N2O Release Research Articles

Application of waste eggshells elevates phytoremediation efficiency of Pb-Zn mine-contaminated farmland and mitigates soil greenhouse gas emissions: A field study

Remediating heavy metal (HM)-contaminated farmlands and sequestering soil carbon for emission reduction have been prominent topics in environmental research in recent years. However, few studies have looked into the soil greenhouse gas (GHG) impacts of growing hyperaccumulators in composite HM-contaminated farmland, as well as agronomic measures to remediate soil HMs while mitigating GHG emissions. To investigate fertilization measures to improve phytoremediation efficiency and mitigate GHG emissions, S. photeinocarpum was planted with three different fertilization measures on farmland contaminated by lead-zinc (Pb-Zn) mines (1200 kg ha−1 eggshell, 125 kg ha−1 28-homobrassinolide, and 16.7 kg ha−1 mineral potassium fulvic acid) during its growth period. The findings are as follows: Eggshell application significantly enhanced the translocation factor (TF) of Pb, Zn, and cadmium (Cd) from the roots to the shoots of Solanum photeinocarpum. Moreover, eggshells notably increased the bioaccumulation factor (BCF) of Cd and Pb in plant shoots by 120.75% and 159.09%, respectively. Regarding GHG emissions, the combined application of eggshells and 28-homobrassinolide substantially lowered the global warming potential (GWP) of the soil. Correlation analyses revealed that eggshell application increased the relative abundance of the Gemmatimonadota bacterial phylum in the soil, facilitating Pb and Cd migration from the roots to shoot tissues in S. photeinocarpum. Eggshell use inhibited nitrate nitrogen (NO3−-N) transformation into nitrous oxide (N2O) by the Myxococcota bacterial phylum and reduced N2O release from the soil. The application of low-cost eggshells can achieve a win-win situation of soil HM remediation and GHG emission reduction, as well as provide simple and scalable management measures for HM-contaminated farmland.

Labile organic matter favors a low N2O yield during nitrogen removal in estuarine sediments

Estuary harbors the active sediment denitrification and nitrous oxide (N2O) emission, while the knowledge of environmental controls on the denitrification-derived N2O yield remains underexplored. Here, we quantitatively assess the potential and in situ rates of N2O production during sediment denitrification in the Pearl River Estuary (PRE), China. Organic matter determines the product stoichiometry and capacity of nitrogen removal. In particular, labile organic matter (LOM) reduces N2O yield via enhancing the complete coupled nitrification-denitrification. Our results reveal that the chain processes, primary production-LOM settling-sedimentary respiration-coupled nitrification-denitrification, control the sediment denitrification and N2O production, linking the carbon and nitrogen biogeochemical cycles in the atmosphere-water column-sediment continuum. The PRE sediments serve as nitrogen removal hotspots but with low efficiency (~25 % of riverine input) and strong N2O release (~66 % of daily sea-air N2O efflux). These findings contribute to policy makers to develop knowledge-based management actions for achieving sustainable coastal environments and mitigating N2O emission.

Key biochar properties linked to denitrification products in a calcareous soil

Meta-analyses show an overall decrease in soil N2O emissions after biochar (BC) amendment. Nonetheless, N2O mitigation with BC cannot be extrapolated to every BC-soil combination, inasmuch as an increase in soil N2O release has been occasionally reported. We hypothesized that BC characteristics are key, and performed two microcosm experiments to advance in the understanding of the properties associated. We first investigated how 22 well-characterized BCs affect N2O emissions in a calcareous soil under denitrification conditions. Whereas most BCs decreased N2O emissions, some substantially increased N2O emissions. In a second experiment, we selected and further characterized eight of the 22 previous BCs. We applied the 15N-gas-flux method to study how these BCs affect denitrification products (N2O and N2) in the same soil. Results indicate that the interaction between BC and the denitrification process depends on the temperature of pyrolysis. Whereas BCs produced at 400 °C tended to increase total denitrification (N2O+N2) by an average of 28%, BCs produced at 600 °C significantly reduced total denitrification by 53%. Nevertheless, this decline in overall denitrification did not result in a decrease of N2O emissions, as there was a strong shift in the N2O/(N2+N2O) ratio favoring N2O. A redundancy analysis revealed a direct correlation between carboxylic groups on BCs surface and N2O emissions. This research enhances our understanding of the interaction of BC with denitrification, particularly concerning the relevance of the temperature of pyrolysis, and opens up new paths for investigation, crucial for optimizing the application of BCs in different soil environments.Graphical

Impact of freeze-thaw cycles and influent C/N ratios on N2O emissions in subsurface wastewater infiltration systems

Subsurface wastewater infiltration system (SWIS) is important source of N2O emission, biological denitrification process relies on organic carbon source as electron donor, enabling denitrifying reductase (NAR, NIR, NOR, and N2OR) to reduce nitrate nitrogen to N2. However, freeze-thaw cycles cause changes in soil structure through physical and biological processes that increase organic matter availability and microbial activity, thereby accelerating upper (aerobic) organic matter degradation. This leads to carbon deficiency in the lower (anaerobic) layer, which reduces denitrification efficiency increasing N2O production and emissions. This study investigated effects of influent C/N ratios on N2O emissions from SWIS under freeze-thaw stress, and changes in denitrifying reductase and microbial communities. Results showed that as influent C/N ratio increased from 6:1–10:1, average TN removal of SWIS decreased from 89.59 % to 84.95 %, while N2O emission rate decreased from 0.106 mg·m−2·h−1 to 0.0333 mg·m−2·h−1, a reduction of 68.61 %. Meanwhile, N2OR activity increased by 29.95 % with C/N ratio increasing from 6 to 10, showing a significant reduction of N2O. High-throughput sequencing results revealed that Proteobacteria and Firmicutes showed a linear relationship with influent C/N. As C/N increased from 6 to 8 and 10, Proteobacteria relative abundance increased from 22.24 % ± 1.79–32.51 % ± 2.51 % and 39.59 % ± 3.45 %, while Firmicutes relative abundance decreased from 31.73 % ± 7.87–3.34 % ± 0.27 % and 2.19 % ± 0.07 %. These results indicated that sufficient supply of organic carbon provided abundant electron donors for denitrifying reductases in freeze-thaw-affected SWIS, promoting influent NO3--N reduction and decreasing N2O release rates. Conversely, under low C/N ratio conditions, electron acceptance capacity of N2OR was limited and N2OR activity was inhibited, resulting in N2O accumulation and emission. SynopsisThis paper shows how increasing the organic carbon supply in SWIS can reduce N2O emissions and improve nitrogen removal under freeze-thaw stress.

Temporal enrichment of comammox Nitrospira and Ca. Nitrosocosmicus in a coastal plastisphere.

Plastic marine debris is known to harbor a unique microbiome (termed the "plastisphere") that can be important in marine biogeochemical cycles. However, the temporal dynamics in the plastisphere and their implications for marine biogeochemistry remain poorly understood. Here, we characterized the temporal dynamics of nitrifying communities in the plastisphere of plastic ropes exposed to a mangrove intertidal zone. The 39-month colonization experiment revealed that the relative abundances of Nitrospira and Candidatus Nitrosocosmicus representatives increased over time according to 16S rRNA gene amplicon sequencing analysis. The relative abundances of amoA genes in metagenomes implied that comammox Nitrospira were the dominant ammonia oxidizers in the plastisphere, and their dominance increased over time. The relative abundances of two metagenome-assembled genomes of comammox Nitrospira also increased with time and positively correlated with extracellular polymeric substances content of the plastisphere but negatively correlated with NH4+ concentration in seawater, indicating the long-term succession of these two parameters significantly influenced the ammonia-oxidizing community in the coastal plastisphere. At the end of the colonization experiment, the plastisphere exhibited high nitrification activity, leading to the release of N2O (2.52ng N2O N g-1) in a 3-day nitrification experiment. The predicted relative contribution of comammox Nitrospira to N2O production (17.9%) was higher than that of ammonia-oxidizing bacteria (4.8%) but lower than that of ammonia-oxidizing archaea (21.4%). These results provide evidence that from a long-term perspective, some coastal plastispheres will become dominated by comammox Nitrospira and thereby act as hotspots of ammonia oxidation and N2O production.

Impact of elevated CO2 on microbial communities and functions in riparian sediments: Role of pollution levels in modulating effects

The impact of elevated CO2 levels on microorganisms is a focal point in studying the environmental effects of global climate change. A growing number of studies have demonstrated the importance of the direct effects of elevated CO2 on microorganisms, which are confounded by indirect effects that are not easily identified. Riparian zones have become key factor in identifying the environmental effects of global climate change because of their special location. However, the direct effects of elevated CO2 levels on microbial activity and function in riparian zone sediments remain unclear. In this study, three riparian sediments with different pollution risk levels of heavy metals and nutrients were selected to explore the direct response of microbial communities and functions to elevated CO2 excluding plants. The results showed that the short-term effects of elevated CO2 did not change the diversity of the bacterial and fungal communities, but altered the composition of their communities. Additionally, differences were observed in the responses of microbial functions to elevated CO2 levels among the three regions. Elevated CO2 promoted the activities of nitrification and denitrification enzymes and led to significant increases in N2O release in the three sediments, with the greatest increase of 76.09 % observed in the Yuyangshan Bay (YYS). Microbial carbon metabolism was promoted by elevated CO2 in YYS but was significantly inhibited by elevated CO2 in Gonghu Bay and Meiliang Bay. Moreover, TOC, TN, and Pb contents were identified as key factors contributing to the different microbial responses to elevated CO2 in sediments with different heavy metal and nutrient pollution. In conclusion, this study provides in-depth insights into the responses of bacteria and fungi in polluted riparian sediments to elevated CO2, which helps elucidate the complex interactions between microbial activity and environmental stressors.

Modified biochar affects CO2 and N2O emissions from coastal saline soil by altering soil pH and elemental stoichiometry

The application of biochar in degraded farmland improves soil productivity while achieving the recycling of agricultural waste. The collapse of the physical structure of coastal saline soils will greatly reduce the carbon sequestration potential of biochar. Phosphorus- and magnesium-modified biochar greatly improve the stability of biochar, which endows them with the potential to greatly improve the organic carbon pool of coastal saline soil. However, changes in the properties of modified biochar increase the uncertainty of microbial driven CO2 and N2O release by affecting soil chemistry properties. In this study, through laboratory soil microcosmic experiment, we investigated the effects of magnesium-modified biochar (BCMg) and phosphorus-modified biochar (BCP) on CO2 and N2O releases from coastal saline soils, and further uncovered their potential mechanisms. Compared with unapplied biochar (CK) and unmodified biochar (BC) treatment, BCMg reduced both the releases of CO2 and N2O, and BCP decreased N2O release but enhanced CO2 release. pH is the medium through which BCMg affects the release of CO2 and N2O. Specifically, BCMg increased soil pH above 8.5, which reduced the metabolic activity of the microbial community, and the abundance of bacteria directly or indirectly involved in N2O production, thereby decreasing the releases of CO2 and N2O. The amendment of BCP changed soil elemental stoichiometry causing microbial N-limitation. Increasing CO2 release and decreasing N2O release were strategies for microorganisms to cope with N-limitation. These findings suggested that BCMg is superior to BCP in mitigating greenhouse gas emissions, providing a basis for the application of modified biochar to improve the carbon pool and reduce greenhouse gas emissions of coastal saline soil.

Half substitution of mineral N with fish protein hydrolysate enhancing microbial residue C and N storage and climate benefits under high straw residue return

The widespread utilization of straw return was a popular practice straw disposal for highly intensive agriculture in China, which has brought about some negative impacts such as less time for straw complete biodegradation, aggravation of greenhouse gas evolution, and lower efficient of carbon accumulation. It was urgent to find an eco-friendly N-rich organic fertilizer instead of mineral N as activator to solve the above problems and lead a carbon accumulation in long tern management. Besides, microbial necromass was considered as a crucial contributor to persistent soil carbon (C) and nitrogen (N) pool. How organic fertilizer activators influence microbial residue under different amount of crop residues input remained unclear. Thus, soils incorporating moderate and high rate of rice straw residue with additions of half and full of organic activators (fish protein hydrolysates vs. manure) were incubated for measuring carbon dioxide (CO2) and nitrous oxide (N2O) emission, microbial community and necromass. It was found that soil CO2 emission was rapidest during the first 13 days of straw decomposition but remained lowest in the treatments of 50% mineral N substituted by fish protein hydrolysate. There were that 81%–89% of total CO2 release and 59%–65% of total N2O emission occurred within 60 days of incubation period, and bacterial community and nitrate positively affected soil CO2 and N2O release respectively. Straw incorporation amount and organic activator application interactively influenced soil CO2 emission but not affected soil N2O emission. After 360 days of incubation, the difference of bacterial necromass was noticeable but fungal necromass remained almost unaltered across all treatments. All treatments showed generally comparable contribution of microbial necromass N to the total N pool. The treatment of 50% mineral N substituted by fish protein hydrolysate under high rate of straw input (HSF50) promoted the highest proportion of microbial necromass C in soil organic C because of alleviating N limitation for microorganisms. Finally, HSF50 was recommended as an eco-friendly strategy for enhancing microbial necromass C and N storage and climate benefits in agroecosystems.

NosZ II/nosZ I ratio regulates the N2O reduction rates in the eutrophic lake sediments

Nitrous oxide (N2O) is a more potent greenhouse gas with an atmospheric lifetime of 121 years, contributing significantly to climate change and stratospheric ozone depletion. Lakes are hotspots for N2O release due to the imbalance between N2O sources and sinks. N2O-reducing bacteria are the only biological means to mitigate N2O emission, yet their roles in lakes are not well studied. This study investigated the potential for N2O reduction, keystones of typical and atypical N2O-reducing bacterial communities, and their correlations with environmental factors in the sediments of Lake Taihu through microcosm experiments, high-throughput sequencing of the nosZ gene, and statistical modeling. The results showed that potential N2O reduction rates in sediments ranged from 13.71 to 76.95 μg N2O g−1 d−1, with lower rates in December compared to March and July. Correlation analysis indicated that the nosZ II/nosZ I ratio and the trophic lake index (TLI) were the primary factors influencing N2O reduction rates and N2O-reducing bacterial community structures. The genera Pseudogulbenkiania and Ardenticatena were identified as the most abundant typical and atypical N2O-reducing bacteria, respectively, and were also recognized as the keystone taxa. Quantitative real-time PCR (qPCR) results revealed that nosZ II was more abundant than nosZ I in the sediments. Partial least squares path modeling (PLS-PM) further demonstrated that atypical N2O-reducing bacteria had significant positive effects on N2O reduction process in the sediments (p < 0.05). Overall, this study highlights the crucial ecological roles of atypical N2O-reducing bacteria in the sediments of the eutrophic lake of Taihu, underscoring their potential in mitigating N2O emissions.

Large nitrogen cycle perturbations during the Early Triassic hyperthermal

Ocean temperature, redox state, circulation, and nutrient levels regulate the marine nitrogen (N) cycle, yet their specific impacts during greenhouse intervals remain poorly understood. Here, we examined the Smithian–Spathian hyperthermal event (∼250.5 Ma) during the Early Triassic greenhouse using stable N isotopes (δ15N) from sedimentary records in the Nanpanjiang Basin and Northern Yangtze Basin of South China. The δ15N profiles in both basins reveal consistent trends that correspond to fluctuations in temperature across the Smithian–Spathian transition. The Smithian hyperthermal interval exhibited low δ15N values (mostly <+2‰), indicating N deficiency and enhanced biological N2 fixation. Bacterial blooms and the release of the potent greenhouse gas N2O, enhanced by high temperatures, may have triggered positive feedback mechanisms that sustained the warming and contributed to the late Smithian extinction. During subsequent cooling across the Smithian–Spathian transition, δ15N increased to a range of +3‰ to +7‰, likely reflecting signals of partial denitrification based on reconstruction of the NO3− inventory associated with oceanic cooling and oxygenation. The prevailing increases in sedimentary TOC/TN ratios signify heightened deamination (removal of amino groups) and N recycling across the Smithian–Spathian boundary. This transition is likely attributed to cooling-driven amelioration of seawater stratification and anoxia from the Smithian to the Spathian, which resulted in increased nitrate availability in the photic zone. Eukaryotic algae thrived while prokaryotes declined during the Spathian, evidenced by elevated δ15N and Δ13Ccarb-org (the difference between carbonate and organic carbon isotopes). The proliferation of eukaryotic algae had a positive impact on environmental conditions and facilitated biotic recovery due to more efficient burial of organic particles. A notable latitudinal gradient in the N cycle response was observed, with low-latitude regions showing a more pronounced response to cooling compared to mid-latitude areas. This significant gradient may suggest that the rapid recovery of nutrient cycles, despite relatively small decline in high temperature, was a key factor in the amelioration of climate and recovery of life in low latitudes. These findings highlight that the marine N cycle is highly sensitive to temperature changes, particularly in low-latitude regions, and that changes in N cycle under high-temperature conditions may be a critical life-limiting factor.

Influence of Catalyst Surface Structure on the Electrochemical Hydrogenation of Cis,Cis-Muconic Acid

Adipic acid (AA) production from petroleum-based cyclohexane is one of the largest chemical processes in terms of annual volumetric turnover accounting for 3 million tons as of 2022. The current commercial approach to synthesize AA is through the oxidation of petroleum-derived cyclohexane using nitric acid. The release of N2O in stoichiometric amounts makes it one of the most significant greenhouse gas (GhG) emitting processes. The abundance of biomass in the Midwestern United States has driven significant research efforts to synthesize bio-derived and sustainable commodity products and lower the chemical industry’s carbon footprint.1 cis,cis-Muconic acid (ccMA), a biobased C6 diunsaturated diacid platform molecule can be transformed to commodity chemicals like caprolactam, adipic acid, and terephthalic acid, with AA being of particular interest for the synthesis of nylon 6,6.2 For the first time in literature, we demonstrate appreciable production of AA (conversion: 91%, selectivity: >95%) through electrochemical hydrogenation (ECH) of ccMA on PGM catalysts. Carbon-supported palladium (Pd/C) and platinum (Pt/C) selectively produced AA while bulk Pd and Pt yielded the monounsaturated trans-3-hexenedioic acid (t3HDA) intermediate and H2 under all tested conditions. Such an influence of surface structure on the electrochemistry of organics is not unprecedented. Koper et. al3 studied Pt single crystals for the electrochemical hydrogenation of acetone and showed how activity, selectivity, and extent of catalytic poisoning are highly sensitive to the Pt surface structure. Similarly, we used density functional calculations to elucidate the structure-sensitive nature of ccMA ECH and its intermediates by identifying thermodynamically preferred reaction pathways as a function of surface geometry (terrace vs steps). The energetics coupled with experimental observations suggest that the reduction of ccMA to t3HDA occurs through an outer sphere proton-coupled electron transfer mechanism, while the reduction of HDA to AA preferentially occurs on Pd and Pt (111), the most abundant facet in Pd/C and Pt/C. Our calculations also explain the exceptional performance of Pd/C compared to Pt/C by the weaker binding of Pd terrace sites compared to Pt. Overall, combining renewable electricity, in-situ hydrogen generation from water, and a biologically-produced intermediate enabled us to open a sustainable route for bio-adipic acid production. This allows us to further design and optimize the catalyst for the selective production of biobased AA.

Effects of aeration control strategies on nitrous oxide emissions in alternating anoxic–oxic sequencing batch reactor systems

Reducing N2O emissions is key to controlling greenhouse gases (GHG) in wastewater treatment plants (WWTPs). Although studies have examined the effects of dissolved oxygen (DO) on N2O emissions during nitrogen removal, the precise effects of aeration rate remain unclear. This study aimed to fill this research gap by investigating the influence of dynamic aeration rates on N2O emissions in an alternating anoxic–oxic sequencing batch reactor system. The emergence of DO breakthrough points indicated that the conversion of ammonia nitrogen to nitrite and the release of N2O were nearly complete. Approximately 91.73 ± 3.35% of N2O was released between the start of aeration and the DO breakthrough point. Compared to a fixed aeration rate, dynamically adjusting the aeration rates could reduce N2O production by up to 48.6%. Structural equation modeling revealed that aeration rate and total nitrogen directly or indirectly had significant effects on the N2O production. A novel regression model was developed to estimate N2O production based on energy consumption (aeration flux), water quality (total nitrogen), and GHG emissions (N2O). This study emphasizes the potential of optimizing aeration strategies in WWTPs to significantly reduce GHG and improve environmental sustainability.

Effect of microbial growth and electron competition on nitrous oxide source and sink function of hyporheic zones

The hyporheic zones (HZs) are key sites of the production of nitrous oxide (N2O), a potent ozone-depleting greenhouse gas. Denitrification is the primary process of N2O production in HZs, including four reduction steps (NO3−→NO2−→NO→N2O→N2). Electron competition occurs between the four reduction steps and can significantly impact the production of N2O. However, denitrification was typically considered as simplified two step reactions for investigating the release of N2O, neglecting the electron competition among the four-step reactions. Moreover, the N2O production/consumption patterns are regulated by both hydraulic and biogeochemical conditions in HZs. Dynamic microbial growth cannot only mediate the biogeochemical reactions, but also change hydraulic properties spatiotemporally by bioclogging. But microbial growth is rarely considered for investigating N2O dynamics of HZs. To assess these effects on hyporheic N2O dynamics and source-sink function, we establish a novel numerical model of N2O dynamics of HZs, coupling porous flow, reactive transport, electron competition, microbial growth and bioclogging. The results show that the weak electron competitiveness of N2O reductase results in a less allocation of electrons to the N2O reduction process, particularly in situations with limited carbon sources, thus increasing the release of N2O into the rives. Microbial growth significantly influences N2O release from HZs into rivers, increasing by more than two orders of magnitude on average compared to the model neglecting microbial dynamics. In contrast to the classical knowledges that HZs in coarse sediments tending to short residence time cannot act as sources of N2O, dynamic microbial growth obviously increases the potential for N2O release from HZs in coarse sediments to the rivers. The global Monte Carlo regional sensitivity analyses indicate that microbial biomass is the most critical factor determined the hyporheic source-sink function for N2O, followed by carbon oxidation rate and residence time. These are significantly different from previous knowledge that the residence time and oxygen/nitrogen uptake rate are the most sensitive parameters, which may lead to misunderstanding of the key controlling factors of N2O release from HZs. In addition, we propose a new Damköhler number (DaO2∗) of dissolved oxygen by multiplying the classical DaO2 with a dimensionless microbial modification factor for identifying N2O source-sink function of HZs, with DaO2∗ < 1 for N2O sink, while DaO2∗ > 1 for N2O source.

Effect of Cubic Crystal Morphology on Thermal Characteristics and Mechanical Sensitivity of PYX

To investigate the influence of the cubic crystal morphology on the thermal properties and sensitivity of 2,6-bis(picrylamino)-3,5-dinitropyridine (PYX), cubic PYX (CPYX) crystals were prepared using the antisolvent method. Scanning electron microscopy (SEM), laser particle size analysis, X-ray diffraction (XRD) and Fourier transform infrared spectroscopy (FT-IR) were used to characterize the morphology, particle size and structure of the prepared products. The thermal behavior, thermal decomposition kinetics, thermal safety parameters and thermal decomposition mechanism of CPYX were investigated by differential scanning calorimetry–thermogravimetry–mass spectrometry–Fourier transform infrared spectrometry (DSC-TG-MS-FT-IR) and in situ FT-IR experiments. Meanwhile, the mechanical sensitivity of CPYX was determined by means of the explosion probability method. The results showed that the product had a smooth cubic morphology and small crystal aspect ratio with an average particle size (d50) of 10.65 μm, but it had no distinct differences from the crystal structure of raw PYX (RPYX). The thermal decomposition peak temperature, the self-accelerating decomposition temperature and the critical temperature of the thermal explosion of CPYX increased by 7.2 °C, 6.1 °C and 10.4 °C, respectively, compared to RPYX. Similarly, the apparent activation energy increased by 15%. Besides these, the impact sensitivity and friction sensitivity of CPYX decreased by 36% and 20%, respectively, compared to RPYX. The decomposition process of CPYX contains two stages. The first stage involves the breakage of N-H bonds and -NO2 groups with the release of CO2, N2O, NO, HCN and H2O, followed by the thermal decomposition of the resulting intermediate and the release of CO2, N2O and HCN in the second stage.

A Strategic NH3-Dosing Approach for the Minimization of N2O Production During NH3-SCR Reactions over Cu-SSZ-13 Catalysts

AbstractThe undesired production of N2O during NH3-SCR reactions is investigated over a reference commercial Cu-CHA catalyst. Steady-state experiments performed in the 150–500 °C temperature range exhibit a bimodal trend in the N2O formation profile, confirming the existence of two different reaction mechanisms occurring at low and high temperatures. Focusing on a low-to-medium T-range, N2O production, usually ascribed to NH4NO3 formation and decomposition, increases with the NO2/NOx ratio. However, an excess of NO2 leads to a decrease in the N2O release due to ammonium nitrate deposition and catalyst clogging phenomena. Steady-state and dynamics experiments show the promoting effect of both NH3 feed concentration and NH3 storage on N2O production at T &gt; 200 °C. Surprisingly, N2O decreases with increasing NH3/NOx ratio at lower temperature. A novel approach based on the strategic injection of NH3 is also applied to mitigate the N2O formation while maintaining high deNOx activity. Remarkably, complete NOx conversion and ~ 11% N2O saving are achieved (with inlet NO2/NOx = 0–0.5) at temperatures exceeding 200 °C; in addition, a peculiar behavior is observed in the N2O profile, which increases and decreases when adding and removing NH3 from the feed, respectively. Notably, the opposite trend is observed in the N2O profile at 200 °C. When under Standard SCR conditions, this so far unreported observation challenges the NH4NO3 formation route for N2O and suggests the existence of different controlling phenomena at different temperature regimes: i) the Cu/redox chemistry at T ≤ 200 °C and ii) the NH3 storage at higher temperature, ideally up to 300 °C.

Differential responses of temperature sensitivity of greenhouse gases emission to seasonal variations in plateau riparian zones

Riparian zones, regarded as hotspots for greenhouse gas (GHG) emissions, where the variation in temperature sensitivity (Q10) of GHG emissions is crucial for assessing GHG budgets under global warming. However, the seasonal Q10 of GHG emissions from high-elevation riparian zones and underlying microbial mechanisms are poorly documented. This study focuses on seasonal Q10 patterns of GHG emissions from riparian zones along the Lhasa River on the Tibetan Plateau. CO2 and CH4 emissions from riparian soils were more sensitive to temperature in spring than in summer. The opposite trend was observed for Q10 of N2O emissions. Soil organic carbon (SOC) had relatively large direct effects on the Q10-CO2 value in summer, whereas soil nitrate nitrogen (SNO3−-N) was the determinant of Q10-CO2 value in spring. mcrA:pmoA and soil microbial biomass C (SMBC) had strong direct effects on the Q10 of CH4 emissions in summer; the Q10-CH4 value in spring was significantly affected by the mcrA abundance. SMBC and the nirK + nirS abundance were key factors affecting the Q10-N2O value. Q10-CO2 and Q10-CH4 values exhibited strong seasonalities in the lower reaches of riparian soils, mainly due to the seasonalities of SNO3−-N and mcrA:pmoA, respectively. The Q10-N2O value in the middle and upper reaches of riparian soils presented seasonality, which was largely due to the seasonalities of soil ammonia nitrogen and microbial biomass carbon. During thawing, plant productivity increased, substrate carbon was sufficient, microbial biomass increased, and inorganic nitorgen and denitrifier abundance decreased, causing 29.67% and 37.47% decreases in the Q10-CO2 and Q10-CH4 values, respectively, and a 70.85% increase in the Q10-N2O value, indicating that the potential release of N2O from riparian zones along the plateau river was more susceptible to seasonal variations. Our findings are conducive to accurately evaluating the potential contribution of GHG emissions from high-elevation riparian zones to global warming.

N2O emission in temperate seagrass meadows: Fluxes, pathway and molecular mechanism

Seagrass meadows act as filters for nitrogen in coastal areas, but whether they are a source or sink for N2O has been still controversy. Additionally, the production pathways of N2O as well as the microbial driving mechanism in seagrass meadows are seldom reported. In this study, the air-sea fluxes, sediment release potential, and production pathway of N2O in a temperate Zostera marina and Z. japonica mixed meadow were investigated by using gas chromatography and 15N isotopic tracing methods. The qPCR and metagenome sequencing were used to compare the difference in functional gene abundance and expression between seagrass vegetated and non-grass sediments. The results showed that the N2O air-sea fluxes in the meadow ranged from −1.97 to −1.77 nmol m⁻2 h⁻1, which was slightly lower in the seagrass region than in the adjacent bare region. Seagrass sediment N2O release potential dramatically increased after warming and nitrogen enrichment treatments. Heterotrophic nitrification was firstly investigated in seagrass meadows, and the process (26.80%–62.41%) and denitrification (37.55%–72.83%) contributed significantly to N2O production in the meadow, affected deeply by sediment organic content, while the contribution of autotrophic nitrification can be neglected. Compared with the bare sediments, the ammonia monooxygenase genes amoA, amoB and amoC, and nitrite oxidoreductase genes nxrA and nxrB, as well as nitrite reductase gene nirS and nitric oxide reductase gene norB were down-regulated, while the nitrous oxide reductase gene nosZ was up-regulated in the seagrass sediments, explaining less N2O emission in seagrass regions from the perspective of molecular. The nosZII-bearing bacteria like Bacteroidia, Polyangia, Anaerolineae, and Verrucomicrobiae could play important roles in N2O reduction in the seagrass meadow. The result is of great significance for highlighting the ability of seagrass meadows to mitigate climate changes.

Mechanism of heterogeneous reduction of NO over graphite-supported single-atom Fe catalyst: DFT study

The mechanism of nitrogen oxide (NO) reduction over graphite carbon-supported single-atom iron (Fe) catalyst (Fe/G) was investigated by density functional theory (DFT) and transition state theory (TST). The catalyst deactivation was also analyzed. The results revealed that the NO reduction, based on the Eley-Rideal (E-R) mechanism, underwent four stages including N2O formation and release as well as N2 formation and release. However, the NO reduction only involved two stages according to Langmuir-Hinshelwood (L-H) mechanism: N2 formation and release. Furthermore, for the E-R mechanism, the rate-controlling step was NO reduction, where a NO molecule was adsorbed on an Fe atom with an N, O-down structure with energy barrier of 15.5 kJ/mol, lower than that of other paths. Energy barrier analysis indicated that the energy barrier for the reduction of reactive oxygen species was higher than that for the formation of N2. Reactive oxygen species remaining on the surface of Fe atoms after NO decomposition inhibited the adsorption and reduction of NO, leading to catalyst deactivation due to the absence of active sites. The single-atom Fe species promoted the NO reduction. Kinetic analysis results suggested that, upon increasing the reaction temperature, the NO reduction rate increased more significantly than the reactive oxygen transfer rate.

Respiration and growth of Paracoccus denitrificans R-1 with nitrous oxide as an electron acceptor.

Nitrous oxide (N2O) is a potent greenhouse gas and contributor to ozone layer destruction, and atmospheric N2O has increased steadily over the past century due to human activities. The release of N2O from fixed N is almost entirely controlled by microbial N2O reductase activities. Here, we investigated the ability to obtain energy for the growth of Paracoccus denitrificans R-1 by coupling the oxidation of various electron donors to N2O reduction. The modular N2O reduction process of denitrifying microorganism not only can consume N2O produced by itself but also can consume the external N2O generated from biological or abiotic pathways under suitable condition, which should be critical for controlling the release of N2O from ecosystems into the atmosphere.

Mitigated N2O emissions from submerged-plant-covered aquatic ecosystems on the Changjiang River Delta

Submerged plants affect nitrogen cycling in aquatic ecosystems. However, whether and how submerged plants change nitrous oxide (N2O) production mechanism and emissions flux remains controversial. Current research primarily focuses on the feedback from N2O release to variation of substrate level and microbial communities. It is deficient in connecting the relative contribution of individual N2O production processes (i.e., the N2O partition). Here, we attempted to offer a comprehensive understanding of the N2O mitigation mechanism in aquatic ecosystems on the Changjiang River Delta according to stable isotopic techniques, metagenome-assembly genome analysis, and statistical analysis. We found that the submerged plant reduced 45 % of N2O emissions by slowing down the dissolved inorganic nitrogen conversion velocity to N2O in sediment (Vf-[DIN]sed). It was attributed to changing the N2O partition and suppressing the potential capacity of net N2O production (i.e., nor/nosZ). The dominated production processes showed a shift with increasing excess N2O. Meanwhile, distinct shift thresholds of planted and unplanted habitats reflected different mechanisms of stimulated N2O production. The hotspot zone of N2O production corresponded to high nor/nosZ and unsaturated oxygen (O2) in unplanted habitat. In contrast, planted habitat hotspot has lower nor/nosZ and supersaturated O2. O2 from photosynthesis critically impacted the activities of N2O producers and consumers. In summary, the presence of submerged plants is beneficial to mitigate N2O emissions from aquatic ecosystems.