White Andrea K, Metcalf William W
Department of Microbiology, University of Illinois, Urbana, Illinois 61801, USA.
J Biol Chem. 2002 Oct 11;277(41):38262-71. doi: 10.1074/jbc.M204605200. Epub 2002 Aug 2.
The htxA gene is required for the oxidation of hypophosphite in Pseudomonas stutzeri WM88 (Metcalf, W. W., and Wolfe, R. S. (1998) J. Bacteriol. 180, 5547-5558). Amino acid sequence comparisons suggest that hypophosphite:2-oxoglutarate dioxygenase (HtxA) is a novel member of the 2-oxoglutarate-dependent dioxygenase enzyme family. To provide experimental support for this hypothesis, HtxA was overproduced in Escherichia coli and purified to apparent homogeneity. Recombinant HtxA is identical to the native enzyme based on amino terminus sequencing and mass spectral analysis, and it catalyzes the oxidation of hypophosphite to phosphite in a process strictly dependent on 2-oxoglutarate, ferrous ions, and oxygen. Succinate and phosphite are stoichiometrically produced, indicating a strict coupling of the reaction. Size exclusion analysis suggests that HtxA is active as a homodimer, and maximal activity is observed at pH 7.0 and at 27 degrees C. The apparent K(m) values for hypophosphite and 2-oxoglutarate were 0.58 +/- 0.04 mm and 10.6 +/- 1.4 microm, respectively. V(max) and k(cat) values were determined to be 10.9 +/- 0.30 micromol min(-1) mg(-1) and 355 min(-1), respectively. 2-Oxoadipate and pyruvate substitute poorly for 2-oxoglutarate as a cosubstrate. The highest specific activity is observed with hypophosphite as substrate, but HtxA is also able to oxidize formate and arsenite at significant rates. The substrate analog inhibitors, formate and nitrate, significantly reduce HtxA activity.
htxA基因是斯氏假单胞菌WM88中次磷酸盐氧化所必需的基因(梅特卡夫,W.W.,和沃尔夫,R.S.(1998年)《细菌学杂志》180,5547 - 5558)。氨基酸序列比较表明,次磷酸盐:2 - 氧代戊二酸双加氧酶(HtxA)是2 - 氧代戊二酸依赖性双加氧酶家族的一个新成员。为了为这一假设提供实验支持,HtxA在大肠杆菌中过量表达并纯化至表观均一性。基于氨基末端测序和质谱分析,重组HtxA与天然酶相同,并且它在一个严格依赖于2 - 氧代戊二酸、亚铁离子和氧气的过程中催化次磷酸盐氧化为亚磷酸盐。化学计量地产生琥珀酸和亚磷酸盐,表明反应严格偶联。尺寸排阻分析表明HtxA作为同型二聚体具有活性,并且在pH 7.0和27℃时观察到最大活性。次磷酸盐和2 - 氧代戊二酸的表观K(m)值分别为0.58±0.04 mM和10.6±1.4 μM。V(max)和k(cat)值分别测定为10.9±0.30 μmol min(-1) mg(-1)和355 min(-1)。2 - 氧代己二酸和丙酮酸作为共底物替代2 - 氧代戊二酸的效果较差。以次磷酸盐为底物时观察到最高的比活性,但HtxA也能够以显著的速率氧化甲酸和亚砷酸盐。底物类似物抑制剂,甲酸和硝酸盐,显著降低HtxA活性。