BACKGROUND: Rivers and streams are important components of the global carbon cycle and methane budget. However, our understanding of the microbial diversity and the metabolic pathways underpinning methylotrophic methane production in river sediments is limited. Dimethylsulfide is an important methylated compound, found in freshwater sediments. Yet, the magnitude of DMS-dependent methanogenesis nor the methanogens carrying out this process in river sediments have been explored before. This study addressed this knowledge gap in DMS-dependent methanogenesis in gravel and sandy river sediments.
RESULTS: Significant methane production via DMS degradation was found in all sediment  microcosms. Sandy, less permeable river sediments had higher methane yields (83 and 92%) than gravel, permeable sediments (40 and 48%). There was no significant difference between the methanogen diversity in DMS-amended gravel and sandy sediment microcosms, which Methanomethylovorans dominated. Metagenomics data analysis also showed the dominance of Methanomethylovorans and Methanosarcina. DMS-specific methyltransferase genes (mts) were found in very low relative abundances whilst the methanol-, trimethylamine- and dimethylamine-specific methyltransferase genes (mtaA, mttB and mtbB) had the highest relative abundances, suggesting their involvement in DMS-dependent methanogenesis.
CONCLUSIONS: This is the first study demonstrating a significant potential for DMS-dependent methanogenesis in river sediments with contrasting geologies. Methanomethylovorans were the dominant methylotrophic methanogen in all river sediment microcosms. Methyltransferases specific to methylotrophic substrates other than DMS are likely key enzymes in DMS-dependent methanogenesis, highlighting their versatility and importance in the methane cycle in freshwater sediments, which would warrant further study.

Dimethylsulfoniopropionate (DMSP), a key organic sulfur compound in marine and subseafloor sediments, is degraded by phytoplankton and bacteria, resulting in the release of the climate-active volatile gas dimethylsulfide (DMS). However, it remains unclear if dominant eukaryotic fungi in subseafloor sediments possess specific abilities and metabolic mechanisms for DMSP degradation and DMS formation. Our study provides the first evidence that fungi from coal-bearing sediments ∼2 km below the seafloor, such as Aspergillus spp., Chaetomium globosum, Cladosporium sphaerospermum, and Penicillium funiculosum, can degrade DMSP and produce DMS. In Aspergillus sydowii 29R-4-F02, which exhibited the highest DMSP-dependent DMS production rate (16.95 pmol/μg protein/min), two DMSP lyase genes, dddP and dddW, were identified. Remarkably, the dddW gene, previously observed only in bacteria, was found to be crucial for fungal DMSP cleavage. These findings not only extend the list of fungi capable of degrading DMSP, but also enhance our understanding of DMSP lyase diversity and the role of fungi in DMSP decomposition in subseafloor sedimentary ecosystems.

Phaeocystis antarctica forms extensive spring blooms in the Southern Ocean that coincide with high concentrations of dimethylsulfoniopropionate (DMSP), dimethylsulfoxide (DMSO), dimethylsulfide (DMS), and acrylate. We determined how concentrations of these compounds changed during the growth of axenic P. antarctica cultures exposed to light-limiting, sub-saturating, and saturating PAR irradiances. Cellular DMSP concentrations per liter cell volume (CV) ranged between 199 and 403 mmol · LCV -1 , with the highest concentrations observed under light-limiting PAR. Cellular acrylate concentrations did not change appreciably with a change in irradiance level or growth, ranging between 18 and 45 mmol · LCV -1 , constituting an estimated 0.2%-2.8% of cellular carbon. Both dissolved acrylate and DMSO increased substantially with irradiance during exponential growth on a per-cell basis, ranging from 0.91 to 3.15 and 0.24 to 1.39 fmol · cell-1 , respectively, indicating substantial export of these compounds into the dissolved phase. Average cellular DMSO:DMSP ratios increased 7.6-fold between exponential and stationary phases of batch growth, with a 3- to 13-fold increase in cellular DMSO likely formed from abiotic reactions of DMSP and DMS with reactive oxygen species (ROS). At mM levels, cellular DMSP and acrylate are proposed to serve as de facto antioxidants in P. antarctica not regulated by oxidative stress or changes in ROS. Instead, cellular DMSP concentrations are likely controlled by other physiological processes including an overflow mechanism to remove excess carbon via acrylate, DMS, and DMSO during times of unbalanced growth brought on by physical stress or nutrient limitation. Together, these compounds should aid P. antarctica in adapting to a range of PAR irradiances by maintaining cellular functions and reducing oxidative stress.

UNASSIGNED: Saltmarshes are hotspots of organosulfur compound cycling due to production of dimethylsulfoniopropionate (DMSP) by benthic microorganisms, macroalgae, and saltmarsh vegetation. Degradation of DMSP is a source of dimethylsulfide (DMS), an important precursor for formation of secondary organic aerosol. Microorganisms degrading DMS play a role in controlling the amount of DMS available for emission into the atmosphere. Previous work has implicated sediment microbial populations as a major sink for DMS. Here, we show that Sporobolus anglicus (previously known as Spartina anglica), a widely distributed saltmarsh plant, is colonized by DMS-degrading microorganisms.
UNASSIGNED: Dimethylsulfide degradation potential was assessed by gas chromatography and 13C-DMS stable isotope probing, microbial community diversity and functional genetic potential in phyllosphere and rhizosphere samples was assessed by high-throughput sequencing of 16S rRNA gene amplicons, cloning and sequencing of methanethiol oxidase genes, and by metagenomic analysis of phyllosphere microbial communities.
UNASSIGNED: The DMS degradation potential of microbial communities recovered from phyllosphere and rhizosphere samples was similar. Active DMS-degraders were identified by 13C-DMS stable isotope probing and included populations related to Methylophaga and other Piscirickettsiaceae in rhizosphere samples. DMS-degraders in the phyllosphere included Xanthomonadaceae and Halothiobacillaceae. The diversity in sediment samples of the methanethiol oxidase (mtoX) gene, a marker for metabolism of methanethiol during DMS and DMSP degradation, was similar to previously detected saltmarsh mtoX, including those of Methylophaga and Methylococcaeae. Phyllosphere mtoX genes were distinct from sediment mtoX and did not include close relatives of cultivated bacteria. Microbial diversity in the phyllosphere of S. anglicus was distinct compared to those of model plants such as rice, soybean, clover and Arabidopsis and showed a dominance of Gammaproteobacteria rather than Alphaproteobacteria.
UNASSIGNED: The potential for microbial DMS degradation in the phyllosphere and rhizosphere of Sporobolus anglicus suggest that DMS cycling in saltmarshes is more complex than previously recognised and calls for a more detailed assessment of how aboveground activities affect fluxes of DMS.

A key component of the marine sulfur cycle is the climate-active gas dimethylsulfide (DMS), which is synthesized by a range of organisms from phytoplankton to corals, and accounts for up to 80% of global biogenic sulfur emissions. The DMS cycle starts with the intracellular synthesis of the non-gaseous precursor dimethylsulfoniopropionate (DMSP), which is released to the water column by various food web processes such as zooplankton grazing. This dissolved DMSP pool is rapidly turned over by microbially mediated conversion using two known pathways: demethylation (releasing methanethiol) and cleavage (producing DMS). Some of the formed DMS is ventilated to the atmosphere, where it undergoes rapid oxidation and contributes to the formation of sulfate aerosols, with the potential to affect cloud microphysics, and thus the regional climate. The marine phase cycling of DMS is complex, however, as heterotrophs also contribute to the consumption of the newly formed dissolved DMS. Interestingly, due to microbial consumption and other water column sinks such as photolysis, the amount of DMS that enters the atmosphere is currently thought to be a relatively minor fraction of the total amount cycled through the marine food web-less than 10%. These microbial processes are mediated by water column temperature, but the response of marine microbial assemblages to ocean warming is poorly characterized, although bacterial degradation appears to increase with an increase in temperature. This review will focus on the potential impact of climate change on the key microbially mediated processes in the marine cycling of DMS. It is likely that the impact will vary across different biogeographical regions from polar to tropical. For example, in the rapidly warming polar oceans, microbial communities associated with the DMS cycle will likely change dramatically during the 21st century with the decline in sea ice. At lower latitudes, where corals form an important source of DMS (P), shifts in the microbiome composition have been observed during thermal stress with the potential to alter the DMS cycle.

The effects of ocean acidification and solar radiation on marine organisms have received increasing attention. Coccolithophores are a major producer of dimethylsulfoniopropionate (DMSP), which is a precursor of dimethylsulfide (DMS), a volatile biogenic active gas related to climate. Here, we investigated the individual and combined effects of elevated CO2 and ultraviolet radiation (UVR) on growth, DMS, and DMSP production of Emiliania huxleyi. Elevated CO2 (1000 μatm, HC) decreased the cell concentration, DMS, and particulate DMSP (DMSPp) concentrations by 17%, 20%, and 13%, respectively, compared with ambient CO2 (400 μatm, LC) in the semi-continuous culture. The addition of UVA to photosynthetically active radiation (PAR) increased cell concentration of E. huxleyi by 16% on day 4, which may be due to the photorepair effects induced by UVA, and the effect was time-dependent. PAR + UVA and PAR + UVA + UVB exposure decreased cellular DMS by 25%-56%, and increased cellular DMSPp by 60%-130% compared with PAR on days 3-4. Cellular DMSPp followed the order: PAR + UVA > PAR + UVA + UVB > PAR, and HC had no significant effects on cellular DMSPp compared with LC in the combined experiment. These results aid our understanding of the effects of ocean acidification and UV radiation on the production of methyl sulfur compounds in the ocean.

The anti-greenhouse gas dimethylsulfide (DMS) is mainly emitted by algae and accounts for more than half of the total natural flux of gaseous sulfur to the atmosphere, strongly reducing the solar radiation and thereby the temperature on Earth. However, the relationship between phytoplankton biomass and DMS emissions is debated and inconclusive. Our study presents field observations from 100 freshwater lakes, in concert with data of global ocean DMS emissions, showing that DMS and algal biomass show a hump-shaped relationship, i.e. DMS emissions to the atmosphere increase up to a pH of about 8.1 but, at higher pH, DMS concentrations decline, likely mainly due to decomposition. Our findings from lake and ocean ecosystems worldwide were corroborated in experimental studies. This novel finding allows assessments of more accurate global patterns of DMS emissions and advances our knowledge on the negative feedback regulation of phytoplankton-driven DMS emissions on climate.

We developed a dimethylsulfide (DMS) module coupled to an ecological dynamics model studying the annual DMS cycle of the Yellow and East China seas (YECS). The model results showed that surface DMS concentrations ([DMS]) peaked in August along the coast, and there exhibited several DMS peaks offshore annually. In addition, surface [DMS] were higher in the Yellow Sea than that in the East China Sea. The annual mean surface [DMS] of the YECS reached to 4.55 nmol/L, and oceanic DMS emissions from this sea area was 6.78 μmol/(m2 day). Several sensitivity experiments demonstrated that phytoplankton community and sea water temperature exerted crucial effects on seasonal variations of surface [DMS]; and phytoplankton community or temperature changed the timing of surface DMS peak while photolysis affected the magnitude of [DMS]. Moreover, the effect size of phytoplankton community or water temperature varied spatially.

The marine organosulfur cycle has been studied intensively for over 30 years motivated by the hypothesis that dimethylsulfide (DMS) affects Earth\'s radiation balance and climate. The main source of DMS is from the enzymatic lysis of dimethylsulfoniopropionate (DMSP), the latter of which is a significant component of carbon, sulfur, and energy fluxes in the oceans. Acrylate is also produced during DMSP lysis, but unlike DMS or DMSP, very little is known about the marine acrylate cycle. Herein, a new source of acrylate was identified in seawater as a product formed from the photolysis of dissolved organic matter (DOM). Photochemical production rates varied from 1.6 to 5.0 pM (μmol quanta cm-2)-1, based on photon exposures determined from nitrite actinometry. A positive correlation (r = 0.87) was observed between acrylate photoproduction and the seawater absorption coefficient at 330 nm. Acrylate photoproduction was initiated by UV radiation, with UV-B and UV-A contributing approximately 32 and 68% to the total production, respectively. Acrylate did not photolyze in high-purity water or seawater at concentrations less than 100 nM. These findings improve our understanding of the role that sunlight plays in the marine acrylate cycle, a reactive form of DOM that significantly affects the carbon cycle and ecology of the upper ocean.

We implement oceanic dimethylsulfide (DMS) emissions and its atmospheric chemical reactions into the Community Multiscale Air Quality (CMAQv53) model and perform annual simulations without and with DMS chemistry to quantify its impact on tropospheric composition and air quality over the Northern Hemisphere. DMS chemistry enhances both sulfur dioxide (SO2) and sulfate ( S O 4 2 - ) over seawater and coastal areas. It enhances annual mean surface SO2 concentration by +46 pptv and S O 4 2 - by +0.33 μg/m3 and decreases aerosol nitrate concentration by -0.07 μg/m3 over seawater compared to the simulation without DMS chemistry. The changes decrease with altitude and are limited to the lower atmosphere. Impacts of DMS chemistry on S O 4 2 - are largest in the summer and lowest in the fall due to the seasonality of DMS emissions, atmospheric photochemistry and resultant oxidant levels. Hydroxyl and nitrate radical-initiated pathways oxidize 75% of the DMS while halogen-initiated pathways oxidize 25%. DMS chemistry leads to more acidic particles over seawater by decreasing aerosol pH. Increased S O 4 2 - from DMS enhances atmospheric extinction while lower aerosol nitrate reduces the extinction so that the net effect of DMS chemistry on visibility tends to remain unchanged over most of the seawater.