Berry Stuart N, Qin Lei, Lewis William, Jolliffe Katrina A
School of Chemistry , The University of Sydney , NSW 2006 , Australia . Email:
Chem Sci. 2020 Jun 18;11(27):7015-7022. doi: 10.1039/d0sc02533j. eCollection 2020 Jul 21.
The effect of chelate cooperativity on the binding of several ditopic anions to two tetrathiourea macrocycles has been analysed in competitive solvent mixtures (HO : DMSO 1 : 9 v/v). The semi-flexible receptors bind dicarboxylates with high affinity dependent on the length and flexibility of the guest. Chemical double mutant cycle (DMC) analysis allowed the chelate cooperativity effects to be measured in detail and revealed both positive and negative cooperativity effects which were dependent on guest size, flexibility and spacer interactions between guest and macrocycle. H NMR and crystallographic studies confirmed the macrocycle hosts are adaptable, changing conformation to match their pore size to a selected guest.
在竞争性溶剂混合物（水：二甲基亚砜，体积比1:9）中，分析了螯合协同作用对几种双位点阴离子与两个四硫脲大环结合的影响。半柔性受体以高亲和力结合二羧酸盐，这取决于客体的长度和柔性。化学双突变循环（DMC）分析能够详细测定螯合协同效应，并揭示了正协同效应和负协同效应，这些效应取决于客体大小、柔性以及客体与大环之间的间隔相互作用。核磁共振氢谱（¹H NMR）和晶体学研究证实，大环主体具有适应性，会改变构象以使孔径与选定的客体相匹配。
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