Citation: BI Yan-Ting, YAO Jun, SHEN Zhong-Hui, ZHANG Hong-Xing, PAN Qing-Jiang. Interaction Behavior Between Hexa-dentate Polypyrrolic Macrocycles and Actinyl Species: Bonding, Thermodynamic and Spectroscopic Properties[J]. Chinese Journal of Inorganic Chemistry, ;2018, 34(6): 1071-1078. doi: 10.11862/CJIC.2018.136 shu

Interaction Behavior Between Hexa-dentate Polypyrrolic Macrocycles and Actinyl Species: Bonding, Thermodynamic and Spectroscopic Properties

1.
Science and Technology Division, School of Chemistry and Materials Science, Heilongjiang University, Harbin 150080, China
2.
Institute of Theoretical Chemistry, Jilin University, Changchun 130023, China

Corresponding author: SHEN Zhong-Hui, shenzhonghui@hlju.edu.cn PAN Qing-Jiang, panqjitc@163.com
Received Date: 7 January 2018
Revised Date: 20 March 2018

Figures(4)

A relativistic density functional theory (DFT) was used to systematically examine a series of uranyl and transuranyl complexes of N-donor macrocyclic ligands, [(AnO₂)(Ln)]^2-(labeled as nAn; n=1~3; An=U, Np and Pu). Further comparison was made with[(UO₂)(L⁰)]^2-(A) that was experimentally synthesized. Cavities of L¹ and L² macrocycles are found to match well with actinyl ions, but the one of L³ is a lot larger. Consequently, the L³ complexes have to adopt distorted geometry to energetically stabilize systems. Infrared vibrational spectra presented that the An=O stretching frequencies decrease in going from U, Np to Pu. This agrees with the trend of optimized bond lengths of An=O and bond orders. Topological analyses of quantum theory of atoms in molecule (QTAIM) indicate that the An-N bonds have largely ionic character. Depending on different actinyl source, free energies reacting with various macrocyclic ligands were calculated around 146.4 kJ·mol^-1, comparable to the calculated values of A. Time-dependent DFT calculations on four uranyl complexes well reproduced absorption spectra of experimentally reported analogue. The absorption bands in the near-IR and visible region have large contribution from ligand-to-metal charge transfer (LMCT), which is responsible for changes of solution color in the process of macrocyclic ligand sensing uranyl species.
- polypyrrollic uranyl/transuranyl complexes,
- QTAIM analysis,
- thermodynamic reaction,
- electronic spectroscopy,
- relativistic DFT
1. [1]
  Hashke J M, Stakebake J L. The Chemistry of the Actinide and Transactinide Elements. Dordrecht:Springer, 2006:3199-3272
2. [2]
  Choppin G R. J. Radioanal. Nucl. Chem., 2007, 273(3):695-703 doi: 10.1007/s10967-007-0933-3
3. [3]
  Rambo B M, Sessler J L. Chem.-Eur. J., 2011, 17(18):4946-4959 doi: 10.1002/chem.v17.18
4. [4]
  GU Jia-Fang, XU Ke, CHEN Wen-Kai. Chinese J. Inorg. Chem., 2017, 33(9):1579-1586 doi: 10.11862/CJIC.2017.179
5. [5]
  Wang D, van Gunsteren W F, Chai Z. Chem. Soc. Rev., 2012, 41(17):5836-5865 doi: 10.1039/c2cs15354h
6. [6]
  Wang D, Su J, Wu J, et al. Radiochim. Acta, 2014, 102(1/2):13-25
7. [7]
  Wu Q Y, Wang C Z, Lan J H, et al. Inorg. Chem., 2014, 53(18):9607-9614 doi: 10.1021/ic501006p
8. [8]
  Wu H, Wu Q Y, Wang C Z, et al. Dalton Trans., 2015, 44(38):16737-16745 doi: 10.1039/C5DT02528A
9. [9]
  Lan J H, Shi W Q, Yuan L Y. Coord. Chem. Rev., 2012, 256(13/14):1406-1417
10. [10]
  Lan J H, Shi W Q, Yuan L Y, et al. Inorg. Chem., 2011, 50(19):9230-9237 doi: 10.1021/ic200078j
11. [11]
  Hu H S, Wei F, Wang X, et al. J. Am. Chem. Soc., 2014, 136(4):1427-1437 doi: 10.1021/ja409527u
12. [12]
  Hu S X, Jian J, Su J, et al. Chem. Sci., 2017, 8(5):4035-4043 doi: 10.1039/C7SC00710H
13. [13]
  Chi C, Wang J Q, Qu H, et al. Angew. Chem. Int. Ed., 2017, 56(24):6932-6936 doi: 10.1002/anie.201703525
14. [14]
  Sessler J L, Seidel D, Vivian A E, et al. Angew. Chem. Int. Ed., 2001, 40(3):591-594 doi: 10.1002/1521-3773(20010202)40:3<>1.0.CO;2-A
15. [15]
  Sessler J L, Gorden A E V, Seidel D, et al. Inorg. Chim. Acta, 2002, 341:54-70 doi: 10.1016/S0020-1693(02)01202-1
16. [16]
  Sessler J L, Melfi P J, Seidel D, et al. Tetrahedron, 2004, 60(49):11089-11097 doi: 10.1016/j.tet.2004.08.055
17. [17]
  Melfi P J, Kim S K, Lee J T, et al. Inorg. Chem., 2007, 46(13):5143-5145 doi: 10.1021/ic700781t
18. [18]
  Ho I T, Zhang Z, Ishida M, et al. J. Am. Chem. Soc., 2014, 136(11):4281-4286 doi: 10.1021/ja412520g
19. [19]
  Zhang Z, Dong S K, Lin C Y, et al. J. Am. Chem. Soc., 2015, 137(24):7769-7774 doi: 10.1021/jacs.5b03131
20. [20]
  Sessler J L, Melfi P J, Lynch V M. J. Porphyrins Phthaloc-yanines, 2007, 11(4):287-293 doi: 10.1142/S1088424607000345
21. [21]
  Cafeo G, Kohnke F H, La Torre G L, et al. Angew. Chem. Int. Ed., 2000, 39(8):1496-1498 doi: 10.1002/(SICI)1521-3773(20000417)39:8<1496::AID-ANIE1496>3.0.CO;2-I
22. [22]
  Jana A, Ishida M, Cho K, et al. Chem. Commun., 2013, 49(79):8937-8939 doi: 10.1039/c3cc44934c
23. [23]
  Fukuzumi S, Ohkubo K, D'Souza F, et al. Chem. Commun., 2012, 48(79):9801-9815 doi: 10.1039/c2cc32848h
24. [24]
  Laikov D N. J. Comput. Chem., 2007, 28(3):698-702 doi: 10.1002/(ISSN)1096-987X
25. [25]
  Klamt A, Jonas V, Burger T, et al. J. Phys. Chem. A, 1998, 102(26):5074-5085 doi: 10.1021/jp980017s
26. [26]
  Zhao H B, Zheng M, Schreckenbach G, et al. Inorg. Chem., 2017, 56(5):2763-2776 doi: 10.1021/acs.inorgchem.6b02927
27. [27]
  CHEN Fang-Yuan, QU Ning, WU Qun-Yan, et al. Acta Chim. Sinica, 2017, 75(5):457-463
28. [28]
  ZHAO Si-Wei, ZHONG Yu-Xi, GUO Yuan -Ru, et al. Acta Chim. Sinica, 2016, 74(8):683-688
29. [29]
  Frisch M J, Trucks G W, Schlegel H B, et al. Gaussian09, Gaussian, Inc., Wallingford CT, 2009.
30. [30]
  Bader R F W. J. Phys. Chem. A, 1998, 102:7314-7323 doi: 10.1021/jp981794v
31. [31]
  Lu T, Chen F. J. Comput. Chem., 2012, 33(5):580-592 doi: 10.1002/jcc.v33.5
32. [32]
  Natrajan L, Burdet F, Pecaut J, et al. J. Am. Chem. Soc., 2006, 128(22):7152-7153 doi: 10.1021/ja0609809
33. [33]
  Perdew J P, Burke K, Ernzerhof M. Phys. Rev. Lett., 1996, 77(18):3865-3868 doi: 10.1103/PhysRevLett.77.3865
34. [34]
  Hlina J A, Pankhurst J R, Kaltsoyannis N, et al. J. Am. Chem. Soc., 2016, 138(10):3333-3345 doi: 10.1021/jacs.5b10698
35. [35]
  Mountain A R, Kaltsoyannis N. Dalton Trans., 2013, 42(37):13477-13486 doi: 10.1039/c3dt51337h
36. [36]
  GU Jia-Fang, MAN Mei-Ling, LU Chun-Hai, et al. Chinese J. Inorg. Chem., 2012, 28(7):1324-1332
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沈阳化工大学材料科学与工程学院沈阳 110142