Hydroxyl radicals (•OH) play a crucial role in the fate of redox-active substances in the environment. Studies of the •OH production in nature has been constrained to surface environments exposed to light irradiation, but is overlooked in the subsurface under dark. Results of this study demonstrate that abundant •OH is produced when subsurface sediments are oxygenated under fluctuating redox conditions at neutral pH values. The cumulative concentrations of •OH produced within 24 h upon oxygenation of 33 sediments sampled from different redox conditions are 2-670 μmol •OH per kg dry sediment or 6.7-2521 μM •OH in sediment pore water. Fe(II)-containing minerals, particularly phyllosilicates, are the predominant contributor to •OH production. This production could be sustainable when sediment Fe(II) is regenerated by the biological reduction of Fe(III) during redox cycles. Production of •OH is further evident in a field injection-extraction test through injecting oxygenated water into a 23-m depth aquifer. The •OH produced can oxidize pollutants such as arsenic and tetracycline and contribute to CO2 emissions at levels that are comparable with soil respiration. These findings indicate that oxygenation of subsurface sediments is an important source of •OH in nature that has not been previously identified, and •OH-mediated oxidation represents an overlooked process for substance transformations at the oxic/anoxic interface.
Reduction by Fe(II)-bearing silicate minerals has been proposed as an important mechanism for the attenuation of chlorinated hydrocarbons (CHCs) in anoxic subsurfaces. The redox condition of subsurface often changes from anoxic to oxic due to natural processes and human activities, but little is known about the transformation of CHCs induced by Fe(II)-bearing silicate minerals under oxic conditions. This study reveals that trichloroethylene (TCE) can be efficiently oxidized during the oxygenation of reduced nontronite at pH 7.5, whereas the reduction was negligible under anoxic conditions. The maximum oxidation of TCE (initially 1 mg/L) attained 89.6% for 3 h oxygenation of 2 g/L nontronite with 50% reduction extent. TCE oxidation is attributed to the strongly oxidizing hydroxyl radicals (OH) produced by the oxygenation of Fe(II) in nontronite. Fe(II) on the edges is preferentially oxygenated for OH production, and the interior Fe(II) serves as an electron pool to regenerate the Fe(II) on the edges. Oxidation of TCE could be sustainable through chemically or biologically reducing the oxidized silicate minerals. Our findings present a new mechanism for the transformation of CHCs and other redox-active substances in the redox-fluctuation environments.
The integration of strapdown inertial navigation system and Doppler velocity log (SINS/DVL) is widely used for navigation in automatic underwater vehicles (AUVs). In the integration of SINS/DVL, the velocity measured by DVL in body frame should be projected into navigation frame with the help of attitude matrix calculated by SINS to participate in data fusion. In the process of data fusion based on standard Kalman filter, the errors in calculated attitude matrix are characterized by state variance and process noise while the errors in measurement vector from DVL are by measurement noise. But the above projection will bring process noise into measurement noise, and thus the assumption of the independence between process noise and measurement noise will not stand. In this paper, the forming mechanism of cross-noise in SINS/DVL is studied in detail and Kalman filter for cross-noise is introduced to deal with this problem. Simulation results indicate that navigation accuracy, especially the position accuracy, can be improved when the cross-noise is processed in Kalman filter.
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