The biocatalytic activity of nitroreductase from Salmonella typhimurium (NRSal) was investigated for the reduction of alpha,beta-unsaturated carbonyl compounds, nitroalkenes, and nitroaromatics. The synthesized gene was subcloned into a pET28 overexpression system in E.coli BL21 strain, and the corresponding expressed protein was purified to homogeneity with 15% protein mass yield and 41% of total activity recovery. NRSal showed broad substrate acceptance for various nitro compounds such as 1-nitrocyclohexene and aliphatic nitroalkenes (alkene reductase activity), as well as nitrobenzene (nitroreductase activity), with substrate conversion efficiency of > 95%. However, the reduction of enones was generally low, proceeding albeit with high stereoselectivity. The efficient biocatalytic reduction of substituted nitroalkenes provides a route for the preparation of the corresponding nitroalkanes. NRSal also demonstrated the first single isolated enzyme-catalyzed reduction of nitrobenzene to aniline through the formation of nitrosobenzene and phenylhydroxylamine as intermediates. However, chemical condensation of the two intermediates to produce azoxybenzene currently limits the yield of aniline.
Asymmetric trans-bioreduction of activated alkenes by KYE1 from Kluyveromyces lactis and Yers-ER from Yersinia bercovieri, two ene-reductases from the Old Yellow Enzyme family, showed a broad substrate spectrum with a moderate to excellent degree of stereoselectivity. Both substrate- and enzyme-based stereocontrols were observed to furnish opposite stereoisomeric products. The effects of organic solvents on enzyme activity and stereoselectivity were outlined in this study, where two-phase systems hexane and toluene are shown to sustain bioreduction efficiency even at high organic solvent content.
Recent studies have linked interannual sea level variability and extreme events along the U.S. northeast coast (NEC) to the North Atlantic Oscillation (NAO), a natural internal climate mode that prevails in the North Atlantic Ocean. The correlation between the NAO index and coastal sea level north of Cape Hatteras was weak from the 1960s to the mid-1980s, but it has markedly increased since around 1987. The causes for the decadal shift remain unknown. Yet understanding the abrupt change is vital for decadal sea level prediction and is essential for risk management. Here we use a robust method, the Bayesian dynamic linear model (DLM), to explore the nonstationary NAO impact on NEC sea level. The results show that a spatial pattern change of NAO-related winds near the NEC is a major cause of the NAO–sea level relationship shift. A new index using regional sea level pressure is developed that is a significantly better predictor of NEC sea level than is the NAO and is strongly linked to the intensity of westerly winds near the NEC. These results point to the vital importance of monitoring regional changes of wind and sea level pressure patterns, rather than the NAO index alone, to achieve more accurate predictions of sea level change along the NEC.
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