2019
DOI: 10.1021/jacs.9b05874
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General Approach to Direct Measurement of the Hydration State of Coordination Complexes in the Gas Phase: Variable Temperature Mass Spectrometry

Abstract: The formation of ternary aqua complexes of metal-based diagnostics and therapeutics is closely correlated to their in vivo efficacy but approaches to quantify the presence of coordinated water ligands are limited. We introduce a general and high-throughput method for characterizing the hydration state of para- and diamagnetic coordination complexes in the gas phase based on variable-temperature ion trap tandem mass spectrometry. Ternary aqua complexes are directly observed in the mass spectrum and quantified a… Show more

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Cited by 20 publications
(25 citation statements)
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“…In total, optimised structures and reaction energetics for 23 different Zr 4+ complexes, using 17 different ligands (Figure 11) were calculated. 2,10,38,[46][47][48][49][50][51][52][53][54][55][56][57][58][59][60][61][62] Structures of the optimised Zr-complexes are presented in Figure 12 and key thermodynamic data are given in Table 2. The ligands chosen were selected based on their reported experimental potential to form stable complexes with 89 Zr 4+…”
Section: Predicting the Absolute And Relative Formation Constants Of Zirconium Complexesmentioning
confidence: 99%
“…In total, optimised structures and reaction energetics for 23 different Zr 4+ complexes, using 17 different ligands (Figure 11) were calculated. 2,10,38,[46][47][48][49][50][51][52][53][54][55][56][57][58][59][60][61][62] Structures of the optimised Zr-complexes are presented in Figure 12 and key thermodynamic data are given in Table 2. The ligands chosen were selected based on their reported experimental potential to form stable complexes with 89 Zr 4+…”
Section: Predicting the Absolute And Relative Formation Constants Of Zirconium Complexesmentioning
confidence: 99%
“…[ZrHL] 2+ [ZrL] + , and [ZrLH –1 ], over the pH range 1–11 . The stability constants and pZr value determined for the Zr­(IV)-DFOB system place DFOB among the best Zr­(IV) chelators, although the formation of six-coordinate unsaturated complexes (i.e., with the coordination sphere of Zr­(IV) completed by two water molecules or hydroxide ligands) and the susceptibility of coordinated water molecules to deprotonation were suggested to be the reason for the in vivo lability of 89 Zr­(IV)-DFOB complexes. The thermodynamic stability of Zr­(IV)-DFOB complexes is in line with in vivo research ,,, and also with Holland’s recent DFT calculations, indicating that our experimental approach was appropriate.…”
Section: Introductionmentioning
confidence: 99%
“…[9,10] The only chelator currently used in clinical trials utilizing 89 Zr-labelled Abs is the siderophore desferrioxamine (DFO 1, Figure 1). However, the hexadentate chelator DFO 1 is not ideal for the complexation of zirconium since the metal ion mostly has coordination numbers >6 [11,12]. Therefore, a chelator with a higher denticity, e.g., hepta-or octadentate, would be the more optimal choice.…”
Section: Introductionmentioning
confidence: 99%