The flux of fluvial carbon from the terrestrial biosphere to the world's oceans is known to be an important component of the global carbon cycle, but within this pathway, the flux and return of carbon to the river network via sewage effluent has not been quantified. In this study, monitoring data from 2000 to 2016 for the dissolved organic carbon (DOC) concentration, biochemical oxygen demand, and chemical oxygen demand of the final effluent of sewage treatment works from across England were examined to assess the amount of DOC contributing to national‐scale fluvial fluxes of carbon. The study shows that the median concentration of DOC in final effluent was 9.4 compared with 4.8 mg C/L for all surface waters for the United Kingdom over the study period and that the DOC in final effluent significantly declined over the study period from 11.0 to 6.4 mg C/L. Rivers receiving sewage effluent showed a significant, on average 19%, increase in DOC concentration downstream of sewage discharges. At the scale of the United Kingdom, the flux of DOC in final effluent was 31 ktonnes C/year with a per capita export of 0.55 kg C/year and compared with an average annual flux of DOC from the United Kingdom of 859 ktonnes C/year, that is, only 3.6% of national‐scale flux. The lability of this DOC was limited, with only 7.4% loss of final effluent DOC concentration over in‐stream residence times of up to 5 days. The direct decline in DOC concentration from sewage treatment works was not large enough on its own to explain the declines observed in DOC concentration in U.K. rivers at their tidal limit. 相似文献
At sub‐arc depths, the release of carbon from subducting slab lithologies is mostly controlled by fluid released by devolatilization reactions such as dehydration of antigorite (Atg‐) serpentinite to prograde peridotite. Here we investigate carbonate–silicate rocks hosted in Atg‐serpentinite and prograde chlorite (Chl‐) harzburgite in the Milagrosa and Almirez ultramafic massifs of the palaeo‐subducted Nevado‐Filábride Complex (NFC, Betic Cordillera, S. Spain). These massifs provide a unique opportunity to study the stability of carbonate during subduction metamorphism at P–T conditions before and after the dehydration of Atg‐serpentinite in a warm subduction setting. In the Milagrosa massif, carbonate–silicate rocks occur as lenses of Ti‐clinohumite–diopside–calcite marbles, diopside–dolomite marbles and antigorite–diopside–dolomite rocks hosted in clinopyroxene‐bearing Atg‐serpentinite. In Almirez, carbonate–silicate rocks are hosted in Chl‐harzburgite and show a high‐grade assemblage composed of olivine, Ti‐clinohumite, diopside, chlorite, dolomite, calcite, Cr‐bearing magnetite, pentlandite and rare aragonite inclusions. These NFC carbonate–silicate rocks have variable CaO and CO2 contents at nearly constant Mg/Si ratio and high Ni and Cr contents, indicating that their protoliths were variable mixtures of serpentine and Ca‐carbonate (i.e., ophicarbonates). Thermodynamic modelling shows that the carbonate–silicate rocks attained peak metamorphic conditions similar to those of their host serpentinite (Milagrosa massif; 550–600°C and 1.0–1.4 GPa) and Chl‐harzburgite (Almirez massif; 1.7–1.9 GPa and 680°C). Microstructures, mineral chemistry and phase relations indicate that the hybrid carbonate–silicate bulk rock compositions formed before prograde metamorphism, likely during seawater hydrothermal alteration, and subsequently underwent subduction metamorphism. In the CaO–MgO–SiO2 ternary, these processes resulted in a compositional variability of NFC serpentinite‐hosted carbonate–silicate rocks along the serpentine‐calcite mixing trend, similar to that observed in serpentinite‐hosted carbonate‐rocks in other palaeo‐subducted metamorphic terranes. Thermodynamic modelling using classical models of binary H2O–CO2 fluids shows that the compositional variability along this binary determines the temperature of the main devolatilization reactions, the fluid composition and the mineral assemblages of reaction products during prograde subduction metamorphism. Thermodynamic modelling considering electrolytic fluids reveals that H2O and molecular CO2 are the main fluid species and charged carbon‐bearing species occur only in minor amounts in equilibrium with carbonate–silicate rocks in warm subduction settings. Consequently, accounting for electrolytic fluids at these conditions slightly increases the solubility of carbon in the fluids compared with predictions by classical binary H2O–CO2 fluids, but does not affect the topology of phase relations in serpentinite‐hosted carbonate‐rocks. Phase relations, mineral composition and assemblages of Milagrosa and Almirez (meta)‐serpentinite‐hosted carbonate–silicate rocks are consistent with local equilibrium between an infiltrating fluid and the bulk rock composition and indicate a limited role of infiltration‐driven decarbonation. Our study shows natural evidence for the preservation of carbonates in serpentinite‐hosted carbonate–silicate rocks beyond the Atg‐serpentinite breakdown at sub‐arc depths, demonstrating that carbon can be recycled into the deep mantle. 相似文献