Wang Shanzhi, Sura Giri R, Dangott Lawrence J, Fitzpatrick Paul F
Department of Biochemistry and Biophysics, Texas A&M University, College Station, Texas 77843-2128, USA.
Biochemistry. 2009 Jun 9;48(22):4972-9. doi: 10.1021/bi9004254.
The activity of tyrosine hydroxylase is regulated by reversible phosphorylation of serine residues in an N-terminal regulatory domain and catecholamine inhibition at the active site. Catecholamines such as dopamine bind very tightly to the resting enzyme; phosphorylation of Ser40 decreases the affinity for catecholamines by 3 orders of magnitude. The effects of dopamine binding and phosphorylation of Ser40 on the kinetics of deuterium incorporation into peptide bonds were examined by mass spectrometry. When dopamine is bound, three peptic peptides show significantly slower deuterium incorporation, 35-41 and 42-71 in the regulatory domain and 295-299 in the catalytic domain. In the phosphorylated enzyme, peptide 295-299 shows more rapid incorporation of deuterium, while 35-41 and 42-71 can not be detected. These results are consistent with tyrosine hydroxylase existing in two different conformations. In the closed conformation, the regulatory domain lies across the active site loop containing residues 295-298; this is stabilized when dopamine is bound in the active site. In the open conformation, the regulatory domain has moved out of the active site, allowing substrate access; this conformation is favored by phosphorylation of Ser40.
酪氨酸羟化酶的活性受N端调节结构域中丝氨酸残基的可逆磷酸化以及活性位点处儿茶酚胺抑制的调控。多巴胺等儿茶酚胺与静息酶紧密结合;Ser40的磷酸化使对儿茶酚胺的亲和力降低3个数量级。通过质谱研究了多巴胺结合和Ser40磷酸化对肽键中氘掺入动力学的影响。当多巴胺结合时,三条胃蛋白酶肽段的氘掺入明显减慢,调节结构域中的35 - 41和42 - 71以及催化结构域中的295 - 299。在磷酸化酶中,肽段295 - 299的氘掺入更快,而35 - 41和42 - 71无法检测到。这些结果与酪氨酸羟化酶以两种不同构象存在一致。在闭合构象中,调节结构域横跨包含295 - 298残基的活性位点环;当多巴胺结合在活性位点时,这种构象得以稳定。在开放构象中,调节结构域已移出活性位点,允许底物进入;这种构象受Ser40磷酸化的青睐。