Division of Child Development, Rehabilitation Medicine, and Metabolic Disease, Children's Hospital of Philadelphia, Philadelphia, Pennsylvania 19104, USA.
J Biol Chem. 2011 Jun 24;286(25):22055-68. doi: 10.1074/jbc.M110.209023. Epub 2011 May 3.
We previously reported that isobutylmethylxanthine (IBMX), a derivative of oxypurine, inhibits citrulline synthesis by an as yet unknown mechanism. Here, we demonstrate that IBMX and other oxypurines containing a 2,6-dione group interfere with the binding of glutamate to the active site of N-acetylglutamate synthetase (NAGS), thereby decreasing synthesis of N-acetylglutamate, the obligatory activator of carbamoyl phosphate synthase-1 (CPS1). The result is reduction of citrulline and urea synthesis. Experiments were performed with (15)N-labeled substrates, purified hepatic CPS1, and recombinant mouse NAGS as well as isolated mitochondria. We also used isolated hepatocytes to examine the action of various oxypurines on ureagenesis and to assess the ameliorating affect of N-carbamylglutamate and/or l-arginine on NAGS inhibition. Among various oxypurines tested, only IBMX, xanthine, or uric acid significantly increased the apparent K(m) for glutamate and decreased velocity of NAGS, with little effect on CPS1. The inhibition of NAGS is time- and dose-dependent and leads to decreased formation of the CPS1-N-acetylglutamate complex and consequent inhibition of citrulline and urea synthesis. However, such inhibition was reversed by supplementation with N-carbamylglutamate. The data demonstrate that xanthine and uric acid, both physiologically occurring oxypurines, inhibit the hepatic synthesis of N-acetylglutamate. An important and novel concept emerging from this study is that xanthine and/or uric acid may have a role in the regulation of ureagenesis and, thus, nitrogen homeostasis in normal and disease states.
我们之前报道过,异丁基甲基黄嘌呤(IBMX)是一种黄嘌呤衍生物,通过一种未知的机制抑制瓜氨酸的合成。在这里,我们证明 IBMX 和其他含有 2,6-二酮基团的黄嘌呤干扰谷氨酸与 N-乙酰谷氨酸合酶(NAGS)活性位点的结合,从而减少 N-乙酰谷氨酸的合成,N-乙酰谷氨酸是氨甲酰磷酸合成酶-1(CPS1)的必需激活剂。其结果是瓜氨酸和尿素合成减少。实验使用(15)N 标记的底物、纯化的肝 CPS1 和重组小鼠 NAGS 以及分离的线粒体进行。我们还使用分离的肝细胞来研究各种黄嘌呤对尿素生成的作用,并评估 N-氨甲酰谷氨酸和/或 l-精氨酸对 NAGS 抑制的改善作用。在测试的各种黄嘌呤中,只有 IBMX、黄嘌呤或尿酸显著增加了谷氨酸的表观 K(m)并降低了 NAGS 的速度,对 CPS1 的影响很小。NAGS 的抑制作用是时间和剂量依赖性的,导致 CPS1-N-乙酰谷氨酸复合物的形成减少,从而抑制瓜氨酸和尿素的合成。然而,这种抑制作用可以通过补充 N-氨甲酰谷氨酸来逆转。这些数据表明,黄嘌呤和尿酸,这两种生理上存在的黄嘌呤,抑制肝 N-乙酰谷氨酸的合成。本研究提出的一个重要而新颖的概念是,黄嘌呤和/或尿酸可能在尿素生成的调节中发挥作用,从而在正常和疾病状态下维持氮平衡。