金属イオンにより誘起される人工ＤＮＡの自発的集合化

幡野, 明彦; ハタノ, アキヒコ; HATANO, Akihiko

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金属イオンにより誘起される人工ＤＮＡの自発的集合化

https://ir.soken.ac.jp/records/311

名前 / ファイル	ライセンス	アクション
要旨・審査要旨 / Abstract, Screening Result (282.2 kB)
本文 / Thesis (5.6 MB)

Item type

学位論文 / Thesis or Dissertation(1)

公開日

2010-02-22

タイトル

金属イオンにより誘起される人工ＤＮＡの自発的集合化

タイトル

Self-Assembly of Artificial DNA induced by Metal Coordination

言語

jpn

資源タイプ

資源タイプ識別子

http://purl.org/coar/resource_type/c_46ec

資源タイプ

thesis

著者名

幡野, 明彦

フリガナ

ハタノ, アキヒコ

著者

HATANO, Akihiko

学位授与機関

学位授与機関名

総合研究大学院大学

学位名

博士（理学）

学位記番号

内容記述タイプ

Other

内容記述

総研大甲第488号

研究科

値

数物科学研究科

専攻

値

08 機能分子科学専攻

学位授与年月日

2000-09-29

学位授与年度

値

2000

要旨

内容記述タイプ

Other

内容記述

The self-assembly of noncovalently linked molecular clusters of unique building blocks has currently received considerable attention. In particular, "template-directed" approaches are becoming common and have been accepted promising for the construction of the ideally predesigned assembly. One of the most appealing paradigms of self-assembly in biological system is sequence-specific association between two complementary nucleic acid strands, and such processes play essential roles in most genetic events. DNA oligonucleotides have been intensively used as templates for reaction control on the template such as self-replication of the guest DNA components.

(Chart 1 was abbreviated.)

As an approach to novel metal-assembled systems directed to a single-stranded DNA as the template (Chart 1), they have synthesized "chelator-type" nucleic acids mimics 1 - 4 (Scheme 1). Two metal binding sites and one nucleobase moiety were introduced into compound 1 - 4 so that they can undergo strand formation by intermolecular metal coordination thereby possibly interacting with a natural DNA strand through Watson-Crick base pairing.

(Scheme 1 was abbreviated.)

Compound 1 was synthesized from 3,5-dimethylphenol, according to Scheme 1. The phenolic intermediate serves as a common intermediate for the introduction of each nucleobase at the phenolic position. Here they present the experimental data with respect to an adenine mimic 1. The adenine mimic 1 reacted with ZnII(NO3)2 in water to form ZnII complex 2. The molecular structure of the ZnII complex was characterized by single-crystal X-ray crystallography. Each ethylenediamine moiety binds to ZnII to form a trans-N4-plane, and two water molecules at the axial positions complete the octahedral structure (Figure 1).

(Figure 1 was abbreviated.)

Adenine analogues 1 are intermolecularly linked together by ZnII ions that provide the driving force for polymerization by imposing an octahedral coordination geometry at each site. Although the ZnII-ZnII distance of 7.718Å is rather longer than the average distance between adjacent phosphodiester groups in the same chain of B-DNA (ca. 6Å), molecular modeling studies indicated that this complex is structurally flexible enough for complementary binding to a single-stranded natural DNA.
They then examined interactions of the ZnII - assembled adenine polymer with oligo (dT)70 using UV absorption changes. Figure 2 shows the temperature-dependency of the absorption at 260 nm for a 1 : 1 mixture of ZnII complex and (dT)70 ([ZnII complex] = [(dT)70] = 15 μM/base, 1 mM Mops buffer at pH 7.0) when the solution temperature was elevated from 0 □C to 80 □C. An absorption break was observed at 39 □C, and almost the same curve was obtained even when the temperature was changed downwardly. This behavior is common in the naturally occurring nucleic acids.

(Figure 2 was abbreviated.)

The ZnII complex thus preferably associates with a natural DNA oligomer probably through electrostatic and hydrogen bonding interactions accompanied by hydrophobic effects. Such artificially-designed nucleic acid components that can undergo metal-assisted assembly in a reversible fashion would provide novel molecular array systems directed to information-bearing DNA or RNA for applications not only to metallo-antisenses for gene regulation but also to molecular memory devices or molecular wires.

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http://purl.org/coar/version/c_ab4af688f83e57aa

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金属イオンにより誘起される人工ＤＮＡの自発的集合化

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× HATANO, Akihiko

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