TY - JOUR A1 - Debatin, Franziska A1 - Thomas, Arne A1 - Kelling, Alexandra A1 - Hedin, Niklas A1 - Bacsik, Zoltan A1 - Senkovska, Irena A1 - Kaskel, Stefan A1 - Junginger, Matthias A1 - Müller, Holger A1 - Schilde, Uwe A1 - Jäger, Christian A1 - Friedrich, Alwin A1 - Holdt, Hans-Jürgen T1 - In situ synthesis of an imidazolate-4-amide-5-imidate ligand and formation of a microporous zinc-organic framework with H2-and CO2-storage ability N2 - Narrow channels with polar walls are the structural and functional features responsible for the high capacity of a zinc-organic framework based on an imidazolate-amide-imidate ligand for the uptake of H2 and CO2 (see structure: orange Zn, blue N, red O, dark gray C, light gray H). The rigid and stable chelating ligand was synthesized in situ by partial hydrolysis of a dicyanoimidazole compound. Y1 - 2010 UR - http://www3.interscience.wiley.com/cgi-bin/jhome/26737/ U6 - https://doi.org/10.1002/anie.200906188 SN - 1433-7851 ER - TY - JOUR A1 - Schwarze, Thomas A1 - Dosche, Carsten A1 - Flehr, Roman A1 - Klamroth, Tillmann A1 - Löhmannsröben, Hans-Gerd A1 - Saalfrank, Peter A1 - Cleve, Ernst A1 - Buschmann, Hans-Jürgen A1 - Holdt, Hans-Jürgen T1 - Combination of a CT modulated PET and an intramolecular excimer formation to quantify PdCl2 by large fluorescence enhancement N2 - The [6.6](9,10)anthracenophane 1 (Scheme 1) is a selective fluoroionophore for the detection of PdCl2 with a large fluorescence enhancement factor (I/I-0 > 250). Y1 - 2010 UR - http://pubs.rsc.org/en/content/articlehtml/2010/cc/b919973j U6 - https://doi.org/10.1039/B919973j SN - 1359-7345 ER - TY - JOUR A1 - Schwarze, Thomas A1 - Dosche, Carsten A1 - Flehr, Roman A1 - Klamroth, Tillmann A1 - Löhmannsröben, Hans-Gerd A1 - Saalfrank, Peter A1 - Cleve, Ernst A1 - Buschmann, Hans-Jürgen A1 - Holdt, Hans-Jürgen T1 - Combination of a CT modulated PET and an intramolecular excimer formation to quantify PdCl2 by large fluorescence enhancement Y1 - 2010 UR - http://www.rsc.org/ej/CC/2010/b919973j.pdf SN - 1359-7345 ER - TY - JOUR A1 - Schwarze, Thomas A1 - Mickler, Wulfhard A1 - Dosche, Carsten A1 - Flehr, Roman A1 - Klamroth, Tillmann A1 - Löhmannsröben, Hans-Gerd A1 - Saalfrank, Peter A1 - Holdt, Hans-Jürgen T1 - Systematic investigation of photoinduced electron transfer controlled by internal charge transfer and its consequences for selective PdCl2 coordination N2 - Fluoroionophores of fluorophore-spacer-receptor format were prepared for detection of PdCl2 by fluorescence enhancement. The fluorophore probes 1-13 consist of a fluorophore group, in alkyl spacer and a dithiomaleonitrile PdCl2 receptor. First, varying the length of the alkylene spacer (compounds 1-3) revealed, dominant through-space pathway for oxidative photoinduced electron transfer (PET) in CH2-bridged dithiomaleonitrile fluoroionophores. Second. fluorescent probes 4-9 containing two anthracene or pyrene fragments connected through CH2 bridges to the dithiomaleonitrile unit were synthesized. Modulation of the oxidation potential (E-Ox) through electron-withdrawing or -donating groups on the anthracene moiety regulates file thermodynamic driving force for oxidative PET (Delta G(PET)) in bis(anthrylmethylthio)maleonitriles and therefore the fluorescence quantum yields (Phi(f)), too. The new concept was confirmed and transferred to pyrenyl ligands, and fluorescence enhancements (FE) greater than 3.2 in the presence of PdCl2 were achieved by 7 and 8 (FE=5.4 and 5.2). Finally, for comparison, monofluorophore ligands 10-13 were synthesized. Y1 - 2010 UR - http://onlinelibrary.wiley.com/doi/10.1002/chem.200902281/pdf U6 - https://doi.org/10.1002/chem.200902281 SN - 0947-6539 ER - TY - JOUR A1 - Schwarze, Thomas A1 - Mickler, Wulfhard A1 - Dosche, Carsten A1 - Flehr, Roman A1 - Klamroth, Tillmann A1 - Löhmannsröben, Hans-Gerd A1 - Saalfrank, Peter A1 - Holdt, Hans-Jürgen T1 - Systematic investigation of photoinduced electron transfer controlled by internal charge transfer and its consequences for selective PdCl2 coordination N2 - Fluoroionophores of fluorophore-spacer-receptor format were prepared for detection of PdCl2 by fluorescence enhancement. The fluorescent probes 1-13 consist of a fluorophore group, an alkyl spacer and a dithiomaleonitrile PdCl2 receptor. First, varying the length of the alkylene spacer (compounds 1-3) revealed a dominant through-space pathway for oxidative photoinduced electron transfer (PET) in CH2-bridged dithiomaleonitrile fluoroionophores. Second, fluorescent probes 4-9 containing two anthracene or pyrene fragments connected through CH2 bridges to the dithiomaleonitrile unit were synthesized. Modulation of the oxidation potential (EOx) through electron-withdrawing or -donating groups on the anthracene moiety regulates the thermodynamic driving force for oxidative PET (GPET) in bis(anthrylmethylthio)maleonitriles and therefore the fluorescence quantum yields (f), too. The new concept was confirmed and transferred to pyrenyl ligands, and fluorescence enhancements (FE) greater than 3.2 in the presence of PdCl2 were achieved by 7 and 8 (FE=5.4 and 5.2). Finally, for comparison, monofluorophore ligands 10-13 were synthesized. Y1 - 2010 UR - http://www3.interscience.wiley.com/journal/26293/home SN - 0947-6539 ER - TY - JOUR A1 - Starke, Ines A1 - Kammer, Stefan A1 - Holdt, Hans-Jürgen A1 - Kleinpeter, Erich T1 - Stability of disubstituted copper complexes in the gas phase analyzed by electrospray ionization mass spectrometry N2 - A series of nitrogen ligand (L)/copper complexes of the type [(CuL)-L-I](+), [(CuL)-L-II(X)](+) and [(CuL2)-L- I](+) (X = Cl-, BF4-, acac(-), CH3COO- and SO3CF3-) was studied in the gas phase by electrospray ionization mass spectrometry. The following ligands (L) were employed: 1,12-diazaperylene (dap), 1,1'-bisiso-quinoline (bis), 2,2'-bipyridine (bpy), 1,10-phenanthroline (phen), 2,11-disubstituted 1,12-diazaperylenes (dap), 3,3'- disubstituted 1,1'-bisisoquinoline (bis), 5,8-dimethoxy-substituted diazaperylene (meodap), 6,6'-dimethoxy- substituted bisisoquinoline (meobis) and 2,9-dimethyl-1,10-phenanthroline (dmphen). Collision-induced decomposition measurements were applied to evaluate the relative stabilities of the different copper complexes. The influence of the spatial arrangement of the ligands, of the type of substituents and of the counter ion of the copper salts employed for the complexation was examined. Correlations were found between the binding constants of the [ML2](+) complexes in solution and the relative stabilities of the analogous complexes in the gas phase. Furthermore, complexation with the ligands 2,11-dialkylated 1,12-diazaperylenes [alkyl = ethyl (dedap) and isopropyl (dipdap)] was studied in the solvents CH3OH and CH3CN. Y1 - 2010 UR - http://www3.interscience.wiley.com/cgi-bin/jhome/4849 U6 - https://doi.org/10.1002/Rcm.4519 SN - 0951-4198 ER -