Bastian N R, Kay C J, Barber M J, Rajagopalan K V
Department of Biochemistry, Duke University Medical Center, Durham, North Carolina 27710.
J Biol Chem. 1991 Jan 5;266(1):45-51.
Absorption and EPR spectroscopic properties of purified dimethyl sulfoxide (Me2SO) reductase from Rhodobacter sphaeroides f. sp. denitrificans have been examined. The absence of prosthetic groups other than the molybdenum center in the enzyme has made it possible to study its absorption properties. The enzyme displays multiple absorbance peaks in both the oxidized and the dithionite-reduced forms. The oxidized enzyme has absorbance peaks at 280, 350, 470, 550, and 720 nm while the dithionite-reduced enzyme has peaks at 280, 374, and 645 nm with a shoulder at 430 nm. A comparison of the absorbance spectrum of oxidized Me2SO reductase with that of the molybdenum fragment of rat liver sulfite oxidase shows that the 350 and 470 peaks are common to both proteins. EPR studies of the Mo(V) form of Me2SO reductase show a rhombic signal with g1 = 1.988, g2 = 1.977, g3 = 1.961, and g(ave) = 1.975. The signal shows evidence of coupling to an exchangeable proton with A1 = 1.05, A2 = 1.13, A3 = 0.98, and Aave = 1.05 millitesla. These parameters are similar to those of other Mo enzymes, however, the epr signal of this enzyme differs from those of other Mo hydroxylases in showing only a slight sensitivity to pH and no detectable anion effect. EPR potentiometric titrations of Me2SO reductase gave midpoint potentials of +144 mV for the Mo(VI)/Mo(V) couple and +160 mV for the Mo(V)/Mo(IV) couple at room temperature and +141 mV for the Mo(VI)/Mo(V) couple and +200 mV for the Mo(V)/Mo(IV) couple at 173 K.
对来自球形红杆菌反硝化亚种的纯化二甲基亚砜(Me2SO)还原酶的吸收和电子顺磁共振(EPR)光谱性质进行了研究。该酶中除钼中心外不存在其他辅基,这使得研究其吸收性质成为可能。该酶在氧化态和连二亚硫酸盐还原态下均显示出多个吸光度峰。氧化态酶在280、350、470、550和720 nm处有吸光度峰,而连二亚硫酸盐还原态酶在280、374和645 nm处有峰,在430 nm处有一个肩峰。将氧化态Me2SO还原酶的吸收光谱与大鼠肝脏亚硫酸盐氧化酶的钼片段的吸收光谱进行比较,结果表明350和470 nm处的峰是这两种蛋白质共有的。对Me2SO还原酶的Mo(V)形式进行的EPR研究显示出一个菱形信号,g1 = 1.988,g2 = 1.977,g3 = 1.961,g(ave) = 1.975。该信号显示出与一个可交换质子偶合的证据,A1 = 1.05,A2 = 1.13,A3 = 0.98,Aave = 1.05毫特斯拉。这些参数与其他钼酶的参数相似,然而,该酶的EPR信号与其他钼羟化酶的信号不同,仅对pH有轻微敏感性,且未检测到阴离子效应。在室温下,Me2SO还原酶的EPR电位滴定给出Mo(VI)/Mo(V)电对的中点电位为 +144 mV,Mo(V)/Mo(IV)电对的中点电位为 +160 mV;在173 K时,Mo(VI)/Mo(V)电对的中点电位为 +141 mV,Mo(V)/Mo(IV)电对的中点电位为 +200 mV。