In this paper,the Ni/Al_(2)O_(3) monolithic catalyst with 15%Ni content was prepared using cordierite as a matrix,and the catalyst was modified with 10%NaOH to study the methanation performance of biomass gasification...In this paper,the Ni/Al_(2)O_(3) monolithic catalyst with 15%Ni content was prepared using cordierite as a matrix,and the catalyst was modified with 10%NaOH to study the methanation performance of biomass gasification simulated gas based on alkali-modified Ni/Al_(2)O_(3) monolithic catalyst.BET,TEM,H_(2)-TPR,XRD,CO_(2)-TPD and TG were used to characterize the physicochemical properties of the catalyst before and after modification.The results indicated that the CO conversion rate trends of unmodified and modified Ni/Al_(2)O_(3) monolithic catalysts over 2 h were fundamentally consistent.However,the Ni/Al_(2)O_(3) catalysts modified for 2 h demonstrated significantly enhanced performance compared to those modified for 1 h.Regarding CH4 selectivity,the modified Ni/Al_(2)O_(3) catalyst exhibited markedly better performance than the unmodified Ni/Al_(2)O_(3) catalyst,confirming the enhanced methane performance of the alkali-modified Ni/Al_(2)O_(3) monolithic catalyst.Under optimized conditions(H_(2)/CO volume ratio of 3∶1,space velocity of 10000 mL/(g·h),and temperature of 400℃),the methanation performance of the Ni/Al_(2)O_(3) monolithic catalyst modified for 2 h reached its peak,achieving a CO conversion rate of 97%with 100%CH4 selectivity.展开更多
Under the backdrop of“Carbon Peak and Carbon Neutrality”(dual carbon)goal in China,the methane-carbon dioxide reforming reaction has attracted considerable attention due to its environmental benefits of converting t...Under the backdrop of“Carbon Peak and Carbon Neutrality”(dual carbon)goal in China,the methane-carbon dioxide reforming reaction has attracted considerable attention due to its environmental benefits of converting two greenhouse gases(methane and carbon dioxide)into syngas and its promising industrial applications.Nickel(Ni)-based catalysts,with high catalytic activity,low cost,and abundant resources,are considered ideal candidates for industrial applications.In this article,three reaction kinetic models were briefly introduced,namely the Power-Law(PL)model,the Eley-Rideal(ER)model,and the Langmuir-Hinshelwood-Hougen-Watson(LHHW)model.Based on the LHHW model,the reaction kinetics and mechanisms of different catalytic systems were systematically discussed,including the properties of supports,the doping of noble metals and transition metals,the role of promoters,and the influence of the geometric and electronic structures of Ni on the reaction mechanism.Furthermore,the kinetics of carbon deposition and elimination on various catalysts were analyzed.Based on the reaction rate expressions for carbon elimination,the reasons for the high activity of transition metal iron(Fe)-doped catalysts and core-shell structured catalysts in carbon elimination were explained.Based on the detailed collation and comparative analysis of the reaction mechanisms and kinetic characteristics across diverse Ni-based catalytic systems,a theoretical guidance for the designing of high-performance catalysts was provided in this work.展开更多
Methane dehydroaromatization(MDA)presents a promising carbon-neutral pathway for benzene,toluene,and xylene(BTX)production,alternative to petroleumderived routes.Elucidating the regulatory mechanisms of Brønsted ...Methane dehydroaromatization(MDA)presents a promising carbon-neutral pathway for benzene,toluene,and xylene(BTX)production,alternative to petroleumderived routes.Elucidating the regulatory mechanisms of Brønsted acid site(BAS)strength on reaction pathways,alongside the spatial proximity effects between BAS and Mo active sites in bifunctional synergy,remains a critical scientific challenge in catalyst design.This study systematically tunes both BAS strength(via isomorphous metal substitution)and Mo-BAS spatial proximity in zeolites,integrating MDA catalytic evaluations with density functional theory(DFT)calculations to dissect their individual contributions.Strongly acidic BAS catalysts(compared to moderately acidic Fe/Ga-substituted counterparts)exhibit superior performance,evidenced by enhanced aromatic yields.Conversely,weakly acidic Bsubstituted zeolites demonstrate optimal mono-/bifunctional synergy,outperforming moderate-acid systems.DFT results reveal that acid strength dictates C−H activation mechanisms by modulating the energy barriers of rate-determining steps.While Al-zeolites deliver the highest activity,B-substituted systems display unique potential for mechanistic investigations.Spatial proximity analysis indicates that micrometer-scale Mo-BAS distances hinder effective synergy due to exceeding electron interaction and mass transfer limits,whereas nanometer-scale proximity enhances activity(via accelerated intermediate transport)and suppresses coke formation.These findings establish a theoretical framework for rationalizing zeolite catalyst optimization through BAS property engineering and spatial control of Mo-BAS cooperation,providing actionable guidelines for designing next-generation MDA catalysts.展开更多
Catalytic decomposition of methane,which produces high-purity hydrogen and high-value-added carbon nanomaterials,has shown considerable potential for development and is expected to yield significant economic benefits ...Catalytic decomposition of methane,which produces high-purity hydrogen and high-value-added carbon nanomaterials,has shown considerable potential for development and is expected to yield significant economic benefits in the future.However,designing catalysts that simultaneously exhibit high activity and long-term stability remains a significant challenge.Tuning the catalyst’s structure and electronic properties is an effective strategy for enhancing the reaction performance.In this work,a series of NixZr/ZSM-5 catalysts were prepared using the incipient wetness impregnation method,and the effect of Zr loadings on catalyst properties and performance was systematically investigated.The calcined and reduced catalysts were characterized by low-temperature N_(2)adsorption-desorption,XRD,SEM,H_(2)-TPR and XPS.The results showed that the addition of Zr significantly increased the specific surface area of the catalyst and reduced the metal particle size.Smaller NiO particles were found to enter the pores of the HZSM-5 support,and electronic interactions between NiO and ZrO_(2)markedly enhanced the metal-support interaction.The catalyst exhibited optimal catalytic performance at a Zr loading of 5%,achieving a maximum methane conversion of 68%at 625℃,maintaining activity for 900 min,and delivering a carbon yield of 1927%.Further increasing the Zr loading yielded only limited improvements in catalytic performance.Characterization of the spent catalysts and carbon products via TEM,Raman spectroscopy,and TGA revealed that the introduction of ZrO_(2)reduced metal sintering and promoted a shift in carbon nanofibers growth mode from tip-growth to base-growth.The mechanism of base-growth enabled the catalyst to maintain reaction activity for an extended period.展开更多
Conductive materials(CM)can improve methane production(MP)efficiency in many methanogenic systems.However,several types of CM exist,and there are uncertainties regarding whether they all improve MP efficiency to the s...Conductive materials(CM)can improve methane production(MP)efficiency in many methanogenic systems.However,several types of CM exist,and there are uncertainties regarding whether they all improve MP efficiency to the same extent and modulate microbial communities in a similar way.To investigate that,different microbial enrichments with and without activated carbon(AC),magnetite(Mag),and zeolites(Zeo)(at 0.5 g/L)were developed.MP profiles and microbial composition changes were compared among enrichments.The behavior of all enrichments was different,although the initial inoculum sludge was the same.Lag phase duration was lower in AC enrichment,while the complete conversion of butyrate to methane was faster in Mag enrichment.Syntrophomonas was the most abundant bacterial genus in all enrichments,but changes in the methanogenic community were evident.Acetoclastic methanogens were more diverse in Mag enrichment,with microorganisms assigned to Methanosarcina and Methanothrix gener1,but Methanothrix was the only acetoclastic methanogen in the other enrichments.On the other hand,different species of hydrogenotrophic methanogens prevailed in distinct enrichments.The metatranscriptomics results revealed that the dominant mechanism of interspecies electron transfer in the AC enrichment utilized hydrogen as the electron carrier,and no evidences of direct interspecies electron transfer(DIET)could be found.These results showed how different CM modulate microbial communities and affect MP efficiency through mechanisms that do not necessarily involve DIET or mediation via CM.展开更多
Rice fields are one of the largest sources of methane(CH4),a potent greenhouse gas contributing significantly to global warming.Elucidating the underlying mechanisms and mitigating CH4 emissions from paddy fields is c...Rice fields are one of the largest sources of methane(CH4),a potent greenhouse gas contributing significantly to global warming.Elucidating the underlying mechanisms and mitigating CH4 emissions from paddy fields is crucial for combating climate change while ensuring sustainable food production.This review investigates the biological processes governing CH4 generation in rice fields,focusing on how soil microorganisms generate CH4 under waterlogged,anaerobic conditions.It also explores the mechanisms by which CH4 escapes into the atmosphere through plant-mediated transport,diffusion,and ebullition.Several factors influencing CH4 emissions are discussed,including soil composition,water management,exogenous organic matter application,rice variety selection,and local climate conditions.Strategies that can be implemented to reduce CH4 emissions are assessed,such as alternate wetting and drying,urea deep placement,biochar application,optimized fertilizer application,and breeding of rice varieties with low CH4 emissions.Novel solutions,such as the enhancement of methane-consuming bacteria in soils using microbial-based approaches,are also explored.The importance of integrating innovative technologies,improved farming practices,and interdisciplinary research is emphasized to develop practical and scalable strategies for reducing CH4 emissions.By addressing these challenges,we can advance towards the attainment of sustainable agriculture and global climate goals.This review aims to serve as a comprehensive resource for researchers,policymakers,and practitioners seeking to understand and mitigate CH4 emissions from rice cultivation.展开更多
Directly burning methane for energy production wastes chemical potential and exacerbates CO_(2) emissions,while catalytic conversion into high-value fuel/chemicals provides economic and environmental sustainability.Ph...Directly burning methane for energy production wastes chemical potential and exacerbates CO_(2) emissions,while catalytic conversion into high-value fuel/chemicals provides economic and environmental sustainability.Photocatalytic CH_(4) conversion has emerged as a transformative technology,enabling selective oxidation under ambient conditions to directly synthesize value-added organic compounds.This addresses the dual challenges of climate mitigation and sustainable energy conversion.This review systematically examines the development of photocata lytic CH_(4) conversion,with three key dimensions.Firstly,we elucidate fundamental reaction mechanisms governing CH_(4) activation,emphasizing critical steps such as C-H bond scission via charge transfer,intermediate stabilization,and product desorption kinetics.Subsequently,we classify emerging photocata lytic pathways(partial oxidation,coupling,and reforming)and analyze material innovations.Finally,the challenges of the current photocata lytic CH_(4)conversion system and catalyst development were discussed,and perspectives were presented.The overarching objective of this work is to provide a comprehensive roadmap for the development of solardriven CH_(4) conversion systems that are aligned with global carbon neutrality goals.展开更多
Lakes are carbon dioxide(CO_(2))and methane(CH_(4))emission hotspots,whose associated flux is spatially vari-able.Many studies have investigated the impact of microorganisms and environmental factors on CO_(2) and CH_...Lakes are carbon dioxide(CO_(2))and methane(CH_(4))emission hotspots,whose associated flux is spatially vari-able.Many studies have investigated the impact of microorganisms and environmental factors on CO_(2) and CH_(4) emissions between different lakes.However,the carbon emissions and their influencing factors of different areas within a single lake remain poorly understood.Accordingly,this study investigates CO_(2) and CH_(4) emission hetero-geneity in a large floodplain lake system and distribution characteristics of associated functional microorganisms.Findings show that mean CO_(2) and CH_(4) flux values in the sub lake area were 62.03±24.21 mg/(m2·day)and 5.97±3.2μg/(m2·day),which were greater by factors of 1.78 and 2.96 compared to the water channel and the main lake area,respectively.The alpha diversity of methanogens in the sub lake area was lower than that in the main lake and water channel areas.The abundance of methanogens in bottom water layer was higher compared with the middle and surface layers.Conversely,the abundance of methane(CH_(4))-oxidizing bacteria in the surface layer was higher than that in the bottom layer.Additionally,the composition of methanogen and CH_(4)-oxidizing bacterial community,chlorophyll a(Chl-a),pH,total phosphorus(TP)and dissolved organic carbon(DOC)con-tent constituted the dominate driving factors affecting lake C emissions.Results from this study can be used to improve our understanding of lake spatial heterogeneous of CO_(2) and CH_(4) emission and the driving mechanisms within floodplain lakes under the coupling effects of functional C microorganisms and environmental factors.展开更多
The research presented in this paper aimed to analyze the evolution of fractures in strata in relation to the progress of longwall mining.To achieve this objective,an introscopic probe equipped with a highresolution c...The research presented in this paper aimed to analyze the evolution of fractures in strata in relation to the progress of longwall mining.To achieve this objective,an introscopic probe equipped with a highresolution camera was developed,along with additional equipment that enables continuous recording of the internal surfaces of drainage boreholes exceeding 100 m in depth.The probe was utilized to test two methane drainage boreholes in the Z-3b longwall,which operates within the 501/3 coal seam of the Jankowice mine in Poland.Automatic image analysis methods were applied to evaluate the recorded images,based on a newly developed classificationsystem for fractures categorized by size and number.The results were compared with an analysis of changes in the methane capture rate from the drainage boreholes,which correlated with longwall mining progress.A strong correlation was observed between the number of fractures and the lithology of the strata layers.The largest number of fractures and their evolution were recorded in the coal layers,followed by the shale layers,while the sandstone layers exhibited the least number of fractures.Based on parallel measurements of the methane capture rate from the drainage boreholes during the progress of longwall mining,the extent of the strata's fracture zone was determined to range from 6 m to 36 m.Within the fracture zone,the strata are highly fractured,which leads to an increase in methane emissions through seepage and diffusion processes.展开更多
Background The enteric methane inhibitor 3-nitrooxypropanol(3-NOP)inhibits the key enzyme in ruminal methanogenesis,but whether short-term(ST)and long-term(LT)dietary supplementation has similar effects on rumen micro...Background The enteric methane inhibitor 3-nitrooxypropanol(3-NOP)inhibits the key enzyme in ruminal methanogenesis,but whether short-term(ST)and long-term(LT)dietary supplementation has similar effects on rumen microbiota in beef cattle and how microbes change after 3-NOP withdrawal have not been studied.This study investigated changes in rumen bacteria,archaea,and protozoa after ST and LT dietary supplementation and removal of 3-NOP using metataxonomic analysis.Results A total of 143 rumen samples were collected from two beef cattle studies with 3-NOP supplementation.The ST study(95 samples)used eight ruminally cannulated beef cattle in a 4×4 Latin square design with four 28-d of 3-NOP treatments[mg/kg of dry matter(DM)]:control:0,low:53,med:161,and high:345.The LT study(48 samples)was a completely randomized design with two 3-NOP treatments[control:0,and high:280 mg/kg of DM)fed for 112-d followed by a 16-d withdrawal(without 3-NOP).Bacterial and archaeal communities were significantly affected by 3-NOP supplementation but limited effects on protozoal communities were observed.Under ST supplementation,the relative abundances of Prevotella,Methanobrevibacter(Mbb.)ruminantium,Methanosphaera sp.ISO3-F5,and Entodinium were increased(Q<0.05),whereas those of Mbb.gottschalkii and Epidinium were decreased(Q<0.05)with 3-NOP supplementation.In LT study,relative abundances of Mbb.ruminantium,and Methanosphaera sp.Group5 were increased(Q<0.05),while those of Saccharofermentans and Mbb.gottschalkii were decreased(Q<0.05)with 3-NOP supplementation.Comparison between 3-NOP supplementation and the withdrawal revealed increased relative abundances of Clostridia UCG-014 and Oscillospiraceae NK4A214 group and decreased those of Eubacterium nodatum group and Methanosphaera sp.Group5(P<0.05)after 3-NOP withdrawal.Further comparison of rumen microbiota between control and 3-NOP withdrawal showed significantly higher(P=0.029)relative abundances of Eggerthellaceae DNF00809,p-1088-a5 gut group,and Family XII UCG-001 in control group while no significant differences were detected for archaea and protozoa.Microbial network analysis revealed that microbial interactions differed by both 3-NOP dose and durations.Conclusions Both ST and LT supplementation affected overall rumen microbial profile,with individual microbial groups responded to 3-NOP supplementation differently.After 3-NOP withdrawal,not all microbes showed recovery,indicating that the 3-NOP driven shifts were only partially reversible.These findings provide an understanding of the effects of 3-NOP on rumen microbial communities and their adaptability to methane mitigation strategies.展开更多
Significant differences exist between deep and medium-shallow coalbed methane(CBM)reservoirs.The unclear understanding of flowback and production behavior severely constrains the development of deep CBM resources.To a...Significant differences exist between deep and medium-shallow coalbed methane(CBM)reservoirs.The unclear understanding of flowback and production behavior severely constrains the development of deep CBM resources.To address this challenge,guided by the gas-liquid two-phase flow theory in ultra-low permeability reservoirs,and integrating theoretical analysis,numerical simulation,and insights from production practices,this study classifies the flowback and production stages of deep CBM well considering the Daning-Jixian Block,Eastern Ordos Basin as a representative case.We summarize the flowback characteristics for each stage and establish a standard flowback production type curve,aiming to guide field operations.The results indicate that:(a)The production process of deep CBM horizontal wells can be divided into five distinct stages:initial single-phase water dewatering stage,initial gas appearance to peak water production stage,gas breakthrough to peak gas production stage,stable production and decline stage,and low-rate production stage.(b)Based on reservoir energy,two standard type curves for horizontal well flowback production are established:the‘Sufficient Reservoir Energy’type and the‘Insufficient Reservoir Energy’type.The former achieves a higher initial gas rate(up to 12×10^(4)m^(3)/d)but exhibits poorer stability,while the latter achieves a lower stable rate(up to 8×10^(4)m^(3)/d)but demonstrates stronger stability.Numerical simulation confirms these behavioral patterns and reveals the underlying mechanisms related to the effectively drained area where pressure is significantly depleted.The findings from this study have guided the flowback production operations in 53 deep CBM wells with positive results,demonstrating high potential for broad application.展开更多
The traditional ammonia synthesis via the Haber–Bosch process requires large consumption of highpurity H_(2) and causes significant carbon emissions owing to the energy-intensive and complex hydrogen production steps...The traditional ammonia synthesis via the Haber–Bosch process requires large consumption of highpurity H_(2) and causes significant carbon emissions owing to the energy-intensive and complex hydrogen production steps conducted under harsh reaction conditions.Herein,we report a cyclic catalytic process for the production of NH_(3) by directly utilizing earth-abundant CH_(4) as a hydrogen source for N_(2) hydrogenation while simultaneously co-producing H_(2) over an alumina-supported iron catalyst(Fe/Al_(2)O_(3)).It achieves exceptional productivities of 2300μmol g^(-1)h^(-1)for NH_(3) and 400 mmol g^(-1)h^(-1)for H_(2) at700℃.By eliminating the coke that results from CH_(4) pyrolysis through a reaction with the greenhouse gas CO_(2) to produce valuable CO,we establish an atom-economic cyclic catalytic process while producing a CO stream intrinsically separated in the regeneration step.Mechanistic investigations indicate that the iron species in Fe/Al_(2) O_(3) serve as tri-functional active sites for CH_(4) pyrolysis,N_(2) hydrogenation,and coke elimination to produce CO,thus enabling an efficient and environmentally friendly cyclic catalytic process.展开更多
Oil and gas pipelines are a vital long-distance liquid and natural gas carrier,but their functionality is being assessed from a two-fold perspective of power economy and environmentalism.This review concurs on the way...Oil and gas pipelines are a vital long-distance liquid and natural gas carrier,but their functionality is being assessed from a two-fold perspective of power economy and environmentalism.This review concurs on the way these outcomes are interdependent throughout the pipeline lifecycle by contending that the efficiency,emissions,reliability,and environmental risk are jointly determined through the shared design decisions,operating plans,integrity platforms,and monitoring and response plans.Our initial conceptualization is pipeline systems and performance measures,which are characterized by boundary and comparability issues of particular energy consumption,methane intensity,and release consequence measures.Next,we look at hydraulic and station optimization,focusing on the need to look at the importance of equipment performance at part loads,constraints consciousness dispatch,and transient management to prevent the erosion of integrity levels by efficiency gains.The integrity management is appraised as one of the key enablers of stewardship that connects the corrosion prevention,in-line inspection and verification,and the risk-based mitigation to less likely failure,less disruptive interventions,and reduced emissions during maintenance.We compare the leak and spill prevention,detection,quantification,and response of the SCADA(supervisory control and data acquisition)-based computational monitoring,distributed sensing,as well as aerial/satellite,focusing on the validation,characterization of uncertainty,and the operational parameters modulating the time-to-detect and isolation performance.Environmental impacts of the lifecycle,not related to releases,are explained,such as routing and construction disturbance,management of right-of-way,station externalities,decommissioning,and climate resilience.Lastly,we assess new technologies,such as continuous monitoring networks,electrification,superior materials,and multi-objective decision-making that collaborates to increase energy,reliability,and environmental performance in heterogeneous pipeline networks.展开更多
Sintering and coking are critical barriers to achieving high performance in dry reforming of methane(DRM)catalysts.A finely dispersed and thermostable Ni-based catalyst is the key to address these issues.By leveraging...Sintering and coking are critical barriers to achieving high performance in dry reforming of methane(DRM)catalysts.A finely dispersed and thermostable Ni-based catalyst is the key to address these issues.By leveraging the intrinsic superiorities of high-entropy oxides in high-temperature stability and low atomic diffusivity,in this study,a highly dispersed Ni-based catalyst is synthesized via an entropycontrolled exsolution of active components.By increasing the number of transition-metal elements in spinel oxides,the active metalsupport interaction(MSI)can be continuously strengthened,which controls the exsolution and thermal stability of Ni-based active metal in harsh reaction conditions of DRM.An optimized medium-entropy spinel(Mg_(0.4)Ni_(0.2)Co_(0.2)Zn_(0.2))Al_(2)O_(4)with the exsolution of finely dispersed Ni–Co nanoparticles displayed superior activity and stability in thermal DRM at 800°C and photothermal DRM.This entropy-controlled MSI and exsolution principle provides a significant strategy for designing robust catalysts resistant to sintering and coking for high-temperature reactions like DRM in thermal and photothermal systems.展开更多
The photocatalytic oxidation of methane(CH_(4)) to valuable chemicals like low alcohols(CH_(3)OH and C_(2)H_(5)OH) represents a significant technological advancement with implications for energy conversion and environ...The photocatalytic oxidation of methane(CH_(4)) to valuable chemicals like low alcohols(CH_(3)OH and C_(2)H_(5)OH) represents a significant technological advancement with implications for energy conversion and environmental purification.A major challenge in this field is the chemical inertness of methane and the strong oxidizing nature of photogenerated holes,which can lead to over-oxidation and reduced selectivity and efficiency.To address these issues,we have developed a sodium-doped zinc oxide(Na-ZnO) modified with cobalt oxide(CoO) catalyst.This catalyst has demonstrated excellent performance in converting methane to low alcohols,achieving a yield of 130 μmol g^(-1)h^(-1) and a selectivity of up to 96 %.The doping of Na in ZnO significantly enhances methane adsorption,while the surface-modified CoO effectively captures photogenerated holes,activates water molecules,and uses hydroxyl radicals to activate methane,thus controlling the dehydrogenation degree of methane and preventing the formation of over-oxidized products.This strategy has successfully improved the efficiency and selectivity of photocatalytic methane oxidation to low alcohols,offering a new perspective for the application of photocatalytic technology in energy and environmental fields.展开更多
In the development of coalbed methane(CBM)reservoirs using multistage fractured horizontal wells,there often exist areas that are either repeatedly stimulated or completely unstimulated between fracturing stages,leadi...In the development of coalbed methane(CBM)reservoirs using multistage fractured horizontal wells,there often exist areas that are either repeatedly stimulated or completely unstimulated between fracturing stages,leading to suboptimal reservoir performance.Currently,there is no well-established method for accurately evaluating the effectiveness of such stimulation.This study introduces,for the first time,the concept of the Fracture Network Bridging Coefficient(FNBC)as a novel metric to assess stimulation performance.By quantitatively coupling the proportions of unstimulated and overstimulated volumes,the FNBC effectively characterizes the connectivity and efficiency of the fracture network.A background grid calibration method is developed to quantify the stage-controlled volume,effectively stimulated volume,unstimulated volume,and repeatedly stimulated volume among different stages of horizontal wells.Furthermore,an optimization model is constructed by taking the FNBC as the objective function and the fracturing injection rate and fluid volume as optimization variables.The Simultaneous Perturbation Stochastic Approximation(SPSA)algorithm is employed to iteratively perturb and optimize these variables,progressively improving the FNBC until the optimal displacement rate and fluid volume corresponding to the maximum FNBC are obtained.Field application in a typical CBM multistage fractured horizontal well in China demonstrates that the FNBC increased from 0.358 to 0.539(a 50.6% improvement),with the injection rate rising from 16 m^(3)/min to 24 m^(3)/min and the average fluid volume per stage increasing from 2490 m^(3) to 3192 m^(3),significantly enhancing the stimulation effectiveness.This research provides theoretical support for designing high-efficiency stimulation strategies in unconventional reservoirs under dynamic limits.展开更多
Methane in-situ deflagration fracturing in shale is a revolutionary anhydrous technology.This paper selects shale samples from the Longmaxi Formation in Southern Sichuan to conduct deflagration fracturing tests with p...Methane in-situ deflagration fracturing in shale is a revolutionary anhydrous technology.This paper selects shale samples from the Longmaxi Formation in Southern Sichuan to conduct deflagration fracturing tests with pressures ranging from 25 MPa to 91 MPa.Pore structure changes were experimentally measured to explore the modification differences of nanoscale pore characteristics under varying deflagration pressures.The results show that within the deflagration pressure range examined in this study,(1)Deflagration fracturing can alter the pore volume and specific surface area but does not affect the distribution characteristics of the pore size's peak position.The maximum increments of total pore volume occur at a pressure of 45 MPa.(2)When the deflagration pressure is less than 45 MPa,porosity gradually increases with rising deflagration pressure.When it is greater than 45 MPa,the porosity does not change significantly.With increasing deflagration pressure,it gradually increases:from nanopores,such as mesopores and macropores,to large pores and microcracks.(3)At the low deflagration pressure stage,under the influence of high temperature,slippage pores gradually increase,which is conducive to gas desorption and diffusion migration.As pressure increases,the impact of the explosion shock wave gradually increases,the volume of seepage pores increases significantly,and seepage dominates the migration mode.展开更多
CO_(2) hydrogenation using protonic ceramic electrolysis cells(PCECs)to produce fuel gases such as CH_(4)and CO has been considered as a promising technology for effective CO_(2) utilization.However,the long-term stab...CO_(2) hydrogenation using protonic ceramic electrolysis cells(PCECs)to produce fuel gases such as CH_(4)and CO has been considered as a promising technology for effective CO_(2) utilization.However,the long-term stability of conventional PCECs based on Y and Yb doped BaZrO_(3)-BaCeO_(3)(BCZYYb)proton conductors is severely limited by their susceptibility to carbonate formation under high concentration CO_(2) .In this work,a new type PCEC based on CO_(2) -tolerant La_(5.6)WO_(11.4-δ)(LWO)material is firstly constructed.A three-layer porous-dense-porous LWO ceramic scaffold is fabricated via a pressing,dip-coating and cosintering process,followed by Ni and La_(0.6)Sr_(0.4)CoO_(3-δ)(LSC)catalyst impregnation to ensure the chemical compatibility among materials and form an efficient PCEC-based CO_(2) hydrogenation reactor.Benefits from the synergistic catalysis of nano nickel and LWO,the reactor gets a CH_(4)selectivity of over 50%at 600℃under 20%CO_(2) concentration,and it operates stably for over 320 h at 600–650℃under high CO_(2) concentrations of 50–80%,showing no degradation in CO_(2) conversion rate or CH_(4)selectivity.Postmortem analysis demonstrates that the CO_(2) absorption characteristics of LWO and the morphological uniformity of nano nickel lead to stable CO_(2) methanation.This study provides a viable strategy for designing highly stable PCEC-based CO_(2) hydrogenation reactors.展开更多
Methane is considered a potential biosignature gas.The Mars Science Laboratory(MSL)Curiosity rover has observed seasonal variations in atmospheric methane within Gale Crater,suggesting possible microbial activity.The ...Methane is considered a potential biosignature gas.The Mars Science Laboratory(MSL)Curiosity rover has observed seasonal variations in atmospheric methane within Gale Crater,suggesting possible microbial activity.The origin of this methane could be either biological or abiotic or a combination of the two.Different physical mechanisms,involving distinct environmental variables,produce varying concentrations of methane.By analyzing the influence of various environmental variables on methane partial pressures and comparing differences between physical models and empirical measurements,we can better discern methane production mechanisms.This study investigates factors affecting methane cycling.We find that temperature and pressure strongly correlate with Martian atmospheric methane,while Ultraviolet(UV)radiation at the atmospheric boundary and surface UV radiation exhibit weaker correlations.Using Fuller’s method,we successfully reproduce the seasonal methane cycle in Gale Crater.Several potential physical models suggest that gas diffusion driven by variations in pressure and temperature within the shallow subsurface regolith may represent a primary mechanism determining methane concentrations observed in Gale Crater.However,errors in the pressure-dominated model cannot be neglected.As Curiosity enters its uphill exploration phase,we suggest that atmospheric pressure will play a significant role in predicting the methane concentrations that it will detect.展开更多
Background Methane(CH_(4))emissions from ruminants significantly contribute to greenhouse gas effects and energy loss in livestock production.Methyl-coenzyme M reductase(MCR)is the key enzyme in methanogenesis,making ...Background Methane(CH_(4))emissions from ruminants significantly contribute to greenhouse gas effects and energy loss in livestock production.Methyl-coenzyme M reductase(MCR)is the key enzyme in methanogenesis,making it a promising target for CH_(4) mitigation.This study aimed to identify and validate plant-derived inhibitors by using molecular docking to screen compounds with strong binding affinity to the F430 active site of MCR and assessing their efficacy in reducing CH_(4) emissions.Results Molecular docking analysis identified salvianolic acid C(SAC)as a potent inhibitor of MCR,showing a strong binding affinity to the F430 active site(binding energy:-8.2 kcal/mol).Enzymatic inhibition assays confirmed its inhibitory effect,with a half-maximal inhibitory concentration(IC50)of 692.3μmol/L.In vitro rumen fermentation experiments demonstrated that SAC supplementation(1.5 mg/g DM)significantly reduced CH_(4)production(P<0.01)without negatively affecting major fermentation parameters.Microbial community analysis using 16S rRNA sequencing and metagenomics revealed that SAC selectively altered the rumen microbiota,increasing the relative abundance of Bacteroidota while significantly reducing Methanobrevibacter(P=0.04).Moreover,metagenomic analysis showed the downregulation of key methanogenesis-related genes(mcrA and rnfC),suggesting a dual mechanism involving direct enzymatic inhibition and microbial community modulation.Conclusions These findings indicate that SAC effectively reduces CH_(4)production by inhibiting MCR activity and reshaping the rumen microbial community.As a plant-derived compound with strong inhibitory effects on methanogenesis,SAC presents a promising and sustainable alternative to synthetic CH_(4) inhibitors,offering potential applications for mitigating CH_(4)emissions in livestock production.展开更多
基金Supported by the National Natural Science Foundation of China(52506188,52476215)Natural Science Foundation of Liaoning Province(2024-MS-139,2024JH3/10200047)Scientific Research Program of Department of Education of Liaoning Province(310125042,LJ212410143033)。
文摘In this paper,the Ni/Al_(2)O_(3) monolithic catalyst with 15%Ni content was prepared using cordierite as a matrix,and the catalyst was modified with 10%NaOH to study the methanation performance of biomass gasification simulated gas based on alkali-modified Ni/Al_(2)O_(3) monolithic catalyst.BET,TEM,H_(2)-TPR,XRD,CO_(2)-TPD and TG were used to characterize the physicochemical properties of the catalyst before and after modification.The results indicated that the CO conversion rate trends of unmodified and modified Ni/Al_(2)O_(3) monolithic catalysts over 2 h were fundamentally consistent.However,the Ni/Al_(2)O_(3) catalysts modified for 2 h demonstrated significantly enhanced performance compared to those modified for 1 h.Regarding CH4 selectivity,the modified Ni/Al_(2)O_(3) catalyst exhibited markedly better performance than the unmodified Ni/Al_(2)O_(3) catalyst,confirming the enhanced methane performance of the alkali-modified Ni/Al_(2)O_(3) monolithic catalyst.Under optimized conditions(H_(2)/CO volume ratio of 3∶1,space velocity of 10000 mL/(g·h),and temperature of 400℃),the methanation performance of the Ni/Al_(2)O_(3) monolithic catalyst modified for 2 h reached its peak,achieving a CO conversion rate of 97%with 100%CH4 selectivity.
基金Supported by Innovation Capability Support Program of Shaanxi(2024RS-CXTD-53,2024ZC-KJXX-096)the Key R&D Program of Shaanxi Province(2022QCY-LL-69)Xi’an Science and Technology Project(24GXFW0089)。
文摘Under the backdrop of“Carbon Peak and Carbon Neutrality”(dual carbon)goal in China,the methane-carbon dioxide reforming reaction has attracted considerable attention due to its environmental benefits of converting two greenhouse gases(methane and carbon dioxide)into syngas and its promising industrial applications.Nickel(Ni)-based catalysts,with high catalytic activity,low cost,and abundant resources,are considered ideal candidates for industrial applications.In this article,three reaction kinetic models were briefly introduced,namely the Power-Law(PL)model,the Eley-Rideal(ER)model,and the Langmuir-Hinshelwood-Hougen-Watson(LHHW)model.Based on the LHHW model,the reaction kinetics and mechanisms of different catalytic systems were systematically discussed,including the properties of supports,the doping of noble metals and transition metals,the role of promoters,and the influence of the geometric and electronic structures of Ni on the reaction mechanism.Furthermore,the kinetics of carbon deposition and elimination on various catalysts were analyzed.Based on the reaction rate expressions for carbon elimination,the reasons for the high activity of transition metal iron(Fe)-doped catalysts and core-shell structured catalysts in carbon elimination were explained.Based on the detailed collation and comparative analysis of the reaction mechanisms and kinetic characteristics across diverse Ni-based catalytic systems,a theoretical guidance for the designing of high-performance catalysts was provided in this work.
基金Supported by the Science and Technology Major Project of Liaoning Province(2024JH2,1025000892)the Fundamental Research Funds for the Universities of Liaoning Province(LJ232410143051)+1 种基金Liaoning Provincial Science and Technology Program 2023JHl/10400006Shenyang Science and Technology Program(24-213-3-09)。
文摘Methane dehydroaromatization(MDA)presents a promising carbon-neutral pathway for benzene,toluene,and xylene(BTX)production,alternative to petroleumderived routes.Elucidating the regulatory mechanisms of Brønsted acid site(BAS)strength on reaction pathways,alongside the spatial proximity effects between BAS and Mo active sites in bifunctional synergy,remains a critical scientific challenge in catalyst design.This study systematically tunes both BAS strength(via isomorphous metal substitution)and Mo-BAS spatial proximity in zeolites,integrating MDA catalytic evaluations with density functional theory(DFT)calculations to dissect their individual contributions.Strongly acidic BAS catalysts(compared to moderately acidic Fe/Ga-substituted counterparts)exhibit superior performance,evidenced by enhanced aromatic yields.Conversely,weakly acidic Bsubstituted zeolites demonstrate optimal mono-/bifunctional synergy,outperforming moderate-acid systems.DFT results reveal that acid strength dictates C−H activation mechanisms by modulating the energy barriers of rate-determining steps.While Al-zeolites deliver the highest activity,B-substituted systems display unique potential for mechanistic investigations.Spatial proximity analysis indicates that micrometer-scale Mo-BAS distances hinder effective synergy due to exceeding electron interaction and mass transfer limits,whereas nanometer-scale proximity enhances activity(via accelerated intermediate transport)and suppresses coke formation.These findings establish a theoretical framework for rationalizing zeolite catalyst optimization through BAS property engineering and spatial control of Mo-BAS cooperation,providing actionable guidelines for designing next-generation MDA catalysts.
基金Supported by Innovative Research Groups of the National Natural Science Foundation of China(22021004)。
文摘Catalytic decomposition of methane,which produces high-purity hydrogen and high-value-added carbon nanomaterials,has shown considerable potential for development and is expected to yield significant economic benefits in the future.However,designing catalysts that simultaneously exhibit high activity and long-term stability remains a significant challenge.Tuning the catalyst’s structure and electronic properties is an effective strategy for enhancing the reaction performance.In this work,a series of NixZr/ZSM-5 catalysts were prepared using the incipient wetness impregnation method,and the effect of Zr loadings on catalyst properties and performance was systematically investigated.The calcined and reduced catalysts were characterized by low-temperature N_(2)adsorption-desorption,XRD,SEM,H_(2)-TPR and XPS.The results showed that the addition of Zr significantly increased the specific surface area of the catalyst and reduced the metal particle size.Smaller NiO particles were found to enter the pores of the HZSM-5 support,and electronic interactions between NiO and ZrO_(2)markedly enhanced the metal-support interaction.The catalyst exhibited optimal catalytic performance at a Zr loading of 5%,achieving a maximum methane conversion of 68%at 625℃,maintaining activity for 900 min,and delivering a carbon yield of 1927%.Further increasing the Zr loading yielded only limited improvements in catalytic performance.Characterization of the spent catalysts and carbon products via TEM,Raman spectroscopy,and TGA revealed that the introduction of ZrO_(2)reduced metal sintering and promoted a shift in carbon nanofibers growth mode from tip-growth to base-growth.The mechanism of base-growth enabled the catalyst to maintain reaction activity for an extended period.
基金supported by the Portuguese Foundation for Science and Technology(FCT)under the scope of the strategic funding of UIDB/04469/2020 unit and by the CM4Methane project(Ref:PTDC/BTA-BTA/2249/2021,DOI 10.54499/PTDC/BTABTA/2249/2021)FCT and European Union(EU),through the Portuguese State Budget and the European Social Fund under the scope of Norte2020-Programa Operacional Regional do Norte,also funded the SFRH/BD/132003/2017 and COVID/BD/152431/2022 grants held by Cátia S.N.Braga.,and the SFRH/BD/147271/2019 grant held by João C.Sequeira.M.SaloméDuarte acknowledges FCT for the Junior Research contract obtained under the scope of the Scientific Stimulus Employment 2022(ref:2022.06569.CEECIND/CP1718/CT0004,doi:https://doi.org/10.54499/2022.06569.CEECIND/CP1718/CT0004)PhD M.Fernando R.Pereira and PhD O.SaloméG.Soares from the Laboratory of Separation and Reaction Engineering-Laboratory of Catalysis and Materials,Faculty of Engineering(University of Porto),for providing the AC used in this study.
文摘Conductive materials(CM)can improve methane production(MP)efficiency in many methanogenic systems.However,several types of CM exist,and there are uncertainties regarding whether they all improve MP efficiency to the same extent and modulate microbial communities in a similar way.To investigate that,different microbial enrichments with and without activated carbon(AC),magnetite(Mag),and zeolites(Zeo)(at 0.5 g/L)were developed.MP profiles and microbial composition changes were compared among enrichments.The behavior of all enrichments was different,although the initial inoculum sludge was the same.Lag phase duration was lower in AC enrichment,while the complete conversion of butyrate to methane was faster in Mag enrichment.Syntrophomonas was the most abundant bacterial genus in all enrichments,but changes in the methanogenic community were evident.Acetoclastic methanogens were more diverse in Mag enrichment,with microorganisms assigned to Methanosarcina and Methanothrix gener1,but Methanothrix was the only acetoclastic methanogen in the other enrichments.On the other hand,different species of hydrogenotrophic methanogens prevailed in distinct enrichments.The metatranscriptomics results revealed that the dominant mechanism of interspecies electron transfer in the AC enrichment utilized hydrogen as the electron carrier,and no evidences of direct interspecies electron transfer(DIET)could be found.These results showed how different CM modulate microbial communities and affect MP efficiency through mechanisms that do not necessarily involve DIET or mediation via CM.
基金supported by the Cooperative Research Program for Agriculture Science and Technology Development,Republic of Korea(Grant No.RS-2022-RD010034)the 2023 Yellow Sea Wetland International Cooperation Key Project,China(Grant No.HHSDKT202303).
文摘Rice fields are one of the largest sources of methane(CH4),a potent greenhouse gas contributing significantly to global warming.Elucidating the underlying mechanisms and mitigating CH4 emissions from paddy fields is crucial for combating climate change while ensuring sustainable food production.This review investigates the biological processes governing CH4 generation in rice fields,focusing on how soil microorganisms generate CH4 under waterlogged,anaerobic conditions.It also explores the mechanisms by which CH4 escapes into the atmosphere through plant-mediated transport,diffusion,and ebullition.Several factors influencing CH4 emissions are discussed,including soil composition,water management,exogenous organic matter application,rice variety selection,and local climate conditions.Strategies that can be implemented to reduce CH4 emissions are assessed,such as alternate wetting and drying,urea deep placement,biochar application,optimized fertilizer application,and breeding of rice varieties with low CH4 emissions.Novel solutions,such as the enhancement of methane-consuming bacteria in soils using microbial-based approaches,are also explored.The importance of integrating innovative technologies,improved farming practices,and interdisciplinary research is emphasized to develop practical and scalable strategies for reducing CH4 emissions.By addressing these challenges,we can advance towards the attainment of sustainable agriculture and global climate goals.This review aims to serve as a comprehensive resource for researchers,policymakers,and practitioners seeking to understand and mitigate CH4 emissions from rice cultivation.
基金supported by the National Natural Science Foundation of China(No.52500142)the National Postdoctoral Program for Innovative Talents under Grant Number BX20250334the China Postdoctoral Science Foundation(Certificate Number:2025M771285)。
文摘Directly burning methane for energy production wastes chemical potential and exacerbates CO_(2) emissions,while catalytic conversion into high-value fuel/chemicals provides economic and environmental sustainability.Photocatalytic CH_(4) conversion has emerged as a transformative technology,enabling selective oxidation under ambient conditions to directly synthesize value-added organic compounds.This addresses the dual challenges of climate mitigation and sustainable energy conversion.This review systematically examines the development of photocata lytic CH_(4) conversion,with three key dimensions.Firstly,we elucidate fundamental reaction mechanisms governing CH_(4) activation,emphasizing critical steps such as C-H bond scission via charge transfer,intermediate stabilization,and product desorption kinetics.Subsequently,we classify emerging photocata lytic pathways(partial oxidation,coupling,and reforming)and analyze material innovations.Finally,the challenges of the current photocata lytic CH_(4)conversion system and catalyst development were discussed,and perspectives were presented.The overarching objective of this work is to provide a comprehensive roadmap for the development of solardriven CH_(4) conversion systems that are aligned with global carbon neutrality goals.
基金supported by the National Natural Science Foundation of China(No.42225103).
文摘Lakes are carbon dioxide(CO_(2))and methane(CH_(4))emission hotspots,whose associated flux is spatially vari-able.Many studies have investigated the impact of microorganisms and environmental factors on CO_(2) and CH_(4) emissions between different lakes.However,the carbon emissions and their influencing factors of different areas within a single lake remain poorly understood.Accordingly,this study investigates CO_(2) and CH_(4) emission hetero-geneity in a large floodplain lake system and distribution characteristics of associated functional microorganisms.Findings show that mean CO_(2) and CH_(4) flux values in the sub lake area were 62.03±24.21 mg/(m2·day)and 5.97±3.2μg/(m2·day),which were greater by factors of 1.78 and 2.96 compared to the water channel and the main lake area,respectively.The alpha diversity of methanogens in the sub lake area was lower than that in the main lake and water channel areas.The abundance of methanogens in bottom water layer was higher compared with the middle and surface layers.Conversely,the abundance of methane(CH_(4))-oxidizing bacteria in the surface layer was higher than that in the bottom layer.Additionally,the composition of methanogen and CH_(4)-oxidizing bacterial community,chlorophyll a(Chl-a),pH,total phosphorus(TP)and dissolved organic carbon(DOC)con-tent constituted the dominate driving factors affecting lake C emissions.Results from this study can be used to improve our understanding of lake spatial heterogeneous of CO_(2) and CH_(4) emission and the driving mechanisms within floodplain lakes under the coupling effects of functional C microorganisms and environmental factors.
基金the PICTO project(RFCR-CT-2018-800711)funded by the European Research Fund for Coal and Steel(RFCS)and the Polish Ministry of Science and Higher Education(W93/FBWiS/2018).
文摘The research presented in this paper aimed to analyze the evolution of fractures in strata in relation to the progress of longwall mining.To achieve this objective,an introscopic probe equipped with a highresolution camera was developed,along with additional equipment that enables continuous recording of the internal surfaces of drainage boreholes exceeding 100 m in depth.The probe was utilized to test two methane drainage boreholes in the Z-3b longwall,which operates within the 501/3 coal seam of the Jankowice mine in Poland.Automatic image analysis methods were applied to evaluate the recorded images,based on a newly developed classificationsystem for fractures categorized by size and number.The results were compared with an analysis of changes in the methane capture rate from the drainage boreholes,which correlated with longwall mining progress.A strong correlation was observed between the number of fractures and the lithology of the strata layers.The largest number of fractures and their evolution were recorded in the coal layers,followed by the shale layers,while the sandstone layers exhibited the least number of fractures.Based on parallel measurements of the methane capture rate from the drainage boreholes during the progress of longwall mining,the extent of the strata's fracture zone was determined to range from 6 m to 36 m.Within the fracture zone,the strata are highly fractured,which leads to an increase in methane emissions through seepage and diffusion processes.
基金funded by the Beef Cattle Research Council Cluster(FDE.18.21C)Natural Sciences and Engineering Research Council of Canada(NSERC)Discovery,NSERC Canadian Research Chair(Tier 1)program+2 种基金NSERC Alliance program(ALLRP 588541‐23)Foundation for Food&Agriculture Research Greener Cattle Initiative(Award ID 22‐000373)DSM Nutritional Products,Kaiseraugst,Switzerland。
文摘Background The enteric methane inhibitor 3-nitrooxypropanol(3-NOP)inhibits the key enzyme in ruminal methanogenesis,but whether short-term(ST)and long-term(LT)dietary supplementation has similar effects on rumen microbiota in beef cattle and how microbes change after 3-NOP withdrawal have not been studied.This study investigated changes in rumen bacteria,archaea,and protozoa after ST and LT dietary supplementation and removal of 3-NOP using metataxonomic analysis.Results A total of 143 rumen samples were collected from two beef cattle studies with 3-NOP supplementation.The ST study(95 samples)used eight ruminally cannulated beef cattle in a 4×4 Latin square design with four 28-d of 3-NOP treatments[mg/kg of dry matter(DM)]:control:0,low:53,med:161,and high:345.The LT study(48 samples)was a completely randomized design with two 3-NOP treatments[control:0,and high:280 mg/kg of DM)fed for 112-d followed by a 16-d withdrawal(without 3-NOP).Bacterial and archaeal communities were significantly affected by 3-NOP supplementation but limited effects on protozoal communities were observed.Under ST supplementation,the relative abundances of Prevotella,Methanobrevibacter(Mbb.)ruminantium,Methanosphaera sp.ISO3-F5,and Entodinium were increased(Q<0.05),whereas those of Mbb.gottschalkii and Epidinium were decreased(Q<0.05)with 3-NOP supplementation.In LT study,relative abundances of Mbb.ruminantium,and Methanosphaera sp.Group5 were increased(Q<0.05),while those of Saccharofermentans and Mbb.gottschalkii were decreased(Q<0.05)with 3-NOP supplementation.Comparison between 3-NOP supplementation and the withdrawal revealed increased relative abundances of Clostridia UCG-014 and Oscillospiraceae NK4A214 group and decreased those of Eubacterium nodatum group and Methanosphaera sp.Group5(P<0.05)after 3-NOP withdrawal.Further comparison of rumen microbiota between control and 3-NOP withdrawal showed significantly higher(P=0.029)relative abundances of Eggerthellaceae DNF00809,p-1088-a5 gut group,and Family XII UCG-001 in control group while no significant differences were detected for archaea and protozoa.Microbial network analysis revealed that microbial interactions differed by both 3-NOP dose and durations.Conclusions Both ST and LT supplementation affected overall rumen microbial profile,with individual microbial groups responded to 3-NOP supplementation differently.After 3-NOP withdrawal,not all microbes showed recovery,indicating that the 3-NOP driven shifts were only partially reversible.These findings provide an understanding of the effects of 3-NOP on rumen microbial communities and their adaptability to methane mitigation strategies.
基金supported by the National Science and Technology Major Project of China(No.2025ZD1405702)the Scientific Research and Technology Development Project of PetroChina Coalbed Methane Co.,Ltd.(Project No.25MQCTSG010)Applied Science and Technology Project of PetroChina Company Limited(2023ZZ18YJ04).
文摘Significant differences exist between deep and medium-shallow coalbed methane(CBM)reservoirs.The unclear understanding of flowback and production behavior severely constrains the development of deep CBM resources.To address this challenge,guided by the gas-liquid two-phase flow theory in ultra-low permeability reservoirs,and integrating theoretical analysis,numerical simulation,and insights from production practices,this study classifies the flowback and production stages of deep CBM well considering the Daning-Jixian Block,Eastern Ordos Basin as a representative case.We summarize the flowback characteristics for each stage and establish a standard flowback production type curve,aiming to guide field operations.The results indicate that:(a)The production process of deep CBM horizontal wells can be divided into five distinct stages:initial single-phase water dewatering stage,initial gas appearance to peak water production stage,gas breakthrough to peak gas production stage,stable production and decline stage,and low-rate production stage.(b)Based on reservoir energy,two standard type curves for horizontal well flowback production are established:the‘Sufficient Reservoir Energy’type and the‘Insufficient Reservoir Energy’type.The former achieves a higher initial gas rate(up to 12×10^(4)m^(3)/d)but exhibits poorer stability,while the latter achieves a lower stable rate(up to 8×10^(4)m^(3)/d)but demonstrates stronger stability.Numerical simulation confirms these behavioral patterns and reveals the underlying mechanisms related to the effectively drained area where pressure is significantly depleted.The findings from this study have guided the flowback production operations in 53 deep CBM wells with positive results,demonstrating high potential for broad application.
基金financial support from the National Key R&D Program of China(2022YFA1504500 and 2023YFA1506300)the National Natural Science Foundation of China(22588201,22225204,and 22472169)+1 种基金the Strategic Priority Research Program of the Chinese Academy of Sciences(XDB0600100)Liaoning Binhai Laboratory(LBLG-2024-03)。
文摘The traditional ammonia synthesis via the Haber–Bosch process requires large consumption of highpurity H_(2) and causes significant carbon emissions owing to the energy-intensive and complex hydrogen production steps conducted under harsh reaction conditions.Herein,we report a cyclic catalytic process for the production of NH_(3) by directly utilizing earth-abundant CH_(4) as a hydrogen source for N_(2) hydrogenation while simultaneously co-producing H_(2) over an alumina-supported iron catalyst(Fe/Al_(2)O_(3)).It achieves exceptional productivities of 2300μmol g^(-1)h^(-1)for NH_(3) and 400 mmol g^(-1)h^(-1)for H_(2) at700℃.By eliminating the coke that results from CH_(4) pyrolysis through a reaction with the greenhouse gas CO_(2) to produce valuable CO,we establish an atom-economic cyclic catalytic process while producing a CO stream intrinsically separated in the regeneration step.Mechanistic investigations indicate that the iron species in Fe/Al_(2) O_(3) serve as tri-functional active sites for CH_(4) pyrolysis,N_(2) hydrogenation,and coke elimination to produce CO,thus enabling an efficient and environmentally friendly cyclic catalytic process.
文摘Oil and gas pipelines are a vital long-distance liquid and natural gas carrier,but their functionality is being assessed from a two-fold perspective of power economy and environmentalism.This review concurs on the way these outcomes are interdependent throughout the pipeline lifecycle by contending that the efficiency,emissions,reliability,and environmental risk are jointly determined through the shared design decisions,operating plans,integrity platforms,and monitoring and response plans.Our initial conceptualization is pipeline systems and performance measures,which are characterized by boundary and comparability issues of particular energy consumption,methane intensity,and release consequence measures.Next,we look at hydraulic and station optimization,focusing on the need to look at the importance of equipment performance at part loads,constraints consciousness dispatch,and transient management to prevent the erosion of integrity levels by efficiency gains.The integrity management is appraised as one of the key enablers of stewardship that connects the corrosion prevention,in-line inspection and verification,and the risk-based mitigation to less likely failure,less disruptive interventions,and reduced emissions during maintenance.We compare the leak and spill prevention,detection,quantification,and response of the SCADA(supervisory control and data acquisition)-based computational monitoring,distributed sensing,as well as aerial/satellite,focusing on the validation,characterization of uncertainty,and the operational parameters modulating the time-to-detect and isolation performance.Environmental impacts of the lifecycle,not related to releases,are explained,such as routing and construction disturbance,management of right-of-way,station externalities,decommissioning,and climate resilience.Lastly,we assess new technologies,such as continuous monitoring networks,electrification,superior materials,and multi-objective decision-making that collaborates to increase energy,reliability,and environmental performance in heterogeneous pipeline networks.
基金supported by the National Key R&D Program of China(2023YFB4104600)National Natural Science Foundation of China(52572313)+1 种基金Tangshan Talent Funding Project(A202202007)Shenzhen Science and Technology Innovation Commission under Grant No.20231120185819001。
文摘Sintering and coking are critical barriers to achieving high performance in dry reforming of methane(DRM)catalysts.A finely dispersed and thermostable Ni-based catalyst is the key to address these issues.By leveraging the intrinsic superiorities of high-entropy oxides in high-temperature stability and low atomic diffusivity,in this study,a highly dispersed Ni-based catalyst is synthesized via an entropycontrolled exsolution of active components.By increasing the number of transition-metal elements in spinel oxides,the active metalsupport interaction(MSI)can be continuously strengthened,which controls the exsolution and thermal stability of Ni-based active metal in harsh reaction conditions of DRM.An optimized medium-entropy spinel(Mg_(0.4)Ni_(0.2)Co_(0.2)Zn_(0.2))Al_(2)O_(4)with the exsolution of finely dispersed Ni–Co nanoparticles displayed superior activity and stability in thermal DRM at 800°C and photothermal DRM.This entropy-controlled MSI and exsolution principle provides a significant strategy for designing robust catalysts resistant to sintering and coking for high-temperature reactions like DRM in thermal and photothermal systems.
基金support from the Zhejiang Provincial Natural Science Foundation of China (No.LQ24B030011)the Ningbo Natural Science Foundation (No.2023J181)+4 种基金the Open Research Fund of Key Laboratory of Functional Inorganic Materials Chemistry of the Ministry of Education (Heilongjiang University)the Start-up Funding offered by Ningbo University of Technology to J.D.LiNational Natural Science Foundation of China (No.U24A2071)Postdoctoral Research Start-up Fund (No.2111224002)Harbin Normal University Talent Plan (No.1305124213) to Y.D.Liu。
文摘The photocatalytic oxidation of methane(CH_(4)) to valuable chemicals like low alcohols(CH_(3)OH and C_(2)H_(5)OH) represents a significant technological advancement with implications for energy conversion and environmental purification.A major challenge in this field is the chemical inertness of methane and the strong oxidizing nature of photogenerated holes,which can lead to over-oxidation and reduced selectivity and efficiency.To address these issues,we have developed a sodium-doped zinc oxide(Na-ZnO) modified with cobalt oxide(CoO) catalyst.This catalyst has demonstrated excellent performance in converting methane to low alcohols,achieving a yield of 130 μmol g^(-1)h^(-1) and a selectivity of up to 96 %.The doping of Na in ZnO significantly enhances methane adsorption,while the surface-modified CoO effectively captures photogenerated holes,activates water molecules,and uses hydroxyl radicals to activate methane,thus controlling the dehydrogenation degree of methane and preventing the formation of over-oxidized products.This strategy has successfully improved the efficiency and selectivity of photocatalytic methane oxidation to low alcohols,offering a new perspective for the application of photocatalytic technology in energy and environmental fields.
基金the financial support from National Natural Science Foundation of China(No.52474029)Strategic and Applied Scientific Research Project of PetroChina Company Limited(2023ZZ18,2023ZZ18YJ04).
文摘In the development of coalbed methane(CBM)reservoirs using multistage fractured horizontal wells,there often exist areas that are either repeatedly stimulated or completely unstimulated between fracturing stages,leading to suboptimal reservoir performance.Currently,there is no well-established method for accurately evaluating the effectiveness of such stimulation.This study introduces,for the first time,the concept of the Fracture Network Bridging Coefficient(FNBC)as a novel metric to assess stimulation performance.By quantitatively coupling the proportions of unstimulated and overstimulated volumes,the FNBC effectively characterizes the connectivity and efficiency of the fracture network.A background grid calibration method is developed to quantify the stage-controlled volume,effectively stimulated volume,unstimulated volume,and repeatedly stimulated volume among different stages of horizontal wells.Furthermore,an optimization model is constructed by taking the FNBC as the objective function and the fracturing injection rate and fluid volume as optimization variables.The Simultaneous Perturbation Stochastic Approximation(SPSA)algorithm is employed to iteratively perturb and optimize these variables,progressively improving the FNBC until the optimal displacement rate and fluid volume corresponding to the maximum FNBC are obtained.Field application in a typical CBM multistage fractured horizontal well in China demonstrates that the FNBC increased from 0.358 to 0.539(a 50.6% improvement),with the injection rate rising from 16 m^(3)/min to 24 m^(3)/min and the average fluid volume per stage increasing from 2490 m^(3) to 3192 m^(3),significantly enhancing the stimulation effectiveness.This research provides theoretical support for designing high-efficiency stimulation strategies in unconventional reservoirs under dynamic limits.
基金supported by the National Key Research and Development Program of China(Grant No.2020YFA0711800)the National Natural Science Foundation of China(Grant No.42372159).
文摘Methane in-situ deflagration fracturing in shale is a revolutionary anhydrous technology.This paper selects shale samples from the Longmaxi Formation in Southern Sichuan to conduct deflagration fracturing tests with pressures ranging from 25 MPa to 91 MPa.Pore structure changes were experimentally measured to explore the modification differences of nanoscale pore characteristics under varying deflagration pressures.The results show that within the deflagration pressure range examined in this study,(1)Deflagration fracturing can alter the pore volume and specific surface area but does not affect the distribution characteristics of the pore size's peak position.The maximum increments of total pore volume occur at a pressure of 45 MPa.(2)When the deflagration pressure is less than 45 MPa,porosity gradually increases with rising deflagration pressure.When it is greater than 45 MPa,the porosity does not change significantly.With increasing deflagration pressure,it gradually increases:from nanopores,such as mesopores and macropores,to large pores and microcracks.(3)At the low deflagration pressure stage,under the influence of high temperature,slippage pores gradually increase,which is conducive to gas desorption and diffusion migration.As pressure increases,the impact of the explosion shock wave gradually increases,the volume of seepage pores increases significantly,and seepage dominates the migration mode.
基金financially supported by the National Key R&D Program of China(2024YFF0506302)the National Natural Science Foundation of China(52372246)+1 种基金the Frontier Technologies R&D Program of Jiangsu(BF2024041)the Shanghai Engineering Research Center of Inorganic Energy Materials and Electric Power Sources(18DZ2280800)。
文摘CO_(2) hydrogenation using protonic ceramic electrolysis cells(PCECs)to produce fuel gases such as CH_(4)and CO has been considered as a promising technology for effective CO_(2) utilization.However,the long-term stability of conventional PCECs based on Y and Yb doped BaZrO_(3)-BaCeO_(3)(BCZYYb)proton conductors is severely limited by their susceptibility to carbonate formation under high concentration CO_(2) .In this work,a new type PCEC based on CO_(2) -tolerant La_(5.6)WO_(11.4-δ)(LWO)material is firstly constructed.A three-layer porous-dense-porous LWO ceramic scaffold is fabricated via a pressing,dip-coating and cosintering process,followed by Ni and La_(0.6)Sr_(0.4)CoO_(3-δ)(LSC)catalyst impregnation to ensure the chemical compatibility among materials and form an efficient PCEC-based CO_(2) hydrogenation reactor.Benefits from the synergistic catalysis of nano nickel and LWO,the reactor gets a CH_(4)selectivity of over 50%at 600℃under 20%CO_(2) concentration,and it operates stably for over 320 h at 600–650℃under high CO_(2) concentrations of 50–80%,showing no degradation in CO_(2) conversion rate or CH_(4)selectivity.Postmortem analysis demonstrates that the CO_(2) absorption characteristics of LWO and the morphological uniformity of nano nickel lead to stable CO_(2) methanation.This study provides a viable strategy for designing highly stable PCEC-based CO_(2) hydrogenation reactors.
基金supported by the National Natural Science Foundation of China NSFC(Grant No.42330602,42275139)the National Key Research and Development Program of China(Grant No.2024YFF0809401)+2 种基金the Anhui Provincial Natural Science Foundation(Grant No.2208085UQ02)Innovation Center for Fengyun Meteorological Satellite Special Project(Grant No.FY-APP-ZX-2022.0211)the Joint Laboratory of Fengyun Remote Sensing.
文摘Methane is considered a potential biosignature gas.The Mars Science Laboratory(MSL)Curiosity rover has observed seasonal variations in atmospheric methane within Gale Crater,suggesting possible microbial activity.The origin of this methane could be either biological or abiotic or a combination of the two.Different physical mechanisms,involving distinct environmental variables,produce varying concentrations of methane.By analyzing the influence of various environmental variables on methane partial pressures and comparing differences between physical models and empirical measurements,we can better discern methane production mechanisms.This study investigates factors affecting methane cycling.We find that temperature and pressure strongly correlate with Martian atmospheric methane,while Ultraviolet(UV)radiation at the atmospheric boundary and surface UV radiation exhibit weaker correlations.Using Fuller’s method,we successfully reproduce the seasonal methane cycle in Gale Crater.Several potential physical models suggest that gas diffusion driven by variations in pressure and temperature within the shallow subsurface regolith may represent a primary mechanism determining methane concentrations observed in Gale Crater.However,errors in the pressure-dominated model cannot be neglected.As Curiosity enters its uphill exploration phase,we suggest that atmospheric pressure will play a significant role in predicting the methane concentrations that it will detect.
基金funded by the Integrated Demonstration of Scalable and Efficient Healthy Breeding for Cattle and Sheep(Grant No.2022YFD1301100)Instant Intelligent Diagnosis and Risk Warning Methods for Nutritional and Metabolic-Type Periparturient Cow Paralysis(Grant No.2024-YWF-ZYSQ-10)。
文摘Background Methane(CH_(4))emissions from ruminants significantly contribute to greenhouse gas effects and energy loss in livestock production.Methyl-coenzyme M reductase(MCR)is the key enzyme in methanogenesis,making it a promising target for CH_(4) mitigation.This study aimed to identify and validate plant-derived inhibitors by using molecular docking to screen compounds with strong binding affinity to the F430 active site of MCR and assessing their efficacy in reducing CH_(4) emissions.Results Molecular docking analysis identified salvianolic acid C(SAC)as a potent inhibitor of MCR,showing a strong binding affinity to the F430 active site(binding energy:-8.2 kcal/mol).Enzymatic inhibition assays confirmed its inhibitory effect,with a half-maximal inhibitory concentration(IC50)of 692.3μmol/L.In vitro rumen fermentation experiments demonstrated that SAC supplementation(1.5 mg/g DM)significantly reduced CH_(4)production(P<0.01)without negatively affecting major fermentation parameters.Microbial community analysis using 16S rRNA sequencing and metagenomics revealed that SAC selectively altered the rumen microbiota,increasing the relative abundance of Bacteroidota while significantly reducing Methanobrevibacter(P=0.04).Moreover,metagenomic analysis showed the downregulation of key methanogenesis-related genes(mcrA and rnfC),suggesting a dual mechanism involving direct enzymatic inhibition and microbial community modulation.Conclusions These findings indicate that SAC effectively reduces CH_(4)production by inhibiting MCR activity and reshaping the rumen microbial community.As a plant-derived compound with strong inhibitory effects on methanogenesis,SAC presents a promising and sustainable alternative to synthetic CH_(4) inhibitors,offering potential applications for mitigating CH_(4)emissions in livestock production.
