From the Department of Pharmacology and Chemical Biology, University of Pittsburgh School of Medicine, Pittsburgh, Pennsylvania 15261.
the Department of Chemistry, Rutgers, the State University of New Jersey, Newark, New Jersey 07102.
J Biol Chem. 2018 Aug 24;293(34):13204-13213. doi: 10.1074/jbc.RA118.003996. Epub 2018 Jul 3.
The pyruvate dehydrogenase multienzyme complex (PDHc) connects glycolysis to the tricarboxylic acid cycle by producing acetyl-CoA via the decarboxylation of pyruvate. Because of its pivotal role in glucose metabolism, this complex is closely regulated in mammals by reversible phosphorylation, the modulation of which is of interest in treating cancer, diabetes, and obesity. Mutations such as that leading to the αV138M variant in pyruvate dehydrogenase, the pyruvate-decarboxylating PDHc E1 component, can result in PDHc deficiency, an inborn error of metabolism that results in an array of symptoms such as lactic acidosis, progressive cognitive and neuromuscular deficits, and even death in infancy or childhood. Here we present an analysis of two X-ray crystal structures at 2.7-Å resolution, the first of the disease-associated human αV138M E1 variant and the second of human wildtype (WT) E1 with a bound adduct of its coenzyme thiamin diphosphate and the substrate analogue acetylphosphinate. The structures provide support for the role of regulatory loop disorder in E1 inactivation, and the αV138M variant structure also reveals that altered coenzyme binding can result in such disorder even in the absence of phosphorylation. Specifically, both E1 phosphorylation at αSer-264 and the αV138M substitution result in disordered loops that are not optimally oriented or available to efficiently bind the lipoyl domain of PDHc E2. Combined with an analysis of αV138M activity, these results underscore the general connection between regulatory loop disorder and loss of E1 catalytic efficiency.
丙酮酸脱氢酶多酶复合物(PDHc)通过丙酮酸脱羧生成乙酰辅酶 A 将糖酵解与三羧酸循环联系起来。由于其在葡萄糖代谢中的关键作用,该复合物在哺乳动物中受到可逆磷酸化的紧密调节,对其调节在治疗癌症、糖尿病和肥胖症方面具有重要意义。 例如,导致丙酮酸脱氢酶中αV138M 变体的突变,即丙酮酸脱羧 PDHc E1 成分,可导致 PDHc 缺乏,这是一种先天性代谢错误,可导致一系列症状,如乳酸酸中毒、进行性认知和神经肌肉缺陷,甚至在婴儿或儿童期死亡。在这里,我们展示了两个 2.7-Å 分辨率的 X 射线晶体结构分析,第一个是与疾病相关的人类αV138M E1 变体,第二个是与人野生型(WT)E1 的结构,其中包含其辅酶硫胺素二磷酸和底物类似物乙酰膦酸盐的结合物。这些结构为 E1 失活中调节环无序的作用提供了支持,并且αV138M 变体结构还表明,即使没有磷酸化,辅酶结合的改变也会导致这种无序。具体来说,E1 在αSer-264 的磷酸化以及αV138M 取代都会导致无序环,这些环不能最佳定向或有效结合 PDHc E2 的脂酰基结构域。结合对αV138M 活性的分析,这些结果强调了调节环无序与 E1 催化效率丧失之间的普遍联系。