Boyd Jeffrey M, Ellsworth Ashley, Ensign Scott A
Department of Chemistry and Biochemistry, Utah State University, 0300 Old Main Hill, Logan, UT 84322, USA.
J Bacteriol. 2006 Dec;188(23):8062-9. doi: 10.1128/JB.00947-06. Epub 2006 Sep 22.
Bacterial growth with short-chain aliphatic alkenes requires coenzyme M (CoM) (2-mercaptoethanesulfonic acid), which serves as the nucleophile for activation and conversion of epoxide products formed from alkene oxidation to central metabolites. In the present work the CoM analog 2-bromoethanesulfonate (BES) was shown to be a specific inhibitor of propylene-dependent growth of and epoxypropane metabolism by Xanthobacter autotrophicus strain Py2. BES (at low [millimolar] concentrations) completely prevented growth with propylene but had no effect on growth with acetone or n-propanol. Propylene consumption by cells was largely unaffected by the presence of BES, but epoxypropane accumulated in the medium in a time-dependent fashion with BES present. The addition of BES to cells resulted in time-dependent loss of epoxypropane degradation activity that was restored upon removal of BES and addition of CoM. Exposure of cells to BES resulted in a loss of epoxypropane-dependent CO(2) fixation activity that was restored only upon synthesis of new protein. Addition of BES to cell extracts resulted in an irreversible loss of epoxide carboxylase activity that was restored by addition of purified 2-ketopropyl-CoM carboxylase/oxidoreductase (2-KPCC), the terminal enzyme of epoxide carboxylation, but not by addition of epoxyalkane:CoM transferase or 2-hydroxypropyl-CoM dehydrogenase, the enzymes which catalyze the first two reactions of epoxide carboxylation. Comparative studies of the propylene-oxidizing actinomycete Rhodococcus rhodochrous strain B276 showed that BES is an inhibitor of propylene-dependent growth in this organism as well but is not an inhibitor of CoM-independent growth with propane. These results suggest that BES inhibits propylene-dependent growth and epoxide metabolism via irreversible inactivation of the key CO(2)-fixing enzyme 2-KPCC.
利用短链脂肪族烯烃进行细菌生长需要辅酶M(CoM,2-巯基乙烷磺酸),它作为亲核试剂,用于激活由烯烃氧化形成的环氧化物产物并将其转化为中心代谢物。在本研究中,CoM类似物2-溴乙烷磺酸盐(BES)被证明是自养黄色杆菌Py2菌株依赖丙烯生长及环氧丙烷代谢的特异性抑制剂。BES(在低[毫摩尔]浓度下)完全抑制了以丙烯为底物的生长,但对以丙酮或正丙醇为底物的生长没有影响。细胞对丙烯的消耗在很大程度上不受BES存在的影响,但在有BES存在时,环氧丙烷会以时间依赖性方式在培养基中积累。向细胞中添加BES会导致环氧丙烷降解活性随时间丧失,去除BES并添加CoM后该活性得以恢复。细胞暴露于BES会导致环氧丙烷依赖性CO₂固定活性丧失,只有合成新蛋白质后该活性才能恢复。向细胞提取物中添加BES会导致环氧羧化酶活性不可逆丧失,添加纯化的2-酮丙基-CoM羧化酶/氧化还原酶(2-KPCC,环氧羧化的末端酶)可恢复该活性,但添加环氧烷:CoM转移酶或2-羟丙基-CoM脱氢酶(催化环氧羧化前两个反应的酶)则不能恢复。对氧化丙烯的放线菌红平红球菌B276菌株的比较研究表明,BES也是该生物体中依赖丙烯生长的抑制剂,但不是丙烷非依赖CoM生长的抑制剂。这些结果表明,BES通过关键的CO₂固定酶2-KPCC的不可逆失活来抑制依赖丙烯的生长和环氧化物代谢。