On the Binding Strength Sequence for Nucleic Acid Bases and C(60) with Density Functional and Dispersion-corrected Density Functional Theories: Whether C(60) could protect nucleic acid bases from radiation-induced damage?
On the Binding Strength Sequence for Nucleic Acid Bases and C(60) with Density Functional and Dispersion-corrected Density Functional Theories: Whether C(60) could protect nucleic acid bases from radiation-induced damage?
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在核酸碱基和C（60）的结合强度序列上，具有密度和分散校正的密度功能理论：C（60）是否可以保护核酸碱基免受辐射诱导的损伤？
DOI：
10.1021/jp108812z
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发表时间：
2011-03-03
影响因子：
3.7
通讯作者：
Wang, Yixuan
中科院分区：
文献类型：
--
作者：
Sun, Wenming;Bu, Yuxiang;Wang, Yixuan
本文的主要目的是解决一个有争议的约束力 核酸碱基（NAB）和C60之间的序列，通过研究 碳60富勒烯对NAB及其阳离子的吸附 包括两个新的混合元GGA泛函的密度泛函理论， M05-2x和M06-2x，以及色散校正的密度泛函PBE-D。 M05-2x/6-311++G** 提供相同的结合 序列如先前报道的，鸟嘌呤（G）>胞嘧啶（C）>腺嘌呤（A） >胸腺嘧啶（T）;然而，M06-2x转换A和C的结合强度，并且 PBE-D最终导致以下序列，G>A>T>C，这是 这与广泛接受的NAB在其他设备上堆叠的层次结构相同。 碳纳米材料，例如单壁碳纳米管和石墨。的 结果表明，可疑的相对结合强度是由于 M05-2x或甚至M06-2x的电子相关处理不足 法通过计算得到G@C60的结合能， M06-2x/6-311++G（d，p）和PBE-D/cc-pVDZ为−7.10， -8.07千卡/摩尔，后者仅略弱 比MP2/6- 31 G（d，p）的预测值（-8.10kca/mol）高。因此 对于观察到的NAB@C60，PDE-D的性能优于M06-2x π-堆叠复合物。讨论C60是否可以预防 辐射损伤引起的NAB、NAB的电离电位和 C_（60）和前线分子轨道 NABs@C60和（NABs@C60）+也是 广泛调查。这些结果表明，当电子逃逸时， 从复合物中，T优先在C60中产生空穴 和C复合物，而对于G和A，空穴在整个复合物上离域， 而不是定位在C60部分上。有趣的发现是 可能会开启一种保护DNA免受辐射损伤的新策略， 为设计基于C60的抗辐射药物提供了新思路。
The major objective of this paper is to address a controversial binding sequence between nucleic acid bases (NABs) and C60 by investigating adsorptions of NABs and their cations on C60 fullerene with a variety of density functional theories including two novel hybrid meta-GGA functionals, M05-2x and M06-2x, as well as a dispersion-corrected density functional, PBE-D. The M05-2x/6-311++G** provides the same binding sequence as previously reported, guanine(G) > cytosine(C) > adenine (A) > thymine (T); however, M06-2x switches the binding strengths of A and C, and PBE-D eventually results in the following sequence, G>A>T>C, which is the same as the widely accepted hierarchy for the stacking of NABs on other carbon nanomaterials such as single-walled carbon nanotube and graphite. The results indicate that the questionable relative binding strength is due to insufficient electron correlation treatment with the M05-2x or even the M06-2x method. The binding energy of G@C60 obtained with the M06-2x/6-311++G(d,p) and the PBE-D/cc-pVDZ is −7.10 and −8.07 kcal/mol, respectively, and the latter is only slightly weaker than that predicted by the MP2/6-31G(d,p) (−8.10kca/mol). Thus, the PDE-D performs better than the M06-2x for the observed NAB@C60 π-stacked complexes. To discuss whether C60 could prevent NABs from radiation-induced damage, ionization potentials of NABs and C60, and frontier molecular orbitals of the complexes NABs@C60 and (NABs@C60)+ are also extensively investigated. These results revealed that when an electron escapes from the complexes, a hole was preferentially created in C60 for T and C complexes, while for G and A the hole delocalizes over the entire complex, rather than a localization on the C60 moiety. The interesting finding might open a new strategy for protecting DNA from radiation-induced damage and offer a new idea for designing C60-based antiradiation drugs.
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