Dais Tyson N, Nixon David J, Brothers Penelope J, Henderson William, Plieger Paul G
School of Fundamental Sciences, Massey University Private Bag 11 222 Palmerston North 4442 New Zealand
School of Chemical Sciences, University of Auckland Private Bag 92019 Auckland 1142 New Zealand.
RSC Adv. 2020 Nov 4;10(66):40142-40147. doi: 10.1039/d0ra08706h. eCollection 2020 Nov 2.
A comparative study between three experimentally known beryllium chelators (EDTA, NTP, and 10-HBQS) and two tetradentate tripodal di-pyridine-based receptors (HL and HL-NH), specifically designed to bind Be cations, has been undertaken in the aqueous phase at the B3LYP/6-311++G(d,p) computational level. The relative binding energies of these five ligand systems to a variety of first row and pre-transition metal cations have been calculated, specifically to investigate their binding strength to Be and the binding enhancement that a second sphere hydrogen bonding interaction could afford to the pyridyl based systems. The complexes of EDTA were calculated to have the highest average binding energy; followed by those of NTP, HL-NH, HL, and finally 10-HBQS. The calculated binding energy of the HL-NHBe complex, which includes second sphere interactions, was found to be almost 9% greater than the HL Be complex, with an average binding energy increase of 13.5% observed across all metals upon inclusion of second sphere hydrogen bonding.
在水相中，于B3LYP/6-311++G(d,p)计算水平下，对三种实验已知的铍螯合剂（乙二胺四乙酸（EDTA）、N-三（2-吡啶甲基）胺（NTP）和1,2-二羟基喹啉-5,7-二磺酸（10-HBQS））与两种专门设计用于结合铍阳离子的四齿三脚架双吡啶基受体（HL和HL-NH）进行了比较研究。已计算出这五种配体体系与各种第一周期和前过渡金属阳离子的相对结合能，具体目的是研究它们与铍的结合强度以及第二球氢键相互作用对基于吡啶基的体系所能提供的结合增强作用。计算得出EDTA配合物具有最高的平均结合能；其次是NTP、HL-NH、HL的配合物，最后是10-HBQS的配合物。发现包含第二球相互作用的HL-NHBe配合物的计算结合能比HL Be配合物几乎高9%，在包含第二球氢键时，观察到所有金属的平均结合能增加了13.5%。
