Citation: Wen-Jie Xu, Qian-Cheng Luo, Yang Fang, Chen-Jie Yuan, Jin-Tao Lu, Yuan-Qi Zhai, Yu Wang, Yan-Zhen Zheng. Pseudo-mono-coordinate dysprosium(Ⅲ)-alkoxide complexes exhibit enhanced magnetic axiality and blocking temperature[J]. Chinese Chemical Letters, ;2026, 37(7): 110975. doi: 10.1016/j.cclet.2025.110975 shu

Pseudo-mono-coordinate dysprosium(Ⅲ)-alkoxide complexes exhibit enhanced magnetic axiality and blocking temperature

Wen-Jie Xu ^{a, 1} ,
Qian-Cheng Luo ^{a, 1} ,
Yang Fang ^a ,
Chen-Jie Yuan ^b ,
Jin-Tao Lu ^{c, d} ,
Yuan-Qi Zhai ^{a, b, *,} ,
Yu Wang ^{b, *,} ,
Yan-Zhen Zheng ^{a, b, *,}

a.
Frontier Institute of Science and Technology (FIST), State Key Laboratory of Electrical Insulation and Power Equipment, Xi’an Key Laboratory of Electronic Devices and Material Chemistry, School of Chemistry, Xi’an Jiaotong University, Xi’an 710054, China
b.
MOE Key Laboratory for Non-Equilibrium Synthesis and Modulation of Condensed Matter, School of Physics, Xi’an Jiaotong University, Xi’an 710049, China
c.
Key Laboratory of the Ministry of Education and International Center for Dielectric Research, School of Electronic Science and Engineering, Xi’an Jiaotong University, Xi’an 710049, China
d.
Xi’an SIMOLDE Science and Technology Co., Ltd., Xi’an 710049, China

zhaiyuanqi@xjtu.edu.cn

yuwang@mail.xjtu.edu.cn

zheng.yanzhen@xjtu.edu.cn

Received Date: 7 December 2024
Revised Date: 7 February 2025
Accepted Date: 18 February 2025
Available Online: 18 February 2025

Figures(5)

Synthesis of pseudo-mono-coordinate dysprosium(Ⅲ) single-molecule magnets (SMMs) with strong axiality is challenging. Here, by using very basic alkoxides as axial ligands and ether type neutral ligands as ancillary parts two targeted complexes, [Dy(O^tBu)(15-C-5)(THF)₂][I₃]₂ 1 and [Dy(1-AdO)(15-C-5)(THF)₂][I₃]₂ 2 were successfully isolated. Structurally they possess very short Dy–O_alkoxide bonds (2.016(4) Å for 1 and 2.028(3) Å for 2) and very long Dy–O_ether bonds (ranging from 2.427(4) Å to 2.523(4) Å for 1 and 2.416(3) Å to 2.509(3) Å for 2). As such, they are very similar to the diatomic model complex [DyO]⁺and can be magnetically perceived as pseudo-mono-coordinate Dy(Ⅲ) complexes. Both 1 and 2 exhibit high effective magnetic anisotropy barriers (1054(6) K for 1 and 1028(9) K for 2). Consequently, both 1 and 2 demonstrate high opening hysteresis temperatures, namely 14 K for 1 and 10 K for 2. This study provides a new insight into of pseudo-mono-coordinate mode and further emphasizes the excellent potential of this model for constructing high-performance SMMs.
- Single-molecule magnets,
- Pseudo-mono-coordinate,
- Alkoxide,
- Dysprosium,
- Axiality
1. [1]
  R. Sessoli, D. Gatteschi, A. Caneschi, M.A. Novak, Nature 365 (1993) 141–143. doi: 10.1038/365141a0
2. [2]
  F.D. Natterer, W. Paul K. Yang, et al., Nature 543 (2017) 226–228. doi: 10.1038/nature21371
3. [3]
  R. Sessoli, Nature 543 (2017) 189–190. doi: 10.1038/543189a
4. [4]
  L. Bogani, W. Wernsdorfer, Nat. Mater. 7 (2008) 179–186. doi: 10.1038/nmat2133
5. [5]
  S. Sanvito, Chem. Soc. Rev. 40 (2011) 3336–3355. doi: 10.1039/c1cs15047b
6. [6]
  M.N. Leuenberger, D. Loss, Nature 410 (2001) 789–793. doi: 10.1038/35071024
7. [7]
  A. Gaita-Ariño, F. Luis, S. Hill, E. Coronado, Nat. Chem. 11 (2019) 301–309. doi: 10.1038/s41557-019-0232-y
8. [8]
  S. Thiele, F. Balestro, R. Ballou, et al., Science 344 (2014) 1135–1138. doi: 10.1126/science.1249802
9. [9]
  J.L. Liu, Y.C. Chen, M.L. Tong, Chem. Soc. Rev. 47 (2018) 2431. doi: 10.1039/c7cs00266a
10. [10]
  N.F. Chilton, Annu. Rev. Mater. Res. 52 (2022) 79–101. doi: 10.1146/annurev-matsci-081420-042553
11. [11]
  V.S. Parmar, D.P. Mills, R.E.P. Winpenny, Chem. Eur. J. 27 (2021) 7625–7645. doi: 10.1002/chem.202100085
12. [12]
  C.A.P. Goodwin, F. Ortu, D. Reta, N.F. Chilton, D.P. Mills, Nature 548 (2017) 439–442. doi: 10.1038/nature23447
13. [13]
  F.S. Guo, B.M. Day, Y.C. Chen, et al., Angew. Chem. Int. Ed. 56 (2017) 11445–11449. doi: 10.1002/anie.201705426
14. [14]
  K.R. McClain, C.A. Gould, K. Chakarawet, et al., Chem. Sci. 9 (2018) 8492–8503. doi: 10.1039/C8SC03907K
15. [15]
  P.E. Evans, D. Reta, G.F.S. Whitehead, N.F. Chilton, D.P. Mills, J. Am. Chem. Soc. 141 (2019) 19935–19940. doi: 10.1021/jacs.9b11515
16. [16]
  C.A. Gould, K.R. McClain, D. Reta, et al., Science 375 (2022) 198–202. doi: 10.1126/science.abl5470
17. [17]
  J.C. Vanjak, B.O. Wilkins, V. Vieru, et al., J. Am. Chem. Soc. 144 (2022) 17743–17747. doi: 10.1021/jacs.2c06698
18. [18]
  A.H. Vincent, Y.L. Whyatt, N.F. Chilton, J.R. Long, J. Am. Chem. Soc. 145 (2023) 1572–1579. doi: 10.1021/jacs.2c08568
19. [19]
  G.K. Gransbury, S.C. Corner, J.G.C. Kragskow, et al., J. Am. Chem. Soc. 145 (2023) 22814–22825. doi: 10.1021/jacs.3c08841
20. [20]
  Y.D. Wang, Q.C. Luo, Y.Z. Zheng, Angew. Chem. Int. Ed. 63 (2024) e202407016. doi: 10.1002/anie.202407016
21. [21]
  F.S. Guo, B.M. Day, Y.C. Chen, M.L. Tong, Science 362 (2018) 1400–1403. doi: 10.1126/science.aav0652
22. [22]
  J. Liu, Y.C. Chen, J.L. Liu, et al., J. Am. Chem. Soc. 138 (2016) 5441–5450. doi: 10.1021/jacs.6b02638
23. [23]
  Y.S. Ding, N.F. Chilton, R.E. Winpenny, Y.Z. Zheng, Angew. Chem. Int. Ed. 55 (2016) 16071–16074. doi: 10.1002/anie.201609685
24. [24]
  K.X. Yu, J.G.C. Kragskow, Y.S. Ding, et al., Chem 6 (2020) 1777–1793. doi: 10.1016/j.chempr.2020.04.024
25. [25]
  X.L. Ding, Q.C. Luo, Y.Q. Zhai, et al., Chin. J. Chem. 40 (2022) 563–570. doi: 10.1002/cjoc.202100722
26. [26]
  Y. Ma, Y.Q. Zhai, Q.C. Luo, Y.S. Ding, Y.Z. Zheng, Angew. Chem. Int. Ed. 61 (2022) e202206022. doi: 10.1002/anie.202206022
27. [27]
  Q.C. Luo, Y.Z. Zheng, Trends Chem. 5 (2023) 869–872. doi: 10.1016/j.trechm.2023.10.004
28. [28]
  X.L. Ding, Y.Q. Zhai, T. Han, et al., Chem. Eur. J. 27 (2021) 2623–2627. doi: 10.1002/chem.202003931
29. [29]
  Z.H. Li, Y.Q. Zhai, W.P. Chen, Y.S. Ding, Y.Z. Zheng, Chem. Eur. J. 25 (2019) 16219–16224. doi: 10.1002/chem.201904325
30. [30]
  Z.H. Zhu, C. Zhao, T.T. Feng, et al., J. Am. Chem. Soc. 143 (2021) 10077–10082. doi: 10.1021/jacs.1c05279
31. [31]
  A.B. Canaj, S. Dey, C. Wilson, et al., Chem. Commun. 56 (2020) 12037–12040. doi: 10.1039/d0cc04559d
32. [32]
  Z.H. Zhu, C. Zhao, Q. Zhou, et al., CCS Chem. 4 (2022) 3762–3771. doi: 10.31635/ccschem.022.202101604
33. [33]
  S.T. Liu, Y. Gil, C. Zhao, et al., Inorg. Chem. Front. 9 (2022) 4982–4989. doi: 10.1039/d2qi01565j
34. [34]
  S.K. Gupta, S. Dey, T. Rajeshkumar, G. Rajaraman, R. Murugavel, Chem. Eur. J. 28 (2022) e202103585. doi: 10.1002/chem.202103585
35. [35]
  X. Zhong, D.Y. Li, C. Cao, et al., Inorg. Chem. 63 (2024) 21909–21918. doi: 10.1021/acs.inorgchem.4c03012
36. [36]
  W.J. Xu, Q.C. Luo, Z.H. Li, Y.Q. Zhai, Y.Z. Zheng, Adv. Sci. 11 (2024) 2308548. doi: 10.1002/advs.202308548
37. [37]
  L. Ungur, L.F. Chibotaru, Phys. Chem. Chem. Phys. 13 (2011) 20086–20090. doi: 10.1039/c1cp22689d
38. [38]
  L. Norel, L.E. Darago, B.L. Guennic, et al., Angew. Chem. Int. Ed. 57 (2018) 1933–1938. doi: 10.1002/anie.201712139
39. [39]
  A.B. Canaj, M.K. Singh, E.R. Marti, et al., Chem. Commun. 55 (2019) 5950–5953. doi: 10.1039/c9cc00965e
40. [40]
  B.K. Ling, Y.Q. Zhai, J. Han, T. Han, Y.Z. Zheng, Dalton Trans. 49 (2020) 6969–6973. doi: 10.1039/d0dt01146k
41. [41]
  R. Sun, C.Y. Li, Z.N. Huang, et al., CCS Chem. 7 (2025) 2054–2064. doi: 10.31635/ccschem.024.202404701
42. [42]
  B. Zhang, Z.J. Cheng, Y.Y. Wu, et al., Chem. Sci. 13 (2022) 13231–13240. doi: 10.1039/d2sc03182e
43. [43]
  Y.S. Ding, W.J.A. Blackmore, Y.Q. Zhai, et al., Inorg. Chem. 61 (2022) 227–235. doi: 10.1021/acs.inorgchem.1c02779
44. [44]
  Y.S. Ding, T. Han, Y.Q. Zhai, et al., Chem. Eur. J. 26 (2020) 5893–5902. doi: 10.1002/chem.202000646
45. [45]
  Y.S. Ding, K.X. Yu, D. Reta, et al., Nat. Commun. 9 (2018) 3134. doi: 10.1038/s41467-018-05587-6
46. [46]
  M. Nespolo, A.H. Benahsene, J. Appl. Cryst. 54 (2021) 1594–1599. doi: 10.1107/s1600576721009109
47. [47]
  A. Matsumoto, S. Takeda, S. Harada, K. Soai, Tetrahedron 27 (2016) 943–946. doi: 10.1016/j.tetasy.2016.07.013
48. [48]
  Q.C. Luo, X.L. Ding, W.J. Xu, Y.Q. Zhai, Y.Z. Zheng, Chin. Chem. Lett. 36 (2025) 110304. doi: 10.1016/j.cclet.2024.110304
49. [49]
  W. Yang, G. Velkos, F.P. Liu, et al., Adv. Sci. 6 (2019) 1901352. doi: 10.1002/advs.201901352
50. [50]
  F. Neese, Comput. Mol. Sci. 12 (2022) e1606. doi: 10.1002/wcms.1606
51. [51]
  D. Aravena, J. Phys. Chem. Lett. 9 (2018) 5327–5333. doi: 10.1021/acs.jpclett.8b02359
52. [52]
  B. Yin, C.C. Li, Phys. Chem. Chem. Phys. 22 (2020) 9923–9933. doi: 10.1039/d0cp00933d
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