The challenges posed by energy and environmental issues have forced mankind to explore and utilize unconventional energy sources.It is imperative to convert the abundant coalbed gas(CBG)into high value-added products,...The challenges posed by energy and environmental issues have forced mankind to explore and utilize unconventional energy sources.It is imperative to convert the abundant coalbed gas(CBG)into high value-added products,i.e.,selective and efficient conversion of methane from CBG.Methane activation,known as the“holy grail”,poses a challenge to the design and development of catalysts.The structural complexity of the active metal on the carrier is of particular concern.In this work,we have studied the nucleation growth of small Co clusters(up to Co_(6))on the surface of CeO_(2)(110)using density functional theory,from which a stable loaded Co/CeO_(2)(110)structure was selected to investigate the methane activation mechanism.Despite the relatively small size of the selected Co clusters,the obtained Co_(x)/CeO_(2)(110)exhibits interesting properties.The optimized Co_(5)/CeO_(2)(110)structure was selected as the optimal structure to study the activation mechanism of methane due to its competitive electronic structure,adsorption energy and binding energy.The energy barriers for the stepwise dissociation of methane to form CH3^(*),CH2^(*),CH^(*),and C^(*)radical fragments are 0.44,0.55,0.31,and 1.20 eV,respectively,indicating that CH^(*)dissociative dehydrogenation is the rate-determining step for the system under investigation here.This fundamental study of metal-support interactions based on Co growth on the CeO_(2)(110)surface contributes to the understanding of the essence of Co/CeO_(2) catalysts with promising catalytic behavior.It provides theoretical guidance for better designing the optimal Co/CeO_(2) catalyst for tailored catalytic reactions.展开更多
Co-combustion of methane(CH4)and acid gas(AG)is required to sustain the temperature in Claus reaction furnace.In this study,oxy-fuel combustion of methane and acid gas has been experimentally studied in a diffusion fl...Co-combustion of methane(CH4)and acid gas(AG)is required to sustain the temperature in Claus reaction furnace.In this study,oxy-fuel combustion of methane and acid gas has been experimentally studied in a diffusion flame.Three equivalence ratios(ER=1.0,1.5,2.0)and CH_(4)-addition ratios(CH_(4)/AG=0.3,0.5,0.7)were examined and the flame was interpreted by analyzing the distributions of the temperature and species concentration along central axial.CH_(4)-AG diffusion flame could be classified into three sections namely initial reaction,oxidation and complex reaction sections.Competitive oxidation of CH_(4)and H_(2)S was noted in the first section wherein H_(2)S was preferred and both were mainly proceeding decomposition and partial oxidation.SO_(2)was formed at oxidation section together with obvious presence of H2 and CO.However,H2 and CO were inclined to be sustained under fuel rich condition in the complex reaction section.Reducing ER and increasing CH4/AG contributed to higher temperature,H_(2)S and CH_(4)oxidation and CO_(2)reactivity.Hence a growing trend for CH_(4)and AG to convert into H_(2),CO and SO_(2)could be witnessed.And this factor enhanced the generation of CS2 and COS in the flame inner core by interactions of CH4 and CO_(2)with sulfur species.COS was formed through the interactions of CO and CO_(2)with sulfur species.The CS_(2)production directly relied on reaction of CH_(4)with sulfur species.The concentration of COS was greater than CS_(2)since CS_(2)was probably inhibited due to the presence of H_(2).COS and CS_(2)could be consumed by further oxidation or other complex reactions.展开更多
Anthropogenic methane emissions are a leading cause of the increase in global averagetemperatures,often referred to as global warming.Flooded soils play a significant role in methaneproduction,where the anaerobic cond...Anthropogenic methane emissions are a leading cause of the increase in global averagetemperatures,often referred to as global warming.Flooded soils play a significant role in methaneproduction,where the anaerobic conditions promote the production of methane by methanogenicmicroorganisms.Rice fields contribute a considerable portion of agricultural methane emissions,as riceplants provide both factors that enhance and limit methane production.Rice plants harbor both methaneproducingand methane-oxidizing microorganisms.Exudates from rice roots provide source for methaneproduction,while oxygen delivered from the root aerenchyma enhances methane oxidation.Studies haveshown that the diversity of these microorganisms depends on rice cultivars with some genes characterizedas harboring specific groups of microorganisms related to methane emissions.However,there is still aneed for research to determine the balance between methane production and oxidation,as rice plantspossess the ability to regulate net methane production.Various agronomical practices,such as fertilizerand water management,have been employed to mitigate methane emissions.Nevertheless,studiescorrelating agronomic and chemical management of methane with productivity are limited.Moreover,evidences for breeding low-methane-emitting rice varieties are scattered largely due to the absence ofcoordinated breeding programs.Research has indicated that phenotypic characteristics,such as rootbiomass,shoot architecture,and aerenchyma,are highly correlated with methane emissions.This reviewdiscusses available studies that involve the correlation between plant characteristics and methaneemissions.It emphasizes the necessity and importance of breeding low-methane-emitting rice varieties inaddition to existing agronomic,biological,and chemical practices.The review also delves into the idealphenotypic and physiological characteristics of low-methane-emitting rice and potential breeding techniques,drawing from studies conducted with diverse varieties,mutants,and transgenic plants.展开更多
The printed circuit heat exchanger(PCHE) is receiving wide attention as a new kind of compact heat exchanger and is considered as a promising vaporizer in the LNG process. In this paper, a PCHE straight channel in the...The printed circuit heat exchanger(PCHE) is receiving wide attention as a new kind of compact heat exchanger and is considered as a promising vaporizer in the LNG process. In this paper, a PCHE straight channel in the length of 500 mm is established, with a semicircular cross section in a diameter of 1.2 mm.Numerical simulation is employed to investigate the flow and heat transfer performance of supercritical methane in the channel. The pseudo-boiling theory is adopted and the liquid-like, two-phase-like, and vapor-like regimes are divided for supercritical methane to analyze the heat transfer and flow features.The results are presented in micro segment to show the local convective heat transfer coefficient and pressure drop. It shows that the convective heat transfer coefficient in segments along the channel has a significant peak feature near the pseudo-critical point and a heat transfer deterioration when the average fluid temperature in the segment is higher than the pseudo-critical point. The reason is explained with the generation of vapor-like film near the channel wall that the peak feature related to a nucleateboiling-like state and heat transfer deterioration related to a film-boiling-like state. The effects of parameters, including mass flow rate, pressure, and wall heat flux on flow and heat transfer were analyzed.In calculating of the averaged heat transfer coefficient of the whole channel, the traditional method shows significant deviation and the micro segment weighted average method is adopted. The pressure drop can mainly be affected by the mass flux and pressure and little affected by the wall heat flux. The peak of the convective heat transfer coefficient can only form at high mass flux, low wall heat flux, and near critical pressure, in which condition the nucleate-boiling-like state is easier to appear. Moreover,heat transfer deterioration will always appear, since the supercritical flow will finally develop into a filmboiling-like state. So heat transfer deterioration should be taken seriously in the design and safe operation of vaporizer PCHE. The study of this work clarified the local heat transfer and flow feature of supercritical methane in microchannel and contributed to the deep understanding of supercritical methane flow of the vaporization process in PCHE.展开更多
The rich accumulation of methane(CH_(4))in tectonic coal layers poses a significant obstacle to the safe and efficient extraction of coal seams and coalbed methane.Tectonic coal samples from three geologically complex...The rich accumulation of methane(CH_(4))in tectonic coal layers poses a significant obstacle to the safe and efficient extraction of coal seams and coalbed methane.Tectonic coal samples from three geologically complex regions were selected,and the main results obtained by using a variety of research tools,such as physical tests,theoretical analyses,and numerical simulations,are as follows:22.4–62.5 nm is the joint segment of pore volume,and 26.7–100.7 nm is the joint segment of pore specific surface area.In the dynamic gas production process of tectonic coal pore structure,the adsorption method of methane molecules is“solid–liquid adsorption is the mainstay,and solid–gas adsorption coexists”.Methane stored in micropores with a pore size smaller than the jointed range is defined as solid-state pores.Pores within the jointed range,which transition from micropore filling to surface adsorption,are defined as gaseous pores.Pores outside the jointed range,where solid–liquid adsorption occurs,are defined as liquid pores.The evolution of pore structure affects the methane adsorption mode,which provides basic theoretical guidance for the development of coal seam resources.展开更多
This study investigates the dry reformation of methane(DRM)over Ni/Al_(2)O_(3)catalysts in a dielectric barrier discharge(DBD)non-thermal plasma reactor.A novel hybrid machine learning(ML)model is developed to optimiz...This study investigates the dry reformation of methane(DRM)over Ni/Al_(2)O_(3)catalysts in a dielectric barrier discharge(DBD)non-thermal plasma reactor.A novel hybrid machine learning(ML)model is developed to optimize the plasma-catalytic DRM reaction with limited experimental data.To address the non-linear and complex nature of the plasma-catalytic DRM process,the hybrid ML model integrates three well-established algorithms:regression trees,support vector regression,and artificial neural networks.A genetic algorithm(GA)is then used to optimize the hyperparameters of each algorithm within the hybrid ML model.The ML model achieved excellent agreement with the experimental data,demonstrating its efficacy in accurately predicting and optimizing the DRM process.The model was subsequently used to investigate the impact of various operating parameters on the plasma-catalytic DRM performance.We found that the optimal discharge power(20 W),CO_(2)/CH_(4)molar ratio(1.5),and Ni loading(7.8 wt%)resulted in the maximum energy yield at a total flow rate of∼51 mL/min.Furthermore,we investigated the relative significance of each operating parameter on the performance of the plasma-catalytic DRM process.The results show that the total flow rate had the greatest influence on the conversion,with a significance exceeding 35%for each output,while the Ni loading had the least impact on the overall reaction performance.This hybrid model demonstrates a remarkable ability to extract valuable insights from limited datasets,enabling the development and optimization of more efficient and selective plasma-catalytic chemical processes.展开更多
Ni/TiO_(2) catalyst is widely employed for photo-driven DRM reaction while the influence of crystal structure of TiO_(2) remains unclear.In this work,the rutile/anatase ratio in supports was successfully controlled by...Ni/TiO_(2) catalyst is widely employed for photo-driven DRM reaction while the influence of crystal structure of TiO_(2) remains unclear.In this work,the rutile/anatase ratio in supports was successfully controlled by varying the calcination temperature of anatase-TiO_(2).Structural characterizations revealed that a distinct TiO_(x) coating on the Ni nanoparticles(NPs)was evident for Ni/TiO_(2)-700 catalyst due to strong metal-support interaction.It is observed that the TiOx overlayer gradually disappeared as the ratio of rutile/anatase increased,thereby enhancing the exposure of Ni active sites.The exposed Ni sites enhanced visible light absorption and boosted the dissociation capability of CH4,which led to the much elevated catalytic activity for Ni/TiO_(2)-950 in which rutile dominated.Therefore,the catalytic activity of solar-driven DRM reaction was significantly influenced by the rutile/anatase ratio.Ni/TiO_(2)-950,characterized by a predominant rutile phase,exhibited the highest DRM reactivity,with remarkable H_(2) and CO production rates reaching as high as 87.4 and 220.2 mmol/(g·h),respectively.These rates were approximately 257 and 130 times higher,respectively,compared to those obtained on Ni/TiO_(2)-700 with anatase.This study suggests that the optimization of crystal structure of TiO_(2) support can effectively enhance the performance of photothermal DRM reaction.展开更多
Deep coalbed methane(DCBM),an unconventional gas reservoir,has undergone significant advancements in recent years,sparking a growing interest in assessing pore pressure dynamics within these reservoirs.While some prod...Deep coalbed methane(DCBM),an unconventional gas reservoir,has undergone significant advancements in recent years,sparking a growing interest in assessing pore pressure dynamics within these reservoirs.While some production data analysis techniques have been adapted from conventional oil and gas wells,there remains a gap in the understanding of pore pressure generation and evolution,particularly in wells subjected to large-scale hydraulic fracturing.To address this gap,a novel technique called excess pore pressure analysis(EPPA)has been introduced to the coal seam gas industry for the first time to our knowledge,which employs dual-phase flow principles based on consolidation theory.This technique focuses on the generation and dissipation for excess pore-water pressure(EPWP)and excess pore-gas pressure(EPGP)in stimulated deep coal reservoirs.Equations have been developed respectively and numerical solutions have been provided using the finite element method(FEM).Application of this model to a representative field example reveals that excess pore pressure arises from rapid loading,with overburden weight transferred under undrained condition due to intense hydraulic fracturing,which significantly redistributes the weight-bearing role from the solid coal structure to the injected fluid and liberated gas within artificial pores over a brief timespan.Furthermore,field application indicates that the dissipation of EPWP and EPGP can be actually considered as the process of well production,where methane and water are extracted from deep coalbed methane wells,leading to consolidation for the artificial reservoirs.Moreover,history matching results demonstrate that the excess-pressure model established in this study provides a better explanation for the declining trends observed in both gas and water production curves,compared to conventional practices in coalbed methane reservoir engineering and petroleum engineering.This research not only enhances the understanding of DCBM reservoir behavior but also offers insights applicable to production analysis in other unconventional resources reliant on hydraulic fracturing.展开更多
Deep coal seams show low permeability,low elastic modulus,high Poisson’s ratio,strong plasticity,high fracture initiation pressure,difficulty in fracture extension,and difficulty in proppants addition.We proposed the...Deep coal seams show low permeability,low elastic modulus,high Poisson’s ratio,strong plasticity,high fracture initiation pressure,difficulty in fracture extension,and difficulty in proppants addition.We proposed the concept of large-scale stimulation by fracture network,balanced propagation and effective support of fracture network in fracturing design and developed the extreme massive hydraulic fracturing technique for deep coalbed methane(CBM)horizontal wells.This technique involves massive injection with high pumping rate+high-intensity proppant injection+perforation with equal apertures and limited flow+temporary plugging and diverting fractures+slick water with integrated variable viscosity+graded proppants with multiple sizes.The technique was applied in the pioneering test of a multi-stage fracturing horizontal well in deep CBM of Linxing Block,eastern margin of the Ordos Basin.The injection flow rate is 18 m^(3)/min,proppant intensity is 2.1 m^(3)/m,and fracturing fluid intensity is 16.5 m^(3)/m.After fracturing,a complex fracture network was formed,with an average fracture length of 205 m.The stimulated reservoir volume was 1987×10^(4)m^(3),and the peak gas production rate reached 6.0×10^(4)m^(3)/d,which achieved efficient development of deep CBM.展开更多
It is urgent to develop catalysts with application potential for oxidative coupling of methane(OCM)at relatively lower temperature.Herein,three-dimensional ordered macro porous(3 DOM)La_(2-x)Sr_(x)Ce_(2-y)CayO_(7-δ)(...It is urgent to develop catalysts with application potential for oxidative coupling of methane(OCM)at relatively lower temperature.Herein,three-dimensional ordered macro porous(3 DOM)La_(2-x)Sr_(x)Ce_(2-y)CayO_(7-δ)(A_(2)B_(2)O_(7)-type)catalysts with disordered defective cubic fluorite phased structure were successfully prepared by a colloidal crystal template method.3DOM structure promotes the accessibility of the gaseous reactants(O2and CH4)to the active sites.The co-doping of Ca and Sr ions in La_(2-x)Sr_(x)Ce_(2-y)CayO_(7-δ)catalysts improved the formation of oxygen vacancies,thereby leading to increased density of surface-active oxygen species(O_(2)^(-))for the activation of CH4and the formation of C2products(C2H6and C2H4).3DOM La_(2-x)Sr_(x)Ce_(2-y)CayO_(7-δ)catalysts exhibit high catalytic activity for OCM at low temperature.3DOM La1.7Sr0.3Ce1.7Ca0.3O7-δcatalyst with the highest density of O_(2)^(-)species exhibited the highest catalytic activity for low-temperature OCM,i.e.,its CH4conversion,selectivity and yield of C2products at 650℃are 32.2%,66.1%and 21.3%,respectively.The mechanism was proposed that the increase in surface oxygen vacancies induced by the co-doping of Ca and Sr ions boosts the key step of C-H bond breaking and C-C bond coupling in catalyzing low-temperature OCM.It is meaningful for the development of the low-temperature and high-efficient catalysts for OCM reaction in practical application.展开更多
Direct methane conversion has advantages such as low energy consumption,less processes,and being more economical.However,it is difficult to activate methane at room temperature due to the high dissociation energy of C...Direct methane conversion has advantages such as low energy consumption,less processes,and being more economical.However,it is difficult to activate methane at room temperature due to the high dissociation energy of C-H bonds of methane.Additionally,the target products,such as methanol,acetic acid,and other oxygenates,are prone to overoxidation,resulting in the generation of CO_(2).Therefore,the design of catalysts with high activity and selectivity is important.展开更多
Power-to-methane(P2M)processes,by converting electricity from renewable energy to H2and then into other high value-added and energy-intense chemicals in the presence of active catalysts,have become an effective soluti...Power-to-methane(P2M)processes,by converting electricity from renewable energy to H2and then into other high value-added and energy-intense chemicals in the presence of active catalysts,have become an effective solution for energy storage.However,the fluctuating electricity from intermittent renewable energy leads to a dynamic composition of reactants for downstream methanation,which requires an excellent heterogeneous catalyst to withstand the harsh conditions.Based on these findings,the objective of this review is to classify the fundamentals and status of CO/CO_(2)methanation and identify the pathways in the presence of various catalysts for methane production.In addition,this review sheds insight into the future development and challenges of CO_(2)or CO methanation,including the deactivation mechanisms and catalyst performance under dynamically harsh conditions.Finally,we elaborated on the advantages and development prospects of P2M,and then we summarized the current stage and ongoing industrialization projects of P2M.展开更多
Background Sustainable strategies for enteric methane(CH_(4))mitigation of dairy cows have been extensively explored to improve production performance and alleviate environmental pressure.The present study aimed to in...Background Sustainable strategies for enteric methane(CH_(4))mitigation of dairy cows have been extensively explored to improve production performance and alleviate environmental pressure.The present study aimed to investigate the effects of dietary xylooligosaccharides(XOS)and exogenous enzyme(EXE)supplementation on milk production,nutrient digestibility,enteric CH_(4) emissions,energy utilization efficiency of lactating Jersey dairy cows.Forty-eight lactating cows were randomly assigned to one of 4 treatments:(1)control diet(CON),(2)CON with 25 g/d XOS(XOS),(3)CON with 15 g/d EXE(EXE),and(4)CON with 25 g/d XOS and 15 g/d EXE(XOS+EXE).The 60-d experimental period consisted of a 14-d adaptation period and a 46-d sampling period.The enteric CO_(2)and CH_(4) emissions and O2 consumption were measured using two GreenFeed units,which were further used to determine the energy utilization efficiency of cows.Results Compared with CON,cows fed XOS,EXE or XOS+EXE significantly(P<0.05)increased milk yield,true protein and fat concentration,and energy-corrected milk yield(ECM)/DM intake,which could be reflected by the significant improvement(P<0.05)of dietary NDF and ADF digestibility.The results showed that dietary supplementation of XOS,EXE or XOS+EXE significantly(P<0.05)reduced CH_(4) emission,CH_(4)/milk yield,and CH_(4)/ECM.Furthermore,cows fed XOS demonstrated highest(P<0.05)metabolizable energy intake,milk energy output but lowest(P<0.05)of CH_(4) energy output and CH_(4) energy output as a proportion of gross energy intake compared with the remaining treatments.Conclusions Dietary supplementary of XOS,EXE or combination of XOS and EXE contributed to the improvement of lactation performance,nutrient digestibility,and energy utilization efficiency,as well as reduction of enteric CH_(4) emissions of lactating Jersey cows.This promising mitigation method may need further research to validate its long-term effect and mode of action for dairy cows.展开更多
Dry reforming of methane(DRM) is an attractive technology for utilizing the greenhouse gases(CO_(2) and CH_(4)) to produce syngas. However, the catalyst pellets for DRM are heavily plagued by deactivation by coking, w...Dry reforming of methane(DRM) is an attractive technology for utilizing the greenhouse gases(CO_(2) and CH_(4)) to produce syngas. However, the catalyst pellets for DRM are heavily plagued by deactivation by coking, which prevents this technology from commercialization. In this work, a pore network model is developed to probe the catalyst deactivation by coking in a Ni/Al_(2)O_(3) catalyst pellet for DRM. The reaction conditions can significantly change the coking rate and then affect the catalyst deactivation. The catalyst lifetime is higher under lower temperature, pressure, and CH_(4)/CO_(2) molar ratio, but the maximum coke content in a catalyst pellet is independent of these reaction conditions. The catalyst pellet with larger pore diameter, narrower pore size distribution and higher pore connectivity is more robust against catalyst deactivation by coking, as the pores in this pellet are more difficult to be plugged or inaccessible.The maximum coke content is also higher for narrower pore size distribution and higher pore connectivity, as the number of inaccessible pores is lower. Besides, the catalyst pellet radius only slightly affects the coke content, although the diffusion limitation increases with the pellet radius. These results should serve to guide the rational design of robust DRM catalyst pellets against deactivation by coking.展开更多
To obtain high yields of monocyclic aromatic hydrocarbons with methyl side chains,such as toluene and xylene,methane(CH_(4))can be introduced into the hydrocracking of polycyclic aromatic hydrocarbons.CH_(4)can partic...To obtain high yields of monocyclic aromatic hydrocarbons with methyl side chains,such as toluene and xylene,methane(CH_(4))can be introduced into the hydrocracking of polycyclic aromatic hydrocarbons.CH_(4)can participate in the reaction,supply methyl side chains to the product,and improve product distribution.In this study,the hydrogenation reaction of polycyclic aromatic hydrocarbons over a carbonized NiMo/Hβcatalyst in a CH_(4)and hydrogen(H_(2))environment was investigated to study the promotional effect of CH_(4)on the hydrocracking of polycyclic aromatics.Under conditions of 3.5 MPa,380℃,volume air velocity of 4 h^(-1),gas-oil volume ratio of 800,and H_(2):CH_(4)molar ratio of 1:1,the conversion rate of naphthalene was 99.97%,the liquid phase yield was 93.62%,and the selectivity of BTX were 17.76%,25.17%,and 20.47%,respectively.In comparison to the use of a H_(2)atmosphere,the selectivity of benzene was significantly decreased,whereas the selectivity of toluene and xylene were increased.It was shown that CH_(4)can participate in the hydrocracking of naphthalene and improve the selectivity of toluene and xylene in the liquid product.The carbonized NiMo/Hβcatalyst was characterized by a range of analytical methods(such as X-ray diffraction(XRD),ammonia-temperature-programmed desorption(NH3-TPD),hydrogen-temperature-programmed reduction(H_(2)-TPR),and X-ray photoelectron spectroscopy(XPS)).The results indicated that Ni and Mo carbides were the major species in the carbonized NiMo/Hβcatalyst and were considered to be active sites for the activation of CH_(4)and H_(2).After loading the metal components,the catalyst displayed prominent weak acidic sites,which may be suitable locations for cracking,alkylation,and other related reactions.Therefore,the carbonized NiMo/Hβcatalyst displayed multiple functions during the hydrocracking of polycyclic aromatic hydrocarbons in a CH_(4)and H_(2)environment.These results could be used to develop a new way to efficiently utilize polycyclic aromatic hydrocarbons and natural gas resources.展开更多
Background:The use of industrial by-products rich in bioactive compounds as animal feeds can reduce greenhouse gas production.Paulownia leaves silage(PLS)was supplemented to dairy cows'diet and evaluated in vitro(...Background:The use of industrial by-products rich in bioactive compounds as animal feeds can reduce greenhouse gas production.Paulownia leaves silage(PLS)was supplemented to dairy cows'diet and evaluated in vitro(Exp.1;Rusitec)and in vivo(Exp.2,cannulated lactating dairy cows and Exp.3,non-cannulated lactating dairy cows).The study investigated the PLS effect on ruminal fermentation,microbial populations,methane production and concentration,dry matter intake(DMI),and fatty acid(FA)proportions in ruminal fluid and milk.Results:Several variables of the ruminal fluid were changed in response to the inclusion of PLS.In Exp.1,the p H increased linearly and quadratically,whereas ammonia and total volatile fatty acid(VFA)concentrations increased linearly and cubically.A linear,quadratic,and cubical decrease in methane concentration was observed with increasing dose of the PLS.Exp.2 revealed an increase in ruminal p H and ammonia concentrations,but no changes in total VFA concentration.Inclusion of PLS increased ruminal propionate(at 3 h and 6 h after feeding),isovalerate,and valerate concentrations.Addition of PLS also affected several populations of the analyzed microorganisms.The abundances of protozoa and bacteria were increased,whereas the abundance of archaea were decreased by PLS.Methane production decreased by 11%and 14%in PLS-fed cows compared to the control in Exp.2 and 3,respectively.Exp.3 revealed a reduction in the milk protein and lactose yield in the PLS-fed cows,but no effect on DMI and energy corrected milk yield.Also,the PLS diet affected the ruminal biohydrogenation process with an increased proportions of C18:3 cis-9 cis-12 cis-15,conjugated linoleic acid,C18:1 trans-11 FA,polyunsaturated fatty acids(PUFA),and reduced n6/n3 ratio and saturated fatty acids(SFA)proportion in milk.The relative transcript abundances of the 5 of 6 analyzed genes regulating FA metabolism increased.Conclusions:The dietary PLS replacing the alfalfa silage at 60 g/kg diet can reduce the methane emission and improve milk quality with greater proportions of PUFA,including conjugated linoleic acid,and C18:1 trans-11 along with reduction of SFA.展开更多
Microplastics(MPs)are important exempla of the Anthropocene and are exerting an increasing impact on Earth’s carbon cycle.The huge imbalance between the MPs floating on the marine surface and those that are estimated...Microplastics(MPs)are important exempla of the Anthropocene and are exerting an increasing impact on Earth’s carbon cycle.The huge imbalance between the MPs floating on the marine surface and those that are estimated to have been introduced into the ocean necessitates a detailed assessment of marine MP sinks.Here,we demonstrate that cold seep sediments,which are characterized by methane fluid seepage and a chemosynthetic ecosystem,effectively capture and accommodate small-scale(<100μm)MPs,with 16 types of MPs being detected.The abundance of MPs in the surface of the sediment is higher in methane-seepage locations than in non-seepage areas.Methane seepage is beneficial to the accumulation,fragmentation,increased diversity,and aging of MPs.In turn,the rough surfaces of MPs contribute to the sequestration of the electron acceptor ferric oxide,which is associated with the anaerobic oxidation of methane(AOM).The efficiency of the AOM determines whether the seeping methane(which has a greenhouse effect 83 times greater than that of CO_(2)over a 20-year period)can enter the atmosphere,which is important to the global methane cycle,since the deep-sea environment is regarded as the largest methane reservoir associated with natural gas hydrates.展开更多
New energy sources that reduce the volume of harmful gases such as SO_(x)and NO_(x)released into the atmosphere are in constant development.Natural gas,primarily made up of methane,is being widely used as one reliable...New energy sources that reduce the volume of harmful gases such as SO_(x)and NO_(x)released into the atmosphere are in constant development.Natural gas,primarily made up of methane,is being widely used as one reliable energy source for heating and electricity generation due to its high combustion value.Currently,natural gas accounts for a large portion of electricity generation and chemical feedstock in manufacturing plastics and other commercially important organic chemicals.In the near future,natural gas will be widely used as a fuel for vehicles.Therefore,a practical storage device for its storage and transportation is very beneficial to the deployment of natural gas as an energy source for new technologies.In this tutorial review,biomaterials-based carbon monoliths(CMs),one kind of carbonaceous material,was reviewed as an adsorbent for natural gas(methane)adsorption and storage.展开更多
To achieve the goals of carbon peaking and carbon neutrality under the backgrounds of poor resource endowments, weak theoretical basis and other factors, the development of the coalbed methane industry of China faces ...To achieve the goals of carbon peaking and carbon neutrality under the backgrounds of poor resource endowments, weak theoretical basis and other factors, the development of the coalbed methane industry of China faces many bottlenecks and challenges. This paper systematically analyzes the coalbed methane resources, key technologies and progress, exploration effect and production performance in China and abroad. The main problems are summarized as low exploration degree, low technical adaptability, low return on investment and small development scale. This study suggests that the coalbed methane industry in China should follow the “two-step”(short-term and long-term) development strategy. The short-term action before 2030, can be divided into two stages:(1) From the present to 2025, to achieve new breakthroughs in theory and technology, and accomplish the target of annual production of 10 billion cubic meters;(2) From 2025 to 2030, to form the technologies suitable for most geological conditions, further expand the industry scale, and achieve an annual output of 30 billion cubic meters, improving the proportion of coalbed methane in the total natural gas production. The long-term action after 2030 is to gradually realize an annual production of 100 billion cubic meters. The strategic countermeasure to achieve the above goals is to adhere to “technology+management dual wheel drive”, realize the synchronous progress of technology and management, and promote the high-quality development of the coalbed methane industry. Technically, the efforts will focus on fine and effective development of coalbed methane in the medium to shallow layers of mature fields, effective development of coalbed methane in new fields, extensive and beneficial development of deep coalbed methane, three-dimensional comingled development of coalbed methane, applying new technologies such as coalbed methane displacement by carbon dioxide, microwave heating and stimulation technology, ultrasonic stimulation, high-temperature heat injection stimulation, rock breaking by high-energy laser. In terms of management, the efforts will focus on coordinative innovation of resource, technology, talent, policy and investment, with technological innovation as the core, to realize an all-round and integrated management and promote the development of coalbed methane industry at a high level.展开更多
The conversion of methane to olefins,aromatics,and hydrogen(MTOAH)can be used to stably obtain hydrocarbons when the effect of the catalytic surface is optimized from the reaction engineering perspective.In this study...The conversion of methane to olefins,aromatics,and hydrogen(MTOAH)can be used to stably obtain hydrocarbons when the effect of the catalytic surface is optimized from the reaction engineering perspective.In this study,Fe/Si C catalysts were packed into a quartz tube reactor.The catalytic surfaces of Si C and the impregnated Fe species decreased the apparent activation energies(E_a)of methane consumption in the blank reactor between 965 and 1020℃.Consequently,the hydrocarbon yield increased by 2.4times at 1020℃.Based on the model reactions of ethane,ethylene,and acetylene mixed with hydrogen in the range of 500-1020℃,an excess amount of Fe in the reactor favored the C-C coupling reaction over the selective hydrogenation of acetylene;consequently,coke formation was favored over the hydrogenation reaction.The gas-phase reactions and catalyst properties were optimized to increase hydrocarbon yields while reducing coke selectivity.The 0.2Fe catalyst-packed reactor(0.26 wt%Fe)resulted in a hydrocarbon yield of 7.1%and a coke selectivity of<2%when the ratio of the void space of the postcatalyst zone to the catalyst space was adjusted to be≥2.Based on these findings,the facile approach of decoupling the reaction zone between the catalyst surface and the gas-phase reaction can provide insights into catalytic reactor design,thereby facilitating the scale-up from the laboratory to the commercial scale.展开更多
基金National Natural Science Foundation of China(52174279)Analysis and Testing Foundation of Kunming University of Science and Technology(2022M20202202138)Yunnan Fundamental Research Projects(202301AU070027).
文摘The challenges posed by energy and environmental issues have forced mankind to explore and utilize unconventional energy sources.It is imperative to convert the abundant coalbed gas(CBG)into high value-added products,i.e.,selective and efficient conversion of methane from CBG.Methane activation,known as the“holy grail”,poses a challenge to the design and development of catalysts.The structural complexity of the active metal on the carrier is of particular concern.In this work,we have studied the nucleation growth of small Co clusters(up to Co_(6))on the surface of CeO_(2)(110)using density functional theory,from which a stable loaded Co/CeO_(2)(110)structure was selected to investigate the methane activation mechanism.Despite the relatively small size of the selected Co clusters,the obtained Co_(x)/CeO_(2)(110)exhibits interesting properties.The optimized Co_(5)/CeO_(2)(110)structure was selected as the optimal structure to study the activation mechanism of methane due to its competitive electronic structure,adsorption energy and binding energy.The energy barriers for the stepwise dissociation of methane to form CH3^(*),CH2^(*),CH^(*),and C^(*)radical fragments are 0.44,0.55,0.31,and 1.20 eV,respectively,indicating that CH^(*)dissociative dehydrogenation is the rate-determining step for the system under investigation here.This fundamental study of metal-support interactions based on Co growth on the CeO_(2)(110)surface contributes to the understanding of the essence of Co/CeO_(2) catalysts with promising catalytic behavior.It provides theoretical guidance for better designing the optimal Co/CeO_(2) catalyst for tailored catalytic reactions.
基金supported by the National Natural Science Foundation of China(21978092).
文摘Co-combustion of methane(CH4)and acid gas(AG)is required to sustain the temperature in Claus reaction furnace.In this study,oxy-fuel combustion of methane and acid gas has been experimentally studied in a diffusion flame.Three equivalence ratios(ER=1.0,1.5,2.0)and CH_(4)-addition ratios(CH_(4)/AG=0.3,0.5,0.7)were examined and the flame was interpreted by analyzing the distributions of the temperature and species concentration along central axial.CH_(4)-AG diffusion flame could be classified into three sections namely initial reaction,oxidation and complex reaction sections.Competitive oxidation of CH_(4)and H_(2)S was noted in the first section wherein H_(2)S was preferred and both were mainly proceeding decomposition and partial oxidation.SO_(2)was formed at oxidation section together with obvious presence of H2 and CO.However,H2 and CO were inclined to be sustained under fuel rich condition in the complex reaction section.Reducing ER and increasing CH4/AG contributed to higher temperature,H_(2)S and CH_(4)oxidation and CO_(2)reactivity.Hence a growing trend for CH_(4)and AG to convert into H_(2),CO and SO_(2)could be witnessed.And this factor enhanced the generation of CS2 and COS in the flame inner core by interactions of CH4 and CO_(2)with sulfur species.COS was formed through the interactions of CO and CO_(2)with sulfur species.The CS_(2)production directly relied on reaction of CH_(4)with sulfur species.The concentration of COS was greater than CS_(2)since CS_(2)was probably inhibited due to the presence of H_(2).COS and CS_(2)could be consumed by further oxidation or other complex reactions.
基金supported by the Improvement of Green Rice Plant Type Using Genetic Information Program, Rural Development Administration, Korea (Grant No. PJ01699202)
文摘Anthropogenic methane emissions are a leading cause of the increase in global averagetemperatures,often referred to as global warming.Flooded soils play a significant role in methaneproduction,where the anaerobic conditions promote the production of methane by methanogenicmicroorganisms.Rice fields contribute a considerable portion of agricultural methane emissions,as riceplants provide both factors that enhance and limit methane production.Rice plants harbor both methaneproducingand methane-oxidizing microorganisms.Exudates from rice roots provide source for methaneproduction,while oxygen delivered from the root aerenchyma enhances methane oxidation.Studies haveshown that the diversity of these microorganisms depends on rice cultivars with some genes characterizedas harboring specific groups of microorganisms related to methane emissions.However,there is still aneed for research to determine the balance between methane production and oxidation,as rice plantspossess the ability to regulate net methane production.Various agronomical practices,such as fertilizerand water management,have been employed to mitigate methane emissions.Nevertheless,studiescorrelating agronomic and chemical management of methane with productivity are limited.Moreover,evidences for breeding low-methane-emitting rice varieties are scattered largely due to the absence ofcoordinated breeding programs.Research has indicated that phenotypic characteristics,such as rootbiomass,shoot architecture,and aerenchyma,are highly correlated with methane emissions.This reviewdiscusses available studies that involve the correlation between plant characteristics and methaneemissions.It emphasizes the necessity and importance of breeding low-methane-emitting rice varieties inaddition to existing agronomic,biological,and chemical practices.The review also delves into the idealphenotypic and physiological characteristics of low-methane-emitting rice and potential breeding techniques,drawing from studies conducted with diverse varieties,mutants,and transgenic plants.
基金provided by Science and Technology Development Project of Jilin Province(No.20230101338JC)。
文摘The printed circuit heat exchanger(PCHE) is receiving wide attention as a new kind of compact heat exchanger and is considered as a promising vaporizer in the LNG process. In this paper, a PCHE straight channel in the length of 500 mm is established, with a semicircular cross section in a diameter of 1.2 mm.Numerical simulation is employed to investigate the flow and heat transfer performance of supercritical methane in the channel. The pseudo-boiling theory is adopted and the liquid-like, two-phase-like, and vapor-like regimes are divided for supercritical methane to analyze the heat transfer and flow features.The results are presented in micro segment to show the local convective heat transfer coefficient and pressure drop. It shows that the convective heat transfer coefficient in segments along the channel has a significant peak feature near the pseudo-critical point and a heat transfer deterioration when the average fluid temperature in the segment is higher than the pseudo-critical point. The reason is explained with the generation of vapor-like film near the channel wall that the peak feature related to a nucleateboiling-like state and heat transfer deterioration related to a film-boiling-like state. The effects of parameters, including mass flow rate, pressure, and wall heat flux on flow and heat transfer were analyzed.In calculating of the averaged heat transfer coefficient of the whole channel, the traditional method shows significant deviation and the micro segment weighted average method is adopted. The pressure drop can mainly be affected by the mass flux and pressure and little affected by the wall heat flux. The peak of the convective heat transfer coefficient can only form at high mass flux, low wall heat flux, and near critical pressure, in which condition the nucleate-boiling-like state is easier to appear. Moreover,heat transfer deterioration will always appear, since the supercritical flow will finally develop into a filmboiling-like state. So heat transfer deterioration should be taken seriously in the design and safe operation of vaporizer PCHE. The study of this work clarified the local heat transfer and flow feature of supercritical methane in microchannel and contributed to the deep understanding of supercritical methane flow of the vaporization process in PCHE.
基金supported by the National Natural Science Foundation of China(52164015)the Technology Funding Projects of Guizhou Province([2022]231).
文摘The rich accumulation of methane(CH_(4))in tectonic coal layers poses a significant obstacle to the safe and efficient extraction of coal seams and coalbed methane.Tectonic coal samples from three geologically complex regions were selected,and the main results obtained by using a variety of research tools,such as physical tests,theoretical analyses,and numerical simulations,are as follows:22.4–62.5 nm is the joint segment of pore volume,and 26.7–100.7 nm is the joint segment of pore specific surface area.In the dynamic gas production process of tectonic coal pore structure,the adsorption method of methane molecules is“solid–liquid adsorption is the mainstay,and solid–gas adsorption coexists”.Methane stored in micropores with a pore size smaller than the jointed range is defined as solid-state pores.Pores within the jointed range,which transition from micropore filling to surface adsorption,are defined as gaseous pores.Pores outside the jointed range,where solid–liquid adsorption occurs,are defined as liquid pores.The evolution of pore structure affects the methane adsorption mode,which provides basic theoretical guidance for the development of coal seam resources.
基金This project received funding from the European Union’s Horizon 2020 research and innovation program under the Marie Sklodowska-Curie grant agreement No. 813393the funding from the National Natural Science Foundation of China (No. 52177149)
文摘This study investigates the dry reformation of methane(DRM)over Ni/Al_(2)O_(3)catalysts in a dielectric barrier discharge(DBD)non-thermal plasma reactor.A novel hybrid machine learning(ML)model is developed to optimize the plasma-catalytic DRM reaction with limited experimental data.To address the non-linear and complex nature of the plasma-catalytic DRM process,the hybrid ML model integrates three well-established algorithms:regression trees,support vector regression,and artificial neural networks.A genetic algorithm(GA)is then used to optimize the hyperparameters of each algorithm within the hybrid ML model.The ML model achieved excellent agreement with the experimental data,demonstrating its efficacy in accurately predicting and optimizing the DRM process.The model was subsequently used to investigate the impact of various operating parameters on the plasma-catalytic DRM performance.We found that the optimal discharge power(20 W),CO_(2)/CH_(4)molar ratio(1.5),and Ni loading(7.8 wt%)resulted in the maximum energy yield at a total flow rate of∼51 mL/min.Furthermore,we investigated the relative significance of each operating parameter on the performance of the plasma-catalytic DRM process.The results show that the total flow rate had the greatest influence on the conversion,with a significance exceeding 35%for each output,while the Ni loading had the least impact on the overall reaction performance.This hybrid model demonstrates a remarkable ability to extract valuable insights from limited datasets,enabling the development and optimization of more efficient and selective plasma-catalytic chemical processes.
基金The project was supported by the National Key R&D Program of China(2021YFF0500702)Natural Science Foundation of Shanghai(22JC1404200)+3 种基金Program of Shanghai Academic/Technology Research Leader(20XD1404000)Natural Science Foundation of China(U22B20136,22293023)Science and Technology Major Project of Inner Mongolia(2021ZD0042)the Youth Innovation Promotion Association of CAS。
文摘Ni/TiO_(2) catalyst is widely employed for photo-driven DRM reaction while the influence of crystal structure of TiO_(2) remains unclear.In this work,the rutile/anatase ratio in supports was successfully controlled by varying the calcination temperature of anatase-TiO_(2).Structural characterizations revealed that a distinct TiO_(x) coating on the Ni nanoparticles(NPs)was evident for Ni/TiO_(2)-700 catalyst due to strong metal-support interaction.It is observed that the TiOx overlayer gradually disappeared as the ratio of rutile/anatase increased,thereby enhancing the exposure of Ni active sites.The exposed Ni sites enhanced visible light absorption and boosted the dissociation capability of CH4,which led to the much elevated catalytic activity for Ni/TiO_(2)-950 in which rutile dominated.Therefore,the catalytic activity of solar-driven DRM reaction was significantly influenced by the rutile/anatase ratio.Ni/TiO_(2)-950,characterized by a predominant rutile phase,exhibited the highest DRM reactivity,with remarkable H_(2) and CO production rates reaching as high as 87.4 and 220.2 mmol/(g·h),respectively.These rates were approximately 257 and 130 times higher,respectively,compared to those obtained on Ni/TiO_(2)-700 with anatase.This study suggests that the optimization of crystal structure of TiO_(2) support can effectively enhance the performance of photothermal DRM reaction.
基金supported by the National Natural Science Foundation of China(Nos.42272195 and 42130802)supported by the Key Applied Science and Technology Project of PetroChina(No.2023ZZ18)the Major Science and Technology Project of Changqing Oilfield(No.2023DZZ01).
文摘Deep coalbed methane(DCBM),an unconventional gas reservoir,has undergone significant advancements in recent years,sparking a growing interest in assessing pore pressure dynamics within these reservoirs.While some production data analysis techniques have been adapted from conventional oil and gas wells,there remains a gap in the understanding of pore pressure generation and evolution,particularly in wells subjected to large-scale hydraulic fracturing.To address this gap,a novel technique called excess pore pressure analysis(EPPA)has been introduced to the coal seam gas industry for the first time to our knowledge,which employs dual-phase flow principles based on consolidation theory.This technique focuses on the generation and dissipation for excess pore-water pressure(EPWP)and excess pore-gas pressure(EPGP)in stimulated deep coal reservoirs.Equations have been developed respectively and numerical solutions have been provided using the finite element method(FEM).Application of this model to a representative field example reveals that excess pore pressure arises from rapid loading,with overburden weight transferred under undrained condition due to intense hydraulic fracturing,which significantly redistributes the weight-bearing role from the solid coal structure to the injected fluid and liberated gas within artificial pores over a brief timespan.Furthermore,field application indicates that the dissipation of EPWP and EPGP can be actually considered as the process of well production,where methane and water are extracted from deep coalbed methane wells,leading to consolidation for the artificial reservoirs.Moreover,history matching results demonstrate that the excess-pressure model established in this study provides a better explanation for the declining trends observed in both gas and water production curves,compared to conventional practices in coalbed methane reservoir engineering and petroleum engineering.This research not only enhances the understanding of DCBM reservoir behavior but also offers insights applicable to production analysis in other unconventional resources reliant on hydraulic fracturing.
基金Supported by the National Natural Science Foundation of China Project(52274014)Comprehensive Scientific Research Project of China National Offshore Oil Corporation(KJZH-2023-2303)。
文摘Deep coal seams show low permeability,low elastic modulus,high Poisson’s ratio,strong plasticity,high fracture initiation pressure,difficulty in fracture extension,and difficulty in proppants addition.We proposed the concept of large-scale stimulation by fracture network,balanced propagation and effective support of fracture network in fracturing design and developed the extreme massive hydraulic fracturing technique for deep coalbed methane(CBM)horizontal wells.This technique involves massive injection with high pumping rate+high-intensity proppant injection+perforation with equal apertures and limited flow+temporary plugging and diverting fractures+slick water with integrated variable viscosity+graded proppants with multiple sizes.The technique was applied in the pioneering test of a multi-stage fracturing horizontal well in deep CBM of Linxing Block,eastern margin of the Ordos Basin.The injection flow rate is 18 m^(3)/min,proppant intensity is 2.1 m^(3)/m,and fracturing fluid intensity is 16.5 m^(3)/m.After fracturing,a complex fracture network was formed,with an average fracture length of 205 m.The stimulated reservoir volume was 1987×10^(4)m^(3),and the peak gas production rate reached 6.0×10^(4)m^(3)/d,which achieved efficient development of deep CBM.
基金supported by the National Key Research and Development Program of China(Nos.2022YFB3504100,2022YFB3506200)the National Natural Science Foundation of China(Nos.22208373,22376217)+1 种基金the Beijing Nova Program(No.20220484215)the Science Foundation of China University of Petroleum,Beijing(No.2462023YJRC030)。
文摘It is urgent to develop catalysts with application potential for oxidative coupling of methane(OCM)at relatively lower temperature.Herein,three-dimensional ordered macro porous(3 DOM)La_(2-x)Sr_(x)Ce_(2-y)CayO_(7-δ)(A_(2)B_(2)O_(7)-type)catalysts with disordered defective cubic fluorite phased structure were successfully prepared by a colloidal crystal template method.3DOM structure promotes the accessibility of the gaseous reactants(O2and CH4)to the active sites.The co-doping of Ca and Sr ions in La_(2-x)Sr_(x)Ce_(2-y)CayO_(7-δ)catalysts improved the formation of oxygen vacancies,thereby leading to increased density of surface-active oxygen species(O_(2)^(-))for the activation of CH4and the formation of C2products(C2H6and C2H4).3DOM La_(2-x)Sr_(x)Ce_(2-y)CayO_(7-δ)catalysts exhibit high catalytic activity for OCM at low temperature.3DOM La1.7Sr0.3Ce1.7Ca0.3O7-δcatalyst with the highest density of O_(2)^(-)species exhibited the highest catalytic activity for low-temperature OCM,i.e.,its CH4conversion,selectivity and yield of C2products at 650℃are 32.2%,66.1%and 21.3%,respectively.The mechanism was proposed that the increase in surface oxygen vacancies induced by the co-doping of Ca and Sr ions boosts the key step of C-H bond breaking and C-C bond coupling in catalyzing low-temperature OCM.It is meaningful for the development of the low-temperature and high-efficient catalysts for OCM reaction in practical application.
文摘Direct methane conversion has advantages such as low energy consumption,less processes,and being more economical.However,it is difficult to activate methane at room temperature due to the high dissociation energy of C-H bonds of methane.Additionally,the target products,such as methanol,acetic acid,and other oxygenates,are prone to overoxidation,resulting in the generation of CO_(2).Therefore,the design of catalysts with high activity and selectivity is important.
基金funded by the National Key Research and Development Program of China(2019YFA0405602)the Hefei Science Center,CAS(2020HSC-KPRD001,2021HSC-UE005)the DNL Cooperation Fund,CAS(DNL202005)。
文摘Power-to-methane(P2M)processes,by converting electricity from renewable energy to H2and then into other high value-added and energy-intense chemicals in the presence of active catalysts,have become an effective solution for energy storage.However,the fluctuating electricity from intermittent renewable energy leads to a dynamic composition of reactants for downstream methanation,which requires an excellent heterogeneous catalyst to withstand the harsh conditions.Based on these findings,the objective of this review is to classify the fundamentals and status of CO/CO_(2)methanation and identify the pathways in the presence of various catalysts for methane production.In addition,this review sheds insight into the future development and challenges of CO_(2)or CO methanation,including the deactivation mechanisms and catalyst performance under dynamically harsh conditions.Finally,we elaborated on the advantages and development prospects of P2M,and then we summarized the current stage and ongoing industrialization projects of P2M.
基金the Key Program for International S&T Cooperation Projects of China(2022YFE0130100)Central Public-interest Scientific Institution Basal Research Fund of Chinese Academy of Agricultural Sciences(Y2022GH12).
文摘Background Sustainable strategies for enteric methane(CH_(4))mitigation of dairy cows have been extensively explored to improve production performance and alleviate environmental pressure.The present study aimed to investigate the effects of dietary xylooligosaccharides(XOS)and exogenous enzyme(EXE)supplementation on milk production,nutrient digestibility,enteric CH_(4) emissions,energy utilization efficiency of lactating Jersey dairy cows.Forty-eight lactating cows were randomly assigned to one of 4 treatments:(1)control diet(CON),(2)CON with 25 g/d XOS(XOS),(3)CON with 15 g/d EXE(EXE),and(4)CON with 25 g/d XOS and 15 g/d EXE(XOS+EXE).The 60-d experimental period consisted of a 14-d adaptation period and a 46-d sampling period.The enteric CO_(2)and CH_(4) emissions and O2 consumption were measured using two GreenFeed units,which were further used to determine the energy utilization efficiency of cows.Results Compared with CON,cows fed XOS,EXE or XOS+EXE significantly(P<0.05)increased milk yield,true protein and fat concentration,and energy-corrected milk yield(ECM)/DM intake,which could be reflected by the significant improvement(P<0.05)of dietary NDF and ADF digestibility.The results showed that dietary supplementation of XOS,EXE or XOS+EXE significantly(P<0.05)reduced CH_(4) emission,CH_(4)/milk yield,and CH_(4)/ECM.Furthermore,cows fed XOS demonstrated highest(P<0.05)metabolizable energy intake,milk energy output but lowest(P<0.05)of CH_(4) energy output and CH_(4) energy output as a proportion of gross energy intake compared with the remaining treatments.Conclusions Dietary supplementary of XOS,EXE or combination of XOS and EXE contributed to the improvement of lactation performance,nutrient digestibility,and energy utilization efficiency,as well as reduction of enteric CH_(4) emissions of lactating Jersey cows.This promising mitigation method may need further research to validate its long-term effect and mode of action for dairy cows.
基金financially supported by the National Natural Science Foundation of China (22078090 and 92034301)the Shanghai Rising-Star Program (21QA1402000)+1 种基金the Natural Science Foundation of Shanghai (21ZR1418100)the Open Project of State Key Laboratory of Chemical Engineering (SKL-ChE-21C02)。
文摘Dry reforming of methane(DRM) is an attractive technology for utilizing the greenhouse gases(CO_(2) and CH_(4)) to produce syngas. However, the catalyst pellets for DRM are heavily plagued by deactivation by coking, which prevents this technology from commercialization. In this work, a pore network model is developed to probe the catalyst deactivation by coking in a Ni/Al_(2)O_(3) catalyst pellet for DRM. The reaction conditions can significantly change the coking rate and then affect the catalyst deactivation. The catalyst lifetime is higher under lower temperature, pressure, and CH_(4)/CO_(2) molar ratio, but the maximum coke content in a catalyst pellet is independent of these reaction conditions. The catalyst pellet with larger pore diameter, narrower pore size distribution and higher pore connectivity is more robust against catalyst deactivation by coking, as the pores in this pellet are more difficult to be plugged or inaccessible.The maximum coke content is also higher for narrower pore size distribution and higher pore connectivity, as the number of inaccessible pores is lower. Besides, the catalyst pellet radius only slightly affects the coke content, although the diffusion limitation increases with the pellet radius. These results should serve to guide the rational design of robust DRM catalyst pellets against deactivation by coking.
基金the financial support from the Graduate Student Innovation and Practical Ability Training Program of Xi’an Shiyou University (No. YCS21212111)Open Fund Project of the State Key Laboratory of Heavy Oil, China (SKLHOP201703)+3 种基金National Natural Science Foundation of China (No. 52274039)Natural Science Foundation of Shaanxi Provincial Department of Education (Grant 2023-JC-YB-414)Natural Science Foundation of Shaanxi Province in China (No. 2022JZ-28)the Open Fund Project of the National Oil Shale Exploitation Research and Development Center, China (No. 33550022-ZC0613-0255)
文摘To obtain high yields of monocyclic aromatic hydrocarbons with methyl side chains,such as toluene and xylene,methane(CH_(4))can be introduced into the hydrocracking of polycyclic aromatic hydrocarbons.CH_(4)can participate in the reaction,supply methyl side chains to the product,and improve product distribution.In this study,the hydrogenation reaction of polycyclic aromatic hydrocarbons over a carbonized NiMo/Hβcatalyst in a CH_(4)and hydrogen(H_(2))environment was investigated to study the promotional effect of CH_(4)on the hydrocracking of polycyclic aromatics.Under conditions of 3.5 MPa,380℃,volume air velocity of 4 h^(-1),gas-oil volume ratio of 800,and H_(2):CH_(4)molar ratio of 1:1,the conversion rate of naphthalene was 99.97%,the liquid phase yield was 93.62%,and the selectivity of BTX were 17.76%,25.17%,and 20.47%,respectively.In comparison to the use of a H_(2)atmosphere,the selectivity of benzene was significantly decreased,whereas the selectivity of toluene and xylene were increased.It was shown that CH_(4)can participate in the hydrocracking of naphthalene and improve the selectivity of toluene and xylene in the liquid product.The carbonized NiMo/Hβcatalyst was characterized by a range of analytical methods(such as X-ray diffraction(XRD),ammonia-temperature-programmed desorption(NH3-TPD),hydrogen-temperature-programmed reduction(H_(2)-TPR),and X-ray photoelectron spectroscopy(XPS)).The results indicated that Ni and Mo carbides were the major species in the carbonized NiMo/Hβcatalyst and were considered to be active sites for the activation of CH_(4)and H_(2).After loading the metal components,the catalyst displayed prominent weak acidic sites,which may be suitable locations for cracking,alkylation,and other related reactions.Therefore,the carbonized NiMo/Hβcatalyst displayed multiple functions during the hydrocracking of polycyclic aromatic hydrocarbons in a CH_(4)and H_(2)environment.These results could be used to develop a new way to efficiently utilize polycyclic aromatic hydrocarbons and natural gas resources.
基金a grant from the National Science Center,Poland(Grant No.2016/23/B/NZ9/03427)co-financed within the framework of the Polish Ministry of Science and Higher Education’s program:“Regional Initiative Excellence”in the years 2019–2022(No.005/RID/2018/19)“financing amount 12000000,00 PLN”。
文摘Background:The use of industrial by-products rich in bioactive compounds as animal feeds can reduce greenhouse gas production.Paulownia leaves silage(PLS)was supplemented to dairy cows'diet and evaluated in vitro(Exp.1;Rusitec)and in vivo(Exp.2,cannulated lactating dairy cows and Exp.3,non-cannulated lactating dairy cows).The study investigated the PLS effect on ruminal fermentation,microbial populations,methane production and concentration,dry matter intake(DMI),and fatty acid(FA)proportions in ruminal fluid and milk.Results:Several variables of the ruminal fluid were changed in response to the inclusion of PLS.In Exp.1,the p H increased linearly and quadratically,whereas ammonia and total volatile fatty acid(VFA)concentrations increased linearly and cubically.A linear,quadratic,and cubical decrease in methane concentration was observed with increasing dose of the PLS.Exp.2 revealed an increase in ruminal p H and ammonia concentrations,but no changes in total VFA concentration.Inclusion of PLS increased ruminal propionate(at 3 h and 6 h after feeding),isovalerate,and valerate concentrations.Addition of PLS also affected several populations of the analyzed microorganisms.The abundances of protozoa and bacteria were increased,whereas the abundance of archaea were decreased by PLS.Methane production decreased by 11%and 14%in PLS-fed cows compared to the control in Exp.2 and 3,respectively.Exp.3 revealed a reduction in the milk protein and lactose yield in the PLS-fed cows,but no effect on DMI and energy corrected milk yield.Also,the PLS diet affected the ruminal biohydrogenation process with an increased proportions of C18:3 cis-9 cis-12 cis-15,conjugated linoleic acid,C18:1 trans-11 FA,polyunsaturated fatty acids(PUFA),and reduced n6/n3 ratio and saturated fatty acids(SFA)proportion in milk.The relative transcript abundances of the 5 of 6 analyzed genes regulating FA metabolism increased.Conclusions:The dietary PLS replacing the alfalfa silage at 60 g/kg diet can reduce the methane emission and improve milk quality with greater proportions of PUFA,including conjugated linoleic acid,and C18:1 trans-11 along with reduction of SFA.
基金financially supported by the National Natural Science Foundation of China(42022046)the National Key Research and Development Program of China(2021YFF0502300)+1 种基金the Key Special Project for Introduced Talent Teams of the Southern Marine Science and Engineering Guangdong Laboratory(Guangzhou)(GML2019ZD0403 and GML2019ZD0401)Guangdong Natural Resources Foundation(GDNRC[2022]45)。
文摘Microplastics(MPs)are important exempla of the Anthropocene and are exerting an increasing impact on Earth’s carbon cycle.The huge imbalance between the MPs floating on the marine surface and those that are estimated to have been introduced into the ocean necessitates a detailed assessment of marine MP sinks.Here,we demonstrate that cold seep sediments,which are characterized by methane fluid seepage and a chemosynthetic ecosystem,effectively capture and accommodate small-scale(<100μm)MPs,with 16 types of MPs being detected.The abundance of MPs in the surface of the sediment is higher in methane-seepage locations than in non-seepage areas.Methane seepage is beneficial to the accumulation,fragmentation,increased diversity,and aging of MPs.In turn,the rough surfaces of MPs contribute to the sequestration of the electron acceptor ferric oxide,which is associated with the anaerobic oxidation of methane(AOM).The efficiency of the AOM determines whether the seeping methane(which has a greenhouse effect 83 times greater than that of CO_(2)over a 20-year period)can enter the atmosphere,which is important to the global methane cycle,since the deep-sea environment is regarded as the largest methane reservoir associated with natural gas hydrates.
基金Acknowledgment is made to the Donors of the American Chemical Society Petroleum Research Fund for support of this research.
文摘New energy sources that reduce the volume of harmful gases such as SO_(x)and NO_(x)released into the atmosphere are in constant development.Natural gas,primarily made up of methane,is being widely used as one reliable energy source for heating and electricity generation due to its high combustion value.Currently,natural gas accounts for a large portion of electricity generation and chemical feedstock in manufacturing plastics and other commercially important organic chemicals.In the near future,natural gas will be widely used as a fuel for vehicles.Therefore,a practical storage device for its storage and transportation is very beneficial to the deployment of natural gas as an energy source for new technologies.In this tutorial review,biomaterials-based carbon monoliths(CMs),one kind of carbonaceous material,was reviewed as an adsorbent for natural gas(methane)adsorption and storage.
基金Supported by the China National Science and Technology Major Project (2016ZX05042)。
文摘To achieve the goals of carbon peaking and carbon neutrality under the backgrounds of poor resource endowments, weak theoretical basis and other factors, the development of the coalbed methane industry of China faces many bottlenecks and challenges. This paper systematically analyzes the coalbed methane resources, key technologies and progress, exploration effect and production performance in China and abroad. The main problems are summarized as low exploration degree, low technical adaptability, low return on investment and small development scale. This study suggests that the coalbed methane industry in China should follow the “two-step”(short-term and long-term) development strategy. The short-term action before 2030, can be divided into two stages:(1) From the present to 2025, to achieve new breakthroughs in theory and technology, and accomplish the target of annual production of 10 billion cubic meters;(2) From 2025 to 2030, to form the technologies suitable for most geological conditions, further expand the industry scale, and achieve an annual output of 30 billion cubic meters, improving the proportion of coalbed methane in the total natural gas production. The long-term action after 2030 is to gradually realize an annual production of 100 billion cubic meters. The strategic countermeasure to achieve the above goals is to adhere to “technology+management dual wheel drive”, realize the synchronous progress of technology and management, and promote the high-quality development of the coalbed methane industry. Technically, the efforts will focus on fine and effective development of coalbed methane in the medium to shallow layers of mature fields, effective development of coalbed methane in new fields, extensive and beneficial development of deep coalbed methane, three-dimensional comingled development of coalbed methane, applying new technologies such as coalbed methane displacement by carbon dioxide, microwave heating and stimulation technology, ultrasonic stimulation, high-temperature heat injection stimulation, rock breaking by high-energy laser. In terms of management, the efforts will focus on coordinative innovation of resource, technology, talent, policy and investment, with technological innovation as the core, to realize an all-round and integrated management and promote the development of coalbed methane industry at a high level.
基金supported by the C1 Gas Refinery Program through the National Research Foundation of Korea (NRF)funded by the Ministry of Science,ICT&Future Planning (NRF2017M3D3A1A01037001)supported by the Ministry of Trade,Industry and Energy (MOTIE),Korea Institute for Advancement of Technology (KIAT)through the Virtual Engineering Platform Program (P0022334)。
文摘The conversion of methane to olefins,aromatics,and hydrogen(MTOAH)can be used to stably obtain hydrocarbons when the effect of the catalytic surface is optimized from the reaction engineering perspective.In this study,Fe/Si C catalysts were packed into a quartz tube reactor.The catalytic surfaces of Si C and the impregnated Fe species decreased the apparent activation energies(E_a)of methane consumption in the blank reactor between 965 and 1020℃.Consequently,the hydrocarbon yield increased by 2.4times at 1020℃.Based on the model reactions of ethane,ethylene,and acetylene mixed with hydrogen in the range of 500-1020℃,an excess amount of Fe in the reactor favored the C-C coupling reaction over the selective hydrogenation of acetylene;consequently,coke formation was favored over the hydrogenation reaction.The gas-phase reactions and catalyst properties were optimized to increase hydrocarbon yields while reducing coke selectivity.The 0.2Fe catalyst-packed reactor(0.26 wt%Fe)resulted in a hydrocarbon yield of 7.1%and a coke selectivity of<2%when the ratio of the void space of the postcatalyst zone to the catalyst space was adjusted to be≥2.Based on these findings,the facile approach of decoupling the reaction zone between the catalyst surface and the gas-phase reaction can provide insights into catalytic reactor design,thereby facilitating the scale-up from the laboratory to the commercial scale.