Developing deep fragmented soft coalbed methane(CBM)can significantly enhance domestic natural gas supplies,reduce reliance on imported energy,and bolster national energy security.This manuscript provides a comprehens...Developing deep fragmented soft coalbed methane(CBM)can significantly enhance domestic natural gas supplies,reduce reliance on imported energy,and bolster national energy security.This manuscript provides a comprehensive review of commonly employed coalbed methane extraction technologies.It then delves into several critical issues in the current stage of CBM exploration and development in China,including the compatibility of existing technologies with CBM reservoirs,the characteristics and occurrence states of CBM reservoirs,critical desorption pressure,and gas generation mechanisms.Our research indicates that current CBM exploration and development technologies in China have reached an internationally advanced level,yet the industry is facing unprecedented challenges.Despite progress in low-permeability,high-value coal seams,significant breakthroughs have not been achieved in exploring other types of coal seams.For different coal reservoirs,integrated extraction technologies have been developed,such as surface pre-depressurisation and segmented hydraulic fracturing of coal seam roof strata.Additionally,techniques like large-scale volume fracturing in horizontal wells have been established,significantly enhancing reservoir stimulation effects and coalbed methane recovery rates.However,all of these technologies are fundamentally based on permeation.These technologies lack direct methods aimed at enhancing the diffusion rate of CBM,thereby failing to fully reflect the unique characteristics of CBM.Current CBM exploration and development theories and technologies are not universally applicable to all coal seams.They do not adequately account for the predominantly adsorbed state of CBM,and the complex and variable gas generation mechanisms further constrain CBM development in China.Finally,continuous exploration of new deep CBM exploration technologies is necessary.Integrating more effective reservoir stimulation technologies is essential to enhance technical adaptability concerning CBM reservoir characteristics,gas occurrence states,and gas generation mechanisms,ultimately achieving efficient CBM development.We conclude that while China possesses a substantial foundation of deep fractured CBM resources,industry development is constrained and requires continuous exploration of new CBM exploration and development technologies to utilize these resources effectively.展开更多
Cutting farming-related methane emissions from ruminants is critical in the battle against climate change.Since scientists initially investigated the potential of marine macroalgae to reduce methane emissions,using se...Cutting farming-related methane emissions from ruminants is critical in the battle against climate change.Since scientists initially investigated the potential of marine macroalgae to reduce methane emissions,using seaweeds as an anti-methanogenic feed additive has become prevailing in recent years.Asparagopsis taxiformis is the preferred species because it contains a relatively higher concentration of bromoform.As a type of halogenated methane analogue,bromoform contained in A.taxiformis can specifically inhibit the activity of coenzyme M methyltransferase,thereby blocking the ruminal methanogenesis.However,bromoform is a potential toxin and ozone-depleting substance.In response,current research focuses on the effects of bromoform-enriched seaweed supplementation on ruminant productivity and safety,as well as the impact of large-scale cultivation of seaweeds on the atmospheric environment.The current research on seaweed still needs to be improved,especially in developing more species with low bromoform content,such as Bonnemaisonia hamifera,Dictyota bartayresii,and Cystoseira trinodis.Otherwise,seaweed is rich in bioactive substances and exhibits antibacterial,anti-inflammatory,and other physiological properties,but research on the role of these bioactive compounds in methane emissions is lacking.It is worthy of deeper investigation to identify more potential bioactive compounds.As a new focus of attention,seaweed has attracted the interest of many scientists.Nevertheless,seaweed still faces some challenges as a feed additive to ruminants,such as the residues of heavy metals(iodine and bromine)and bromoform in milk or meat,as well as the establishment of a supply chain for seaweed cultivation,preservation,and processing.We have concluded that the methane-reducing efficacy of seaweed is indisputable.However,its application as a commercial feed additive is still influenced by factors such as safety,costs,policy incentives,and regulations.展开更多
Natural gas hydrates widely accumulate in submarine sediments composed of clay minerals.However,due to the complex physiochemistry and micron-sized particles of clay minerals,their effects on methane hydrate(MH)format...Natural gas hydrates widely accumulate in submarine sediments composed of clay minerals.However,due to the complex physiochemistry and micron-sized particles of clay minerals,their effects on methane hydrate(MH)formation and dissociation are still in controversy.In this study,montmorillonite and illite were separately mixed with quartz sand to investigate their effects on MH formation and dissociation.The microstructure of synthesized samples was observed by cryo-SEM innovatively to understand the effects of montmorillonite and illite on MH phase transition in micron scale.Results show that montmorillonite and illite both show the inhibition on MH formation kinetics and water-to-hydrate conversion,and illite shows a stronger inhibition.The 10 wt%montmorillonite addition significantly retards MH formation rate,and the 20 wt%montmorillonite has a less inhibition on the rate.The increase of illite mass ratio(0-20 wt%)retards the rate of MH formation.As the content of clay minerals increase,the water-to-hydrate conversion decreases.Cryo-SEM images presented that montmorillonite aggregates separate as individual clusters while illite particles pack as face-to-face configuration under the interaction with water.The surface-overlapped illite aggregates would make sediments pack tightly,hinder the contact between gas and water,and result in the more significant inhibition on MH formation kinetics.Under the depressurization method,the addition of clay minerals facilitates MH dissociation rate.Physicochemical properties of clay minerals and MH distribution in the pore space lead to the faster dissociation rate in clay-containing sediments.The results of this study would provide beneficial guides on geological investigations and optimizing strategies of natural gas production in marine hydrate-bearing sediments.展开更多
Methane contributes to global warming,and livestock is one of the sources of methane production.However,methane emission studies using bibliometric tools in livestock are lacking.Given the negative impact of climate c...Methane contributes to global warming,and livestock is one of the sources of methane production.However,methane emission studies using bibliometric tools in livestock are lacking.Given the negative impact of climate change on the ecosystem and the rise in methane emissions,it is essential to conduct a bibliometrics study to provide an overview and research trends.We used the Bibliometrix package and VOSviewer to decipher bibliometric indices for methane emissions in cattle farms(MECF).Current dataset were collected from the Web of Science(Core Collection)database,and 8,998 publications were analyzed.The most co-occurring keywords scientists preferred were methane(1,528),greenhouse gas(443),methane emissions(440),and cattle(369).Methane was the most frequently used keyword in the published scientific literature.Thematic evolution of research themes and trend results highlighted carbon dioxide,methane,dairy cattle,cattle,and risk factors during 1999–2017.Chinese Academy of Sciences ranked on top with 485 publications,followed by Agriculture&Agri-Food Canada,University of Colorado,National Oceanic and Atmospheric Administration,and Aarhus University.Chinese Academy of Sciences was also the most cited organization,followed by the University of Colorado,Agriculture&Agri-Food Canada,National Oceanic and Atmospheric Administration,and United States Geological Survey.Source analysis showed that the Science of the Total Environment was cited with the highest total link strength.Science of the Total Environment ranked first in source core 1 with 290 citation frequencies,followed by Journal of Dairy Science with 223 citation frequencies.Currently,no bibliometric study has been conducted on MECF,and to fill this knowledge gap,we carried out this study to highlight methane emissions in cattle farms,aiming at a climate change perspective.In this regard,we focused on the research productivity of countries authors,journals and institutions,co-occurrence of keywords,evolution of research trends,and collaborative networking.Based on relevance degree of centrality,methane emissions and greenhouse gases appeared as basic themes,cattle,and dairy cattle appeared as emerging/declining themes,whereas,methane,greenhouse gas and nitrous oxide appeared to fall amongst basic and motor themes.On the other hand,beef cattle,rumen and dairy cow seem to be between motor and niche themes,and risk factors lie in niche themes.The present bibliometric analysis provides research progress on methane emissions in cattle farms.Current findings may provide a framework for understanding research trends and themes in MECF research.展开更多
Yaks are well-adapted to the harsh environment of the Tibetan Plateau,and they emit less enteric methane(CH_(4))and digest poor-quality forage better than cattle.To examine the potential of yak rumen inoculum to mitig...Yaks are well-adapted to the harsh environment of the Tibetan Plateau,and they emit less enteric methane(CH_(4))and digest poor-quality forage better than cattle.To examine the potential of yak rumen inoculum to mitigate CH_(4)production and improve digestibility in cattle,we incubated substrate with rumen inoculum from yak(YRI)and cattle(CRI)in vitro in five ratios(YRI:CRI):(1)0:100(control),(2)25:75,(3)50:50,(4)75:25 and(5)100:0 for 72 h.The YRI:CRI ratios of 50:50,75:25 and 100:0 produced less total gas and CH_(4)and accumulated less hydrogen(H_(2))than0:100(control)at most time points.From 12 h onwards,there was a linear decrease(P<0.05)in carbon dioxide(CO_(2))production with increasing YRI:CRI ratio.At 72 h,the ratios of 50:50 and 75:25 had higher dry matter(+7.71%and+4.11%,respectively),as well as higher acid detergent fiber digestibility(+15.5%and+7.61%,respectively),when compared to the 0:100 ratio(P<0.05).Increasing the proportion of YRI generally increased total VFA concentrations,and,concomitantly,decreased the proportion of metabolic hydrogen([2H])incorporated into CH_(4),and decreased the recovery of[2H].The lower[2H]recovery indicates unknown[2H]sinks in the culture.Estimated Gibbs free energy changes(ΔG)for reductive acetogenesis were negative,indicating the thermodynamic feasibility of this process.It would be beneficial to identify:1)the alternative[2H]sinks,which could help mitigate CH_(4)emission,and 2)core microbes involved in fiber digestion.This experiment supported lower CH_(4)emission and greater nutrient digestibility of yaks compared to cattle.Multi-omics combined with microbial culture technologies developed in recent years could help to better understand fermentation differences among species.展开更多
As a major contributor to methane production in agriculture,there is a need for a suitable methane inhibitor to reduce ruminant methane emissions and minimize the impact on the climate.This work aimed to explore the i...As a major contributor to methane production in agriculture,there is a need for a suitable methane inhibitor to reduce ruminant methane emissions and minimize the impact on the climate.This work aimed to explore the influence of cordycepin on rumen fermentation,gas production,microbiome and their metabolites.A total of 0.00,0.08,0.16,0.32,and 0.64 g L^(–1)cordycepin were added into fermentation bottles containing 2 g total mixed ration for in vitro ruminal fermentation,and then the gas produced and fermentation parameters were measured for each bottle.Samples from the 0 and 0.64 g L^(–1)cordycepin addition were selected for 16S rRNA gene sequencing and metabolome analysis.The result of this experiment indicated that the addition of cordycepin could linearly increase the concentration of total volatile fatty acid,ammonia nitrogen,the proportion of propionate,valerate,and isovalerate,and linearly reduce ruminal pH and methane,carbon dioxide,hydrogen and total gas production,as well as the methane proportion,carbon dioxide proportion and proportion of butyrate.In addition,there was a quadratic relationship between hydrogen and cordycepin addition.At the same time,the relative abundance of Succiniclasticum,Prevotella,Rikenellaceae_RC9_gut_group,NK4A214_group,Christensenellaceae_R_(7)_group,unclassified_F082,Veillonellaceae_UCG_001,Dasytricha,Ophryoscolex,Isotricha,unclassified_Eukaryota,Methanobrevibacter,and Piromyces decreased significantly after adding the maximum dose of cordycepin.In contrast,the relative abundance of Succinivibrio,unclassified_Succinivibrionaceae,Prevotellaceae_UCG_001,unclassified_Lachnospiraceae,Lachnospira,Succinivibrionaceae_UCG_002,Pseudobutyrivibrio,Entodinium,Polyplastron,unclassified_Methanomethylophilaceae,Methanosphaera,and Candidatus_Methanomethylophilus increased significantly.Metabolic pathways such as biosynthesis of unsaturated fatty acids and purine metabolism and metabolites such as arachidonic acid,adenine,and 2′-deoxyguanosine were also affected by the addition of cordycepin.Based on this,we conclude that cordycepin is an effective methane emission inhibitor that can change the rumen metabolites and fermentation parameters by influencing the rumen microbiome,thus regulating rumen methane production.This experiment may provide a potential theoretical reference for developing Cordyceps byproduct or additives containing cordycepin as methane inhibitors.展开更多
Methane(CH4),the predominant component of natural gas and shale gas,is regarded as a promising carbon feedstock for chemical synthesis[1].However,considering the extreme stability of CH4 molecules,it's quite chall...Methane(CH4),the predominant component of natural gas and shale gas,is regarded as a promising carbon feedstock for chemical synthesis[1].However,considering the extreme stability of CH4 molecules,it's quite challenging in simultaneously achieving high activity and selectivity for target products under mild conditions,especially when synthesizing high-value C2t chemicals such as ethanol[2].The conversion of methane to ethanol by photocatalysis is promising for achieving transformation under ambient temperature and pressure conditions.Currently,the apparent quantum efficiency(AQE)of solar-driven methane-to-ethanol conversion is generally below 0.5%[3,4].Furthermore,the stability of photocatalysts remains inadequate,offering substantial potential for further improvement.展开更多
Coal measures are significant hydrocarbon source rocks and reservoirs in petroliferous basins.Many large gas fields and coalbed methane fields globally are originated from coal-measure source rocks or accumulated in c...Coal measures are significant hydrocarbon source rocks and reservoirs in petroliferous basins.Many large gas fields and coalbed methane fields globally are originated from coal-measure source rocks or accumulated in coal rocks.Inspired by the discovery of shale oil and gas,and guided by“the overall exploration concept of considering coal rock as reservoir”,breakthroughs in the exploration and development of coal-rock gas have been achieved in deep coal seams with favorable preservation conditions,thereby opening up a new development frontier for the unconventional gas in coal-rock reservoirs.Based on the data from exploration and development practices,a systematic study on the accumulation mechanism of coal-rock gas has been conducted.The mechanisms of“three fields”controlling coal-rock gas accumulation are revealed.It is confirmed that the coal-rock gas is different from CBM in accumulation process.The whole petroleum systems in the Carboniferous–Permian transitional facies coal measures of the eastern margin of the Ordos Basin and in the Jurassic continental facies coal measures of the Junggar Basin are characterized,and the key research directions for further developing the whole petroleum system theory of coal measures are proposed.Coal rocks,compared to shale,possess intense hydrocarbon generation potential,strong adsorption capacity,dual-medium reservoir properties,and partial or weak oil and gas self-sealing capacity.Additionally,unlike other unconventional gas such as shale gas and tight gas,coal-rock gas exhibits more complex accumulation characteristics,and its accumulation requires a certain coal-rock play form lithological and structural traps.Coal-rock gas also has the characteristics of conventional fractured gas reservoirs.Compared with the basic theory and model of the whole petroleum system established based on detrital rock formations,coal measures have distinct characteristics and differences in coal-rock reservoirs and source-reservoir coupling.The whole petroleum system of coal measures is composed of various types of coal-measure hydrocarbon plays with coal(and dark shale)in coal measures as source rock and reservoir,and with adjacent tight layers as reservoirs or cap or transport layers.Under the action of source-reservoir coupling,coal-rock gas is accumulated in coal-rock reservoirs with good preservation conditions,tight oil/gas is accumulated in tight layers,conventional oil/gas is accumulated in traps far away from sources,and coalbed methane is accumulated in coal-rock reservoirs damaged by later geological processes.The proposed whole petroleum system of coal measures represents a novel type of whole petroleum system.展开更多
The objective of this study is to propose an optimal plant design for blue hydrogen production aboard a liquefiednatural gas(LNG)carrier.This investigation focuses on integrating two distinct processes—steam methaner...The objective of this study is to propose an optimal plant design for blue hydrogen production aboard a liquefiednatural gas(LNG)carrier.This investigation focuses on integrating two distinct processes—steam methanereforming(SMR)and ship-based carbon capture(SBCC).The first refers to the common practice used to obtainhydrogen from methane(often derived from natural gas),where steam reacts with methane to produce hydrogenand carbon dioxide(CO_(2)).The second refers to capturing the CO_(2) generated during the SMR process on boardships.By capturing and storing the carbon emissions,the process significantly reduces its environmental impact,making the hydrogen production“blue,”as opposed to“grey”(which involves CO_(2) emissions without capture).For the SMR process,the analysis reveals that increasing the reformer temperature enhances both the processperformance and CO_(2) emissions.Conversely,a higher steam-to-carbon(s/c)ratio reduces hydrogen yield,therebydecreasing thermal efficiency.The study also shows that preheating the air and boil-off gas(BOG)before theyenter the combustion chamber boosts overall efficiency and curtails CO_(2) emissions.In the SBCC process,puremonoethanolamine(MEA)is employed to capture the CO_(2) generated by the exhaust gases from the SMR process.The results indicate that with a 90%CO_(2) capture rate,the associated heat consumption amounts to 4.6 MJ perkilogram of CO_(2) captured.This combined approach offers a viable pathway to produce blue hydrogen on LNGcarriers while significantly reducing the carbon footprint.展开更多
CeO_(2) based semiconductor are widely used in solar-driven photothermal catalytic dry reforming of methane(DRM)reaction,but still suffer from low activity and low light utilization efficiency.This study developed gra...CeO_(2) based semiconductor are widely used in solar-driven photothermal catalytic dry reforming of methane(DRM)reaction,but still suffer from low activity and low light utilization efficiency.This study developed graphite-CeO_(2) interfaces to enhance solar-driven photothermal catalytic DRM.Compared with carbon nanotubes-modified CeO_(2)(CeO_(2)-CNT),graphite-modified CeO_(2)(CeO_(2)-GRA)constructed graphite-CeO_(2) interfaces with distortion in CeO_(2),leading to the formation abundant oxygen vacancies.These graphite-CeO_(2) interfaces with oxygen vacancies enhanced optical absorption and promoted the generation and separation of photogenerated carriers.The high endothermic capacity of graphite elevated the catalyst surface temperature from 592.1−691.3℃,boosting light-to-thermal conversion.The synergy between photogenerated carriers and localized heat enabled Ni/CeO_(2)-GRA to achieve a CO production rate of 9985.6 mmol/(g·h)(vs 7192.4 mmol/(g·h)for Ni/CeO_(2))and a light-to-fuel efficiency of 21.8%(vs 13.8%for Ni/CeO_(2)).This work provides insights for designing graphite-semiconductor interfaces to advance photothermal catalytic efficiency.展开更多
In order to solve the shortcomings of MoO_(3)/γ-Al_(2)O_(3)catalyst for sulfur-resistant methanation,a segmented plasma fluidized bed reactor was designed,where plasma discharge zone and the fluidization zone were se...In order to solve the shortcomings of MoO_(3)/γ-Al_(2)O_(3)catalyst for sulfur-resistant methanation,a segmented plasma fluidized bed reactor was designed,where plasma discharge zone and the fluidization zone were separated under higher discharge power.At the bed height of 30 mm,the gas velocity of 0.10 m·s^(-1)can provide a better fluidization state.The suitable discharge results can be achieved when the input power is 27 W and the discharge interval is 2.0 mm.With the extension of catalyst plasma treatment time,the conversion of CO decreases,but the selectivity of CH_(4)increases.Combined with N_(2)physical adsorption-desorption,XRD,TEM,Raman,TGA and TPR characterization,it was found that the active components of the catalyst are uniformly dispersed on the γ-Al_(2)O_(3)support.After plasma treatment,tetrahedral Mo species was used as the active center,and the interaction between Mo and the carrier was strengthened.It provides a novel approach for preparing catalyst with dielectric barrier discharge(DBD)fluidized bed reactor.展开更多
Methane(CH_(4))has a higher heat capacity(104.9 kcal/mol)than carbon dioxide(CO_(2)),and this has inspired research aimed at reducing methane levels to retard global warming.Hydroxylation under ambient conditions thro...Methane(CH_(4))has a higher heat capacity(104.9 kcal/mol)than carbon dioxide(CO_(2)),and this has inspired research aimed at reducing methane levels to retard global warming.Hydroxylation under ambient conditions through methanotrophs can provide crucial information for understanding the harsh C-H activation of methane.Soluble methane monooxygenase(sMMO)belongs to the bacterial multi-component monooxygenase superfamily and requires hydroxylase(MMOH),regulatory(MMOB),and reductase(MMOR)components.Recent structural and biophysical studies have demonstrated that these components accelerate and retard methane hydroxylation in MMOH through protein-protein interactions.Complex structures of sMMO,including MMOH-MMOB and MMOH-MMOD,illustrate how these regulatory and inhibitory components orchestrate the di-iron active sites located within the four-helix bundles of MMOH,specifically at the docking surface known as the canyon region.In addition,recent biophysical studies have demonstrated the role of MmoR,aσ54-dependent transcriptional regulator,in regulating sMMO expression.This perspective article introduces remarkable discoveries in recent reports on sMMO components that are crucial for understanding sMMO expression and activities.Our findings provide insight into how sMMO components interact with MMOH to control methane hydroxylation,shedding light on the mechanisms governing sMMO expression and the interactions between activating enzymes and promoters.展开更多
CO_(2)-free H_(2)refers to H_(2)production process without CO_(2)emission,which is a promising clean energy in the future.Catalytic decomposition of methane(CDM)is a competitive technology to produce CO_(2)-free H2 wi...CO_(2)-free H_(2)refers to H_(2)production process without CO_(2)emission,which is a promising clean energy in the future.Catalytic decomposition of methane(CDM)is a competitive technology to produce CO_(2)-free H2 with large-scale.However,CDM reaction is highly endothermic and is kinetically and thermodynamically unfavorable,which typically requires a harsh reaction temperature above 800℃.In this work,solar-driven photothermal catalytic decomposition of methane was firstly introduced to produce CO_(2)-free H_(2)relying solely on solar energy as the driving force.A high H_(2)yield of 204.6 mmol g^(–1)h^(–1)was observed over Ni-CeO2 interface under photothermal conditions,along with above 87%reduction in the apparent activation energy(11.2 vs.87.3 kJ mol^(–1))when comparing with the traditional thermal catalysis.Further studies suggested that Ni/CeO_(2)catalyst enhanced optical absorption in visible-infrared region to ensure the heat energy for methane decomposition.The generated electrons and holes participated in the redox process of photo-driven CDM reaction with enhanced separation ability of hot carriers excited by ultraviolet-visible light,which lowered activation energy and improved the photothermal catalytic activity.This work provides a promising photothermal catalytic strategy to produce CO_(2)-free H^(2)under mild conditions.展开更多
The conversion of the greenhouse gas methane to value-added chemicals such as alcohols is a promising technology to mitigate environmental issue and the energy crisis.Especially,the sustainable photocatalytic,electroc...The conversion of the greenhouse gas methane to value-added chemicals such as alcohols is a promising technology to mitigate environmental issue and the energy crisis.Especially,the sustainable photocatalytic,electrocatalytic and photoelectrocatalytic conversion of methane at ambient conditions is regarded as an alternative technology to replace with thermocatalysis.In this review,we summarize recent advances in photocatalytic,electrocatalytic and photoelectrocatalytic conversion of methane into alcohols.We firstly introduce the general principles of photocatalysis,electrocatalysis and photoelectrocatalysis.Then,we discuss the mechanism for selective activation of C-H bond and following oxygenation over metal,inorganic semiconductor,organic semiconductor,and heterojunction composite systems in the photocatalytic,electrocatalytic and photoelectrocatalytic methane oxidation in detail.Later,we present insights into the construction of effective photocatalyst,electrocatalyst and photoelectrocatalyst for methane conversion into alcohols from the perspective of band structures and active sites.Finally,the challenges and outlook for future designs of photocatalytic,electrocatalytic and photoelectrocatalytic methane oxidation systems are also proposed.展开更多
Methane, an abundant one-carbon(C_(1)) resource, is extensively used in the industrial production of vital fuels and value-added chemicals. However, current industrial methane conversion technologies are energy-and ca...Methane, an abundant one-carbon(C_(1)) resource, is extensively used in the industrial production of vital fuels and value-added chemicals. However, current industrial methane conversion technologies are energy-and carbon-intensive, mainly due to the high activation energy required to break the inert C–H bond, low selectivity, and problematic side reactions, including CO_(2)emissions and coke deposition. Electrochemical conversion of methane(ECM) using intermittent renewable energy offers an attractive solution, due to its modular reactor design and operational flexibility across a broad spectrum of temperatures and pressures. This review emphasizes conversion pathways of methane in various reaction systems, highlighting the significance and advantages of ECM in facilitating a sustainable artificial carbon cycle. This work provides a comprehensive overview of conventional methane activation mechanisms and delineates the complete pathways of methane conversion in electrolysis contexts. Based on surface/interface chemistry, this work systematically analyzes proposed reaction pathways and corresponding strategies to enhance ECM efficiency towards various target products, including syngas, hydrocarbons, oxygenates, and advanced carbon materials. The discussion also encompasses opportunities and challenges for the ECM process, including insights into ECM pathways, rational electrocatalyst design, establishment of benchmarking protocols, electrolyte engineering, enhancement of CH4conversion rates, and minimization of CO_(2)emission.展开更多
The direct oxidation of methane to methanol(DOMM) has been recognized as a significant technology for efficiently utilizing low-concentration coalbed methane(LCMM) and supplying liquid fuel.Herein,the noble metals(Pt,...The direct oxidation of methane to methanol(DOMM) has been recognized as a significant technology for efficiently utilizing low-concentration coalbed methane(LCMM) and supplying liquid fuel.Herein,the noble metals(Pt,Pd and Ru) modified Cu/alkalized sepiolite(CuX/SEPA) catalysts were prepared and used for the DOMM in a gas-phase system at low temperatures.The CuRu/SEPA exhibited the highest methanol production of 53 μmol·g^(-1)·h^(-1) and methanol selectivity of 90% under the optimal reaction conditions.Various characterizations demonstrated that the addition of Ru promoted the formation of Cu^(2+)and the contraction of Cu—Si/Al bonds to reduce the distance between framework Al atoms of SEPA to further generate more Al pairs,which facilitated the formation of reactive dicopper species([Cu_(2)O]^(2+)or [Cu_(2)O_(2)]^(2+)).Investigation of the reaction mechanism revealed that [Cu_(2)O]^(2+) or [Cu_(2)O_(2)]^(2+) species could adsorb and activate methane to form CH_(3)O^(*) species and ultimately generated methanol with the assistance of water.展开更多
Field tests have demonstrated that depressurization with controlled sand production is an effective technique for natural gas hydrate extraction.Variations in depositional environments and processes result in signific...Field tests have demonstrated that depressurization with controlled sand production is an effective technique for natural gas hydrate extraction.Variations in depositional environments and processes result in significant heterogeneity within subsea natural gas hydrate-bearing sediments.However,the influence of permeability heterogeneity on production performance during depressurization with controlled sand production remains inadequately understood.In this study,a multiphase,multi-component mathematical model is developed to simulate depressurization with controlled sand production in methane hydrate-bearing sediments,incorporating geological conditions representative of unconsolidated argillaceous siltstone hydrate deposits in the Shenhu area of the South China Sea.The effects of permeability heterogeneity-specifically,horizontal autocorrelation length and global permeability heterogeneity-on production performance during depressurization with sand production are investigated using geostatistical modeling combined with finite difference method based numerical simulations.Results show that as the horizontal autocorrelation length of permeability distribution increases,cumulative gas production first rises and then declines,reaching its peak at λ_(Dh)=0.1,whereas sand production steadily increases.In addition,higher formation permeability heterogeneity results in increased cumulative gas and sand production,suggesting that greater heterogeneity promotesmethane hydrate decomposition and gas recovery.These findings can offer valuable insights for optimizing future field development of hydrate-bearing sediments by depressurization with controlled sand production.展开更多
This study explores,for the first time,the influence of various C1 gases,such as methane(CH_(4)),carbon dioxide(CO_(2)),and biogas(CH4+CO_(2)),on catalytic pyrolysis of plastic waste(polypropylene)to evaluate their po...This study explores,for the first time,the influence of various C1 gases,such as methane(CH_(4)),carbon dioxide(CO_(2)),and biogas(CH4+CO_(2)),on catalytic pyrolysis of plastic waste(polypropylene)to evaluate their potential in producing aromatic hydrocarbons.Also,this study used the 0.5 wt%,1 wt%,3 wt%,and 5 wt%Ga-modified ZSM-5 catalyst and its reduction-oxidation processed catalysts owing to their promising catalytic properties.According to the results,the highest yield(39.5 wt%)of BTEX(benzene,toluene,xylene,and ethylbenzene)was achieved under CH4 over RO-GHZ(1)catalyst among all tested conditions.The reduction-oxidation process not only promotes a significant reduction of the Ga-size but also induces its diffusion inside the pore,compared to GHZ(1).This leads to the formation of highly active GaO^(+)ionic species,balancing the Lewis/Brönsted ratio,thereby accelerating the aromatization reaction.The effect of Ga loading on the RO-GHZ catalyst was also evaluated systematically,which showed a negative impact on the BTEX yield owing to the lowering in the concentration of active GaO+species.A detailed catalyst characterization supports the experimental results well.展开更多
Chinese coal reservoirs are characterized by low pressure and low permeability,which need to be enhanced so as to increase production.However,conventional methods for permeability enhancement can only increase the per...Chinese coal reservoirs are characterized by low pressure and low permeability,which need to be enhanced so as to increase production.However,conventional methods for permeability enhancement can only increase the permeability in fractures,but not the ultra-low permeability in coal matrices.Attempts to enhance such impermeable structures lead to rapid attenuation of gas production,especially in the late stage of gas extraction.Thermal stimulation by injecting high-temperature steam is a promising method to increase gas production.The critical scientific challenges that still hinder its widespread application are related to the evolution law of permeability of high-temperature steam in coal and the thermal deformation of coal.In this study,an experimental approach is developed to explore the high-temperature steam seepage coupled with the thermal deformation in coal under triaxial stress.The tests were conducted using cylindrical coal specimens of?50 mm×100 mm.The permeability and thermal strain in coal were investigated when high-temperature steam was injected at151.11,183.20,213.65,and 239.76°C.The experimental results reveal for the first time that as the amount of injected fluid increases,the steam permeability shows periodic pulsation changes.This paper introduces and explains the main traits of this discovery that may shed more light on the seepage phenomenon.When the injected steam temperature increases,the amplitude of pulsating permeability decreases,whereas the frequency increases;meanwhile,the period becomes shorter,the pulsation peak appears earlier,and the stabilization time becomes longer.The average peak permeability shows a“U-shaped”trend,decreasing first and then increasing as the steam temperature increases.Meanwhile,with the extension of steam injection time,the axial,radial,and volumetric strains of coal show a stage-wise expansion characteristic at different temperatures of steam injection,except for the radial strains at 151.11°C.A two-phase flow theory of gas–liquid is adopted to elucidate the mechanism of pulsating seepage of steam.Moreover,the influencing mechanism of inward and outward thermal expansion on the permeability of coal is interpreted.The results presented in this paper provide new insight into the feasibility of thermal gas recovery by steam injection.展开更多
Two kinds of oxide-zeolite composite support,Ce-beta and Zr-beta were prepared by a simple wet impregnation method and adopted for the preparation of palladium-based catalysts for catalytic oxidation of methane.The Pd...Two kinds of oxide-zeolite composite support,Ce-beta and Zr-beta were prepared by a simple wet impregnation method and adopted for the preparation of palladium-based catalysts for catalytic oxidation of methane.The Pd/6.8Zr-beta catalyst showed superiormethane oxidation performance,achieving T_(50) and T90 of 417℃ and 451℃,respectively,together with robust hydrothermal stability.Kinetic analysis has shown that incorporating Zr into the catalyst significantly enhanced its efficiency,nearly tripling the turnover frequency(TOF)for methane combustion compared to the Pd/beta catalyst.This enhanced performance was attributed to the dispersion of Zr on the zeolite surface,which not only promoted the formation of active PdO sites but also helped maintain the high Pd^(2+)content via facilitating the oxygen migration during the reaction,thus improving both the catalyst’s activity and stability.In the Pd/8.6Ce-beta catalyst,doped CeO_(2) tended to aggregate in the zeolite’s pores,adversely affecting the catalyst’s efficiency.This aggregation promoted the formation of inactive Pd^(4+) species,a result of the enhanced metal-support interaction.This finding is critical for understanding the implications of dopant selection in the design of high-activity methane oxidation catalysts.展开更多
基金supported by the National Natural Science Foundation of China(52074045,52274074)the Science Fund for Distinguished Young Scholars of Chongqing(CSTB2022NSCQ-JQX0028).
文摘Developing deep fragmented soft coalbed methane(CBM)can significantly enhance domestic natural gas supplies,reduce reliance on imported energy,and bolster national energy security.This manuscript provides a comprehensive review of commonly employed coalbed methane extraction technologies.It then delves into several critical issues in the current stage of CBM exploration and development in China,including the compatibility of existing technologies with CBM reservoirs,the characteristics and occurrence states of CBM reservoirs,critical desorption pressure,and gas generation mechanisms.Our research indicates that current CBM exploration and development technologies in China have reached an internationally advanced level,yet the industry is facing unprecedented challenges.Despite progress in low-permeability,high-value coal seams,significant breakthroughs have not been achieved in exploring other types of coal seams.For different coal reservoirs,integrated extraction technologies have been developed,such as surface pre-depressurisation and segmented hydraulic fracturing of coal seam roof strata.Additionally,techniques like large-scale volume fracturing in horizontal wells have been established,significantly enhancing reservoir stimulation effects and coalbed methane recovery rates.However,all of these technologies are fundamentally based on permeation.These technologies lack direct methods aimed at enhancing the diffusion rate of CBM,thereby failing to fully reflect the unique characteristics of CBM.Current CBM exploration and development theories and technologies are not universally applicable to all coal seams.They do not adequately account for the predominantly adsorbed state of CBM,and the complex and variable gas generation mechanisms further constrain CBM development in China.Finally,continuous exploration of new deep CBM exploration technologies is necessary.Integrating more effective reservoir stimulation technologies is essential to enhance technical adaptability concerning CBM reservoir characteristics,gas occurrence states,and gas generation mechanisms,ultimately achieving efficient CBM development.We conclude that while China possesses a substantial foundation of deep fractured CBM resources,industry development is constrained and requires continuous exploration of new CBM exploration and development technologies to utilize these resources effectively.
基金supported by the Youth Innovation Program of the Chinese Academy of Agricultural Sciences(Y2022QC10)the Agricultural Science and Technology Innovation Program,China(CAAS-ASTIP-2023-IFR-03,CAAS-IFR-ZDRW202302 and CAAS-IFR-ZDRW202404)the Basal Research Fund of the Institute of Feed Research of Chinese Academy of Agricultural Sciences(1610382024009)。
文摘Cutting farming-related methane emissions from ruminants is critical in the battle against climate change.Since scientists initially investigated the potential of marine macroalgae to reduce methane emissions,using seaweeds as an anti-methanogenic feed additive has become prevailing in recent years.Asparagopsis taxiformis is the preferred species because it contains a relatively higher concentration of bromoform.As a type of halogenated methane analogue,bromoform contained in A.taxiformis can specifically inhibit the activity of coenzyme M methyltransferase,thereby blocking the ruminal methanogenesis.However,bromoform is a potential toxin and ozone-depleting substance.In response,current research focuses on the effects of bromoform-enriched seaweed supplementation on ruminant productivity and safety,as well as the impact of large-scale cultivation of seaweeds on the atmospheric environment.The current research on seaweed still needs to be improved,especially in developing more species with low bromoform content,such as Bonnemaisonia hamifera,Dictyota bartayresii,and Cystoseira trinodis.Otherwise,seaweed is rich in bioactive substances and exhibits antibacterial,anti-inflammatory,and other physiological properties,but research on the role of these bioactive compounds in methane emissions is lacking.It is worthy of deeper investigation to identify more potential bioactive compounds.As a new focus of attention,seaweed has attracted the interest of many scientists.Nevertheless,seaweed still faces some challenges as a feed additive to ruminants,such as the residues of heavy metals(iodine and bromine)and bromoform in milk or meat,as well as the establishment of a supply chain for seaweed cultivation,preservation,and processing.We have concluded that the methane-reducing efficacy of seaweed is indisputable.However,its application as a commercial feed additive is still influenced by factors such as safety,costs,policy incentives,and regulations.
基金supported by the Key Research Program of the Institute of Geology&Geophysics,CAS(Grant No.IGGCAS-201903).
文摘Natural gas hydrates widely accumulate in submarine sediments composed of clay minerals.However,due to the complex physiochemistry and micron-sized particles of clay minerals,their effects on methane hydrate(MH)formation and dissociation are still in controversy.In this study,montmorillonite and illite were separately mixed with quartz sand to investigate their effects on MH formation and dissociation.The microstructure of synthesized samples was observed by cryo-SEM innovatively to understand the effects of montmorillonite and illite on MH phase transition in micron scale.Results show that montmorillonite and illite both show the inhibition on MH formation kinetics and water-to-hydrate conversion,and illite shows a stronger inhibition.The 10 wt%montmorillonite addition significantly retards MH formation rate,and the 20 wt%montmorillonite has a less inhibition on the rate.The increase of illite mass ratio(0-20 wt%)retards the rate of MH formation.As the content of clay minerals increase,the water-to-hydrate conversion decreases.Cryo-SEM images presented that montmorillonite aggregates separate as individual clusters while illite particles pack as face-to-face configuration under the interaction with water.The surface-overlapped illite aggregates would make sediments pack tightly,hinder the contact between gas and water,and result in the more significant inhibition on MH formation kinetics.Under the depressurization method,the addition of clay minerals facilitates MH dissociation rate.Physicochemical properties of clay minerals and MH distribution in the pore space lead to the faster dissociation rate in clay-containing sediments.The results of this study would provide beneficial guides on geological investigations and optimizing strategies of natural gas production in marine hydrate-bearing sediments.
基金supported by the Special Fund for Science and Technology Innovation Strategy of Guangdong Province,China(2022660500250009604)。
文摘Methane contributes to global warming,and livestock is one of the sources of methane production.However,methane emission studies using bibliometric tools in livestock are lacking.Given the negative impact of climate change on the ecosystem and the rise in methane emissions,it is essential to conduct a bibliometrics study to provide an overview and research trends.We used the Bibliometrix package and VOSviewer to decipher bibliometric indices for methane emissions in cattle farms(MECF).Current dataset were collected from the Web of Science(Core Collection)database,and 8,998 publications were analyzed.The most co-occurring keywords scientists preferred were methane(1,528),greenhouse gas(443),methane emissions(440),and cattle(369).Methane was the most frequently used keyword in the published scientific literature.Thematic evolution of research themes and trend results highlighted carbon dioxide,methane,dairy cattle,cattle,and risk factors during 1999–2017.Chinese Academy of Sciences ranked on top with 485 publications,followed by Agriculture&Agri-Food Canada,University of Colorado,National Oceanic and Atmospheric Administration,and Aarhus University.Chinese Academy of Sciences was also the most cited organization,followed by the University of Colorado,Agriculture&Agri-Food Canada,National Oceanic and Atmospheric Administration,and United States Geological Survey.Source analysis showed that the Science of the Total Environment was cited with the highest total link strength.Science of the Total Environment ranked first in source core 1 with 290 citation frequencies,followed by Journal of Dairy Science with 223 citation frequencies.Currently,no bibliometric study has been conducted on MECF,and to fill this knowledge gap,we carried out this study to highlight methane emissions in cattle farms,aiming at a climate change perspective.In this regard,we focused on the research productivity of countries authors,journals and institutions,co-occurrence of keywords,evolution of research trends,and collaborative networking.Based on relevance degree of centrality,methane emissions and greenhouse gases appeared as basic themes,cattle,and dairy cattle appeared as emerging/declining themes,whereas,methane,greenhouse gas and nitrous oxide appeared to fall amongst basic and motor themes.On the other hand,beef cattle,rumen and dairy cow seem to be between motor and niche themes,and risk factors lie in niche themes.The present bibliometric analysis provides research progress on methane emissions in cattle farms.Current findings may provide a framework for understanding research trends and themes in MECF research.
基金supported by the National Natural Science Foundation of China(32072757 and U21A20250)。
文摘Yaks are well-adapted to the harsh environment of the Tibetan Plateau,and they emit less enteric methane(CH_(4))and digest poor-quality forage better than cattle.To examine the potential of yak rumen inoculum to mitigate CH_(4)production and improve digestibility in cattle,we incubated substrate with rumen inoculum from yak(YRI)and cattle(CRI)in vitro in five ratios(YRI:CRI):(1)0:100(control),(2)25:75,(3)50:50,(4)75:25 and(5)100:0 for 72 h.The YRI:CRI ratios of 50:50,75:25 and 100:0 produced less total gas and CH_(4)and accumulated less hydrogen(H_(2))than0:100(control)at most time points.From 12 h onwards,there was a linear decrease(P<0.05)in carbon dioxide(CO_(2))production with increasing YRI:CRI ratio.At 72 h,the ratios of 50:50 and 75:25 had higher dry matter(+7.71%and+4.11%,respectively),as well as higher acid detergent fiber digestibility(+15.5%and+7.61%,respectively),when compared to the 0:100 ratio(P<0.05).Increasing the proportion of YRI generally increased total VFA concentrations,and,concomitantly,decreased the proportion of metabolic hydrogen([2H])incorporated into CH_(4),and decreased the recovery of[2H].The lower[2H]recovery indicates unknown[2H]sinks in the culture.Estimated Gibbs free energy changes(ΔG)for reductive acetogenesis were negative,indicating the thermodynamic feasibility of this process.It would be beneficial to identify:1)the alternative[2H]sinks,which could help mitigate CH_(4)emission,and 2)core microbes involved in fiber digestion.This experiment supported lower CH_(4)emission and greater nutrient digestibility of yaks compared to cattle.Multi-omics combined with microbial culture technologies developed in recent years could help to better understand fermentation differences among species.
基金financially supported by the National Key Research and Development Program of China(2023YFD2000701)the Natural Science Foundation of Heilongjiang Province,China(YQ2023C011)+1 种基金the Key Research and Development Program of Heilongjiang Province,China(Grant no.2022ZX01A24)the Key Laboratory of Low-carbon Green Agriculture in Northeastern China,Ministry of Agriculture and Rural Affairs of China(LCGANE14)。
文摘As a major contributor to methane production in agriculture,there is a need for a suitable methane inhibitor to reduce ruminant methane emissions and minimize the impact on the climate.This work aimed to explore the influence of cordycepin on rumen fermentation,gas production,microbiome and their metabolites.A total of 0.00,0.08,0.16,0.32,and 0.64 g L^(–1)cordycepin were added into fermentation bottles containing 2 g total mixed ration for in vitro ruminal fermentation,and then the gas produced and fermentation parameters were measured for each bottle.Samples from the 0 and 0.64 g L^(–1)cordycepin addition were selected for 16S rRNA gene sequencing and metabolome analysis.The result of this experiment indicated that the addition of cordycepin could linearly increase the concentration of total volatile fatty acid,ammonia nitrogen,the proportion of propionate,valerate,and isovalerate,and linearly reduce ruminal pH and methane,carbon dioxide,hydrogen and total gas production,as well as the methane proportion,carbon dioxide proportion and proportion of butyrate.In addition,there was a quadratic relationship between hydrogen and cordycepin addition.At the same time,the relative abundance of Succiniclasticum,Prevotella,Rikenellaceae_RC9_gut_group,NK4A214_group,Christensenellaceae_R_(7)_group,unclassified_F082,Veillonellaceae_UCG_001,Dasytricha,Ophryoscolex,Isotricha,unclassified_Eukaryota,Methanobrevibacter,and Piromyces decreased significantly after adding the maximum dose of cordycepin.In contrast,the relative abundance of Succinivibrio,unclassified_Succinivibrionaceae,Prevotellaceae_UCG_001,unclassified_Lachnospiraceae,Lachnospira,Succinivibrionaceae_UCG_002,Pseudobutyrivibrio,Entodinium,Polyplastron,unclassified_Methanomethylophilaceae,Methanosphaera,and Candidatus_Methanomethylophilus increased significantly.Metabolic pathways such as biosynthesis of unsaturated fatty acids and purine metabolism and metabolites such as arachidonic acid,adenine,and 2′-deoxyguanosine were also affected by the addition of cordycepin.Based on this,we conclude that cordycepin is an effective methane emission inhibitor that can change the rumen metabolites and fermentation parameters by influencing the rumen microbiome,thus regulating rumen methane production.This experiment may provide a potential theoretical reference for developing Cordyceps byproduct or additives containing cordycepin as methane inhibitors.
基金the support from the National Natural Science Foundation of China(52202306)Program from Guangdong Introducing Innovative and Entrepreneurial Teams(2019ZT08L101 and RCTDPT-2020-001)+1 种基金Shenzhen Key Laboratory of Eco-materials and Renewable Energy(ZDSYS20200922160400001)the Provincial Talent Plan of Guangdong(2023TB0012).
文摘Methane(CH4),the predominant component of natural gas and shale gas,is regarded as a promising carbon feedstock for chemical synthesis[1].However,considering the extreme stability of CH4 molecules,it's quite challenging in simultaneously achieving high activity and selectivity for target products under mild conditions,especially when synthesizing high-value C2t chemicals such as ethanol[2].The conversion of methane to ethanol by photocatalysis is promising for achieving transformation under ambient temperature and pressure conditions.Currently,the apparent quantum efficiency(AQE)of solar-driven methane-to-ethanol conversion is generally below 0.5%[3,4].Furthermore,the stability of photocatalysts remains inadequate,offering substantial potential for further improvement.
基金Supported by the PetroChina Basic Project(2024DJ23)CNPC Science Research and Technology Development Project(2021DJ0101)。
文摘Coal measures are significant hydrocarbon source rocks and reservoirs in petroliferous basins.Many large gas fields and coalbed methane fields globally are originated from coal-measure source rocks or accumulated in coal rocks.Inspired by the discovery of shale oil and gas,and guided by“the overall exploration concept of considering coal rock as reservoir”,breakthroughs in the exploration and development of coal-rock gas have been achieved in deep coal seams with favorable preservation conditions,thereby opening up a new development frontier for the unconventional gas in coal-rock reservoirs.Based on the data from exploration and development practices,a systematic study on the accumulation mechanism of coal-rock gas has been conducted.The mechanisms of“three fields”controlling coal-rock gas accumulation are revealed.It is confirmed that the coal-rock gas is different from CBM in accumulation process.The whole petroleum systems in the Carboniferous–Permian transitional facies coal measures of the eastern margin of the Ordos Basin and in the Jurassic continental facies coal measures of the Junggar Basin are characterized,and the key research directions for further developing the whole petroleum system theory of coal measures are proposed.Coal rocks,compared to shale,possess intense hydrocarbon generation potential,strong adsorption capacity,dual-medium reservoir properties,and partial or weak oil and gas self-sealing capacity.Additionally,unlike other unconventional gas such as shale gas and tight gas,coal-rock gas exhibits more complex accumulation characteristics,and its accumulation requires a certain coal-rock play form lithological and structural traps.Coal-rock gas also has the characteristics of conventional fractured gas reservoirs.Compared with the basic theory and model of the whole petroleum system established based on detrital rock formations,coal measures have distinct characteristics and differences in coal-rock reservoirs and source-reservoir coupling.The whole petroleum system of coal measures is composed of various types of coal-measure hydrocarbon plays with coal(and dark shale)in coal measures as source rock and reservoir,and with adjacent tight layers as reservoirs or cap or transport layers.Under the action of source-reservoir coupling,coal-rock gas is accumulated in coal-rock reservoirs with good preservation conditions,tight oil/gas is accumulated in tight layers,conventional oil/gas is accumulated in traps far away from sources,and coalbed methane is accumulated in coal-rock reservoirs damaged by later geological processes.The proposed whole petroleum system of coal measures represents a novel type of whole petroleum system.
文摘The objective of this study is to propose an optimal plant design for blue hydrogen production aboard a liquefiednatural gas(LNG)carrier.This investigation focuses on integrating two distinct processes—steam methanereforming(SMR)and ship-based carbon capture(SBCC).The first refers to the common practice used to obtainhydrogen from methane(often derived from natural gas),where steam reacts with methane to produce hydrogenand carbon dioxide(CO_(2)).The second refers to capturing the CO_(2) generated during the SMR process on boardships.By capturing and storing the carbon emissions,the process significantly reduces its environmental impact,making the hydrogen production“blue,”as opposed to“grey”(which involves CO_(2) emissions without capture).For the SMR process,the analysis reveals that increasing the reformer temperature enhances both the processperformance and CO_(2) emissions.Conversely,a higher steam-to-carbon(s/c)ratio reduces hydrogen yield,therebydecreasing thermal efficiency.The study also shows that preheating the air and boil-off gas(BOG)before theyenter the combustion chamber boosts overall efficiency and curtails CO_(2) emissions.In the SBCC process,puremonoethanolamine(MEA)is employed to capture the CO_(2) generated by the exhaust gases from the SMR process.The results indicate that with a 90%CO_(2) capture rate,the associated heat consumption amounts to 4.6 MJ perkilogram of CO_(2) captured.This combined approach offers a viable pathway to produce blue hydrogen on LNGcarriers while significantly reducing the carbon footprint.
文摘CeO_(2) based semiconductor are widely used in solar-driven photothermal catalytic dry reforming of methane(DRM)reaction,but still suffer from low activity and low light utilization efficiency.This study developed graphite-CeO_(2) interfaces to enhance solar-driven photothermal catalytic DRM.Compared with carbon nanotubes-modified CeO_(2)(CeO_(2)-CNT),graphite-modified CeO_(2)(CeO_(2)-GRA)constructed graphite-CeO_(2) interfaces with distortion in CeO_(2),leading to the formation abundant oxygen vacancies.These graphite-CeO_(2) interfaces with oxygen vacancies enhanced optical absorption and promoted the generation and separation of photogenerated carriers.The high endothermic capacity of graphite elevated the catalyst surface temperature from 592.1−691.3℃,boosting light-to-thermal conversion.The synergy between photogenerated carriers and localized heat enabled Ni/CeO_(2)-GRA to achieve a CO production rate of 9985.6 mmol/(g·h)(vs 7192.4 mmol/(g·h)for Ni/CeO_(2))and a light-to-fuel efficiency of 21.8%(vs 13.8%for Ni/CeO_(2)).This work provides insights for designing graphite-semiconductor interfaces to advance photothermal catalytic efficiency.
基金supported by the National Natural Science Foundation of China(22178255).
文摘In order to solve the shortcomings of MoO_(3)/γ-Al_(2)O_(3)catalyst for sulfur-resistant methanation,a segmented plasma fluidized bed reactor was designed,where plasma discharge zone and the fluidization zone were separated under higher discharge power.At the bed height of 30 mm,the gas velocity of 0.10 m·s^(-1)can provide a better fluidization state.The suitable discharge results can be achieved when the input power is 27 W and the discharge interval is 2.0 mm.With the extension of catalyst plasma treatment time,the conversion of CO decreases,but the selectivity of CH_(4)increases.Combined with N_(2)physical adsorption-desorption,XRD,TEM,Raman,TGA and TPR characterization,it was found that the active components of the catalyst are uniformly dispersed on the γ-Al_(2)O_(3)support.After plasma treatment,tetrahedral Mo species was used as the active center,and the interaction between Mo and the carrier was strengthened.It provides a novel approach for preparing catalyst with dielectric barrier discharge(DBD)fluidized bed reactor.
基金This research was supported by"Regional Innovation Strategy"(2023RIS-008)and"C1 Gas Refinery Program"(NRF-2015M3D3D3A1A01064876)through the National Research Foundation of Koreafunded by the Ministry of Education(NRF-2017R1A6A1A03015876).
文摘Methane(CH_(4))has a higher heat capacity(104.9 kcal/mol)than carbon dioxide(CO_(2)),and this has inspired research aimed at reducing methane levels to retard global warming.Hydroxylation under ambient conditions through methanotrophs can provide crucial information for understanding the harsh C-H activation of methane.Soluble methane monooxygenase(sMMO)belongs to the bacterial multi-component monooxygenase superfamily and requires hydroxylase(MMOH),regulatory(MMOB),and reductase(MMOR)components.Recent structural and biophysical studies have demonstrated that these components accelerate and retard methane hydroxylation in MMOH through protein-protein interactions.Complex structures of sMMO,including MMOH-MMOB and MMOH-MMOD,illustrate how these regulatory and inhibitory components orchestrate the di-iron active sites located within the four-helix bundles of MMOH,specifically at the docking surface known as the canyon region.In addition,recent biophysical studies have demonstrated the role of MmoR,aσ54-dependent transcriptional regulator,in regulating sMMO expression.This perspective article introduces remarkable discoveries in recent reports on sMMO components that are crucial for understanding sMMO expression and activities.Our findings provide insight into how sMMO components interact with MMOH to control methane hydroxylation,shedding light on the mechanisms governing sMMO expression and the interactions between activating enzymes and promoters.
文摘CO_(2)-free H_(2)refers to H_(2)production process without CO_(2)emission,which is a promising clean energy in the future.Catalytic decomposition of methane(CDM)is a competitive technology to produce CO_(2)-free H2 with large-scale.However,CDM reaction is highly endothermic and is kinetically and thermodynamically unfavorable,which typically requires a harsh reaction temperature above 800℃.In this work,solar-driven photothermal catalytic decomposition of methane was firstly introduced to produce CO_(2)-free H_(2)relying solely on solar energy as the driving force.A high H_(2)yield of 204.6 mmol g^(–1)h^(–1)was observed over Ni-CeO2 interface under photothermal conditions,along with above 87%reduction in the apparent activation energy(11.2 vs.87.3 kJ mol^(–1))when comparing with the traditional thermal catalysis.Further studies suggested that Ni/CeO_(2)catalyst enhanced optical absorption in visible-infrared region to ensure the heat energy for methane decomposition.The generated electrons and holes participated in the redox process of photo-driven CDM reaction with enhanced separation ability of hot carriers excited by ultraviolet-visible light,which lowered activation energy and improved the photothermal catalytic activity.This work provides a promising photothermal catalytic strategy to produce CO_(2)-free H^(2)under mild conditions.
文摘The conversion of the greenhouse gas methane to value-added chemicals such as alcohols is a promising technology to mitigate environmental issue and the energy crisis.Especially,the sustainable photocatalytic,electrocatalytic and photoelectrocatalytic conversion of methane at ambient conditions is regarded as an alternative technology to replace with thermocatalysis.In this review,we summarize recent advances in photocatalytic,electrocatalytic and photoelectrocatalytic conversion of methane into alcohols.We firstly introduce the general principles of photocatalysis,electrocatalysis and photoelectrocatalysis.Then,we discuss the mechanism for selective activation of C-H bond and following oxygenation over metal,inorganic semiconductor,organic semiconductor,and heterojunction composite systems in the photocatalytic,electrocatalytic and photoelectrocatalytic methane oxidation in detail.Later,we present insights into the construction of effective photocatalyst,electrocatalyst and photoelectrocatalyst for methane conversion into alcohols from the perspective of band structures and active sites.Finally,the challenges and outlook for future designs of photocatalytic,electrocatalytic and photoelectrocatalytic methane oxidation systems are also proposed.
基金National Key R&D Program of China (2023YFA1508001 and 2023YFA1508002)National Natural Science Foundation of China (22272120 and U2202251)+1 种基金Hainan Province Science and Technology Special Fund(ZDYF2023SHFZ120)Research Foundation of Marine Science and Technology Collaborative Innovation Center of Hainan University (XTCX2022HYB01)。
文摘Methane, an abundant one-carbon(C_(1)) resource, is extensively used in the industrial production of vital fuels and value-added chemicals. However, current industrial methane conversion technologies are energy-and carbon-intensive, mainly due to the high activation energy required to break the inert C–H bond, low selectivity, and problematic side reactions, including CO_(2)emissions and coke deposition. Electrochemical conversion of methane(ECM) using intermittent renewable energy offers an attractive solution, due to its modular reactor design and operational flexibility across a broad spectrum of temperatures and pressures. This review emphasizes conversion pathways of methane in various reaction systems, highlighting the significance and advantages of ECM in facilitating a sustainable artificial carbon cycle. This work provides a comprehensive overview of conventional methane activation mechanisms and delineates the complete pathways of methane conversion in electrolysis contexts. Based on surface/interface chemistry, this work systematically analyzes proposed reaction pathways and corresponding strategies to enhance ECM efficiency towards various target products, including syngas, hydrocarbons, oxygenates, and advanced carbon materials. The discussion also encompasses opportunities and challenges for the ECM process, including insights into ECM pathways, rational electrocatalyst design, establishment of benchmarking protocols, electrolyte engineering, enhancement of CH4conversion rates, and minimization of CO_(2)emission.
基金financial assistance from the Anhui Provincial Major Science and Technology Project(202003a05020022)the Institute of Energy,Hefei Comprehensive National Science Center(21KZS219)。
文摘The direct oxidation of methane to methanol(DOMM) has been recognized as a significant technology for efficiently utilizing low-concentration coalbed methane(LCMM) and supplying liquid fuel.Herein,the noble metals(Pt,Pd and Ru) modified Cu/alkalized sepiolite(CuX/SEPA) catalysts were prepared and used for the DOMM in a gas-phase system at low temperatures.The CuRu/SEPA exhibited the highest methanol production of 53 μmol·g^(-1)·h^(-1) and methanol selectivity of 90% under the optimal reaction conditions.Various characterizations demonstrated that the addition of Ru promoted the formation of Cu^(2+)and the contraction of Cu—Si/Al bonds to reduce the distance between framework Al atoms of SEPA to further generate more Al pairs,which facilitated the formation of reactive dicopper species([Cu_(2)O]^(2+)or [Cu_(2)O_(2)]^(2+)).Investigation of the reaction mechanism revealed that [Cu_(2)O]^(2+) or [Cu_(2)O_(2)]^(2+) species could adsorb and activate methane to form CH_(3)O^(*) species and ultimately generated methanol with the assistance of water.
基金funded by the National Key Research and Development Program of China(grant number 2023YFC3009204)the National Natural Science Foundation of China(grant number 52174015).
文摘Field tests have demonstrated that depressurization with controlled sand production is an effective technique for natural gas hydrate extraction.Variations in depositional environments and processes result in significant heterogeneity within subsea natural gas hydrate-bearing sediments.However,the influence of permeability heterogeneity on production performance during depressurization with controlled sand production remains inadequately understood.In this study,a multiphase,multi-component mathematical model is developed to simulate depressurization with controlled sand production in methane hydrate-bearing sediments,incorporating geological conditions representative of unconsolidated argillaceous siltstone hydrate deposits in the Shenhu area of the South China Sea.The effects of permeability heterogeneity-specifically,horizontal autocorrelation length and global permeability heterogeneity-on production performance during depressurization with sand production are investigated using geostatistical modeling combined with finite difference method based numerical simulations.Results show that as the horizontal autocorrelation length of permeability distribution increases,cumulative gas production first rises and then declines,reaching its peak at λ_(Dh)=0.1,whereas sand production steadily increases.In addition,higher formation permeability heterogeneity results in increased cumulative gas and sand production,suggesting that greater heterogeneity promotesmethane hydrate decomposition and gas recovery.These findings can offer valuable insights for optimizing future field development of hydrate-bearing sediments by depressurization with controlled sand production.
文摘This study explores,for the first time,the influence of various C1 gases,such as methane(CH_(4)),carbon dioxide(CO_(2)),and biogas(CH4+CO_(2)),on catalytic pyrolysis of plastic waste(polypropylene)to evaluate their potential in producing aromatic hydrocarbons.Also,this study used the 0.5 wt%,1 wt%,3 wt%,and 5 wt%Ga-modified ZSM-5 catalyst and its reduction-oxidation processed catalysts owing to their promising catalytic properties.According to the results,the highest yield(39.5 wt%)of BTEX(benzene,toluene,xylene,and ethylbenzene)was achieved under CH4 over RO-GHZ(1)catalyst among all tested conditions.The reduction-oxidation process not only promotes a significant reduction of the Ga-size but also induces its diffusion inside the pore,compared to GHZ(1).This leads to the formation of highly active GaO^(+)ionic species,balancing the Lewis/Brönsted ratio,thereby accelerating the aromatization reaction.The effect of Ga loading on the RO-GHZ catalyst was also evaluated systematically,which showed a negative impact on the BTEX yield owing to the lowering in the concentration of active GaO+species.A detailed catalyst characterization supports the experimental results well.
基金Fundamental Research Funds for the Universities of Henan Province,Grant/Award Number:NSFRF180305。
文摘Chinese coal reservoirs are characterized by low pressure and low permeability,which need to be enhanced so as to increase production.However,conventional methods for permeability enhancement can only increase the permeability in fractures,but not the ultra-low permeability in coal matrices.Attempts to enhance such impermeable structures lead to rapid attenuation of gas production,especially in the late stage of gas extraction.Thermal stimulation by injecting high-temperature steam is a promising method to increase gas production.The critical scientific challenges that still hinder its widespread application are related to the evolution law of permeability of high-temperature steam in coal and the thermal deformation of coal.In this study,an experimental approach is developed to explore the high-temperature steam seepage coupled with the thermal deformation in coal under triaxial stress.The tests were conducted using cylindrical coal specimens of?50 mm×100 mm.The permeability and thermal strain in coal were investigated when high-temperature steam was injected at151.11,183.20,213.65,and 239.76°C.The experimental results reveal for the first time that as the amount of injected fluid increases,the steam permeability shows periodic pulsation changes.This paper introduces and explains the main traits of this discovery that may shed more light on the seepage phenomenon.When the injected steam temperature increases,the amplitude of pulsating permeability decreases,whereas the frequency increases;meanwhile,the period becomes shorter,the pulsation peak appears earlier,and the stabilization time becomes longer.The average peak permeability shows a“U-shaped”trend,decreasing first and then increasing as the steam temperature increases.Meanwhile,with the extension of steam injection time,the axial,radial,and volumetric strains of coal show a stage-wise expansion characteristic at different temperatures of steam injection,except for the radial strains at 151.11°C.A two-phase flow theory of gas–liquid is adopted to elucidate the mechanism of pulsating seepage of steam.Moreover,the influencing mechanism of inward and outward thermal expansion on the permeability of coal is interpreted.The results presented in this paper provide new insight into the feasibility of thermal gas recovery by steam injection.
基金supported by the National Natural Science Foundation of China(Nos.U20B6004 and 22072179)。
文摘Two kinds of oxide-zeolite composite support,Ce-beta and Zr-beta were prepared by a simple wet impregnation method and adopted for the preparation of palladium-based catalysts for catalytic oxidation of methane.The Pd/6.8Zr-beta catalyst showed superiormethane oxidation performance,achieving T_(50) and T90 of 417℃ and 451℃,respectively,together with robust hydrothermal stability.Kinetic analysis has shown that incorporating Zr into the catalyst significantly enhanced its efficiency,nearly tripling the turnover frequency(TOF)for methane combustion compared to the Pd/beta catalyst.This enhanced performance was attributed to the dispersion of Zr on the zeolite surface,which not only promoted the formation of active PdO sites but also helped maintain the high Pd^(2+)content via facilitating the oxygen migration during the reaction,thus improving both the catalyst’s activity and stability.In the Pd/8.6Ce-beta catalyst,doped CeO_(2) tended to aggregate in the zeolite’s pores,adversely affecting the catalyst’s efficiency.This aggregation promoted the formation of inactive Pd^(4+) species,a result of the enhanced metal-support interaction.This finding is critical for understanding the implications of dopant selection in the design of high-activity methane oxidation catalysts.
