Greenhouse Gas N2O Research Articles

Selective conversion of thermal decomposition products of ammonium perchlorate by amorphous CoSnOx

The directional transformation of products in the multiphase decomposition process of ammonium perchlorate (AP) still faces significant challenges, one of which is the conversion of greenhouse gas N2O. Furthermore, additional elucidation of the structure and potential catalytic mechanisms of catalysts with high thermal stability is imperative for the aforementioned process. This study proposes a cobalt-based amorphous oxide with high thermal stability for catalysing the thermal decomposition of AP and achieving the transformation of catalytic products from N2O to NO (and its derivatives). The results indicate that the type of catalytic decomposition products is related to the structural transformation of the catalyst, suggesting a synergistic oxidation mechanism by active oxygen and lattice oxygen. The peak decomposition temperature of AP has dropped to near the limit of 257.2 °C, TG-IR test and MD simulation results indicate the selective generation of NO under the lattice oxygen mechanism. In addition, kinetic calculations elucidated the transition of catalysts from amorphous to crystalline state in catalysis. Finally, suggestions were made for the current characterization techniques of catalysts. This study offers a reference point for the catalyst design of AP decomposition-oriented products, which is beneficial for the transition to more environmentally-friendly products.

Temporal and spatial analysis of fertilizer application intensity and its environmental risks in China from 1978 to 2022

Fertilizers are an essential input in agriculture as they can enhance crop yields. However, their use also poses significant environmental risks. To thoroughly explore the intensity of fertilizer use and its potential threats to the ecological environment, this study analyzed the environmental risks of fertilizer use from a temporal and spatial perspective based on fertilizer application data in China from 1978 to 2022. Additionally, the contribution of fertilizer application in Chinese farmland to greenhouse gas N2O emissions was quantified using IPCC emission factor methodology. The results indicated that fertilizer application intensity and N2O emissions in China initially increased and then decreased from 1978 to 2022. Despite the implementation of various fertilizer control measures at the policy level, such as the Zero Growth of Fertilizer Action in 2015 and the Efficiency-Increasing Action for Reducing Fertilizer Use in 2022, the intensity of fertilizer application in China still exceeded international safety standards by 1.33-fold in 2022, reaching 298.79 kg/hm2. Furthermore, N2O emissions amounted to 50.17 × 104t, accounting for 16% of China's total agricultural greenhouse gas emissions that year. Correlation and regression analyses demonstrated that with increasing fertilizer application, crop production exhibits an inverted U-shaped growth trend, indicating limited effectiveness of high-intensity fertilizer use in increasing crop yields. These findings highlight the profound greenhouse effect resulting from the use of agricultural nitrogen fertilizer. Therefore, this study proposed technical and policy-level mitigation measures to address the issues caused by excessive fertilizer application, aiming to provide insights for controlling agricultural non-point source pollution and preserving the agroecological environment.

Elucidating redox pathways for N2O selective catalytic reduction with NO and NH3 over Fe-chabazite zeolites

We combined kinetics and in situ X-ray absorption spectroscopy to investigate redox pathways of N2O-selective catalytic reduction (SCR) by NH3 and NO over Fe-exchanged Chabazite zeolites, a strategy to mitigate emissions of greenhouse gas N2O and toxic NOx from sources such as NH3 engines. N2O-SCR occurs via FeII/FeIII redox cycles with N2O as the oxidant, and parallel reactions involving NO+NH3 or NH3 as reductants, where in situ XAS shows that most Fe ions are redox-active. NO co-reduces FeIII with NH3 rather than oxidizing to NO2. Net rates of N2O-SCR in gas mixtures containing NH3 versus NO+NH3 are both limited by FeII oxidation, resulting in similar apparent activation energies. In contrast, reduction pathway selectivity reflects the intrinsic kinetics of FeIII reduction steps with NO+NH3 versus NH3, implying that reduction involving NO+NH3 dominates at lower temperatures and higher NO pressures. This work provides fundamental insights into kinetics and mechanisms of N2O-SCR.

Dose Effect of Drinking Water Nitrate on Health, Feed Intake, Rumen Fermentation and Microbiota, and Nitrogen Excretion in Holstein Heifers for a Sustainable Water Use

The present study aimed to evaluate the potential hazardous effects of NO3− concentration in drinking water on health, feed intake, rumen fermentation and microbiota, and nitrogen excretion of Holstein heifers fed a high-concentrate diet for a sustainable water use. Twenty-four Holstein heifers were individually allocated and assigned to one of four treatments with increasing drinking water NO3− concentration: CTR, without NO3−; LOW, with 44 mg NO3−/L; MOD, with 110 mg NO3−/L; and HIGH, with 220 mg NO3−/L. The entire study lasted 168 days. Fortnightly water NO3− concentration and daily feed and water intake were recorded. Blood parameters, rumen pH, volatile fatty acids, NO3− and NO2− concentration, microbiota, and apparent total tract digestibility were determined at the beginning and at the end of the study. Most of the analyzed parameters were similar among treatments. Denitrifying bacteria population, estimated as nosZ gene copies, were greater in HIGH animals than in CTR animals at the end of the study. In conclusion, drinking water NO3− concentration up to 220 mg/L has no detrimental effect on health, feed intake, rumen fermentation, nor N excretion in dairy beef cattle for periods up to 168 days; moreover, denitrifying bacteria population increased, which are related with the neutralization of the greenhouse gas N2O.

Moderate effects of distance to air-filled macropores on denitrification potentials in soils

AbstractDenitrification is a major source of the greenhouse gas N2O. As a result of spatial heterogeneity of organic carbon, oxygen and nitrate, denitrification is observed even under relatively dry conditions. However, it is unclear whether denitrification potentials of microbial communities exhibit spatial patterns relative to variations in distance to soil pores facilitating oxygen exchange and nutrient transfer. Thus, we determined genetic and process-level denitrification potentials in two contrasting soils, a cropland and a grassland, with respect to the distance to air-filled pores. An X-ray computed tomography aided sampling strategy was applied for precise sampling of soil material. Process-level and genetic denitrification potentials in both soils were spatially variable, and similar with respect to distance to macropores. In the cropland soil, a minor increase of process-level potentials with distance to pores was observed and related to changes in NO3− rather than oxygen availability. Genetic denitrification potentials after the short-term incubations revealed a certain robustness of the local community. Thus, distance to macropores has a minor impact on denitrification potentials relative to the observed spatial variability. Our findings support the notion that the impact of macropore induced changes of the environmental conditions in soil does not overrule the high spatial variability due to other controlling factors, so that the rather minor proportion of spatial heterogeneity of functional genes and activity potentials related to macropore distances in soil need not be considered explicitly in modelling denitrification.

Determining how oxygen legacy affects trajectories of soil denitrifier community dynamics and N2O emissions

Denitrification – a key process in the global nitrogen cycle and main source of the greenhouse gas N2O – is intricately controlled by O2. While the transition from aerobic respiration to denitrification is well-studied, our understanding of denitrifier communities’ responses to cyclic oxic/anoxic shifts, prevalent in natural and engineered systems, is limited. Here, agricultural soil is exposed to repeated cycles of long or short anoxic spells (LA; SA) or constant oxic conditions (Ox). Surprisingly, denitrification and N2O reduction rates are three times greater in Ox than in LA and SA during a final anoxic incubation, despite comparable bacterial biomass and denitrification gene abundances. Metatranscriptomics indicate that LA favors canonical denitrifiers carrying nosZ clade I. Ox instead favors nosZ clade II-carrying partial- or non-denitrifiers, suggesting efficient partnering of the reduction steps among organisms. SA has the slowest denitrification progression and highest accumulation of intermediates, indicating less functional coordination. The findings demonstrate how adaptations of denitrifier communities to varying O2 conditions are tightly linked to the duration of anoxic episodes, emphasizing the importance of knowing an environment’s O2 legacy for accurately predicting N2O emissions originating from denitrification.

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.

Relevance and prediction of N2O in small-scale multi-fuel biomass furnaces using primary NOx reduction measures

The relevance of the greenhouse gas N2O was investigated in two small-scale biomass combustion plants, a 30-kW fixed bed and a 70-kW moving grate furnace, both of which use double air staging. Furthermore, the 70-kW furnace was simulated with ideal reactor models, applying a detailed nitrogen chemistry mechanism to gain insights into N2O formation mechanisms that occur during double air-staged combustion.The experimental and simulated results confirm the existence of correlations between CO, NOx and N2O. For all investigated fuels, N2O reached the highest levels (increase of up to 300 %) when high CO and low NOx concentrations were present. Therefore, caution is advised when looking for minimum NOx emissions, due to the risk of having high N2O emissions, an aspect which is often overlooked.A deeper analysis of the N2O formation mechanisms revealed that N2O is mainly generated from HCN in the oxidation zone and it is thermally dissociated at high temperatures. Finally, a comparison between the results of both plants showed that the concern about high N2O emissions at minimum NOx concentrations is not a reactor-specific problem; therefore, it is necessary to ensure that CO and N2O are kept at a low level during NOx reduction with primary measures.

Nitrous oxide respiration in acidophilic methanotrophs

Aerobic methanotrophic bacteria are considered strict aerobes but are often highly abundant in hypoxic and even anoxic environments. Despite possessing denitrification genes, it remains to be verified whether denitrification contributes to their growth. Here, we show that acidophilic methanotrophs can respire nitrous oxide (N2O) and grow anaerobically on diverse non-methane substrates, including methanol, C-C substrates, and hydrogen. We study two strains that possess N2O reductase genes: Methylocella tundrae T4 and Methylacidiphilum caldifontis IT6. We show that N2O respiration supports growth of Methylacidiphilum caldifontis at an extremely acidic pH of 2.0, exceeding the known physiological pH limits for microbial N2O consumption. Methylocella tundrae simultaneously consumes N2O and CH4 in suboxic conditions, indicating robustness of its N2O reductase activity in the presence of O2. Furthermore, in O2-limiting conditions, the amount of CH4 oxidized per O2 reduced increases when N2O is added, indicating that Methylocella tundrae can direct more O2 towards methane monooxygenase. Thus, our results demonstrate that some methanotrophs can respire N2O independently or simultaneously with O2, which may facilitate their growth and survival in dynamic environments. Such metabolic capability enables these bacteria to simultaneously reduce the release of the key greenhouse gases CO2, CH4, and N2O.

Soil gross N2O emission and uptake under two contrasting agroforestry systems: riparian tree buffer versus alley-cropping tree row

In addition to the removal of excess mineral nitrogen (N) via root uptake, trees in agroforestry systems may mitigate negative effects of high N fertilization of adjacent crops by enhancing complete denitrification of excess mineral N aside from root uptake. Presently, little is known about the potential for NO3− reduction through denitrification (conversion to greenhouse gas N2O and subsequently to non-reactive N2) in contrasting agroforestry systems: riparian tree buffer versus tree row of an upland alley-cropping system. Our study aimed to (1) quantify gross N2O emissions (both N2O + N2 emissions) and gross N2O uptake (N2O reduction to N2), and (2) determine their controlling factors. We employed the 15N2O pool dilution technique to quantify gross N2O fluxes from 0 to 5 cm (topsoil) and 40 to 60 cm (subsoil) depths with seasonal field measurements in 2019. The riparian tree buffer exhibited higher topsoil gross N2O emissions and uptake than the alley-cropping tree row (P < 0.03). Gross N2O emissions were regulated by N and carbon (C) availabilities and aeration status rather than denitrification gene abundance. Gross N2O uptake was directly linked to available C and nirK gene abundance. In the subsoil, gross N2O emission and uptake were low in both agroforestry systems, resulting from low mineral N contents possibly due to N uptake by deep tree roots. Nonetheless, the larger available C and soil moisture in the subsoil of riparian tree buffer than in alley-cropping tree row (P < 0.05) suggest its large potential for N2O uptake whenever NO3− is transported to the subsoil.

Inventory and Distribution Characteristics of Carbon Emissions from Agricultural Sources in Henan Province from 2011 to 2020

Agriculture is an important part of Henan's economic development, and agricultural production is also an important source of greenhouse gas emissions. In this paper, the activity level data of agricultural carbon emissions in 18 cities in Henan Province were collected. Based on the calculation method provided by the Guidelines for Compiling Provincial Greenhouse Gas Inventories and referring to the 2006 IPCC Guidelines for National Greenhouse Gas Inventories, agricultural CO2, CH4 and N2O emissions were carefully estimated. An agricultural greenhouse gas inventory was compiled for Henan Province from 2011 to 2020. Then, based on the spatial distribution and emission intensity, the carbon emissions of each city in Henan Province in 2019 were further analyzed. The results show that carbon emissions decreased from 57,603,500 tons in 2011 to 44,517,300 tons in 2020, with an average annual decrease rate of about 2.66%. The total agricultural carbon emissions in Henan showed a downward trend, and agricultural land was the dominant factor of carbon emissions, accounting for about 47% of the total carbon emissions over the years.

Revisiting the metal sites of nitrous oxide reductase in a low-dose structure from Marinobacter nauticus

Copper-containing nitrous oxide reductase catalyzes a 2-electron reduction of the green-house gas N2O to yield N2. It contains two metal centers, the binuclear electron transfer site CuA, and the unique, tetranuclear CuZ center that is the site of substrate binding. Different forms of the enzyme were described previously, representing variations in oxidation state and composition of the metal sites. Hypothesizing that many reported discrepancies in the structural data may be due to radiation damage during data collection, we determined the structure of anoxically isolated Marinobacter nauticus N2OR from diffraction data obtained with low-intensity X-rays from an in-house rotating anode generator and an image plate detector. The data set was of exceptional quality and yielded a structure at 1.5 Å resolution in a new crystal form. The CuA site of the enzyme shows two distinct conformations with potential relevance for intramolecular electron transfer, and the CuZ cluster is present in a [4Cu:2S] configuration. In addition, the structure contains three additional types of ions, and an analysis of anomalous scattering contributions confirms them to be Ca2+, K+, and Cl–. The uniformity of the present structure supports the hypothesis that many earlier analyses showed inhomogeneities due to radiation effects. Adding to the earlier description of the same enzyme with a [4Cu:S] CuZ site, a mechanistic model is presented, with a structurally flexible CuZ center that does not require the complete dissociation of a sulfide prior to N2O binding.Graphical The [4Cu:2S] CuZ site in M. nauticus N 2O reductase. The electron density map shown is contoured at the 5 σ level, highlighting the presence of two sulfide ligands. 705x677mm (72 x 72 DPI)

Impact of aerobic granular sludge sizes and dissolved oxygen concentration on greenhouse gas N2O emission

Aerobic granular sludge (AGS) at wastewater treatment plants (WWTPs) are known to produce nitrous oxide (N2O), a greenhouse gas which has a ∼300 times higher global warming potential than carbon dioxide. In this research, we studied N2O emissions from different sizes of AGS developed at a dissolved oxygen (DO) level of 2 mgO2/L while exposing them to disturbances at various DO concentrations ranging from 1 to 4 mgO2/L. Five different AGS size classes were studied: 212–600 µm, 600–1000 µm, 1000–1400 µm, 1400–2000 µm, and > 2000 µm. Metagenomic data showed N2O reductase genes (nosZ) were more abundant in the smaller AGS sizes which aligned with the observation of higher N2O reduction rates in small AGS under anaerobic conditions. However, when oxygen was present, the activity measurements of N2O emission showed an opposite trend compared to metagenomic data, smaller AGS (212 to 1000 µm) emitted significantly higher N2O (p < 0.05) than larger AGS (1000 µm to >2000 µm) at DO of 2, 3, and 4 mgO2/L. The N2O emission rate showed positive correlation with both oxygen levels and nitrification rate. This pattern indicates a connection between N2O emission and nitrification. In addition, the data suggested the penetration of oxygen into the anoxic zone of granules might have hindered nitrous oxide reduction, resulting in incomplete denitrification stopping at N2O and consequently contributing to an increase in N2O emissions. This work sets the stage to better understand the impacts of AGS size on N2O emissions in WWTPs under different disturbance of DO conditions, and thus ensure that wastewater treatment will comply with possible future regulations demanding lowering greenhouse gas emissions in an effort to combat climate change.

Exploring Si-centered phthalocyanine as a single atom catalyst for N2O reduction: a DFT study.

To remove the greenhouse gas N2O from the environment, recently, researchers have taken great interest in single-atom catalysts (SACs). In this study, we investigated various reaction pathways and barrier energies for the N2O reduction process onto Si-coordinated phthalocyanine (Si@PthC) employing density functional theory. The outcomes validate that Si decoration in PthC is energetically stable while the corresponding electronic properties show that the Si atom acts as the reactive site for catalytic activity. The N2O molecule exhibits spontaneous dissociation over the catalyst surface from the O-end with -4.01 eV dissociation energy. Meanwhile, N2O dissociation via the N-end involves chemisorption onto the Si@PthC surface with an adsorption energy (Ead) of -1.16 eV, and the dissociation needs an energy barrier of 0.51 eV. The bond distances and negative adsorption energies (-1.11 and -2.40 eV) evince that CO and O2 species chemisorbed onto the Si@PthC surface. However, these energies are smaller than the N2O dissociation energy, which demonstrates that the presence of CO and O2 molecules cannot interrupt the N2O reduction process. Additionally, the CO + O* → CO2 reaction was executed for catalyst recovery, and the reaction proceeds very quickly on the Si@PthC catalyst, with a very small energy barrier (0.37 eV), indicating the excellent catalytic reactivity of the studied catalyst. These results propose that the designed catalyst can be valuable in the progress of novel noble metal-free catalysts for the elimination of harmful N2O from the environment.

氮磷添加下典型温带、亚热带森林土壤氮循环功能基因丰度和微生物群落属性数据集

Nitrogen (N) and phosphorus (P) are essential nutrients for soil microbial growth and activities. There are notable differences in the concentrations of N and P and the characteristics of microbial communities observed between temperate and subtropical forests soils, and this is also true for soil vertical profiles. As a consequence of the rise in global atmospheric N deposition, soil nutrient imbalances and P limitation are increasingly aggravated in eastern China. However, there is a lack of systematic dataset showing how N deposition and P addition affect soil N cycling microbes and soil physicochemical properties in eastern China; hence a comprehensive dataset is needed to a better understanding of the impact of N deposition and P addition on soil nitrogen cycle. This dataset is constructed based on the field experimental setup in the forests of Chinese Ecosystem Research Network (CERN). To obtain a systematic dataset on N-cycling microbial communities, we conducted measurements and collected data of soil N-cycling functional genes abundance, N-cycling microbial community diversities and compositions and enzyme activities in three typical forests with N and/or P additions. We collected 0-10 cm top soils from a temperate forest (Changbai Mountain) and two subtropical forests (Qianyanzhou and Dinghu Mountain) with field N and/or P additions, and the soils along 0-80 cm vertical profiles without nutrient additions. The N-cycling functional genes involved in the datasets cover ammonia oxidizing archaea amoA, ammonia oxidizing bacteria amoA, nirK, nirS, nosZ, qnorB, narG, nir, nifH and chiA. The potential activities included in the datasets cover nitrification activity, denitrification activity, nitrogen fixation activity and organic nitrogen decomposition enzyme activity. The datasets also include soil physiochemical properties, including soil pH, moisture content, N2O emission, net nitrification rate and the concentrations of organic carbon, NH4+ , NO3− , available phosphorus, total nitrogen, total carbon, total phosphorus and dissolved organic carbon. The creation and sharing of the datasets can provide data and support for understanding the microbial mechanisms of soil N-cycling and the modelling processes under the scenario of aggravated N deposition and P addition. The datasets will also provide support for forest management efforts with regard to greenhouse gas N2O emission, N and nutrient loss in forest ecosystems.

Potential Risk of Significant N2O Emission without Changing NOx Conversion on Commercial V2O5/TiO2 Catalyst under Working Conditions.

Vanadium-based catalysts play a pivotal role in the emission control of industrial NOx via selective catalytic reduction (SCR) technology. However, little attention has been paid to the potential emission of greenhouse gas N2O under complex working conditions. This work reports that a commercial V2O5/TiO2 catalyst may lead to significant N2O emission without greatly changing the outlet NOx concentration after chromium (Cr) deposition. With a Cr loading of 2 wt %, N2O concentration increased from 27.8 to 199.2 ppm at 350 °C with the value of outlet N2O/(N2O+N2) from 2.5% to 19.4%. Experimental results combined with DFT+U calculations suggest that nonselective catalytic reduction (NSCR) is the main route for N2O formation in a wide temperature range of 250 ∼ 400 °C. It is stemmed from the fact that the covalent interaction between Cr and V species on the V2O5/TiO2 surface accelerates the conversion of V4+ + Cr6+ → V5+ + Cr3+, leading to a larger proportion of surface V5+. More importantly, surface V5+ is highly related to the redox property of the V2O5/TiO2 catalyst, which is beneficial to NSCR reaction rather than the standard SCR process. The work suggests that to better inhibit the emission of greenhouse gases during the NH3-SCR process, monitoring N2O emission should be included along with the NOx concentrations, especially in complex flue gases.

Spatial distribution characteristics of denitrification functional genes and the environmental drivers in Liaohe estuary wetland.

Genes nirS, nirK, and nosZ are specific for the denitrification process, which is associated with greenhouse gas N2O emission. The abundances and diversities of community containing these three genes are usually used as a common index to reflect the denitrification process, and they would be affected by differences in environmental factors caused by changes from warm to cold conditions. The quantification of denitrification in natural wetlands is complex, and straightforward identification of spatial distribution and drivers affecting the process is still developing. In this study, the bacterial communities, gene diversities, and relative abundances involved in denitrification were investigated in Liaohe Estuary Wetland. We analyzed the relative abundances, diversities, and communities of bacteria containing the three genes at warm and cold conditions using Illumina MiSeq sequencing and detected the potential environmental factors influencing their distribution by using a random forest algorithm. There are great differences in the community composition of the bacteria containing genes nirS, nirK, and nosZ. All the abundant taxa of nirS and nirK communities belonged to phylum Proteobacteria. Compared with the community composition of bacteria containing nirS and nirK, the community of bacteria containing nosZ is more diverse, and the subdivision taxa of phylum Euryarchaeota was also abundant in the community containing nosZ. The distribution characteristics of the relative abundance of nirS and nirK showed obvious differences both at warm and cold climate conditions. The oxidation-reduction potential, nitrite nitrogen, and salinity were detected as potential variables that might explain the diversity of nirS. The total nitrogen and nitrite nitrogen were the important variables for predicting the relative abundance of nirS at warm climate condition, while oxidation-reduction potential and pH contributed to the diversity of nirS at cold condition. The bulk density of sediment was detected as a potential variable affecting the relative abundance of nirK at warm and cold conditions, and diversity of nirK at warm condition, while nitrite nitrogen was detected as an important environmental factor for predicting the diversity of nirK at cold condition. Overall, our results show that the key environmental factors, which affect the relative abundance, diversity, and community of bacteria containing the functional denitrification genes, are not exactly the same, and the diversities of nirS, nirK, and nosZ have a higher environmental sensitivity than their relative abundances.

Graphdiyne as an Electron Modifier for Boosting Electrochemical Production of Adipic Acid

AbstractAdipic acid (AA) is a crucial feedstock for nylon polymers, and is industrially produced by thermal oxidation of cyclohexanone/cyclohexanol mixture (KA oil). However, this process consumes large quantities of corrosive nitric acid as oxidants, while emits ozone‐depleting greenhouse gas N2O. Here, an electrocatalytic strategy for selective oxidation of KA oil to AA coupled with H2 evolution over a Co3O4/graphdiyne cooperative catalyst (Co3O4/GDY) is reported. The Co3O4/GDY displays high electrooxidation activity of KA oil to AA (100 mA cm−2 at ≈1.5 V vs RHE), outperforming all the reported findings. Detailed ex situ and in situ experimental studies, theoretical calculations, and molecular dynamic simulations reveal that GDY not only facilitates the enrichment of cyclohexanone on the catalyst surface in aqueous medium, but also upshifts the d‐band center of Co sites, strengthening the adsorption/activation of cyclohexanone. This study offers a green route for AA synthesis and proposes a GDY interface engineering strategy for efficient electrooxidation.

Estimated mangrove carbon stocks and fluxes to inform MRV for REDD+ using a process-based model

Mangrove forests are important due to their strong capability for carbon storage, especially in soils. Understanding carbon dynamics in these forests is fundamental to estimate their roles in carbon storage and mitigating climate change. This study used a process-based model, MCAT-DNDC, to assess mangrove carbon sequestration and fluxes at a 30-m spatial resolution in three African countries, Gabon, Mozambique and Tanzania. The simulated above- and below-ground biomass at inventory plots in each country was approximate to actual observations with mean errors <5% for aboveground biomass and <8% for belowground biomass, indicating that the MCAT-DNDC model can be a useful tool for assessing mangrove carbon storage and fluxes. The results from assessing mangrove carbon storage and fluxes for the three countries showed that the mangroves in these countries are large carbon pools, they export large amounts of dissolved and particulate carbon components to riverine and oceanic ecosystems, and they bury a large amount of carbon in soils. However, soil-borne greenhouse gases CO2, CH4 and N2O fluxes from mangrove forest lands were low. There were large differences in all mangrove carbon components among the mangroves in the three countries, indicating that regional or global mangrove carbon stocks estimated using a process-based model may be better than the extrapolations using limited inventories.

Suggested role of NosZ in preventing N2O inhibition of dissimilatory nitrite reduction to ammonium.

Dissimilatory nitrate/nitrite reduction to ammonium (DNRA) is a microbial energy-conserving process that reduces NO3 - and/or NO2 - to NH4 +. Interestingly, DNRA-catalyzing microorganisms possessing nrfA genes are occasionally found harboring nosZ genes encoding nitrous oxide reductases, i.e., the only group of enzymes capable of removing the potent greenhouse gas N2O. Here, through a series of physiological experiments examining DNRA metabolism in one of such microorganisms, Bacillus sp. DNRA2, we have discovered that N2O may delay the transition to DNRA upon an oxic-to-anoxic transition, unless timely removed by the nitrous oxide reductases. These observations suggest a novel explanation as to why some nrfA-possessing microorganisms have retained nosZ genes: to remove N2O that may otherwise interfere with the transition from O2 respiration to DNRA.