在水界面的磷脂单层中增强了精氨酸-磷酸盐的识别,The Journal of Physical Chemistry C

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在水界面的磷脂单层中增强了精氨酸-磷酸盐的识别
The Journal of Physical Chemistry C ( IF 3.3 ) Pub Date : 2018-07-23 , DOI: 10.1021/acs.jpcc.8b03531
Jennifer F. Neal ₁ , Wei Zhao ₂ , Alexander J. Grooms ₁ , Amar H. Flood ₂ , Heather C. Allen ₁

Affiliation

由于世界人口的增长，对开发更好的受体以回收和再循环用于农业过程的磷酸盐的需求不断增长。这种需求是由农业需求和环境问题驱动的，因为磷酸盐富营养化通过为藻华提供燃料而对淡水供应产生破坏性影响。空气/水界面提供具有介电常数（ε）的独特区域，该介电常数从高体积水（ε= 80）减小到单层表面附近的明显降低（例如ε<40），从而潜在地增强分子识别期间的亲和力。此处介绍的工作使用了磷酸盐与氨基酸精氨酸结合的模型系统，并利用了磷脂单层1,2-二棕榈酰-sn的界面性质-甘油-3-磷脂酸，作为定量结合的磷酸盐来源。采用精氨酸作为探针分子可以评估其胍基部分的磷酸盐螯合作用。Langmuir单层研究的表面压力-面积等温线以及相应的红外反射吸收光谱与Brewster角显微镜一起用于原位测定磷酸-胍盐配合物的分子结合相互作用和表面结合常数，如下所示：大于10 ³ M ^–1。通过磷酸盐和精氨酸的NMR滴定确定的本体溶液中的结合常数约为0.1 M ^–1。从本体水溶液到空气/水界面的大于10,000倍的增加表明该界面提供了增强的结合亲和力的区域。

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Arginine–Phosphate Recognition Enhanced in Phospholipid Monolayers at Aqueous Interfaces

Due to the growing world population, there is an ever-increasing need to develop better receptors to recover and recycle phosphate for use in agricultural processes. This need is driven by agricultural demand and environmental concerns because phosphate eutrophication has a damaging effect on fresh water supplies by fueling algal blooms. The air/water interface provides a unique region with a dielectric constant (ε) that diminishes from high in bulk water (ε = 80) to significantly lower (e.g., ε < 40) near the monolayer surface to potentially enhance affinities during molecular recognition. The work presented here uses a model system of phosphate binding to an amino acid, arginine, and utilizes the interfacial properties of the phospholipid monolayer, 1,2-dipalmitoyl-sn-glycero-3-phosphatidic acid, as the phosphate source to quantify binding. Employing arginine as a probe molecule allows for the evaluation of its guanidinium moiety for phosphate chelation. Surface pressure–area isotherms from Langmuir monolayer studies, and the corresponding infrared reflection absorption spectroscopy, were used along with Brewster angle microscopy for in situ determination of molecular binding interactions and the surface binding constants of the phosphate–guanidinium complex, which are shown here to be greater than 10³ M^–1. The binding constant in bulk solution, determined by NMR titrations of phosphate and arginine, is determined to be on the order of 0.1 M^–1. The greater than 10 000-fold increase from the bulk aqueous solution to the air/water interface reveals that the interface provides a region of enhanced binding affinity.

更新日期：2018-07-24

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