Shuck Sarah C, Wauchope Orrette R, Rose Kristie L, Kingsley Philip J, Rouzer Carol A, Shell Steven M, Sugitani Norie, Chazin Walter J, Zagol-Ikapitte Irene, Boutaud Olivier, Oates John A, Galligan James J, Beavers William N, Marnett Lawrence J
A. B. Hancock Jr. Memorial Laboratory for Cancer Research, Departments of Biochemistry, ‡Chemistry, and §Pharmacology, ∥Mass Spectrometry Research Center, ⊥Center in Molecular Toxicology, #Center for Structural Biology, ∇Department of Medicine, Vanderbilt Institute of Chemical Biology, and Vanderbilt-Ingram Cancer Center, Vanderbilt University School of Medicine , Nashville, Tennessee 37232-0146, United States.
Chem Res Toxicol. 2014 Oct 20;27(10):1732-42. doi: 10.1021/tx500218g. Epub 2014 Sep 24.
Base propenals are products of the reaction of DNA with oxidants such as peroxynitrite and bleomycin. The most reactive base propenal, adenine propenal, is mutagenic in Escherichia coli and reacts with DNA to form covalent adducts; however, the reaction of adenine propenal with protein has not yet been investigated. A survey of the reaction of adenine propenal with amino acids revealed that lysine and cysteine form adducts, whereas histidine and arginine do not. N(ε)-Oxopropenyllysine, a lysine-lysine cross-link, and S-oxopropenyl cysteine are the major products. Comprehensive profiling of the reaction of adenine propenal with human serum albumin and the DNA repair protein, XPA, revealed that the only stable adduct is N(ε)-oxopropenyllysine. The most reactive sites for modification in human albumin are K190 and K351. Three sites of modification of XPA are in the DNA-binding domain, and two sites are subject to regulatory acetylation. Modification by adenine propenal dramatically reduces XPA's ability to bind to a DNA substrate.
碱基丙烯醛是DNA与过氧亚硝酸盐和博来霉素等氧化剂反应的产物。反应活性最高的碱基丙烯醛,即腺嘌呤丙烯醛,在大肠杆菌中具有致突变性,并与DNA反应形成共价加合物;然而,腺嘌呤丙烯醛与蛋白质的反应尚未得到研究。一项关于腺嘌呤丙烯醛与氨基酸反应的调查显示,赖氨酸和半胱氨酸会形成加合物,而组氨酸和精氨酸则不会。赖氨酸-赖氨酸交联物N(ε)-氧代丙烯基赖氨酸和S-氧代丙烯基半胱氨酸是主要产物。对腺嘌呤丙烯醛与人血清白蛋白和DNA修复蛋白XPA反应的全面分析表明,唯一稳定的加合物是N(ε)-氧代丙烯基赖氨酸。人白蛋白中最易发生修饰的位点是K190和K351。XPA的三个修饰位点位于DNA结合结构域,两个位点会发生调节性乙酰化。腺嘌呤丙烯醛的修饰显著降低了XPA与DNA底物结合的能力。