CH4 Concentrations Research Articles

Carbon dioxide emissions from temperate reservoirs and pit lakes of different trophic states

The abundance of human-made inland waters, such as artificial ponds and reservoirs, has multiplied over the last decades. Compared to natural lakes, reservoirs and retention basins can exhibit a higher accumulation of organic carbon and a higher emission of greenhouse gases. Magnitude and dynamics of related emission fluxes are important to understand the role of inland waters in the global carbon cycle. However, origin and use of artificial waterbodies are diverse, and it is unclear whether current gas flux estimates adequately represent all important types and conditions of artificial inland waters. This study compares drivers of CO2 and CH4 emissions from two types of temperate artificial waters that are widespread in central Europe: reservoirs and artificial lakes in former open-pit lignite mines (pit lakes). We measured CO2 exchange at the water surface, calculated surface water CO2 from long-term DIC and pH data, and measured CO2 and CH4 concentrations throughout the water column. We found that an older, eutrophic pit lake showed seasonal variations in CO2 fluxes including uptake during summer and release during turnover, similar to three studied freshwater reservoirs. In contrast, reacidification and repeated addition of carbonate (liming) led to sustained CO2 supersaturation in a young, oligotrophic pit lake throughout the year, potentially making it a steady source of CO2 to the atmosphere. This implies that on an annual level, pH regulation and lake maturity largely determine whether pit lakes act as sources of CO2 (young, slightly acidic) or sinks of CO2 (older, neutral pH).

The Influence of the Fire Point on the Thermal Dynamic Disaster in the Goaf

A thermal dynamic disaster in the goaf is one of the most serious coal mine disasters formed by coal spontaneous combustion and gas interweaving. However, the influence of the high-temperature hidden fire source formed in the goaf on the evolution law of thermal dynamic disasters is not clear, and effective prevention and control measures cannot be taken. Therefore, this paper uses the experimental platform of thermal dynamic disaster in the goaf to study the influence of different fire point positions on the development of thermal dynamic disaster in the goaf through a similar simulation experiment of thermal dynamic disaster evolution in the goaf and analyzes the corresponding relationship between temperature and CO concentration in the upper corner. The results show that under different locations of heat source, the high-temperature heat source of coal spontaneous combustion migrates to the air leakage side with sufficient oxygen supply, and an oxygen-poor circle is formed near the ignition point. Under the action of air leakage flow, CH4 accumulates in the deep part of the goaf on the return air side. Due to the increase in coal, part of CH4 is produced, which leads to the increase in concentration of CH4 at the ignition point. Under the action of different heat sources, the changing trend of concentration of CO and temperature in the return air corner is the same, but the temperature change in the return air corner shows a lag compared with the change in the concentration of CO, so concentration monitoring of CO can reflect the evolution process of the fire field in the goaf more quickly than temperature monitoring.

Land use and urbanization indirectly control riverine CH4 and CO2 emissions by altering nutrient input

Urban rivers are recognized as significant sources of methane (CH4) and carbon dioxide (CO2) emissions. Despite this, the influence of land use and urbanization on carbon emissions across rural-urban rivers at the watershed scale has been insufficiently explored. This study utilized in-situ surveys of the Liao River in northern China to investigate the spatial and temporal variations of CH4 and CO2 emissions and their relationship with urbanization and its potential controlling factors. The findings revealed that CH4 emissions peaked in fall, whereas CO2 emissions were highest in summer. The average fluxes of CH4 and CO2 at the water-gas interface were 1387.22 ± 2474.98 µmol·m−2·d−1 and 52.78 ± 54.44 mmol·m−2·d−1, respectively. Water quality parameters accounted for 80.49 % of the total variation in CH4 and CO2 concentrations and fluxes. Structural equation modeling indicated that TN, TP, DTC, and conductivity had direct effects on riverine CH4 and CO2 emissions, with standardized direct effects of 0.50 and 0.49, respectively. Nutrient input emerged as the primary driver, increasing CH4 and CO2 concentrations and fluxes, particularly in urban-adjacent river sections likely receiving higher nutrient loads. This study underscores that land use and urbanization indirectly influence riverine CH4 and CO2 emissions by modifying nutrient inputs. Effective land use management and nutrient input control are recommended strategies to mitigate riverine CH4 and CO2 emissions.

The effect of CO content on CH4/CO/H2 rotating detonation wave propagation characteristics

Rotating detonation experiments were conducted using CH4/CO/H2 (methane/carbon monoxide/hydrogen) mixtures with varying CO contents, the modes of rotating detonation wave (RDW) propagation in the mixtures were analyzed, and the impact of CO content on the propagation characteristics of the RDW in the gas mixture was compared. Three propagation modes of RDW were observed: sawtooth wave mode, mixed mode, and single wave mode. An increase in the CO content resulted in an upward shift in the range of working equivalence ratios for different gas mixtures. Additionally, the propagation modes of the same gas mixture change with increased fuel flow rate. When the equivalence ratio is below 1.13, it is observed that the gas mixture with the lowest CO content exhibits the highest RDW velocity and the shortest time required to establish RDW. This was attributed to the higher content of oxygen-containing functional groups, such as OH (hydroxyl), HO2 (peroxyhydroxyl), and O (oxygen atom), which were present under lean combustion conditions, along with the highest mass content of H2 in the gas mixture with the lowest CO content. Conversely, for equivalence ratios above 1.13, it is observed that the gas mixture with the highest CO content exhibits the highest propagation velocity and the shortest time required to establish RDW. This was attributed to the lowest mass content of CH4 and H2 in the gas mixture with the highest CO content at the same equivalence ratio, along with the inhibitory effect of elevated CO content on CH4 consumption under fuel-rich combustion conditions. The increase in the CO content resulted in maximum propagation velocities of the detonation wave being achieved for the three gas mixtures at equivalence ratios of 0.91, 1.09, and 1.19, with corresponding velocities of 1136.7, 1108.7, and 1113.2 m/s, and the shortest times required to establish RDW were measured at 1.5, 1.1, and 0.8 ms for the respective mixtures.

SF6 Tracer Technique to Estimate Methane Emission in a Dual-Flow Continuous Culture System: Test and Application

This study aimed to evaluate the sulfur hexafluoride (SF6) tracer technique for estimating methane (CH4) emissions in dual-flow continuous culture systems (DFCCS). In experiment 1 (Exp1), fermenters were filled with water, and known CH4 concentrations (0, 1.35, 2.93, or 4.43 g/d) were injected using permeation tubes with SF6 release rates (3.30 or 9.65 mg/d). Headspace gas was collected using canisters, and the SF6 technique estimated CH4 recovery. Experiment 2 (Exp2) involved a DFCCS fermentation trial with ruminal fluid from three Holstein cows, testing diets with soybean meal or its partial replacement (50%) by Chlorella or Spirulina. Headspace gas was collected at intervals post-feeding. Standard curves for SF6 and CH4 quantification were inadequate for DFCCS samples, with the CH4:SF6 ratio differing from standards, indicating the data needs further SF6 release rate evaluation. In Exp1, a high correlation (r = 0.97) was found between infused and calculated CH4, indicating good repeatability. Low and high SF6 rates performed similarly at low CH4 infusion, but high SF6 overestimated CH4 at high infusion. Exp2 showed CH4 emissions irrespective of SF6 rate and indicated reduced CH4 emissions and increased NDF degradation with algae-containing diets. Further evaluation of the SF6 tracer technique is warranted for DFCCS.

Experimental investigation of steam and carbon dioxide influence on methane filtration combustion in a reversal flow porous media reactor

A reverse flow porous medium reactor with premixed and non-premixed flames was experimentally investigated to evaluate the influence of steam and carbon dioxide on methane (CH4) filtration combustion for syngas production. Premixed, non-premixed, and non-premixed with steam were the tested cases for different injection configurations. Thermal profiles, combustion products, hydrogen (H2) and carbon monoxide (CO) yields for several equivalence ratios are analyzed. Non-premixed case exposed higher maximum temperatures due to the reactant accumulation at the crosswise injection position, with a temperature of 1615 K. The lack of homogenization of the reactants in this configuration leads to low H2 and high CO concentrations compared to the premixed case. The maximum CO yield was 92.81% for the non-premixed configuration with alternated air injection, while the maximum H2 yield was 37.8% for the premixed air-methane-steam case. It was found that the air-methane-carbon dioxide mixtures had lower temperatures, combustion wave velocities, and H2 and CO concentrations, compared to the air-methane, and air-methane-steam mixtures, but higher CH4 and CO2 concentrations. The premixed configuration with air-methane-carbon dioxide mixture showed higher temperatures, and H2 and CO concentrations, compared to the non-premixed configuration. Further studies are necessary to optimize the operation of these types of reactors.

Methodology and Uncertainty Analysis of Methane Flux Measurement for Small Sources Based on Unmanned Aerial Vehicles

The top–down emission rate retrieval algorithm (TERRA) method for calculating the net flux out of a box has been employed by other researchers to assess large sources of methane release. This usually requires a manned aircraft drone with powerful performance to fly over the boundary layer. Few studies have focused on low-altitude box sampling mass balance methods for small sources of methane release, such as at maximum flight altitudes of less than 100 m. The accuracy and sources of uncertainty in such a method still need to be determined as they differ from the conditions of large sources. Nineteen flights were conducted to detect methane emissions from Chinese oil field well sites using a measurement system consisting of a quadcopter and methane, wind speed, wind direction, air pressure, and temperature sensors. The accuracy and uncertainty of the method are discussed. The average absolute relative error of the measurement is 18.5%, with an average uncertainty of 55.75%. The uncertainty is mainly caused by the wind speed and direction, and the background CH4 concentration. The main paths to reduce uncertainty and improve accuracy for low-altitude box sampling include subtracting the background concentration during flux retrieval, enhancing the accuracy of methane measurements, selecting a period of downwind dominant or wind direction change of less than 30 degrees, and ensuring a maximum flight height greater than 50 m with a horizontal distance from the pollution source center of less than 75 m. The results show that TERRA-based low-altitude box sampling is suitable for quantifying methane release rates from small sources.

Advanced UV Spectrophotometry-Classical Least Squares Determination of Paracetamol, Phenylpropanolamine HCl, and Chlorpheniramine Maleate in Tablet Dosage Form

This study aims to develop and validate an advanced UV spectrophotometry- Classical Least Squares (CLS) for the simultaneous determination of Paracetamol (PA), Phenylpropanolamine HCl (PH), and Chlorpheniramine Maleate (CH) in tablet dosage form. The method involves the preparation of standard solutions of the three compounds across their respective concentration ranges 3-9 µg/mL for PA, 170-512 µg/mL for PH, and 7-19 µg/mL for CH. The CLS spectrophotometry UV method was applied to these spectra to construct calibration, which were then used to predict the concentrations of PA, PH, and CH in tablet dosage form. Validation of the method demonstrated excellent linearity, precision, and accuracy, with recovery rates of 99.26% for PA, 100.06% for PH, and 99.41% for CH. Sensitivity analysis revealed Limits of Detection (LOD) of 0.10 µg/mL for PA, 1.20 µg/mL for PH, and 0.30 µg/mL for CH, and Limits of Quantification (LOQ) of 0,30 µg/mL for PA, 4.00 µg/mL for PH, and 1.50 µg/mL for CH. The method’s robustness and reliability make it an excellent choice for routine quality control of these compounds in pharmaceutical tablet formulations.

Effect of Tectonic Deformation on the Pore System and Methane Adsorption of Anthracite Coal.

Tectonic deformation significantly alters the physical structure of coals, holding great importance to the coal mining industry and coalbed methane. In this study, eight anthracite coal samples with varying degrees of deformation were collected to investigate the effects of tectonic deformation on the pore system and CH4 adsorption of anthracite coals. In addition, low-temperature gas adsorption (N2 and CO2), Raman spectroscopy, and CH4 isothermal experiments were performed. The results revealed that coal samples with higher degrees of deformation exhibited larger ratios of D-band intensity to G-band intensity (I D/I G), indicating increased molecular defects induced by tectonic deformation. As the deformation degree of the coal samples increased, the mesopore volume increased from 0.00044 cm3/g (primary coal) to 0.0019 cm3/g (scaly coal). Conversely, the micropore volume tended to decrease with the increasing deformation degree of the coal samples. Moreover, the impact of deformation degree on the CH4 adsorption capacity of anthracite coals was complex. With the deformation degree increasing, the Langmuir volume initially decreased from 32.0 to 24.55 cm3/g and then rose to 30.14 cm3/g. This complexity arose from the differential effects of tectonic deformation on various pore types, where micropores and mesopores collectively determined the CH4 adsorption capacity of anthracite coals. This study analyzed the influence of tectonic deformation on the pore structure and CH4 adsorption capacity at the molecular level, providing valuable insights for evaluating the in situ CH4 content in anthracite coal seams.

Methane dynamics altered by reservoir operations in a typical tributary of the Three Gorges Reservoir

Substantial nutrient inputs from reservoir impoundment typically increase sedimentation rate and primary production. This can greatly enhance methane (CH4) production, making reservoirs potentially significant sources of atmospheric CH4. Consequently, elucidating CH4 emissions from reservoirs is crucial for assessing their role in the global methane budget. Reservoir operations can also influence hydrodynamic and biogeochemical processes, potentially leading to pronounced spatiotemporal heterogeneity, especially in reservoirs with complex tributaries, such as the Three Gorges Reservoir (TGR). Although several studies have investigated the spatial and temporal variations in CH4 emissions in the TGR and its tributaries, considerable uncertainties remain regarding the impact of reservoir operations on CH4 dynamics. These uncertainties primarily arise from the limited spatial and temporal resolutions of previous measurements and the complex underlying mechanisms of CH4 dynamics in reservoirs. In this study, we employed a fast-response automated gas equilibrator to measure the spatial distribution and seasonal variations of dissolved CH4 concentrations in XXB, a representative area significantly impacted by TGR operations and known for severe algal blooms. Additionally, we measured CH4 production rates in sediments and diffusive CH4 flux in the surface water. Our multiple campaigns suggest substantial spatial and temporal variability in CH4 concentrations across XXB. Specifically, dissolved CH4 concentrations were generally higher upstream than downstream and exhibited a vertical stratification, with greater concentrations in bottom water compared to surface water. The peak dissolved CH4 concentration was observed in May during the drained period. Our results suggest that the interplay between aquatic organic matter, which promotes CH4 production, and the dilution process caused by intrusion flows from the mainstream primarily drives this spatiotemporal variability. Importantly, our study indicates the feasibility of using strategic reservoir operations to regulate these factors and mitigate CH4 emissions. This eco-environmental approach could also be a pivotal management strategy to reduce greenhouse gas emissions from other reservoirs.

Numerical simulation of CO2-ECBM for deep coal reservoir with strong stress sensitivity

CH4 production rate of coalbed methane (CBM) well decreases rapidly during primary recovery in the deeply buried coal seam, resulting in a lot of CH4 residues. CO2 pour into deep coal seam with high stress sensitivity is available for enhancing CH4 recovery by improving permeability for reservoir fracture and displacing CH4 adsorbed in matrix. A coupled adsorp-hydro-thermo-mechanical (AHTM) model for deep methane development is established by considering the coupling relationships of non-isothermal and non-constant pressure competitive adsorption between CO2 and CH4, multi-phase flow, unsteady diffusion, heat transmission and in-situ stress variety. The model is verified by historical production and then used for CO2 enhanced CBM (CO2-ECBM) of deep coal reservoir in a sedimentary basin in Northwest China. The simulation results show that: (1) For primary recovery, permeability in coal reservoir drops rapidly with the development of CBM, which seriously restricts the production of CH4. The permeability of the reservoir decreases from 7.89 × 10−16 m2 to less than 1.50 × 10−16 m2, CH4 production rate in CBM well reduces to below 2000 m3/d, and the average total CH4 content of coal reservoir is reduced by 5.49 m3/t with the decrease of only 1.12 m3/t of average adsorbed CH4 in a production duration of 2000 d (2) With 10 MPa CO2 continuous injection into coal seam after 700d of primary, the permeability for reservoir and CH4 production rate increase while the total CH4 content and adsorption CH4 content in reservoir decrease compared with the primary recovery. (3) CO2 pouring into coal reservoir increases the CH4 production time and rate, which improves CH4 recovery of coal reservoir. And it increases by 23.36 %, 23.07 % and 22.46 % with shut-in thresholds of CH4 production rate of 1000 m3/d, 800 m3/d and 600 m3/d, respectively. The investigation is of great significance for the development of deep coalbed methane.

In Situ High-Precision Measurement of Deep-Sea Dissolved Methane by Quartz-Enhanced Photoacoustic and Light-Induced Thermoelastic Spectroscopy.

Rapid and accurate realization of in situ analysis of deep-sea dissolved gases imperative to the study of ecological geology, oil and gas resource exploration, and global climate change. Herein, we report for the first time the deep-sea dissolved methane (CH4) in situ sensor based on quartz-enhanced photoacoustic and light-induced thermoelastic spectroscopy. The developed sensor system has a volume of φ120 mm × 430 mm and a power consumption of 7.6 W. The sensor, in the manner of frequency division multiplexing, is able to simultaneously measure the photoacoustic signals and light-induced thermoelastic signals, which can accurately correct laser-intensity induced influence on concentration. The spectral response of CH4 concentration varying from 0.01 to 5% is calibrated in detail based on the pressure and temperature in the application environment. The trend of the photoacoustic signal of CH4 at different water molecule (H2O) concentrations is investigated. An Allan variance analysis of several hours demonstrates a minimum detection limit of 0.21 ppm for the CH4 spectrometer. The sensor combined with the gas-liquid separation and enrichment unit is integrated into a compact marine standalone system. Since the specifically designed photoacoustic cell has a volume of only 1.2 mL, the time response for dissolved CH4 detection is reduced to 4 min. Furthermore, the sensor is successfully deployed in the vicinity of the "HaiMa" cold seeps at 1380 m underwater in the South China Sea, completing three consecutive days of measurements of dissolved CH4.

Continuous biogas production and ex-situ biomethanation in a trickling bed bioreactor under mesophilic and thermophilic conditions

The utilization of biogas as a renewable energy source necessitates a reduction in its CO2 content. "Ex-situ biomethanation" is employed to convert CO2 in biogas to CH4 through hydrogenotrophic methanogens. In this study, a biogas stream (32–36 % CO2) originating from cow manure digestion was subjected to treatment in a trickle bed bioreactor (4 liters). The presence of microorganisms on the packing material was confirmed by using a 16 S rRNA test and SEM images. This study stands out by considering all four combinations of thermophilic and mesophilic conditions, monitoring the transition and steady-state phases in a two-reactor series setup. The mesophilic-thermophilic mode yielded the highest purity (92 %) with an 86 % CO2 conversion rate and an energy density of 13,870 kJ/m3. Additionally, the performance consistency was also assessed using a larger TBB (8 liters). Extending the residence time, the thermophilic-thermophilic mode yielded the highest CH4 concentration at 98 %. The 16 S rRNA results revealed that, influenced by the designated growth conditions encompassing culture media, pH, temperature, and reactor retention time, an enrichment of hydrogenotrophic methanogens occurred. Furthermore, promising results in terms of CH4 concentration and process efficiency were demonstrated by the trickled bed bioreactor employing liquid-in-gas dispersion.

Real-time monitoring of CH4 and N2O emissions from livestock using mid-infrared external cavity quantum cascade laser absorption spectroscopy

The largest share of greenhouse gas (GHG) emissions related to livestock originates from methane (CH4) and nitrous oxide (N2O) which have a far higher influence on global warming, it is therefore necessary to accurately monitor CH4 and N2O emissions to provide theoretical and practical basis for further estimating and regulating GHG emissions from livestock and improving livestock production performance. For the purpose of sensing CH4 and N2O emissions during livestock living process in real time, an optical sensor based on continuous-wave (CW) external cavity quantum cascade laser (EC-QCL) operating at room temperature was developed. CH4 and N2O absorption lines, located around 8 μm, of the ν4 and ν1 fundamental vibrational bands, respectively, were chosen for direct absorption spectroscopy, which allows for sensitive, selective and simultaneous measurement of CH4 and N2O concentrations. Use of a Herriot multi-pass cell with an effective path-length of 100 m, 1σ (SNR = 1) limits of detection of 26.8 ppbv, 20.3 ppbv and 0.01 % for CH4, N2O and H2O vapor were achieved, respectively. Field measurement of CH4 and N2O emissions from horses has been carried out in a stable over two weeks at the Vernaelde farm in Couderkerque Branche city, France. Concentrations of CH4 and N2O up to 10 times and 1.5 times higher than their levels in the local ambient air (∼ 2.12 ppmv and ∼ 427 ppbv) were observed, respectively.

In-situ biological biogas upgrading using upflow anaerobic polyfoam bioreactor: Operational and biological aspects.

A high rate upflow anaerobic polyfoam-based bioreactor (UAPB) was developed for lab-scale in-situ biogas upgrading by H2 injection. The reactor, with a volume of 440 mL, was fed with synthetic wastewater at an organic loading rate (OLR) of 3.5 g COD/L·day and a hydraulic retention time (HRT) of 7.33 h. The use of a porous diffuser, alongside high gas recirculation, led to a higher H2 liquid mass transfer, and subsequently to a better uptake for high CH4 content of 56% (starting from 26%). Our attempts to optimize both operational parameters (H2 flow rate and gas recirculation ratio, which is the total flow rate of recirculated gas over the total outlet of gas flow rate) were not initially successful, however, at a very high recirculation ratio (32) and flow rate (54 mL/h), a significant improvement of the hydrogen consumption was achieved. These operational conditions have in turn driven the methanogenic community towardthe dominance of Methanosaetaceae, which out-competed Methanosarcinaceae. Nevertheless, highly stable methane production rates of 1.4-1.9 L CH4/Lreactor.day were observed despite the methanogenic turnover. During the different applied operational conditions, the bacterial community was especially impacted, resulting in substantial shifts of taxonomic groups. Notably, Aeromonadaceae was the only bacterial group positively correlated with increasing hydrogen consumption rates. The capacity of Aeromonadaceae to extracellularly donate electrons suggests that direct interspecies electron transfer (DIET) enhanced biogas upgrading. Overall, the proposed innovative biological in-situ biogas upgrading technology using the UAPB configuration shows promising results for stable, simple, and effective biological biogas upgrading.

In-situ biomethanation of high CO content syngas in agricultural biogas digesters

To meet global energy demands, syngas with high CO content (>50 %) generated from hydrothermal gasification of agricultural residues or wood, could be utilized as a co-substrate in anaerobic digestion (AD) processes for conversion into CH4. This study investigated in-situ biomethanation using synthetic gas (55 % CO, 35 % H2, and 15 % CO2), mimicking wood gasification syngas, during AD of cow manure, the most abundant agricultural waste. A continuously stirred tank reactor (CSTR) served as a control and was fed only cow manure, while the other two reactors were fed syngas with or without gas recirculation at different gas loading rates (GLRs).In-situ syngas injection in AD of cow manure at GLRs ≤0.3 L LRV−1 d−1 improved overall CH4 productivity compared to the control (0.35 ± 0.1 vs. 0.29 ± 0.1 L LRV−1 d−1), though the CH4 content (45 ± 5 %) was lower than the control reactor (62 ± 3 %), indicating a need for biogas upgrading. Gas recirculation enabled higher CO and H2 conversion efficiencies of 99–100 % but considerably decreased CH4 productivity from cow manure. In-situ biomethanation enhanced the relative abundance of hydrogenotrophic methanogens, highlighting their role in syngas conversion to CH4.

Surprising concentrations of hydrogen and non-geological methane and carbon dioxide in the soil

Due to its potential use as a carbon-free energy resource with minimal environmental and climate impacts, natural hydrogen (H2) produced by subsurface geochemical processes is today the target of intensive research. In H2 exploration practices, bacteria are thought to swiftly consume H2 and, therefore, small near-surface concentrations of H2, even orders of 102 ppmv in soils, are considered a signal of active migration of geological gas, potentially revealing underground resources. Here, we document an extraordinary case of a widespread occurrence of H2 (up to 1 vol%), together with elevated concentrations of CH4 and CO2 (up to 51 and 27 vol%, respectively), in aerated meadow soils along Italian Alps valleys. Based on current literature, this finding would be classified as a discovery of pervasive and massive geological H2 seepage. Nevertheless, an ensemble of gas geochemical and soil microbiological analyses, including bulk and clumped CH4 isotopes, radiocarbon of CH4 and CO2, and DNA and mcrA gene quantitative polymerase chain reaction analyses, revealed that H2 was only coupled to modern microbial gas. The H2-CO2-CH4-H2S association, wet soil proximity, and the absence of other geogenic gases in soils and springs suggest that H2 derives from near-surface fermentation, rather than geological degassing. H2 concentrations up to 1 vol% in soils are not conclusive evidence of deep gas seepage. This study provides a new reference for the potential of microbial H2, CH4 and CO2 in soils, to be considered in H2 exploration guidelines and soil carbon and greenhouse-gas cycle research.

Direct reduction of calcium carbonate by coupling with methane dry reforming using NiO/S-1 as catalyst

Thermal decomposition of carbonate is an important process in the production of cement, refractory materials, and steel. Nevertheless, this process requires high temperature and is always accompanied with large amounts of CO2 emission. To reduce the decomposition temperature and simultaneously mitigate CO2 emissions, direct reduction of carbonate under a reducing atmosphere has been proposed as a novel strategy. This work mainly investigated the feasibility of direct reduction of CaCO3 by CH4 in the presence of a highly dispersed NiO/S-1 catalyst. It was found that the introduction of a CH4 atmosphere without a catalyst had little promotion effect on CaCO3 decomposition (as compared to air atmosphere), and no notable conversion of CO2 was observed. However, the presence of a highly dispersed NiO/S-1 catalyst significantly decreased the decomposition temperature of CaCO3 in a CH4 atmosphere, and most of the carbon species in CaCO3 can be converted to CO. To gain a comprehensive understanding of CaCO3 reduction in CH4, the effects of reaction temperature, CH4 concentration, and NiO loading in the NiO/S-1 catalyst were systematically explored. With the best-performing catalyst, i.e., 7NiO/S-1, complete CaCO3 decomposition and approximate 90 % CH4/CO2 conversion can be achieved under the condition of 750 °C and 25 vol% CH4. Characterization results indicated that the CaO particles obtained in the CH4 reducing atmosphere exhibited a more porous structure compared to that attained in air, due to the more intensive CaCO3 decomposition in CH4. Further data analysis revealed that reverse water-gas shift reaction also contributed to CO2 conversion during the reduction of CaCO3 in CH4. The findings obtained in this research can provide new perspectives for CO2 emission control and energy saving in traditional heavy-emission and high energy consumption industries.

Channel selection method for the CH4 profile retrieval using the Atmospheric Sounder Spectrometer by Infrared Spectral Technology

Methane (CH4) is the second-largest greenhouse gas contributing to global warming, surpassed only by CO2, has a large difference in its vertical concentration distribution, and closely affects the global environment and climate change. The variations in the vertical concentrations of CH4 need to be monitored. Ground-based infrared hyperspectrometers can measure the fine variations of the CH4 concentrations in the vertical distribution within the planetary boundary layer (PBL). However, different detection channels are easily affected by instrumental noise and other environmental factors, leading to differences in the channel spectral characteristics and thereby affecting the accuracy of the CH4 profile retrieval. In this study, an information-weighted channel selection method is proposed for the CH4 profile retrieval using the Atmospheric Sounder Spectrometer by Infrared Spectral Technology (ASSIST) to address the differences in the channel characteristics from the different interference factors. This method leverages the information content of CH4 and its environmental interference factors in each channel to derive the weighting factors, and a comprehensive weighting approach is subsequently applied to ascertain the effective information content of CH4. The method then establishes the threshold for the effective CH4 information content, considering the influence of noise, to select the optimal channels. We employ this method in our study, and 22 channels are selected as the optimal channels for the CH4 profile retrieval. We also evaluate the retrieval capability of the CH4 profile and the anti-interference ability of the selected channels using simulated spectra under clear-sky conditions. When retrieving the CH4 profile using the 1200–1390 cm−1 band (394 channels in total), the CH4 profile is mainly affected by temperature, water vapor, aerosol optical depth (AOD) and N2O. In addition, the mean absolute error (MAE) and the root mean square error (RMSE) for the CH4 profile retrieval using the selected channels are substantially reduced.

Optimizing methane plasma pyrolysis for instant hydrogen and high-quality carbon production

The European Green Deal has set a target for Europe to achieve net-zero greenhouse gas emissions by 2050, necessitating a transition to more sustainable energy sources. Hydrogen gas (H2) has emerged as a promising solution, with methane pyrolysis presenting a viable method for its production. This study explores the optimization of methane plasma pyrolysis for hydrogen and high-quality carbon production. Employing a statistical approach by a design of experiment software, critical process parameters are systematically analyzed to predict their impact within a defined range. Additionally, the paper conducts comprehensive characterization of the solid carbon produced during pyrolysis using imaging, spectroscopic and elemental analysis, and gas sorption analysis methods. The experimental investigation was conducted using a thermal plasma reactor with several settings of influential parameters including methane gas (CH4) content in the plasma gas, electric current, and arc length. The DC-transferred plasma arc is formed using a variable gas mixture of argon gas (Ar) and CH4, with a constant flow rate of 5 Nl/min. Thirteen tests were designed, evaluating responses such as power input, process stability, and H2 yield. The H2 yield indicates the hydrogen produced from CH4, with 100% representing total conversion. While the process exhibited inconstancy, attributed to reactor design constraints, a high H2 yield of 67%–100% was achieved. The results indicate that a higher CH4 content in the plasma gas and extended arc lengths disturb the plasma arc, hence reducing the H2 yield. Increased power input, achieved through higher amperage levels, and a wider reaction zone eased by extending the arc length both led to an improved H2 yield. Scanning electron microscopy (SEM) and energy dispersive X-ray spectroscopy (EDS) revealed microstructural differences, with carbon samples from the filter exhibiting finer textures and carbon samples from the reactor larger sizes and dendritic particles. Raman spectroscopy confirmed crystalline graphitic-like structures with low defect concentrations, a finding supported by X-ray diffraction (XRD) analysis. Inductively coupled plasma mass spectroscopy (ICP-MS) analysis confirmed high-purity carbon with slight impurities from initial filter contamination. Brunauer-Emmett-Teller (BET) specific surface area calculations based on gas sorption analysis showed significant variations, with filter-collected samples exhibiting 40–170 m2/g and reactor-collected ones showing 7–30 m2/g.