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首页> 外文期刊>Chemistry: A European journal >Equilibrium, Kinetic and Structural Properties of Gallium(III) and Some Divalent Metal Complexes Formed with the New DATAm and DATA5m Ligands
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Equilibrium, Kinetic and Structural Properties of Gallium(III) and Some Divalent Metal Complexes Formed with the New DATAm and DATA5m Ligands

机译：镓（III）的平衡，动力学和结构性能，与新的DataM和Data5M配体形成的一些二价金属配合物

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摘要

The development of 68Ge/68Ga generators has made the positron-emitting 68Ga isotope widely accessible and raised interest in new chelate complexes of Ga~(3+). The hexadentate 1,4-di(acetate)-6-methyl[amino(methyl)acetate]-perhydro-1,4-diazepane (DATAm) ligand and its bifunctional analogue, 1,4-di(acetate)-6-pentanoic acid[amino(methyl)acetate] perhydro-1,4-diazepane (DATA5m), rapidly form complexes with 68Ga in high radiochemical yield. The stability constants of DATAm and DATA5m complexes formed with Ga~(3+), Zn~(2+), Cu~(2+), Mn~(2+) and Ca~(2+) have been determined by using pH potentiometry, spectrophotometry (Cu~(2+)) and ~1H and 71Ga NMR spectroscopy (Ga~(3+)). The stability constants of Ga(DATAm) and Ga(DATA5m) complexes are slightly higher than those of Ga(AAZTA). The species distribution calculations indicated the predominance of Ga(L)OH mixed-hydroxo complexes at physiological pH. The ~1H and 71Ga NMR spectroscopy studies provided information about the coordinated functional groups of ligands and on the kinetics of exchange between the Ga(L) and Ga(L)OH complexes. The transmetalation reactions between the Ga(L) complexes and Cu~(2+) citrate (6H<8.5) occur through both spontaneous and OH--assisted dissociation of the Ga(L)OH species. At pH 7.4 and 25°C, the half-lives of the dissociation of Ga(DATAm), Ga(DATA5m) and Ga(AAZTA) were 11, 44 and 24 h, respectively. Similar half-lives have been obtained for the ligand-exchange reactions between the Ga(L)OH complexes and transferrin. The equilibrium and kinetic data indicate that the Ga(DATA5m) complex is a good 68Ga-based radiodiagnostic candidate.
机译：68GE / 68GA发电机的开发使正电子发射68Ga同位素广泛访问，并对Ga〜（3+）的新螯合物复合物提高了兴趣。六次戊酸1,4-二（乙酸盐）-6-甲基[氨基（甲基）乙酸酯] - 氢-1,4-二氮杂己烷（DATAM）配体及其双官能类似物，1,4-DI（醋酸）-6-戊烯酸[氨基（甲基）乙酸盐] perydro-1,4-二氮己（Data5m），快速形成68ga的复合物，高放射化学产率。通过使用pH确定与Ga〜（3+），Zn〜（2+），Cu〜（2+），Cu〜（2+），Cu〜（2+），Cu〜（2+），Cu〜（2+）和Ca〜（2+）形成的DATAM和DATA5M复合物的稳定性常数已经确定电位测量，分光光度法（Cu〜（2+））和〜1H和71Ga NMR光谱（Ga〜（3+））。 Ga（DataM）和Ga（Data5M）复合物的稳定性常数略高于Ga（Aazta）。物种分布计算表明Ga（L）OH混合 - 羟基复合物在生理pH下的优势。 〜1H和71GA NMR光谱研究提供了有关配体的协调官能团的信息以及Ga（L）和Ga（L）OH复合物之间的交换动力学。通过自发和OH辅助解离Ga（L）OH物种，通过自发和OH辅助解离，柠檬酸盐（L）复合物和Cu〜（2+）之间的透射率反应进行柠檬酸盐（6-<8.5）。在pH 7.4和25℃下，Ga（DATAM），Ga（Data5M）和Ga（Aazta）解离的半衰期分别为11,44和24小时。已经获得了Ga（L）OH复合物和转铁蛋白之间的配体交换反应的类似半衰期。均衡和动力学数据表明GA（DATA5M）复合物是良好的68GA基于无线电诊所候选者。

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  • 来源
    《Chemistry: A European journal》 |2017年第43期|共14页
  • 作者

    Edit Farkas; Johannes Nagel; Bradley P. Waldron; David Parker; Imre Tjth; Ern? Brecher; Frank R?sch; Zsolt Baranyai;

  • 作者单位

    Department of Inorganic and Analytical Chemistry University of Debrecen Egyetem tér 1 4032 Debrecen (Hungary);

    Institute of Nuclear Chemistry University of Mainz Fritz-Strassmann-Weg 2 55128 Mainz (Germany);

    Department of Chemistry Durham University South Road Durham DH1 3LE (UK);

    Department of Chemistry Durham University South Road Durham DH1 3LE (UK);

    Department of Inorganic and Analytical Chemistry University of Debrecen Egyetem tér 1 4032 Debrecen (Hungary);

    Department of Inorganic and Analytical Chemistry University of Debrecen Egyetem tér 1 4032 Debrecen (Hungary);

    Institute of Nuclear Chemistry University of Mainz Fritz-Strassmann-Weg 2 55128 Mainz (Germany);

    Department of Inorganic and Analytical Chemistry University of Debrecen Egyetem tér 1 4032 Debrecen (Hungary);

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  • 原文格式 PDF
  • 正文语种 eng
  • 中图分类 应用化学;
  • 关键词

    gallium; kinetics; molecular imaging; NMR spectroscopy; reaction mechanisms; thermodynamics;

    机译：镓;动力学;分子成像;NMR光谱;反应机制;热力学;

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