title: Investigation of DOTA-Metal Chelation Effects on the Chemical Shift of (129) Xe.
abstract: Recent work has shown that xenon chemical shifts in cryptophane-cage sensors are affected when tethered chelators bind to metals. Here, we explore the xenon shifts in response to a wide range of metal ions binding to diastereomeric forms of 1,4,7,10-tetraazacyclododecane-1,4,7,10-tetraacetic acid (DOTA) linked to cryptophane-A. The shifts induced by the binding of Ca(2+) , Cu(2+) , Ce(3+) , Zn(2+) , Cd(2+) , Ni(2+) , Co(2+) , Cr(2+) , Fe(3+) , and Hg(2+) are distinct. In addition, the different responses of the diastereomers for the same metal ion indicate that shifts are affected by partial folding with a correlation between the expected coordination number of the metal in the DOTA complex and the chemical shift of (129) Xe. These sensors may be used to detect and quantify many important metal ions, and a better understanding of the basis for the induced shifts could enhance future designs.
authors.affiliation: Department of Chemistry, University of California, Berkeley, CA, 94720-1460, USA.|Material Science Division, Lawrence Berkeley National Laboratory, Berkeley, CA, 94720-1460, USA.
authors.forename: Keunhong
authors.initials: K
authors.lastname: Jeong
authors.affiliation: Department of Chemistry, University of California, Berkeley, CA, 94720-1460, USA.|Material Science Division, Lawrence Berkeley National Laboratory, Berkeley, CA, 94720-1460, USA.
authors.forename: Clancy C
authors.initials: CC
authors.lastname: Slack
authors.affiliation: Department of Chemistry, University of California, Berkeley, CA, 94720-1460, USA.|Material Science Division, Lawrence Berkeley National Laboratory, Berkeley, CA, 94720-1460, USA.
authors.forename: Christophoros C
authors.initials: CC
authors.lastname: Vassiliou
authors.affiliation: Department of Chemistry, University of California, Berkeley, CA, 94720-1460, USA.|Material Science Division, Lawrence Berkeley National Laboratory, Berkeley, CA, 94720-1460, USA.
authors.forename: Phuong
authors.initials: P
authors.lastname: Dao
authors.affiliation: Department of Chemistry, University of California, Berkeley, CA, 94720-1460, USA.|Material Science Division, Lawrence Berkeley National Laboratory, Berkeley, CA, 94720-1460, USA.
authors.forename: Muller D
authors.initials: MD
authors.lastname: Gomes
authors.affiliation: Department of Chemistry, University of California, Berkeley, CA, 94720-1460, USA.|Material Science Division, Lawrence Berkeley National Laboratory, Berkeley, CA, 94720-1460, USA.
authors.forename: Daniel J
authors.initials: DJ
authors.lastname: Kennedy
authors.affiliation: Department of Chemistry, University of California, Berkeley, CA, 94720-1460, USA.|Material Science Division, Lawrence Berkeley National Laboratory, Berkeley, CA, 94720-1460, USA.
authors.forename: Ashley E
authors.initials: AE
authors.lastname: Truxal
authors.affiliation: Department of Chemistry and Biochemistry, Santa Clara University, Sata Clara, CA, 95053-0270, USA.
authors.forename: Lindsay J
authors.initials: LJ
authors.lastname: Sperling
authors.affiliation: Department of Chemistry, University of California, Berkeley, CA, 94720-1460, USA.|Material Science Division, Lawrence Berkeley National Laboratory, Berkeley, CA, 94720-1460, USA.
authors.forename: Matthew B
authors.initials: MB
authors.lastname: Francis
authors.affiliation: Department of Chemistry, University of California, Berkeley, CA, 94720-1460, USA.|Physical Bioscience Division, Lawrence Berkeley National Laboratory, Berkeley, CA, 94720-1460, USA.
authors.forename: David E
authors.initials: DE
authors.lastname: Wemmer
authors.affiliation: Department of Chemistry, University of California, Berkeley, CA, 94720-1460, USA. pines@berkeley.edu.|Material Science Division, Lawrence Berkeley National Laboratory, Berkeley, CA, 94720-1460, USA. pines@berkeley.edu.
authors.forename: Alexander
authors.initials: A
authors.lastname: Pines
mesh_terms: D002614:Chelating Agents / Q000737:chemistry*; D018360:Crystallography, X-Ray; D006573:Heterocyclic Compounds, 1-Ring / Q000737:chemistry*; D008673:Metals, Alkaline Earth / Q000737:chemistry*; D019216:Metals, Heavy / Q000737:chemistry*; D008958:Models, Molecular; D015394:Molecular Structure; D014979:Xenon Isotopes / Q000737:chemistry
chemical_list: D002614:Chelating Agents; D006573:Heterocyclic Compounds, 1-Ring; D008673:Metals, Alkaline Earth; D019216:Metals, Heavy; D014979:Xenon Isotopes; C071349:1,4,7,10-tetraazacyclododecane- 1,4,7,10-tetraacetic acid
keywords: DOTA; NMR spectroscopy; cryptophane; metal-ion sensors; xenon