Abstract
Reactions of ortho-, para- and substituted meta-xylenyl bridged bis(tacn) ligands with two or three molar equivalents of Zn(NO3)2·6H2O at pH 5.0 in the presence of NaClO4 or NH4PF6 resulted in the formation of a range of crystalline zinc complexes. In the presence of perchlorate counter ions the Lpx and Lphx ligands gave rise to dinuclear Zn2+ coordination complexes [Zn2Cl2(Lpx)(H2O)2](ClO4)2(H2O) and [Zn2Cl2(Lphx)(H2O)2](ClO4)2(H2O)2 respectively, which formed infinite 1D polymeric chains. In contrast, in the presence of the hexafluorophosphate counter ion, the Lnix ligand formed a unique tetranuclear Zn2+ complex, [Zn2Cl2(Lnix)(H2O)3](Cl)(PF6)2(H2O)4, the Lcax ligand formed an octanuclear complex [Zn8Cl4(Lcax)4(H2O)10](PF6)6.7(NO3)1.3(H2O)3.3, whilst the Lox ligand formed a mononuclear sandwich structure, [Zn(Lox)](PF6)2(H2O). The protonated metal-free Lpx ligand crystallised as [H4(Lpx)](NO3)2(PF6)(H2O)2 with the stacked ligand cations forming a hydrogen-bonded network. These structural attributes provide an explanation for the significant differences in binding behaviour of recombinant N-terminally tagged proteins with the corresponding Zn2+-azamacrocyclic complexes, compared to the analogous Cu2+- or Ni2+-azamacrocyclic complexes, when immobilised onto support materials and used as immobilised metal affinity chromatographic (IMAC) adsorbents.
| Original language | English |
|---|---|
| Pages (from-to) | 187-197 |
| Number of pages | 11 |
| Journal | Polyhedron |
| Volume | 144 |
| DOIs | |
| Publication status | Published - 1 Apr 2018 |
Keywords
- Bis(tacn) ligands
- Crystal structures
- IMAC separations
- Xylenyl linkers
- Zinc(II) aza-macrocyclic complexes
Cite this
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Impact of the substitution pattern of xylyl-bridged 1,4-bis(1,4,7-triazacyclononane) ligands on the crystal structures of their zinc(II) complexes and their ability to bind to N-terminally tagged proteins. / Coghlan, Campbell J.; Campi, Eva M.; Batten, Stuart R.; Jackson, W. Roy; Hearn, Milton T.W.
In: Polyhedron, Vol. 144, 01.04.2018, p. 187-197.Research output: Contribution to journal › Article › Research › peer-review
TY - JOUR
T1 - Impact of the substitution pattern of xylyl-bridged 1,4-bis(1,4,7-triazacyclononane) ligands on the crystal structures of their zinc(II) complexes and their ability to bind to N-terminally tagged proteins
AU - Coghlan, Campbell J.
AU - Campi, Eva M.
AU - Batten, Stuart R.
AU - Jackson, W. Roy
AU - Hearn, Milton T.W.
PY - 2018/4/1
Y1 - 2018/4/1
N2 - Reactions of ortho-, para- and substituted meta-xylenyl bridged bis(tacn) ligands with two or three molar equivalents of Zn(NO3)2·6H2O at pH 5.0 in the presence of NaClO4 or NH4PF6 resulted in the formation of a range of crystalline zinc complexes. In the presence of perchlorate counter ions the Lpx and Lphx ligands gave rise to dinuclear Zn2+ coordination complexes [Zn2Cl2(Lpx)(H2O)2](ClO4)2(H2O) and [Zn2Cl2(Lphx)(H2O)2](ClO4)2(H2O)2 respectively, which formed infinite 1D polymeric chains. In contrast, in the presence of the hexafluorophosphate counter ion, the Lnix ligand formed a unique tetranuclear Zn2+ complex, [Zn2Cl2(Lnix)(H2O)3](Cl)(PF6)2(H2O)4, the Lcax ligand formed an octanuclear complex [Zn8Cl4(Lcax)4(H2O)10](PF6)6.7(NO3)1.3(H2O)3.3, whilst the Lox ligand formed a mononuclear sandwich structure, [Zn(Lox)](PF6)2(H2O). The protonated metal-free Lpx ligand crystallised as [H4(Lpx)](NO3)2(PF6)(H2O)2 with the stacked ligand cations forming a hydrogen-bonded network. These structural attributes provide an explanation for the significant differences in binding behaviour of recombinant N-terminally tagged proteins with the corresponding Zn2+-azamacrocyclic complexes, compared to the analogous Cu2+- or Ni2+-azamacrocyclic complexes, when immobilised onto support materials and used as immobilised metal affinity chromatographic (IMAC) adsorbents.
AB - Reactions of ortho-, para- and substituted meta-xylenyl bridged bis(tacn) ligands with two or three molar equivalents of Zn(NO3)2·6H2O at pH 5.0 in the presence of NaClO4 or NH4PF6 resulted in the formation of a range of crystalline zinc complexes. In the presence of perchlorate counter ions the Lpx and Lphx ligands gave rise to dinuclear Zn2+ coordination complexes [Zn2Cl2(Lpx)(H2O)2](ClO4)2(H2O) and [Zn2Cl2(Lphx)(H2O)2](ClO4)2(H2O)2 respectively, which formed infinite 1D polymeric chains. In contrast, in the presence of the hexafluorophosphate counter ion, the Lnix ligand formed a unique tetranuclear Zn2+ complex, [Zn2Cl2(Lnix)(H2O)3](Cl)(PF6)2(H2O)4, the Lcax ligand formed an octanuclear complex [Zn8Cl4(Lcax)4(H2O)10](PF6)6.7(NO3)1.3(H2O)3.3, whilst the Lox ligand formed a mononuclear sandwich structure, [Zn(Lox)](PF6)2(H2O). The protonated metal-free Lpx ligand crystallised as [H4(Lpx)](NO3)2(PF6)(H2O)2 with the stacked ligand cations forming a hydrogen-bonded network. These structural attributes provide an explanation for the significant differences in binding behaviour of recombinant N-terminally tagged proteins with the corresponding Zn2+-azamacrocyclic complexes, compared to the analogous Cu2+- or Ni2+-azamacrocyclic complexes, when immobilised onto support materials and used as immobilised metal affinity chromatographic (IMAC) adsorbents.
KW - Bis(tacn) ligands
KW - Crystal structures
KW - IMAC separations
KW - Xylenyl linkers
KW - Zinc(II) aza-macrocyclic complexes
UR - http://www.scopus.com/inward/record.url?scp=85041514995&partnerID=8YFLogxK
U2 - 10.1016/j.poly.2018.01.013
DO - 10.1016/j.poly.2018.01.013
M3 - Article
VL - 144
SP - 187
EP - 197
JO - Polyhedron
JF - Polyhedron
SN - 0277-5387
ER -