Citation: Hongdao LI, Shengjian ZHANG, Hongmei DONG. Magnetic relaxation and luminescent behavior in nitronyl nitroxide-based annuluses of rare-earth ions[J]. Chinese Journal of Inorganic Chemistry, ;2024, 40(5): 972-978. doi: 10.11862/CJIC.20230411 shu

Magnetic relaxation and luminescent behavior in nitronyl nitroxide-based annuluses of rare-earth ions

Taiyuan Institute of Technology, Department of Chemistry and Chemical Engineering, Taiyuan 030008, China

Corresponding author: Hongdao LI, lihong.dao@163.com
Received Date: 30 October 2023
Revised Date: 24 January 2024

Figures(8)

Employing the reaction of chiral nitronyl nitroxide radical and rare-earth ions, two 2p-4f hetero-spin meso complexes [Ln(hfac)₃((R)-MePP-Ph-NIT)]₂, where Ln=Eu (1) and Dy (2), hfac=hexafluoroacetylacetone; (R)-MePP-Ph-NIT=2-(4-((R)-tert-butyl-2-methylpiperazine-1-carboxylate)phenyl)-4,4,5,5-tetramethylimidazoline-1-oxyl-3-oxide, have been assembled. In both complexes, two chiral radicals ligate to two Ln(Ⅲ) ions to produce a cyclic dinuclear structure. Complex 1 shows the characteristic fluorescence emission of the Eu(Ⅲ) ion. In complex 2, the frequency-dependent out-of-phase susceptibility signals connected with magnetic relaxation confirm single-molecule magnet (SMM) behavior.
- nitronyl nitroxide,
- single-molecule magnet,
- rare-earth ion,
- 2p-4f hetero-spin
1. [1]
  Sessoli R, Gatteschi D, Caneschi A, Novak M A. Magnetic bistability in a metal-ion cluster[J]. Nature, 1993,365:141-143. doi: 10.1038/365141a0
2. [2]
  Sorace L, Benelli C, Gatteschi D. Lanthanides in molecular magnetism: Old tools in a new field[J]. Chem. Soc. Rev., 2011,40:3092-3104. doi: 10.1039/c0cs00185f
3. [3]
  Ashebr T G, Li H, Ying X, Li X L, Zhao C, Liu S T, Tang J K. Emerging trends on designing high-performance dysprosium(Ⅲ) single-molecule magnets[J]. ACS Mater. Lett., 2022,4:307-319. doi: 10.1021/acsmaterialslett.1c00765
4. [4]
  Rinehart J D, Long J R. Exploiting single-ion anisotropy in the design of f-element single-molecule magnets[J]. Chem. Sci., 2011,2:2078-2085. doi: 10.1039/c1sc00513h
5. [5]
  Guo F S, Day B M, Chen Y C, Tong M L, Mansikkamäki A, Layfield R A. Magnetic hysteresis up to 80 Kelvin in a dysprosium metallocene single-molecule magnet[J]. Science, 2018,362:1400-1403. doi: 10.1126/science.aav0652
6. [6]
  Gould C A, McClain K R, Reta D, Kragskow J G C, Marchiori D A, Lachman E, Choi E S, Analytis J G, Britt R D, Chilton N F, Harvey B G, Long J R. Ultrahard magnetism from mixed-valence dilanthanide complexes with metal-metal bonding[J]. Science, 2022,375:198-202. doi: 10.1126/science.abl5470
7. [7]
  Demir S, Jeon I R, Long J R, Harris T D. Radical ligand-containing single-molecule magnets[J]. Coord. Chem. Rev., 2015,289:149-176.
8. [8]
  Sessoli R, Powell A K. Strategies towards single molecule magnets based on lanthanide ions[J]. Coord. Chem. Rev., 2009,253:2328-2341. doi: 10.1016/j.ccr.2008.12.014
9. [9]
  Li H D, Wu S G, Tong M L. Lanthanide-radical single-molecule magnets: Current status and future challenges[J]. Chem. Commun., 2023,59:6159-6170. doi: 10.1039/D2CC07042A
10. [10]
  Demir S, Gonzalez M I, Darago L E, Evans W J, Long J R. Giant coercivity and high magnetic blocking temperatures for N₂^3- radical-bridged dilanthanide complexes upon ligand dissociation[J]. Nat. Commun., 2017,82144. doi: 10.1038/s41467-017-01553-w
11. [11]
  Li H D, Jing P, Lu J, Xie J, Zhai L J, Xi L. Dipyridyl-decorated nitronyl nitroxide-Dy^Ⅲ single-molecule magnet with a record energy barrier of 146 K[J]. Inorg. Chem., 2021,60:7622-7626. doi: 10.1021/acs.inorgchem.1c00809
12. [12]
  Jia J H, Li Q W, Chen Y C, Liu J L, Tong M L. Luminescent single-molecule magnets based on lanthanides: Design strategies, recent advances and magneto-luminescent studies[J]. Coord. Chem. Rev., 2019,378:365-381. doi: 10.1016/j.ccr.2017.11.012
13. [13]
  Ziessel R, Ulrich G, Lawson R C, Echegoyen L. Oligopyridine bis (nitronyl nitroxides): Synthesis, structures, electrochemical, magnetic and electronic properties[J]. J. Mater. Chem., 1999,9:1435-1448. doi: 10.1039/a810044f
14. [14]
  Kahn O. Molecular magnetism. Weinheim: VCH, 1993.
15. [15]
  SAINT Version 7.68A. Bruker AXS, Inc., Madison, WI, 2009.
16. [16]
  Sheldrick G M. SADABS, Version 2008/1. Bruker AXS, Inc., Madison, WI, 2008.
17. [17]
  Sheldrick G M. SHELXS-2014, Program for structure solution. University of Göttingen, Germany, 2014.
18. [18]
  Sheldrick G M. SHELXL-2014, Program for structure refinement. University of Göttingen, Germany, 2014.
19. [19]
  Kahn M L, Sutter J P, Guionneau S G P, Ouahab L, Kahn O, Chasseau D. Systematic investigation of the nature of the coupling between an Ln(Ⅲ) Ion (Ln=Ce(Ⅲ) to Dy(Ⅲ)) and its aminoxyl radical ligands: Structural and magnetic characteristics of a series of {Ln(organic radical)₂} compounds and the related {Ln(Nitrone)₂} derivatives[J]. J. Am. Chem. Soc., 2000,122:3413-3421. doi: 10.1021/ja994175o
20. [20]
  Wang Y J, Wu D F, Gou J, Duan Y Y, Li L, Chen H H, Gao H L, Cui J Z. Modulation of the properties of dinuclear lanthanide complexes through utilizing different β-diketonate co-ligands: Near-infrared luminescence and magnetization dynamics[J]. Dalton Trans., 2020,49:2850-2861. doi: 10.1039/C9DT04093E
21. [21]
  Xi L, Li H D, Sun J, Ma Y, Tang J K, Li L C. Designing multicoordinating nitronyl nitroxide radical toward multinuclear lanthanide aggregates[J]. Inorg. Chem., 2020,59:443-451. doi: 10.1021/acs.inorgchem.9b02739
22. [22]
  Casanova D, Llunell M, Alemany P, Alvarez S. The rich stereochemistry of eight vertex polyhedra: A continuous shape measures study[J]. Chem.-Eur. J., 2005,11:1479-1494. doi: 10.1002/chem.200400799
23. [23]
  Llunell M, Casanova D, Cirera J, Alemany P, Alvarez S. SHAPE 2.1. University of Barcelona, Spain, 2013.
24. [24]
  Liu Y, Anh Ho L T, Huang G Z, Chen Y C, Ungur L, Liu J L, Tong M L. Magnetization dynamics on isotope-isomorphic holmium single-molecule magnets[J]. Angew. Chem. Int. Ed., 2021,60:27282-27287. doi: 10.1002/anie.202112764
25. [25]
  Yang Q Q, Ungur L, Chibotarud L F, Tang J K. Toroidal versus centripetal arrangement of the magnetic moment in a Dy₄ tetrahedron[J]. Chem. Commun., 2022,58:1784-1787. doi: 10.1039/D1CC06265D
26. [26]
  Dolinar B S, Coca S G, Alexandropoulos D I, Dunbar K R. An air stable radical-bridged dysprosium single molecule magnet and its neutral counterpart: Redox switching of magnetic relaxation dynamics[J]. Chem. Commun., 2017,53:2283-2286. doi: 10.1039/C6CC09824J
27. [27]
  Wang J, Miao H, Xiao Z X, Zhou Y, Deng L D, Zhang Y Q, Wang X Y. Syntheses, structures and magnetic properties of the lanthanide complexes of the pyrimidyl-substituted nitronyl nitroxide radical[J]. Dalton Trans., 2017,46:10452-10461. doi: 10.1039/C7DT01037K
28. [28]
  Liu C M, Sun R, Hao X, Wang B W. Chiral co-crystals of (S)- or (R)-1,1'-binaphthalene-2,2'-diol and Zn₂Dy₂ tetranuclear complexes behaving as single-molecule magnets[J]. Cryst. Growth Des., 2021,21:4346-4353. doi: 10.1021/acs.cgd.1c00246
29. [29]
  Shi J Y, Wu M Z, Chen P Y, Li T, Tian L, Zhang Y Q. Terbium triangle bridged by a triazole nitronyl nitroxide radical with single-molecule-magnet behavior[J]. Inorg. Chem., 2019,58:14285-14288. doi: 10.1021/acs.inorgchem.9b01647
30. [30]
  JI W J, XIA C C, ZHANG X Y, WANG X Y. Anionic modification of the Cu-Tb single-molecule magnets based on the compartmental Schiff-base ligand[J]. Chinese J. Inorg. Chem., 2022,38:1199-1208.
31. [31]
  Chilton N F, Collison D, McInnes E J L, Winpenny R E P, Soncini A. An electrostatic model for the determination of magnetic anisotropy in dysprosium complexes[J]. Nat. Commun., 2013,42551. doi: 10.1038/ncomms3551
32. [32]
  Miao H, Li H Q, Shen F X, Wei H Y, Wang B L, Wang X Y. A family of lanthanide complexes with a bis-tridentate nitronyl nitroxide radical: Syntheses, structures and magnetic properties[J]. Dalton Trans., 2019,48:10337-10345. doi: 10.1039/C9DT01397K
33. [33]
  Xiao Z X, Miao H, Shao D, Wei H Y, Zhang Y Q, Wang X Y. Single-molecule magnet behaviour in a dysprosium-triradical complex[J]. Chem. Commun., 2018,54:9726-9729. doi: 10.1039/C8CC04739A
34. [34]
  Liu J L, Chen Y C, Zheng Y Z, Lin W Q, Ungur L, Wernsdorfer W, Chibotaru L F, Tong M L. Switching the anisotropy barrier of a single-ion magnet by symmetry change from quasi-D_5h to quasi-O_h[J]. Chem. Sci., 2013,4:3310-3316. doi: 10.1039/c3sc50843a
1. [1]
  Haodong Wang , Xiaoxu Lai , Chi Chen , Pei Shi , Houzhao Wan , Hao Wang , Xingguang Chen , Dan Sun . Novel 2D bifunctional layered rare-earth hydroxides@GO catalyst as a functional interlayer for improved liquid-solid conversion of polysulfides in lithium-sulfur batteries. Chinese Chemical Letters, 2024, 35(5): 108473-. doi: 10.1016/j.cclet.2023.108473
2. [2]
  Shuyan ZHAO . Field-induced Co^Ⅱ single-ion magnet with pentagonal bipyramidal configuration. Chinese Journal of Inorganic Chemistry, 2024, 40(8): 1583-1591. doi: 10.11862/CJIC.20240231
3. [3]
  Tsegaye Tadesse Tsega , Jiantao Zai , Chin Wei Lai , Xin-Hao Li , Xuefeng Qian . Earth-abundant CuFeS2 nanocrystals@graphite felt electrode for high performance aqueous polysulfide/iodide redox flow batteries. Chinese Journal of Structural Chemistry, 2024, 43(1): 100192-100192. doi: 10.1016/j.cjsc.2023.100192
4. [4]
  Binyang Qin , Mengqi Wang , Shimei Wu , Yining Li , Chilin Liu , Yufei Zhang , Haosen Fan . Carbon dots confined nanosheets assembled NiCo₂S₄@CDs cross-stacked architecture for enhanced sodium ion storage. Chinese Chemical Letters, 2024, 35(7): 108921-. doi: 10.1016/j.cclet.2023.108921
5. [5]
  Mianying Huang , Zhiguang Xu , Xiaoming Lin . Mechanistic analysis of Co2VO4/X (X = Ni, C) heterostructures as anode materials of lithium-ion batteries. Chinese Journal of Structural Chemistry, 2024, 43(7): 100309-100309. doi: 10.1016/j.cjsc.2023.100309
6. [6]
  Shengyu Zhao , Xuan Yu , Yufeng Zhao . A water-stable high-voltage P3-type cathode for sodium-ion batteries. Chinese Chemical Letters, 2024, 35(9): 109933-. doi: 10.1016/j.cclet.2024.109933
7. [7]
  Lu LIU , Huijie WANG , Haitong WANG , Ying LI . Crystal structure of a two-dimensional Cd(Ⅱ) complex and its fluorescence recognition of p-nitrophenol, tetracycline, 2, 6-dichloro-4-nitroaniline. Chinese Journal of Inorganic Chemistry, 2024, 40(6): 1180-1188. doi: 10.11862/CJIC.20230489
8. [8]
  Muhammad Humayun , Mohamed Bououdina , Abbas Khan , Sajjad Ali , Chundong Wang . Designing single atom catalysts for exceptional electrochemical CO2 reduction. Chinese Journal of Structural Chemistry, 2024, 43(1): 100193-100193. doi: 10.1016/j.cjsc.2023.100193
9. [9]
  Yinglian LI , Chengcheng ZHANG , Xinyu ZHANG , Xinyi WANG . Spin crossover in [Co(pytpy)₂]²⁺ complexes modified by organosulfonate anions. Chinese Journal of Inorganic Chemistry, 2024, 40(6): 1162-1172. doi: 10.11862/CJIC.20240087
10. [10]
  Jin Long , Xingqun Zheng , Bin Wang , Chenzhong Wu , Qingmei Wang , Lishan Peng . Improving the electrocatalytic performances of Pt-based catalysts for oxygen reduction reaction via strong interactions with single-CoN₄-rich carbon support. Chinese Chemical Letters, 2024, 35(5): 109354-. doi: 10.1016/j.cclet.2023.109354
11. [11]
  Shiqi Peng , Yongfang Rao , Tan Li , Yufei Zhang , Jun-ji Cao , Shuncheng Lee , Yu Huang . Regulating the electronic structure of Ir single atoms by ZrO₂ nanoparticles for enhanced catalytic oxidation of formaldehyde at room temperature. Chinese Chemical Letters, 2024, 35(7): 109219-. doi: 10.1016/j.cclet.2023.109219
12. [12]
  Qian-Qian Tang , Li-Fang Feng , Zhi-Peng Li , Shi-Hao Wu , Long-Shuai Zhang , Qing Sun , Mei-Feng Wu , Jian-Ping Zou . Single-atom sites regulation by the second-shell doping for efficient electrochemical CO₂ reduction. Chinese Chemical Letters, 2024, 35(9): 109454-. doi: 10.1016/j.cclet.2023.109454
13. [13]
  Jing Wang , Zhongliao Wang , Jinfeng Zhang , Kai Dai . Single-layer crystalline triazine-based organic framework photocatalysts with different linking groups for H2O2 production. Chinese Journal of Structural Chemistry, 2023, 42(12): 100202-100202. doi: 10.1016/j.cjsc.2023.100202
14. [14]
  Kun Zhang , Ni Dan , Dan-Dan Ren , Ruo-Yu Zhang , Xiaoyan Lu , Ya-Pan Wu , Li-Lei Zhang , Hong-Ru Fu , Dong-Sheng Li . A small D-A molecule with highly heat-resisting room temperature phosphorescence for white emission and anti-counterfeiting. Chinese Journal of Structural Chemistry, 2024, 43(3): 100244-100244. doi: 10.1016/j.cjsc.2024.100244
15. [15]
  Jin Wang , Xiaoyan Pan , Junyu Zhang , Qingqing Zhang , Yanchen Li , Weiwei Guo , Jie Zhang . Active molecule-based theranostic agents for tumor vasculature normalization and antitumor efficacy. Chinese Chemical Letters, 2024, 35(8): 109187-. doi: 10.1016/j.cclet.2023.109187
16. [16]
  Aolei Tan , Xiaoxiao Ma . Exploring the functional roles of small-molecule metabolites in disease research: Recent advancements in metabolomics. Chinese Chemical Letters, 2024, 35(8): 109276-. doi: 10.1016/j.cclet.2023.109276
17. [17]
  Kunyao Peng , Xianbin Wang , Xingbin Yan . Converting LiNO₃ additive to single nitrogenous component Li₂N₂O₂ SEI layer on Li metal anode in carbonate-based electrolyte. Chinese Chemical Letters, 2024, 35(9): 109274-. doi: 10.1016/j.cclet.2023.109274
18. [18]
  Xingyan Liu , Chaogang Jia , Guangmei Jiang , Chenghua Zhang , Mingzuo Chen , Xiaofei Zhao , Xiaocheng Zhang , Min Fu , Siqi Li , Jie Wu , Yiming Jia , Youzhou He . Single-atom Pd anchored in the porphyrin-center of ultrathin 2D-MOFs as the active center to enhance photocatalytic hydrogen-evolution and NO-removal. Chinese Chemical Letters, 2024, 35(9): 109455-. doi: 10.1016/j.cclet.2023.109455
19. [19]
  Xinlong WANG , Zhenguo CHENG , Guo WANG , Xiaokuen ZHANG , Yong XIANG , Xinquan WANG . Enhancement of the fragile interface of high voltage LiCoO₂ by surface gradient permeation of trace amounts of Mg/F. Chinese Journal of Inorganic Chemistry, 2024, 40(3): 571-580. doi: 10.11862/CJIC.20230259
20. [20]
  Yu-Yu Tan , Lin-Heng He , Wei-Min He . Copper-mediated assembly of SO₂F group via radical fluorine-atom transfer strategy. Chinese Chemical Letters, 2024, 35(9): 109986-. doi: 10.1016/j.cclet.2024.109986

Get Citation

PDF

XML

Metrics

PDF Downloads(0)
Abstract views(62)
HTML views(11)

通讯作者: 陈斌, bchen63@163.com

1.
沈阳化工大学材料科学与工程学院沈阳 110142