期刊
LANGMUIR
卷 27, 期 4, 页码 1448-1456出版社
AMER CHEMICAL SOC
DOI: 10.1021/la104152s
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资金
- EPSRC [EP/C004396/1, EP/F055315/1]
- EPSRC [EP/F055315/1] Funding Source: UKRI
- Engineering and Physical Sciences Research Council [EP/F055315/1, EP/C004396/1] Funding Source: researchfish
A membrane-spanning bis(meso-3-pyridyl) porphyrin I has been synthesized, embedded in EYPC vesicles, and upon Pd(II) addition has been shown to form ionophores that allow the passage of anionic 5/6-carboxyfluorescein through membranes. The geometric matching of bis(meso-3-pyridyl) porphyrin 1 and trans-Pd(II) was designed to give a cyclic porphyrin trimer [PdCl2(1)](3). However, solution-phase studies showed that PdCl2(PhCN)2 cross linked 1 into linear oligomers at porphyrin concentrations above 10 mM, although the formation of cyclic species was inferred from studies at concentrations below 2 mu M. Fluorescence titrations showed that embedding porphyrin 1 in bilayers greatly reduced its affinity for Pd(II), but the combination of porphyrin 1 and Pd(II) gave an ionophoric species that increased the rate of 5/6-carboxyfluorescein (5/6-CF) transit through the phospholipid bilayer 12-fold. A maximum in the 5/6-CF release rate was observed at a Pd(II) concentration of 4 mu M, and the application of a solution-phase binding model to the membrane phase showed that this peak in ionophoric activity corresponded to the greatest extent of porphyrin oligomerization. Further studies suggested these Pd(II)/porphyrin oligomers transported 5/6-CF via a channel mechanism.
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