RESUMEN
Waste-derived nitrogen-containing porous carbons were widely accepted as promising carbon capture materials. However, roles of nitrogen in CO2 uptake were highly controversial, posing a challenge in designing high CO2 uptake porous carbons. Herein, nitrogen-containing species was firstly introduced into machine learning (ML) models to uncover the complex relationship of nitrogen, micropore and CO2 uptake by combining ML models, DFT computations and experiments. The results revealed that micropore volume (Vmicro) was the most important property influencing CO2 uptake, but was not the only determinant factor. Nitrogen-containing species (pyrrolic/pyridonic-N (N5) and pyridinic-N (N6)) rather than total nitrogen content, also played an essential role. On the one hand, they can enhanced CO2 adsorption by Lewis acid-base and hydrogen bonding. On the other hand, they promoted development of micropores by participating in activation reactions. The model further indicated that excessive N5 (>1.5 wt%) or N6 (>1.7 wt%) led to restriction on developments of micropores, which was attributed to enlargement of pore size, collapses or blockage of micropores. The double edged-sword effect of N5 and N6 on changes of microporous structures was responsible for the long-standing controversy over nitrogen. The result was further verified by synthesizing eight porous carbons with different textural and chemical properties. This study provided not only a new perspective for resolving the controversy of nitrogen in CO2 uptake, but also a graphical user interface prediction software meaningful for designing porous carbons.
RESUMEN
Organophosphate flame retardants (OPFRs) are widely used in consumer products, leading to their unavoidable release into the environment, especially accumulation in anaerobic environments and posing potential risks. This study focused on Tris(2-chloroethyl) phosphate (TCEP), a representative OPFR, to investigate its effects on carbon transformation and methane production in anaerobic digestion. Increasing TCEP concentrations from control to 16 mg/L resulted in decreased cumulative methane yield (from 235.4 to 196.3 mL/g COD) and maximum daily methane yield (from 40.8 to 16.17 mL/(g COD·d)), along with an extended optimal anaerobic digestion time (from 15 to 20 days). Mechanistic analysis revealed TCEP binding to tyrosine-like proteins in extracellular polymeric substances, causing cell membrane integrity impairment. The TCEP-caused alteration of the physiological status of cells was demonstrated to be a significant contribution to the inhibited bioprocesses including acidogenesis, acetogenesis, and methanogenesis. Illumina Miseq sequencing showed TCEP decreasing the relative abundance of acidogens (58.8 % to 46.0 %) and acetogens (7.1 % to 5.0 %), partly shifting the methanogenesis pathway from acetoclastic to hydrogenotrophic methanogenesis. These findings enhance understanding of TCEP's impact on anaerobic digestion, emphasizing the environmental risk associated with its continued accumulation.
Asunto(s)
Retardadores de Llama , Metano , Organofosfatos , Metano/metabolismo , Anaerobiosis , Organofosfatos/metabolismo , Organofosfatos/toxicidad , Retardadores de Llama/metabolismo , Retardadores de Llama/toxicidad , Reactores Biológicos , Microbiota/efectos de los fármacos , Bacterias/metabolismo , Bacterias/efectos de los fármacosRESUMEN
The effects of grazing on the cycling of carbon (C), nitrogen (N) and phosphorus (P) in grassland ecosystems are complex. Uncertainty still exists as regards the allocation of C, N and P storage amounts in grazed ecosystems in Inner Mongolia, situated at the eastern end of the Eurasian dryland. Based on the long-term cattle grazing experimental platform in the Hulun Buir meadow steppe of Inner Mongolia, a 3-year (2019-2021) field control experiment was conducted to assess how the grazing intensity influenced the quantities of C, N and P stored in canopy biomass, root, litter and soil compartments. We examined the relationships between the different pools and their regulatory pathways at the ecosystem level across six grazing intensities. In general, grazing increased the aboveground N and P contents but decreased the aboveground biomass C content and nutrient storage amounts in aboveground biomass, roots and litter. The grazing intensity of 0.34 AU ha-1 increased soil organic carbon, total nitrogen and total phosphorus storage amounts, with the soil accounting for 98 % of total reserves on average. Grazing affected soil pHï¼ nutrient contents, above- and belowground biomass and soil environmental factors such as soil bulk density, which in turn affected C, N and P storage in the ecosystem according to the results of the structural equation model; therefore, grazing intensity can be an important factor regulating the input and output of nutrients in the ecosystem. In the future, for adaptive management of grasslands, moderate grazing could effectively increase C, N and P storage in meadow steppe ecosystems and ensure the nutrient balance and long-term sustainable development.
Asunto(s)
Ecosistema , Pradera , Animales , Bovinos , Carbono/análisis , Fósforo , Suelo/química , Nitrógeno/análisis , Plantas , Biomasa , ChinaRESUMEN
Soil acidifications become one of the main causes restricting the sustainable development of agriculture and causing issues of agricultural product safety. In order to explore the effect of different acidification on soil cadmium (Cd) availability, soil pot culture and hydroponic (soil potting solution extraction) were applied, and non-invasive micro-test technique (NMT) was combined. Here three different soil acidification processes were simulated, including direct acidification by adding sulfuric acid (AP1), acid rain acidification (AP2) by adding artificial simulated acid rain and excessive fertilization acidification by adding (NH4)2SO4 (AP3). The results showed that for direct acidification (AP1), DTPA-Cd concentration in field soils in Liaoning (S1) and Zhejiang (S2) increased by 0.167 - 0.217 mg/kg and 0.181 - 0.346 mg/kg, respectively, compared with control group. When soil pH decreased by 0.45 units in S1, the Cd content of rice stems, leaves and roots increased by 0.48 to 6.04 mg/kg and 2.58 to 12.84 mg/kg, respectively, When the pH value of soil S1 and S2 decreased by 0.20 units, the average velocity of Cd2+ at 200 µm increased by 10.03 - 33.11 pmol/cm2/sec and 21.33 -52.86 pmol/cm2/sec, respectively, and followed the order of AP3 > AP2 > AP1. In summary, different acidification measures would improve the effectiveness of Cd, under the same pH reduction condition, fertilization acidification increased Cd availability most significantly.
Asunto(s)
Lluvia Ácida , Oryza , Contaminantes del Suelo , Cadmio/toxicidad , Cadmio/análisis , Suelo/química , Oryza/química , Contaminantes del Suelo/toxicidad , Contaminantes del Suelo/análisis , Concentración de Iones de HidrógenoRESUMEN
Both soil irrigation and sulfur (S) are associated with the precipitation of cadmium (Cd)-sulfide in paddy soil, their interaction affecting on Cd solubility and extractability is still unknown. This study primarily discusses the effect of exogenous S addition on the bioavailability of Cd in paddy soil under unsteady pe + pH conditions. The experiment was treated with three different water strategies: continuous dryness (CD), continuous flooding (CF), and alternating dry-wet cycles for one cycle (DW). These strategies were combined with three different S concentrations. The results indicate that the CF treatment, particularly when combined with S addition, had the most significant effect on reducing pe + pH and Cd bioavailability in the soil. The reduction of pe + pH from 10.2 to 5.5 resulted in a decrease in soil Cd availability by 58.3%, and Cd accumulation in rice grain by 52.8%, compared to the other treatments. While it was more conducive to the formation of iron plaque on the root surface in DW treatment with S addition at rice maturing stage and enhanced the gathering of Fe/S/Cd. Structural equation model (SEM) analysis further confirmed a significant negative correlation (r = -0.916) between the abundance of soil Fer-reducing bacteria (FeRB) and sulfate-reducing bacteria (SRB) like Desulfuromonas, Pseudomonas, Geobacter, and the Cd content in rice grains. This study provides a basic mechanistic understanding of how soil redox status (pe + pH), S addition, and FeRB/SRB interacted with Cd transfer in paddy soil-rice tissues.
Asunto(s)
Desulfovibrio , Oryza , Contaminantes del Suelo , Suelo/química , Oryza/química , Cadmio/análisis , Contaminantes del Suelo/análisis , Hierro/análisis , Bacterias , Concentración de Iones de HidrógenoRESUMEN
Microplastics (MPs) and Cd have been proven to inhibit methane production from anaerobic digestion of sewage sludge. However, the published studies mainly focused on their single inhibition. This cannot reflect the real-world situations where MPs and Cd co-exist. This study therefore aims to reveal the combined effect of MPs and Cd on anaerobic digestion of sewage sludge. Experimental results showed that PVC-MPs at environmentally relevant levels (e.g., 1, 10 particles/g total solids (TS)) did not affect methane yield but decrease the toxicity of Cd. When PVC-MPs were 30 particles/g TS, the cumulative methane production recovered from 58.8 % (in the presence of 5 mg Cd/g TS) to 89.7 % of the control. Organic fluxes were significantly increased compared with the control, particularly affecting the content of dissolved substances and short-chain fatty acids during anaerobic digestion. Mechanistic exploration showed that the adsorption of Cd by PVC-MPs was higher than that of sludge-substrate, which reduced the bioavailability of Cd by anaerobes, as evidenced by the increased anaerobes driven carbon flux from solid-phase to bio-methane during anaerobic digestion. Overall, these findings identified important factors in determining the toxicity of pollutants on anaerobic digestion process, providing precise data for toxicity evaluation of MPs and metals in anaerobic environment.
Asunto(s)
Microplásticos , Aguas del Alcantarillado , Aguas del Alcantarillado/química , Cadmio/toxicidad , Plásticos , Anaerobiosis , Reactores Biológicos , MetanoRESUMEN
Soil nitrogen (N) supply is essential in influencing plant functional traits and regulating plant morphological and physiological performances. The effects of N on plants can be altered by complex environmental changes. However, conflicting results have been reported on the co-effects of N and climatic variables on plant performance, which may be attributed to differences in experiment setting and approach, e.g., ecosystem, duration, plant type, and fertilizer form. To elucidate the general response of plant performance to increasing soil N availability under climate change, a global meta-analysis was conducted to synthesize 380 publications studying interactions of N enrichment and four climatic variables (e.g., elevated atmospheric CO2 (eCO2), drought, precipitation, and warming) on performance-related traits (e.g., size, nutrient, and fitness). Results showed that N enrichment increased shoot and root size, nutrient, and fitness of terrestrial plants. The synergistic interactions of N × eCO2 and antagonistic interactions of N × drought were found on plant overall performance (mainly on plant size), indicating that the N effects can be aggregated by eCO2 and mitigated by drought. The co-effects of N and climatic variables on plant overall performance rely on experiment approach, duration, ecosystem type, or plant functional type. Synergistic interactions of N × eCO2 and antagonistic interactions of N × drought, N × precipitation, and N × warming on plant overall performance were found mainly in greenhouse experiments and short-term experiments (duration ≤ one year), but not in the field or longer-term experiments. The results highlighted that N effects on plant performance were not isolated, but can be modified by climate changes. These findings can improve the future modeling predictions of plant performance under complex climate change and provide a fundamental basis for N management strategies to optimize plant performance in production, N nutrient, and reproduction while enabling sustainability of plant production systems.