.61986 (9) | −0.00351 (5) | 0.01426 (16) | |
| C4B | 0.73344 (7) | 0.57847 (10) | 0.53216 (5) | 0.01579 (17) | |
| C5A | 0.67944 (7) | 0.52052 (10) | −0.05393 (5) | 0.01702 (17) | |
| H5A | 0.5903 (8) | 0.5023 (12) | −0.0456 (6) | 0.031 (3)* | |
| C5B | 0.61878 (7) | 0.59683 (11) | 0.54546 (5) | 0.02024 (18) | |
| H5B | 0.5665 (9) | 0.6653 (14) | 0.5054 (6) | 0.040 (3)* | |
| C6A | 0.73229 (7) | 0.44423 (10) | −0.11365 (5) | 0.01900 (18) | |
| H6A | 0.6838 (9) | 0.3643 (13) | −0.1510 (6) | 0.036 (3)* | |
| C6B | 0.57384 (8) | 0.52971 (11) | 0.61061 (5) | 0.0245 (2) | |
| H6B | 0.4841 (9) | 0.5440 (13) | 0.6203 (6) | 0.039 (3)* | |
| C7A | 0.84716 (7) | 0.46702 (11) | −0.12364 (5) | 0.01942 (18) | |
| H7A | 0.8874 (9) | 0.4069 (13) | −0.1685 (7) | 0.043 (3)* | |
| C7B | 0.64302 (8) | 0.44385 (12) | 0.66256 (5) | 0.0257 (2) | |
| H7B | 0.6084 (9) | 0.3926 (13) | 0.7137 (7) | 0.041 (3)* | |
| C8A | 0.90950 (7) | 0.56615 (11) | −0.07371 (5) | 0.01958 (18) | |
| H8A | 0.9988 (9) | 0.5834 (13) | −0.0805 (6) | 0.038 (3)* | |
| C8B | 0.75664 (8) | 0.42286 (11) | 0.64873 (5) | 0.0247 (2) | |
| H8B | 0.8100 (9) | 0.3533 (14) | 0.6870 (7) | 0.048 (3)* | |
| C9A | 0.85757 (7) | 0.64189 (10) | −0.01341 (5) | 0.01796 (18) | |
| H9A | 0.9041 (8) | 0.7182 (12) | 0.0273 (6) | 0.028 (3)* | |
| C9B | 0.80233 (7) | 0.48971 (10) | 0.58373 (5) | 0.01967 (18) | |
| H9B | 0.8907 (9) | 0.4737 (13) | 0.5731 (6) | 0.039 (3)* |
| U11 | U22 | U33 | U12 | U13 | U23 | |
| O1A | 0.0218 (3) | 0.0163 (3) | 0.0205 (3) | 0.0027 (2) | −0.0014 (3) | −0.0006 (2) |
| O1B | 0.0229 (3) | 0.0159 (3) | 0.0225 (3) | −0.0039 (2) | −0.0036 (3) | −0.0006 (2) |
| N1A | 0.0115 (3) | 0.0197 (4) | 0.0190 (4) | −0.0028 (3) | −0.0002 (3) | −0.0001 (3) |
| N1B | 0.0151 (3) | 0.0180 (4) | 0.0182 (4) | 0.0037 (3) | −0.0015 (3) | 0.0009 (3) |
| N2A | 0.0120 (3) | 0.0199 (4) | 0.0187 (4) | −0.0036 (3) | −0.0004 (3) | −0.0019 (3) |
| N2B | 0.0140 (3) | 0.0197 (4) | 0.0188 (4) | 0.0044 (3) | −0.0006 (3) | 0.0011 (3) |
| N3A | 0.0125 (3) | 0.0189 (4) | 0.0164 (4) | −0.0045 (3) | −0.0005 (3) | −0.0008 (3) |
| N3B | 0.0149 (3) | 0.0211 (4) | 0.0210 (4) | 0.0054 (3) | −0.0016 (3) | 0.0015 (3) |
| N4A | 0.0145 (3) | 0.0174 (4) | 0.0160 (3) | −0.0038 (3) | −0.0006 (3) | −0.0005 (3) |
| N4B | 0.0145 (3) | 0.0215 (4) | 0.0215 (4) | 0.0035 (3) | −0.0000 (3) | 0.0010 (3) |
| C1A | 0.0161 (4) | 0.0211 (5) | 0.0217 (5) | 0.0003 (3) | 0.0019 (3) | −0.0022 (4) |
| C1B | 0.0196 (4) | 0.0174 (4) | 0.0212 (5) | −0.0018 (3) | 0.0007 (3) | −0.0013 (3) |
| C2A | 0.0132 (4) | 0.0141 (4) | 0.0162 (4) | −0.0005 (3) | −0.0003 (3) | 0.0010 (3) |
| C2B | 0.0146 (4) | 0.0154 (4) | 0.0173 (4) | 0.0007 (3) | −0.0012 (3) | −0.0018 (3) |
| C3A | 0.0117 (4) | 0.0151 (4) | 0.0144 (4) | −0.0025 (3) | −0.0008 (3) | 0.0015 (3) |
| C3B | 0.0141 (4) | 0.0151 (4) | 0.0160 (4) | 0.0020 (3) | −0.0014 (3) | −0.0018 (3) |
| C4A | 0.0131 (4) | 0.0156 (4) | 0.0139 (4) | −0.0026 (3) | −0.0009 (3) | 0.0015 (3) |
| C4B | 0.0166 (4) | 0.0149 (4) | 0.0157 (4) | 0.0011 (3) | −0.0013 (3) | −0.0017 (3) |
| C5A | 0.0152 (4) | 0.0197 (4) | 0.0160 (4) | −0.0035 (3) | −0.0009 (3) | −0.0005 (3) |
| C5B | 0.0176 (4) | 0.0230 (5) | 0.0202 (5) | 0.0023 (3) | 0.0013 (3) | −0.0010 (4) |
| C6A | 0.0198 (4) | 0.0207 (4) | 0.0164 (4) | −0.0035 (3) | −0.0003 (3) | −0.0017 (3) |
| C6B | 0.0234 (5) | 0.0287 (5) | 0.0217 (5) | −0.0027 (4) | 0.0048 (4) | −0.0015 (4) |
| C7A | 0.0201 (4) | 0.0219 (4) | 0.0165 (4) | 0.0002 (3) | 0.0029 (3) | −0.0004 (3) |
| C7B | 0.0320 (5) | 0.0267 (5) | 0.0183 (5) | −0.0086 (4) | 0.0015 (4) | 0.0006 (4) |
| C8A | 0.0147 (4) | 0.0245 (5) | 0.0196 (4) | −0.0009 (3) | 0.0022 (3) | −0.0002 (3) |
| C8B | 0.0289 (5) | 0.0243 (5) | 0.0203 (5) | −0.0049 (4) | −0.0057 (4) | 0.0039 (4) |
| C9A | 0.0134 (4) | 0.0221 (4) | 0.0183 (4) | −0.0030 (3) | 0.0002 (3) | −0.0010 (3) |
| C9B | 0.0201 (4) | 0.0194 (4) | 0.0190 (4) | −0.0005 (3) | −0.0043 (3) | 0.0012 (3) |
| O1A—H1A | 0.969 (12) | C3B—C4B | 1.4742 (12) |
| O1A—C1A | 1.4022 (10) | C4A—C5A | 1.4018 (11) |
| O1B—H1B | 0.972 (13) | C4A—C9A | 1.3988 (11) |
| O1B—C1B | 1.4036 (10) | C4B—C5B | 1.3999 (11) |
| N1A—N2A | 1.3086 (10) | C4B—C9B | 1.4003 (11) |
| N1A—C2A | 1.3448 (10) | C5A—H5A | 1.085 (10) |
| N1B—N2B | 1.3242 (10) | C5A—C6A | 1.3926 (12) |
| N1B—C2B | 1.3336 (10) | C5B—H5B | 1.078 (11) |
| N2A—C3A | 1.3534 (10) | C5B—C6B | 1.3909 (13) |
| N2B—C3B | 1.3413 (10) | C6A—H6A | 1.082 (10) |
| N3A—N4A | 1.3214 (10) | C6A—C7A | 1.3961 (12) |
| N3A—C3A | 1.3421 (10) | C6B—H6B | 1.093 (11) |
| N3B—N4B | 1.3101 (10) | C6B—C7B | 1.3932 (13) |
| N3B—C3B | 1.3533 (10) | C7A—H7A | 1.061 (11) |
| N4A—C2A | 1.3314 (10) | C7A—C8A | 1.3922 (12) |
| N4B—C2B | 1.3466 (10) | C7B—H7B | 1.084 (11) |
| C1A—H1Aa | 1.098 (11) | C7B—C8B | 1.3925 (13) |
| C1A—H1Ab | 1.078 (11) | C8A—H8A | 1.082 (10) |
| C1A—C2A | 1.5042 (12) | C8A—C9A | 1.3929 (12) |
| C1B—H1Ba | 1.089 (11) | C8B—H8B | 1.071 (11) |
| C1B—H1Bb | 1.075 (10) | C8B—C9B | 1.3918 (13) |
| C1B—C2B | 1.5083 (12) | C9A—H9A | 1.087 (10) |
| C3A—C4A | 1.4745 (11) | C9B—H9B | 1.082 (11) |
| C1A—O1A—H1A | 107.3 (7) | C9A—C4A—C3A | 119.68 (7) |
| C1B—O1B—H1B | 107.0 (7) | C9A—C4A—C5A | 119.95 (8) |
| C2A—N1A—N2A | 117.96 (7) | C5B—C4B—C3B | 119.95 (7) |
| C2B—N1B—N2B | 118.46 (7) | C9B—C4B—C3B | 120.17 (7) |
| C3A—N2A—N1A | 118.29 (7) | C9B—C4B—C5B | 119.87 (8) |
| C3B—N2B—N1B | 117.83 (7) | H5A—C5A—C4A | 119.8 (5) |
| C3A—N3A—N4A | 117.73 (7) | C6A—C5A—C4A | 119.63 (8) |
| C3B—N3B—N4B | 118.29 (7) | C6A—C5A—H5A | 120.6 (5) |
| C2A—N4A—N3A | 118.46 (7) | H5B—C5B—C4B | 119.3 (6) |
| C2B—N4B—N3B | 118.11 (7) | C6B—C5B—C4B | 120.07 (8) |
| H1Aa—C1A—O1A | 111.4 (6) | C6B—C5B—H5B | 120.6 (6) |
| H1Ab—C1A—O1A | 108.9 (6) | H6A—C6A—C5A | 119.1 (6) |
| H1Ab—C1A—H1Aa | 107.6 (8) | C7A—C6A—C5A | 120.31 (8) |
| C2A—C1A—O1A | 113.97 (7) | C7A—C6A—H6A | 120.5 (6) |
| C2A—C1A—H1Aa | 106.4 (6) | H6B—C6B—C5B | 119.6 (6) |
| C2A—C1A—H1Ab | 108.3 (6) | C7B—C6B—C5B | 119.93 (9) |
| H1Ba—C1B—O1B | 112.6 (6) | C7B—C6B—H6B | 120.5 (6) |
| H1Bb—C1B—O1B | 108.8 (6) | H7A—C7A—C6A | 120.0 (6) |
| H1Bb—C1B—H1Ba | 106.9 (8) | C8A—C7A—C6A | 120.02 (8) |
| C2B—C1B—O1B | 113.76 (7) | C8A—C7A—H7A | 119.9 (6) |
| C2B—C1B—H1Ba | 106.7 (6) | H7B—C7B—C6B | 120.1 (6) |
| C2B—C1B—H1Bb | 107.7 (6) | C8B—C7B—C6B | 120.14 (9) |
| N4A—C2A—N1A | 123.99 (8) | C8B—C7B—H7B | 119.8 (6) |
| C1A—C2A—N1A | 116.60 (7) | H8A—C8A—C7A | 120.6 (6) |
| C1A—C2A—N4A | 119.40 (7) | C9A—C8A—C7A | 120.08 (8) |
| N4B—C2B—N1B | 123.68 (8) | C9A—C8A—H8A | 119.3 (6) |
| C1B—C2B—N1B | 119.98 (7) | H8B—C8B—C7B | 120.9 (6) |
| C1B—C2B—N4B | 116.27 (7) | C9B—C8B—C7B | 120.31 (9) |
| N3A—C3A—N2A | 123.45 (8) | C9B—C8B—H8B | 118.8 (6) |
| C4A—C3A—N2A | 118.18 (7) | C8A—C9A—C4A | 120.01 (8) |
| C4A—C3A—N3A | 118.36 (7) | H9A—C9A—C4A | 118.0 (5) |
| N3B—C3B—N2B | 123.33 (8) | H9A—C9A—C8A | 122.0 (5) |
| C4B—C3B—N2B | 118.84 (7) | C8B—C9B—C4B | 119.66 (8) |
| C4B—C3B—N3B | 117.83 (7) | H9B—C9B—C4B | 120.0 (6) |
| C5A—C4A—C3A | 120.37 (7) | H9B—C9B—C8B | 120.3 (6) |
| O1A—C1A—C2A—N1A | −162.92 (7) | N3B—C3B—C4B—C5B | −174.15 (7) |
| O1A—C1A—C2A—N4A | 18.03 (9) | N3B—C3B—C4B—C9B | 7.26 (9) |
| O1B—C1B—C2B—N1B | 16.06 (9) | N4A—N3A—C3A—C4A | −177.69 (7) |
| O1B—C1B—C2B—N4B | −166.93 (7) | N4B—N3B—C3B—C4B | −176.25 (7) |
| N1A—N2A—C3A—N3A | −2.39 (9) | C2A—N1A—N2A—C3A | −0.78 (9) |
| N1A—N2A—C3A—C4A | 178.34 (7) | C2A—N4A—N3A—C3A | −0.49 (8) |
| N1A—C2A—N4A—N3A | −2.73 (9) | C2B—N1B—N2B—C3B | 0.77 (9) |
| N1B—N2B—C3B—N3B | −5.01 (9) | C2B—N4B—N3B—C3B | 0.23 (9) |
| N1B—N2B—C3B—C4B | 175.76 (7) | C3A—C4A—C5A—C6A | −179.25 (8) |
| N1B—C2B—N4B—N3B | −4.47 (10) | C3A—C4A—C9A—C8A | 179.81 (8) |
| N2A—N1A—C2A—N4A | 3.38 (9) | C3B—C4B—C5B—C6B | −177.30 (8) |
| N2A—N1A—C2A—C1A | −175.62 (7) | C3B—C4B—C9B—C8B | 177.35 (8) |
| N2A—C3A—N3A—N4A | 3.04 (9) | C4A—C5A—C6A—C7A | −0.35 (10) |
| N2A—C3A—C4A—C5A | −0.12 (9) | C4A—C9A—C8A—C7A | −0.75 (10) |
| N2A—C3A—C4A—C9A | −179.41 (7) | C4B—C5B—C6B—C7B | −0.14 (10) |
| N2B—N1B—C2B—N4B | 3.95 (9) | C4B—C9B—C8B—C7B | 0.03 (10) |
| N2B—N1B—C2B—C1B | −179.28 (7) | C5A—C4A—C9A—C8A | 0.51 (9) |
| N2B—C3B—N3B—N4B | 4.50 (9) | C5A—C6A—C7A—C8A | 0.12 (10) |
| N2B—C3B—C4B—C5B | 5.13 (9) | C5B—C4B—C9B—C8B | −1.23 (9) |
| N2B—C3B—C4B—C9B | −173.46 (8) | C5B—C6B—C7B—C8B | −1.07 (11) |
| N3A—N4A—C2A—C1A | 176.25 (7) | C6A—C5A—C4A—C9A | 0.04 (10) |
| N3A—C3A—C4A—C5A | −179.42 (7) | C6A—C7A—C8A—C9A | 0.43 (10) |
| N3A—C3A—C4A—C9A | 1.29 (9) | C6B—C5B—C4B—C9B | 1.29 (10) |
| N3B—N4B—C2B—C1B | 178.65 (7) | C6B—C7B—C8B—C9B | 1.13 (11) |
| D—H···A | D—H | H···A | D···A | D—H···A |
| O1A—H1A···N1B | 0.969 (12) | 1.963 (13) | 2.9019 (9) | 162.7 (10) |
| O1B—H1B···N4A | 0.972 (13) | 1.871 (13) | 2.8287 (9) | 168.2 (11) |
| C9H7BrN4 | Z = 2 |
| Mr = 251.09 | F(000) = 247.736 |
| Triclinic, P1 | Dx = 1.814 Mg m−3 |
| a = 5.2376 (4) Å | Mo Kα radiation, λ = 0.71073 Å |
| b = 7.5069 (6) Å | Cell parameters from 3207 reflections |
| c = 12.0638 (8) Å | θ = 3.2–30.6° |
| α = 89.632 (6)° | µ = 4.44 mm−1 |
| β = 80.517 (6)° | T = 100 K |
| γ = 79.451 (7)° | Block, clear red |
| V = 459.80 (6) Å3 | 0.35 × 0.29 × 0.09 mm |
| SuperNova, Single source at offset/far, Eos diffractometer | 2531 independent reflections |
| Radiation source: micro-focus sealed X-ray tube, SuperNova (Mo) X-ray Source | 2136 reflections with I ≥ 2u(I) |
| Mirror monochromator | Rint = 0.048 |
| Detector resolution: 8.0951 pixels mm-1 | θmax = 29.6°, θmin = 1.7° |
| ω scans | h = −7→7 |
| Absorption correction: gaussian (CrysAlisPro; Rigaku OD, 2025) | k = −10→10 |
| Tmin = 0.394, Tmax = 1.000 | l = −17→16 |
| 7431 measured reflections |
| Refinement on F2 | 7 constraints |
| Least-squares matrix: full | Primary atom site location: dual |
| R[F2 > 2σ(F2)] = 0.033 | H-atom parameters constrained |
| wR(F2) = 0.061 | w = 1/[σ2(Fo2) + (0.0159P)2] where P = (Fo2 + 2Fc2)/3 |
| S = 1.03 | (Δ/σ)max = −0.0002 |
| 2531 reflections | Δρmax = 0.81 e Å−3 |
| 148 parameters | Δρmin = −0.70 e Å−3 |
| 0 restraints |
Refinement. Refinement using NoSpherA2, an implementation of NOn-SPHERical Atom-form-factors in Olex2. The following options were used: SOFTWARE: ORCA 6.1 PARTITIONING: NoSpherA2 INT ACCURACY: Normal METHOD: r2SCAN BASIS SET: def2-TZVPP CHARGE: 0 MULTIPLICITY: 1 SOLVATION: Water DATE: 2026-09-01_14-39-25. Hydrogen atoms were refined isotropically. |
| x | y | z | Uiso*/Ueq | ||
| Br1 | 0.65100 (5) | 0.72768 (3) | 0.010906 (19) | 0.02391 (8) | |
| N1 | 0.8794 (3) | 0.7258 (3) | 0.28825 (15) | 0.0176 (4) | |
| N2 | 0.7978 (3) | 0.6944 (3) | 0.39466 (15) | 0.0178 (4) | |
| N3 | 0.3775 (3) | 0.8719 (2) | 0.38276 (15) | 0.0172 (4) | |
| N4 | 0.4589 (3) | 0.9025 (3) | 0.27664 (16) | 0.0191 (4) | |
| C1 | 0.8027 (5) | 0.8656 (3) | 0.11273 (19) | 0.0212 (5) | |
| H1a | 1.023 (5) | 0.823 (3) | 0.0968 (19) | 0.0254 (6)* | |
| H1b | 0.726 (5) | 1.015 (3) | 0.097 (2) | 0.0254 (6)* | |
| C2 | 0.7078 (4) | 0.8275 (3) | 0.23224 (18) | 0.0159 (4) | |
| C3 | 0.5477 (4) | 0.7671 (3) | 0.43979 (18) | 0.0144 (4) | |
| C4 | 0.4543 (4) | 0.7315 (3) | 0.55885 (17) | 0.0134 (4) | |
| C5 | 0.6212 (4) | 0.6175 (3) | 0.62007 (18) | 0.0148 (4) | |
| H5 | 0.817 (4) | 0.550 (3) | 0.5826 (18) | 0.0178 (5)* | |
| C6 | 0.5325 (4) | 0.5841 (3) | 0.73262 (19) | 0.0174 (5) | |
| H6 | 0.664 (4) | 0.495 (3) | 0.7779 (19) | 0.0209 (5)* | |
| C7 | 0.2781 (4) | 0.6636 (3) | 0.78360 (19) | 0.0171 (5) | |
| H7 | 0.211 (4) | 0.629 (3) | 0.8726 (19) | 0.0205 (5)* | |
| C8 | 0.1121 (4) | 0.7774 (3) | 0.72290 (19) | 0.0178 (5) | |
| H8 | −0.086 (4) | 0.841 (3) | 0.7634 (19) | 0.0214 (5)* | |
| C9 | 0.1997 (4) | 0.8101 (3) | 0.61046 (18) | 0.0152 (4) | |
| H9 | 0.075 (4) | 0.900 (3) | 0.5609 (19) | 0.0182 (5)* |
| U11 | U22 | U33 | U12 | U13 | U23 | |
| Br1 | 0.02876 (14) | 0.02440 (14) | 0.01709 (13) | −0.00081 (10) | −0.00401 (9) | −0.00149 (9) |
| N1 | 0.0139 (9) | 0.0189 (10) | 0.0180 (10) | 0.0008 (7) | −0.0008 (7) | −0.0004 (8) |
| N2 | 0.0124 (9) | 0.0200 (10) | 0.0189 (10) | 0.0018 (8) | −0.0022 (7) | 0.0004 (8) |
| N3 | 0.0134 (9) | 0.0171 (10) | 0.0194 (10) | 0.0015 (7) | −0.0024 (7) | 0.0004 (8) |
| N4 | 0.0159 (10) | 0.0192 (10) | 0.0205 (10) | 0.0012 (8) | −0.0030 (7) | 0.0022 (8) |
| C1 | 0.0201 (12) | 0.0232 (13) | 0.0195 (12) | −0.0036 (10) | −0.0020 (9) | 0.0040 (10) |
| C2 | 0.0149 (11) | 0.0156 (11) | 0.0171 (11) | −0.0015 (8) | −0.0036 (8) | 0.0004 (9) |
| C3 | 0.0116 (10) | 0.0135 (11) | 0.0180 (11) | −0.0010 (8) | −0.0032 (8) | −0.0010 (9) |
| C4 | 0.0121 (10) | 0.0098 (10) | 0.0183 (11) | −0.0003 (8) | −0.0041 (8) | −0.0015 (8) |
| C5 | 0.0114 (10) | 0.0134 (11) | 0.0181 (11) | 0.0019 (8) | −0.0023 (8) | −0.0008 (9) |
| C6 | 0.0145 (11) | 0.0153 (11) | 0.0214 (12) | 0.0012 (9) | −0.0045 (9) | −0.0006 (9) |
| C7 | 0.0166 (11) | 0.0153 (11) | 0.0186 (12) | −0.0013 (9) | −0.0023 (9) | 0.0012 (9) |
| C8 | 0.0129 (11) | 0.0181 (12) | 0.0206 (12) | 0.0003 (9) | −0.0008 (9) | −0.0009 (9) |
| C9 | 0.0115 (10) | 0.0152 (11) | 0.0179 (11) | −0.0000 (8) | −0.0021 (8) | 0.0004 (9) |
| Br1—C1 | 1.962 (2) | C4—C5 | 1.404 (3) |
| N1—N2 | 1.318 (2) | C4—C9 | 1.399 (3) |
| N1—C2 | 1.338 (3) | C5—H5 | 1.09 (2) |
| N2—C3 | 1.348 (3) | C5—C6 | 1.397 (3) |
| N3—N4 | 1.314 (2) | C6—H6 | 1.08 (2) |
| N3—C3 | 1.351 (3) | C6—C7 | 1.397 (3) |
| N4—C2 | 1.345 (3) | C7—H7 | 1.12 (2) |
| C1—H1a | 1.13 (2) | C7—C8 | 1.397 (3) |
| C1—H1b | 1.15 (3) | C8—H8 | 1.09 (2) |
| C1—C2 | 1.489 (3) | C8—C9 | 1.394 (3) |
| C3—C4 | 1.478 (3) | C9—H9 | 1.10 (2) |
| C2—N1—N2 | 117.68 (17) | C9—C4—C3 | 120.19 (18) |
| C3—N2—N1 | 117.92 (17) | C9—C4—C5 | 119.94 (19) |
| C3—N3—N4 | 118.14 (18) | H5—C5—C4 | 122.4 (11) |
| C2—N4—N3 | 117.46 (18) | C6—C5—C4 | 119.76 (19) |
| H1a—C1—Br1 | 109.3 (12) | C6—C5—H5 | 117.8 (11) |
| H1b—C1—Br1 | 105.8 (12) | H6—C6—C5 | 118.5 (12) |
| H1b—C1—H1a | 115.0 (17) | C7—C6—C5 | 119.9 (2) |
| C2—C1—Br1 | 110.83 (15) | C7—C6—H6 | 121.6 (12) |
| C2—C1—H1a | 107.5 (12) | H7—C7—C6 | 118.0 (12) |
| C2—C1—H1b | 108.4 (12) | C8—C7—C6 | 120.4 (2) |
| N4—C2—N1 | 125.0 (2) | C8—C7—H7 | 121.5 (12) |
| C1—C2—N1 | 117.44 (19) | H8—C8—C7 | 120.2 (12) |
| C1—C2—N4 | 117.57 (19) | C9—C8—C7 | 119.8 (2) |
| N3—C3—N2 | 123.82 (19) | C9—C8—H8 | 120.0 (12) |
| C4—C3—N2 | 118.23 (18) | C8—C9—C4 | 120.18 (19) |
| C4—C3—N3 | 117.95 (18) | H9—C9—C4 | 118.2 (12) |
| C5—C4—C3 | 119.87 (18) | H9—C9—C8 | 121.6 (12) |
| Br1—C1—C2—N1 | 107.43 (16) | N3—C3—C4—C9 | −2.1 (2) |
| Br1—C1—C2—N4 | −74.63 (17) | N4—N3—C3—C4 | −179.36 (18) |
| N1—N2—C3—N3 | −0.9 (2) | C2—N1—N2—C3 | −0.2 (2) |
| N1—N2—C3—C4 | 179.59 (18) | C2—N4—N3—C3 | −0.3 (2) |
| N1—C2—N4—N3 | −0.8 (2) | C3—C4—C5—C6 | 179.94 (19) |
| N2—N1—C2—N4 | 1.0 (2) | C3—C4—C9—C8 | −179.63 (19) |
| N2—N1—C2—C1 | 178.79 (19) | C4—C5—C6—C7 | 0.3 (2) |
| N2—C3—N3—N4 | 1.1 (2) | C4—C9—C8—C7 | −0.9 (2) |
| N2—C3—C4—C5 | −2.9 (2) | C5—C4—C9—C8 | 0.7 (2) |
| N2—C3—C4—C9 | 177.44 (19) | C5—C6—C7—C8 | −0.5 (2) |
| N3—N4—C2—C1 | −178.56 (19) | C6—C5—C4—C9 | −0.4 (2) |
| N3—C3—C4—C5 | 177.48 (18) | C6—C7—C8—C9 | 0.8 (2) |
Acknowledgements
The authors are deeply grateful to Professor Dr Norbert Sewald for his constant encouragement and for providing infrastructure and research materials. Jona Voss thanks the Studienstiftung des deutschen Volkes for its support. We also thank Dr Jascha Rüter for fruitful discussions and proof-reading of the manuscript. Open access funding enabled and organised by Projekt DEAL. We acknowledge support for the publication costs by the Open Access Publication Fund of Bielefeld University.
Funding information
Funding for this research was provided by: Studienstiftung des deutschen Volkes (scholarship to Jona Voss).
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