Kubata Bruno Kilunga, Kabututu Zakayi, Nozaki Tomoyoshi, Munday Craig J, Fukuzumi Shunichi, Ohkubo Kei, Lazarus Michael, Maruyama Toshihiko, Martin Samuel K, Duszenko Michael, Urade Yoshihiro
Department of Molecular Behavioral Biology, Osaka Bioscience Institute, Osaka 565-0874, Japan.
J Exp Med. 2002 Nov 4;196(9):1241-51. doi: 10.1084/jem.20020885.
Trypanosoma cruzi is the etiological agent of Chagas' disease. So far, first choice anti-chagasic drugs in use have been shown to have undesirable side effects in addition to the emergence of parasite resistance and the lack of prospect for vaccine against T. cruzi infection. Thus, the isolation and characterization of molecules essential in parasite metabolism of the anti-chagasic drugs are fundamental for the development of new strategies for rational drug design and/or the improvement of the current chemotherapy. While searching for a prostaglandin (PG) F(2alpha) synthase homologue, we have identified a novel "old yellow enzyme" from T. cruzi (TcOYE), cloned its cDNA, and overexpressed the recombinant enzyme. Here, we show that TcOYE reduced 9,11-endoperoxide PGH(2) to PGF(2alpha) as well as a variety of trypanocidal drugs. By electron spin resonance experiments, we found that TcOYE specifically catalyzed one-electron reduction of menadione and beta-lapachone to semiquinone-free radicals with concomitant generation of superoxide radical anions, while catalyzing solely the two-electron reduction of nifurtimox and 4-nitroquinoline-N-oxide drugs without free radical production. Interestingly, immunoprecipitation experiments revealed that anti-TcOYE polyclonal antibody abolished major reductase activities of the lysates toward these drugs, identifying TcOYE as a key drug-metabolizing enzyme by which quinone drugs have their mechanism of action.
克氏锥虫是恰加斯病的病原体。到目前为止,已表明目前使用的首选抗锥虫病药物除了会出现寄生虫耐药性以及缺乏针对克氏锥虫感染的疫苗前景外,还具有不良副作用。因此,分离和鉴定抗锥虫病药物寄生虫代谢中必需的分子对于开发合理药物设计的新策略和/或改善当前化疗至关重要。在寻找前列腺素(PG)F(2α)合酶同源物时,我们从克氏锥虫中鉴定出一种新型的“老黄色酶”(TcOYE),克隆了其cDNA,并使重组酶过量表达。在此,我们表明TcOYE将9,11-内过氧化物PGH(2)还原为PGF(2α)以及多种杀锥虫药物。通过电子自旋共振实验,我们发现TcOYE特异性催化甲萘醌和β-拉帕醌单电子还原为半醌自由基,同时伴随超氧阴离子自由基的产生,而仅催化硝呋替莫和4-硝基喹啉-N-氧化物药物的双电子还原且不产生自由基。有趣的是,免疫沉淀实验表明,抗TcOYE多克隆抗体消除了裂解物对这些药物的主要还原酶活性,确定TcOYE是醌类药物发挥作用机制的关键药物代谢酶。