title: Programming A Molecular Relay for Ultrasensitive Biodetection through (129)Xe NMR.
abstract: A supramolecular strategy for detecting specific proteins in complex media by using hyperpolarized (129) Xe NMR is reported. A cucurbit[6]uril (CB[6])-based molecular relay was programmed for three sequential equilibrium conditions by designing a two-faced guest (TFG) that initially binds CB[6] and blocks the CB[6]-Xe interaction. The protein analyte recruits the TFG and frees CB[6] for Xe binding. TFGs containing CB[6]- and carbonic anhydrase II (CAII)-binding domains were synthesized in one or two steps. X-ray crystallography confirmed TFG binding to Zn(2+) in the deep CAII active-site cleft, which precludes simultaneous CB[6] binding. The molecular relay was reprogrammed to detect avidin by using a different TFG. Finally, Xe binding by CB[6] was detected in buffer and in E. coli cultures expressing CAII through ultrasensitive (129) Xe NMR spectroscopy.
authors.affiliation: Department of Chemistry, University of Pennsylvania, 231 South 34th Street, Philadelphia, PA, 19104-6323, USA.
authors.forename: Yanfei
authors.identifier: 0000-0002-9358-4759
authors.initials: Y
authors.lastname: Wang
authors.affiliation: Department of Chemistry, University of Pennsylvania, 231 South 34th Street, Philadelphia, PA, 19104-6323, USA.
authors.forename: Benjamin W
authors.identifier: 0000-0003-3333-5053
authors.initials: BW
authors.lastname: Roose
authors.affiliation: Department of Chemistry, University of Pennsylvania, 231 South 34th Street, Philadelphia, PA, 19104-6323, USA.
authors.forename: John P
authors.initials: JP
authors.lastname: Philbin
authors.affiliation: Department of Chemistry, University of Pennsylvania, 231 South 34th Street, Philadelphia, PA, 19104-6323, USA.
authors.forename: Jordan L
authors.initials: JL
authors.lastname: Doman
authors.affiliation: Department of Chemistry, University of Pennsylvania, 231 South 34th Street, Philadelphia, PA, 19104-6323, USA. ivandmo@sas.upenn.edu.
authors.forename: Ivan J
authors.identifier: 0000-0001-7162-1347
authors.initials: IJ
authors.lastname: Dmochowski
mesh_terms: D018360:Crystallography, X-Ray; D057230:Limit of Detection; D009682:Magnetic Resonance Spectroscopy / Q000379:methods*; D014978:Xenon / Q000737:chemistry*
chemical_list: D014978:Xenon
keywords: NMR spectroscopy; bioinorganic chemistry; biosensors; host-guest systems; molecular recognition