Dai MingHua, Rogers Julie Bull, Warner Joseph R, Copley Shelley D
Department of Molecular, Cellular, and Developmental Biology, and Cooperative Institute for Research in Environmental Sciences, University of Colorado at Boulder, Boulder, CO 80309, USA.
J Bacteriol. 2003 Jan;185(1):302-10. doi: 10.1128/JB.185.1.302-310.2003.
The first step in the pentachlorophenol (PCP) degradation pathway in Sphingobium chlorophenolicum has been believed for more than a decade to be conversion of PCP to tetrachlorohydroquinone. We show here that PCP is actually converted to tetrachlorobenzoquinone, which is subsequently reduced to tetrachlorohydroquinone by PcpD, a protein that had previously been suggested to be a PCP hydroxylase reductase. pcpD is immediately downstream of pcpB, the gene encoding PCP hydroxylase (PCP monooxygenase). Expression of PcpD is induced in the presence of PCP. A mutant strain lacking functional PcpD has an impaired ability to remove PCP from the medium. In contrast, the mutant strain removes tetrachlorophenol from the medium at the same rate as does the wild-type strain. These data suggest that PcpD catalyzes a step necessary for degradation of PCP, but not for degradation of tetrachlorophenol. Based upon the known mechanisms of flavin monooxygenases such as PCP hydroxylase, hydroxylation of PCP should produce tetrachlorobenzoquinone, while hydroxylation of tetrachlorophenol should produce tetrachlorohydroquinone. Thus, we proposed and verified experimentally that PcpD is a tetrachlorobenzoquinone reductase that catalyzes the NADPH-dependent reduction of tetrachlorobenzoquinone to tetrachlorohydroquinone.
十多年来,人们一直认为,在嗜氯鞘氨醇菌中,五氯苯酚(PCP)降解途径的第一步是PCP转化为四氯对苯二酚。我们在此表明,PCP实际上转化为四氯苯醌,随后四氯苯醌被PcpD还原为四氯对苯二酚,PcpD是一种之前被认为是PCP羟化酶还原酶的蛋白质。pcpD位于pcpB的下游紧邻位置,pcpB是编码PCP羟化酶(PCP单加氧酶)的基因。在PCP存在的情况下,PcpD的表达被诱导。缺乏功能性PcpD的突变菌株从培养基中去除PCP的能力受损。相比之下,该突变菌株从培养基中去除四氯苯酚的速率与野生型菌株相同。这些数据表明,PcpD催化PCP降解所必需的一步,但不是四氯苯酚降解所必需的一步。基于已知的黄素单加氧酶(如PCP羟化酶)的机制,PCP的羟基化应产生四氯苯醌,而四氯苯酚的羟基化应产生四氯对苯二酚。因此,我们提出并通过实验验证,PcpD是一种四氯苯醌还原酶,催化依赖于NADPH的四氯苯醌还原为四氯对苯二酚。