Copper availability governs nitrous oxide accumulation in wetland soils and stream sediments

Sharma, Neha; Flynn, Elaine D.; Catalano, Jeffrey G.; Giammar, Daniel E.

doi:10.1016/j.gca.2022.04.019

Copper availability governs nitrous oxide accumulation in wetland soils and stream sediments

Journal Article · Tue Apr 26 00:00:00 EDT 2022 · Geochimica et Cosmochimica Acta

DOI:https://doi.org/10.1016/j.gca.2022.04.019· OSTI ID:1868027

Sharma, Neha ^[1]; Flynn, Elaine D. ^[1]; ^[1]; ^[1]

Washington Univ., St. Louis, MO (United States)

Denitrification is microbially-mediated through enzymes containing metal cofactors. Laboratory studies of pure cultures have highlighted that the availability of Cu, required for the multicopper enzyme nitrous oxide reductase, can limit N2O reduction. However, in natural aquatic systems, such as wetlands and hyporheic zones in stream beds, the role of Cu in controlling denitrification remains incompletely understood. In this study, we collected soils and sediments from three natural environments -- riparian wetlands, marsh wetlands, and a stream -- to investigate their nitrogen species transformation activity at background Cu levels and different supplemented Cu loadings. All of the systems contained solid-phase associated Cu below or around geological levels (40 - 280 nmol g-1) and exhibited low dissolved Cu (3-50 nM), which made them appropriate sites for evaluating the effect of limited Cu availability on denitrification. In laboratory incubation experiments, high concentrations of N2O accumulated in all microcosms lacking Cu amendment except for one stream sediment sample. With Cu added to provide dissolved concentrations at trace levels (10-300 nM), reduction rate of N2O to N₂ in the wetland soils and stream sediments was enhanced. A kinetic model could account for the trends in nitrogen species by combining the reactions for microbial reduction of NO₃- to NO₂-/N₂O/N₂ and abiotic reduction of NO₂- to N₂. The model revealed that the rate of N₂O to N₂ conversion increased significantly in the presence of Cu. For riparian wetland soils and stream sediments, the kinetic model also suggested that overall denitrification is driven by abiotic reduction of NO2- in the presence of inorganic electron donors. This study demonstrated that natural aquatic systems containing Cu at concentrations less than or equal to crustal abundances may display incomplete reduction of N₂O to N₂ that would cause N₂O accumulation and release to the atmosphere.

View Accepted Manuscript (DOE)

Research Organization:: Washington Univ., St. Louis, MO (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Biological and Environmental Research (BER). Earth and Environmental Systems Science Division

Grant/Contract Number:: SC0019422

OSTI ID:: 1868027

Journal Information:: Geochimica et Cosmochimica Acta, Vol. 327; ISSN 0016-7037

Publisher:: Elsevier; The Geochemical Society; The Meteoritical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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54 ENVIRONMENTAL SCIENCES
58 GEOSCIENCES
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
wetlands
hyporheic zone
denitrification
nitrous oxide
copper
bioavailability
organic carbon

Copper availability governs nitrous oxide accumulation in wetland soils and stream sediments

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