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三元铜（II）配合物，Cu（H⁻¹L）（ACys⁻）和Cu（H⁻²L）（ACys⁻）；L =肽，ACys⁻ = N-乙酰半胱氨酸盐。与铜（II）从Cu（H⁻²L）转运至半胱氨酸过程中的中间体类似的配合物。

Ternary Cu(II) complexes, Cu(H(-1)L)(ACys-) and Cu(H(-2)L)(ACys-); L = peptides, ACys- = N-acetyl-cysteinate. Analogous complexes to the intermediates in the transport of Cu(II) from Cu(H(-2)L) to cysteine.

作者信息

Hanaki Akira, Funahashi Yasuhiro, Odani Akira

机构信息

National Institute of Radiological Sciences, Anagawa 4-9, Inage-ku, Chiba 263-8555, Japan.

出版信息

J Inorg Biochem. 2006 Mar;100(3):305-15. doi: 10.1016/j.jinorgbio.2005.11.017. Epub 2006 Jan 10.

DOI:10.1016/j.jinorgbio.2005.11.017
PMID:16406099
Abstract

The Cu(II) in Cu(H(-2)L) has been postulated to be successively transported to cysteine (Cys) as follows; Cu(H(-2)L) <==> Cu(H(-2)L)(Cys*-) <==> Cu(H(-1)L)(Cys*-) --> Cu(H(-1)L)(Cys-), where Cys*- denotes the monodentate Cys-. N-acetyl-cysteinate (ACys-) complexes Cu(H(-2)L)(ACys-) and Cu(H(-1)L)(ACys-), having similar coordination modes to Cu(H(-2)L)(Cys*-) and Cu(H(-1)L)(Cys*-), respectively, exhibited the S --> Cu(II) charge transfer absorption at 325-355 nm and the d-d absorption at 530-610 nm. A linear interrelation existed between the energies of the CD and d-d absorptions. Cu(H(-2)L)(ACys-) were in rapid equilibrium with Cu(H(-1)L)(ACys-). Upon forming the ternary complex, pK(c2) of the parent Cu(H(-1)L) was raised to more than 1.0. The formation constants (K) of the Cu(H(-1)L)(ACys-) species from Cu(H(-1)L) were bigger than those of Cu(H(-2)L)(ACys-) from Cu(H(-2)L). The linear free-energy relationship existed between the free-energy change (deltaG) and the entropy change (deltaS) for the ternary complex formation. The rate constants (k1+) for the Cu(H(-1)L)(Cys-) formation closely correlated with the K values for Cu(H(-2)L)(ACys-). The ternary complexes containing ACys are considered to be analogous complexes to the intermediates in the transport of Cu(II) from peptides to cysteine.

摘要

据推测，Cu(H(-2)L)中的Cu(II)会按以下方式依次转移至半胱氨酸（Cys）：Cu(H(-2)L) <==> Cu(H(-2)L)(Cys*-) <==> Cu(H(-1)L)(Cys*-) --> Cu(H(-1)L)(Cys-)，其中Cys*-表示单齿Cys-。N-乙酰半胱氨酸盐（ACys-）形成的配合物Cu(H(-2)L)(ACys-)和Cu(H(-1)L)(ACys-)，分别具有与Cu(H(-2)L)(Cys*-)和Cu(H(-1)L)(Cys*-)相似的配位模式，在325 - 355 nm处表现出S --> Cu(II)电荷转移吸收，在530 - 610 nm处表现出d-d吸收。圆二色（CD）吸收和d-d吸收的能量之间存在线性相互关系。Cu(H(-2)L)(ACys-)与Cu(H(-1)L)(ACys-)处于快速平衡状态。形成三元配合物后，母体Cu(H(-1)L)的pK(c2)升高至1.0以上。由Cu(H(-1)L)形成Cu(H(-1)L)(ACys-)物种的形成常数（K）大于由Cu(H(-2)L)形成Cu(H(-2)L)(ACys-)的形成常数。三元配合物形成的自由能变化（deltaG）和熵变化（deltaS）之间存在线性自由能关系。Cu(H(-1)L)(Cys-)形成的速率常数（k1+）与Cu(H(-2)L)(ACys-)的K值密切相关。含ACys的三元配合物被认为是Cu(II)从肽转移至半胱氨酸过程中中间体的类似配合物。

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