Andreev Oleg A, Dupuy Allison D, Segala Michael, Sandugu Srikanth, Serra David A, Chichester Clinton O, Engelman Donald M, Reshetnyak Yana K
Physics Department, University of Rhode Island, 2 Lippitt Road, Kingston, RI 02881, USA.
Proc Natl Acad Sci U S A. 2007 May 8;104(19):7893-8. doi: 10.1073/pnas.0702439104. Epub 2007 May 1.
The pH-selective insertion and folding of a membrane peptide, pHLIP [pH (low) insertion peptide], can be used to target acidic tissue in vivo, including acidic foci in tumors, kidneys, and inflammatory sites. In a mouse breast adenocarcinoma model, fluorescently labeled pHLIP finds solid acidic tumors with high accuracy and accumulates in them even at a very early stage of tumor development. The fluorescence signal is stable for >4 days and is approximately five times higher in tumors than in healthy counterpart tissue. In a rat antigen-induced arthritis model, pHLIP preferentially accumulates in inflammatory foci. pHLIP also maps the renal cortical interstitium; however, kidney accumulation can be reduced significantly by providing mice with bicarbonate-containing drinking water. The peptide has three states: soluble in water, bound to the surface of a membrane, and inserted across the membrane as an alpha-helix. At physiological pH, the equilibrium is toward water, which explains its low affinity for cells in healthy tissue; at acidic pH, titration of Asp residues shifts the equilibrium toward membrane insertion and tissue accumulation. The replacement of two key Asp residues located in the transmembrane part of pHLIP by Lys or Asn led to the loss of pH-sensitive insertion into membranes of liposomes, red blood cells, and cancer cells in vivo, as well as to the loss of specific accumulation in tumors. pHLIP nanotechnology introduces a new method of detecting, targeting, and possibly treating acidic diseased tissue by using the selective insertion and folding of membrane peptides.
膜肽pHLIP[pH(低)插入肽]的pH选择性插入和折叠可用于在体内靶向酸性组织,包括肿瘤、肾脏和炎症部位的酸性病灶。在小鼠乳腺腺癌模型中,荧光标记的pHLIP能高精度地发现实体酸性肿瘤,甚至在肿瘤发展的早期阶段就能在其中积聚。荧光信号在4天以上保持稳定,肿瘤中的信号强度约为健康对照组织的五倍。在大鼠抗原诱导的关节炎模型中,pHLIP优先积聚在炎症病灶中。pHLIP还可描绘肾皮质间质;然而,通过给小鼠提供含碳酸氢盐的饮用水,可显著减少肾脏中的积聚。该肽有三种状态:溶于水、结合在膜表面以及以α螺旋形式插入膜中。在生理pH值下,平衡倾向于水相,这解释了其对健康组织中细胞的低亲和力;在酸性pH值下,天冬氨酸残基的滴定使平衡向膜插入和组织积聚方向移动。将pHLIP跨膜部分的两个关键天冬氨酸残基替换为赖氨酸或天冬酰胺,导致其在体内对脂质体、红细胞和癌细胞膜的pH敏感插入丧失,以及在肿瘤中的特异性积聚丧失。pHLIP纳米技术引入了一种利用膜肽的选择性插入和折叠来检测、靶向并可能治疗酸性疾病组织的新方法。