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
Urban growth has promoted the use of underground spaces,where explosion accidents can be catastrophic.In this study,we investigated the effect of placing flexible construction in front of rigid obstacles on methane ex...Urban growth has promoted the use of underground spaces,where explosion accidents can be catastrophic.In this study,we investigated the effect of placing flexible construction in front of rigid obstacles on methane explosion protection by using an experimental platform and adjusting the blockage rate and spacing of the obstacles.It aims to reduce the risk of gas explosions in urban underground spaces.The results of the study show that the flame propagation peak speed and peak overpressure are reduced with the decrease in the blocking rate of the flexible obstacle when the blocking rate of the flexible obstacle is less than or equal to the blocking rate of the rigid obstacle,with the decrease in the spacing,the better the protection effect of the methane explosion.When the blockage rate of the flexible obstacle is greater than the blockage rate of the rigid obstacle and spacing is less than the height of the flexible obstacle,rigid and flexible obstacles are connected as a whole,increasing the strength of the explosion.This study can provide a theoretical basis and scientific guidance for optimizing rigid and flexible object hybrid layouts and methane explosion protection technology in urban underground spaces.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
Different mesoporous activated carbons were prepared by both chemical and physical activation processes and were examined for methane uptake in the presence of water.Methane isotherms were obtained at wet condition by...Different mesoporous activated carbons were prepared by both chemical and physical activation processes and were examined for methane uptake in the presence of water.Methane isotherms were obtained at wet condition by wetting samples with water at mass ratio of water/carbon(R) close to 1.0.To compare,the amount of methane storage were also measured at dry situation.The maximum amount of methane stored was attained as 237 V/V at R=1.0 by hydrate formation at the methane critical pressure.In the next step,mass ratios of water/carbon were changed to investigate various amount of water for methane storage enhancement.Two other values of mass ratio of water/carbon(R=0.8 and 1.4) were selected and methane isotherms were obtained at the same conditions.Maximum values of 210 and 248 V/V were reached for methane storage,respectively.It was also observed that,in the pressure range lower than hydrate pressure,by increasing water ratio the hydrate formation pressure was decreased and methane uptake was much less than that of dry condition due to pore filling by water.展开更多
Three experiments of static state storage method, low-temperature and constant-pressure storage method and low-temperature and constant-pressure storage method were carried out to investigate which method was best in ...Three experiments of static state storage method, low-temperature and constant-pressure storage method and low-temperature and constant-pressure storage method were carried out to investigate which method was best in gas hydrate. The relationships of hydrate rate, capacity and liquid temperature versus time were derived and three results were contrasted. The experimental results show lowtemperature and constant-pressure method is better than the other two methods because it's operation period is shorter and storage capacity is larger than the other two. Low-temperature and constant-pressure method is the best method. So new method will be new research objective.展开更多
Methane decomposition into hydrogen and carbon nanomaterials(CNMs)was carded out over Ni/ZSM-5 catalysts with different Ni contents at different temperatures.The yields of hydrogen and the CNMs increase significantly ...Methane decomposition into hydrogen and carbon nanomaterials(CNMs)was carded out over Ni/ZSM-5 catalysts with different Ni contents at different temperatures.The yields of hydrogen and the CNMs increase significantly with Ni content and reaction temperature,but they level off at high temperatures when the Ni content is over 8 wt.%.The morphology of the CNMs strongly depended on the temperature.Multiwall carbon nanotubes were formed at higher temperature,while carbon nanofibers formed at the lower temperature.The catalytic activity of the Ni/ZSM-5 decreased with time.展开更多
Caprocks play an important role in the trapping of coalbed methane(CBM)reservoirs.To study the sealing capacities of caprocks,five samples with different lithologies of Neogene clayrock,Paleogene redbeds,Permian sands...Caprocks play an important role in the trapping of coalbed methane(CBM)reservoirs.To study the sealing capacities of caprocks,five samples with different lithologies of Neogene clayrock,Paleogene redbeds,Permian sandstone,Permian mudstone and Permian siltstone were collected and tested using experimental methods of microstructure observation,pore structure measurement and diffusion properties determination.Results indicate that with denser structures,lower porosities,much more developed micropores/transition pores and higher pore/throat ratios,mudstone and siltstone have the more ideal sealing capacities for CBM preservation when comparing to other kinds of caprocks;the methane diffusion coefficients of mudstone/siltstone are about 6 times higher than sandstone and almost 90 times higher than clayrock/redbeds.To further estimate the CBM escape through caprocks,a one-dimensional CBM diffusion model is derived.Modeling calculation result demonstrates that under the same thickness,the CBM sealing abilities of mudstone/siltstone are almost 100 times higher than those of clayrock/redbeds,and nearly 17 times higher than sandstone,which indicates that the coal seam below caprocks like clayrock,redbeds or sandstone may suffer stronger CBM diffusion effect than that below mudstone or siltstone.Such conclusion is verified by the case study from III3 District,Xutuan Colliery,where the coal seam capped by Paleogene redbeds has a much lower CBM content than that capped by the Permian strata like mudstone,siltstone and sandstone.展开更多
The main objective of this paper was to characterize the voltammetric profiles of the Pt/C,Pt/C-ATO,Pd/C and Pd/CATO electrocatalysts and study their catalytic activities for methane oxidation in an acidic electrolyte...The main objective of this paper was to characterize the voltammetric profiles of the Pt/C,Pt/C-ATO,Pd/C and Pd/CATO electrocatalysts and study their catalytic activities for methane oxidation in an acidic electrolyte at 25 ℃ and in a direct methane proton exchange membrane fuel cell at 80 ℃. The electrocatalysts prepared also were characterized by X-ray diffraction( XRD) and transmission electron microscopy( TEM). The diffractograms of the Pt/C and Pt/C-ATO electrocatalysts show four peaks associated with Pt face-centered cubic( fcc) structure,and the diffractograms of Pd/C and Pd/C-ATO show four peaks associated with Pd face-centered cubic( fcc) structure. For Pt/C-ATO and Pd/C-ATO,characteristic peaks of cassiterite( SnO_2) phase are observed,which are associated with Sb-doped SnO_2( ATO) used as supports for electrocatalysts. Cyclic voltammograms( CV) of all electrocatalysts after adsorption of methane show that there is a current increase during the anodic scan. However,this effect is more pronounced for Pt/C-ATO and Pd/C-ATO. This process is related to the oxidation of the adsorbed species through the bifunctional mechanism,where ATO provides oxygenated species for the oxidation of CO or HCO intermediates adsorbed in Pt or Pd sites. From in situ ATR-FTIR( Attenuated Total Reflectance-Fourier Transform Infrared) experiments for all electrocatalysts prepared the formation of HCO or CO intermediates are observed,which indicates the production of carbon dioxide. Polarization curves at 80 ℃in a direct methane fuel cell( DMEFC) show that Pd/C and Pt/C electroacatalysts have superior performance to Pd/C-ATO and Pt/C-ATO in methane oxidation.展开更多
Thermal shocking effect occurs when the coalbed methane(CBM)reservoirs meet liquid nitrogen(LN2)of extremely low temperature.In this study,3D via X-ray microcomputer tomography(μCT)and scanning electron microscope(SE...Thermal shocking effect occurs when the coalbed methane(CBM)reservoirs meet liquid nitrogen(LN2)of extremely low temperature.In this study,3D via X-ray microcomputer tomography(μCT)and scanning electron microscope(SEM)are employed to visualize and quantify morphological evolution characteristics of fractures in coal after LN2 thermal shocking treatments.LN2 thermal shocking leads to a denser fracture network than its original state with coal porosity growth rate increasing up to 183.3%.The surface porosity of theμCT scanned layers inside the coal specimen is influenced by LN2 thermal shocking which rises from 18.76%to 215.11%,illustrating the deformation heterogeneity of coal after LN2 thermal shocking.The cracking effect of LN2 thermal shocking on the surface of low porosity is generally more effective than that of high surface porosity,indicating the applicability of LN2 thermal shocking on low-permeability CBM reservoir stimulation.The characteristics of SEM scanned coal matrix in the coal powder and the coal block after the LN2 thermal shocking presented a large amount of deep and shallow progressive scratch layers,fracture variation diversity(i.e.extension,propagation,connectivity,irregularity)on the surface of the coal block and these were the main reasons leading to the decrease of the uniaxial compressive strength of the coal specimen.展开更多
Diamond films were deposited on high-speed steel substrates by hot filament chemical vapor deposition （HFCVD） method. To minimize the early formation of graphite and to enhance the diamond film adhesion, a WC-Co coa...Diamond films were deposited on high-speed steel substrates by hot filament chemical vapor deposition （HFCVD） method. To minimize the early formation of graphite and to enhance the diamond film adhesion, a WC-Co coating was used as an interlayer on the steel substrates by high velocity oxy-fuel spraying. The effects of methane content on nucleation, quality, residual stress and adhesion of diamond films were investigated. The results indicate that the increasing methane content leads to the increase in nucleation density, residual stress, the degradation of quality and adhesion of diamond films. Diamond films deposited on high-speed steel （HSS） substrate with a WC-Co interlayer exhibit high nucleation density and good adhesion under the condition of the methane content initially set to be a higher value （4%, volume fraction） for 30 min, and then reduced to 2% for subsequent growth at pressure of 3 kPa and substrate temperature of 800 ℃.展开更多
The easy acidification and high hydrogen sulfide （H2S） production during anaerobic digestion of macroalgae limited its application in biomethane production. In order to investigate the effects of ceramsite on methan...The easy acidification and high hydrogen sulfide （H2S） production during anaerobic digestion of macroalgae limited its application in biomethane production. In order to investigate the effects of ceramsite on methane and HzS productions during anaerobic digestion of macroalgae, batch experiments ofMacrocystis pyrifera were carried out. Four groups named C0, C1, C2 and C3 added with 0, 1.5, 3.0 and 4.5 g/g substrate of ceramsite, respectively, were studied and compared. The highest cumulative methane yield of 286.3 mL/g substrate is obtained in C2, which is 40.11% higher than that of CO. The cumulative HzS yields of C1, C2 and C3 are 32.67%, 44.66% and 53.21% lower than that of CO, respectively. Results indicate that ceramsite addition permits higher methane yields, shorter lag-phase time and lower HzS yields during anaerobic digestion of Macrocystispyrifera.展开更多
The reaction of CO2 reforming of CH4 has been investigated with y-A1203-supported platinum and ruthenium bimetallic catalysts, with the specific purpose of thermochemical energy storage. The catalysts were prepared by...The reaction of CO2 reforming of CH4 has been investigated with y-A1203-supported platinum and ruthenium bimetallic catalysts, with the specific purpose of thermochemical energy storage. The catalysts were prepared by using the wetness impregnation method. The prepared catalysts were characterized by a series of physico-chemical characterization techniques such as BET surface area, thermo-gravimetric （TG）, transmission electron microscope （TEM） and X-ray photoelectron spectroscopy （XPS）. In addition, the amount of carbon deposits on the surface of the catalysts and the type of the carbonaceous species were discussed by TG. It was found that the bimetallic Pt-Ru/7-A1203 catalysts exhibit both superior catalytic activity and remarkable stability by comparison of monometallic catalysts. During the 500 h stability test, the bimetallic catalyst showed a good performance at 800 ~C in CO2 reforming of CH4, exhibiting an excellent anti-carbon performance with the mass loss of less than 8.5%. The results also indicate that CO2 and CH4 have quite stable conversions of 96.0 % and 94.0 %, respectively. Also, the selectivity of the catalysts is excellent with the products ratio of CO/H2 maintaining at 1.02. Furthermore, it was found in TEM images that the active carbonaceous species were formed during the catalytic reaction, and well-distributed dot-shaped metallic particles with a relatively uniform size of about 3 nm as well as amorphous carbon structures were observed. Combined with BET, TG, TEM tests, it is concluded that the selected bimetallic catalysts can work continuously in a stable state at the high temperature, which has a potential to be utilized for the closed-loop cycle of the solar thermochemical energy storage in future industry applications.展开更多
Recently,methane of possible abiogenic origin has been reported from many localities within the Earth’s crust.However,little is known about the mechanisms of abiogenic methane formation during such processes.The Fisc...Recently,methane of possible abiogenic origin has been reported from many localities within the Earth’s crust.However,little is known about the mechanisms of abiogenic methane formation during such processes.The Fischer-Tropsch reaction as a well known process for converting CO<sub>2</sub> to hydrocarbon gas by reaction with H<sub>2</sub> may take place on a metallic iron or iron oxide catalyst and also may take place on展开更多
Coalbed methane enrichment will be controlled by many good macro geological dynamical conditions; there is evident difference of enrichment grade in different area and different geological conditions.This paper has st...Coalbed methane enrichment will be controlled by many good macro geological dynamical conditions; there is evident difference of enrichment grade in different area and different geological conditions.This paper has studied tectonic dynamical conditions, thermal dynamical conditions and hydraulic conditions, which affect coalbed methane enrichment in Qinshui basin.Coalbed methane enrichment units have been divided based on tectonic dynamical conditions of Qinshui basin,combined with thermal dynamical conditions and hydraulic conditions.展开更多
Highly active and stable nickel catalyst for dehydrogenation of methane and hydrogenation of benzene is prepared from a precursor with hydrotalcite-like anionic clam structure by coprecipitation. The nickel particles ...Highly active and stable nickel catalyst for dehydrogenation of methane and hydrogenation of benzene is prepared from a precursor with hydrotalcite-like anionic clam structure by coprecipitation. The nickel particles have a narrow size distribution in several nanometers, and have a strong interaction with other components such as Al2O3. This catalyst is highly sensitive to further modification by doping and to reaction condition. On a modified catalyst, benzene hydrogenation to cyclohexane proceeds to complete at 373 K. While on another catalyst, different structured nanocarbons are obtained at moderate temperatures. It is found that the thioresistance of the nickel catalyst in hydrogenation can be improved by doping.展开更多
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(Grant No.52274177)Science and Technology Research Program of Chongqing Municipal Education Commission(Grant No.KJZD-K202401501)+1 种基金Chongqing Graduate Student Research Innovation Program(Grant No.CYS240800)The Science and Technology Innovation Project for Graduate Students of Chongqing University of Science and Technology(Grant No.YKJCX2420702).
文摘Urban growth has promoted the use of underground spaces,where explosion accidents can be catastrophic.In this study,we investigated the effect of placing flexible construction in front of rigid obstacles on methane explosion protection by using an experimental platform and adjusting the blockage rate and spacing of the obstacles.It aims to reduce the risk of gas explosions in urban underground spaces.The results of the study show that the flame propagation peak speed and peak overpressure are reduced with the decrease in the blocking rate of the flexible obstacle when the blocking rate of the flexible obstacle is less than or equal to the blocking rate of the rigid obstacle,with the decrease in the spacing,the better the protection effect of the methane explosion.When the blockage rate of the flexible obstacle is greater than the blockage rate of the rigid obstacle and spacing is less than the height of the flexible obstacle,rigid and flexible obstacles are connected as a whole,increasing the strength of the explosion.This study can provide a theoretical basis and scientific guidance for optimizing rigid and flexible object hybrid layouts and methane explosion protection technology in urban underground spaces.
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Shahid Hashemi Nejad Gas refinery for supporting this project
文摘Different mesoporous activated carbons were prepared by both chemical and physical activation processes and were examined for methane uptake in the presence of water.Methane isotherms were obtained at wet condition by wetting samples with water at mass ratio of water/carbon(R) close to 1.0.To compare,the amount of methane storage were also measured at dry situation.The maximum amount of methane stored was attained as 237 V/V at R=1.0 by hydrate formation at the methane critical pressure.In the next step,mass ratios of water/carbon were changed to investigate various amount of water for methane storage enhancement.Two other values of mass ratio of water/carbon(R=0.8 and 1.4) were selected and methane isotherms were obtained at the same conditions.Maximum values of 210 and 248 V/V were reached for methane storage,respectively.It was also observed that,in the pressure range lower than hydrate pressure,by increasing water ratio the hydrate formation pressure was decreased and methane uptake was much less than that of dry condition due to pore filling by water.
基金supported by the National Natural Science Foundation of China(No.50176051)the State Key Development Program for Basic Research of China(No.2000026306).
文摘Three experiments of static state storage method, low-temperature and constant-pressure storage method and low-temperature and constant-pressure storage method were carried out to investigate which method was best in gas hydrate. The relationships of hydrate rate, capacity and liquid temperature versus time were derived and three results were contrasted. The experimental results show lowtemperature and constant-pressure method is better than the other two methods because it's operation period is shorter and storage capacity is larger than the other two. Low-temperature and constant-pressure method is the best method. So new method will be new research objective.
基金financed by the National Science Centre(Nr N N507306240)
文摘Methane decomposition into hydrogen and carbon nanomaterials(CNMs)was carded out over Ni/ZSM-5 catalysts with different Ni contents at different temperatures.The yields of hydrogen and the CNMs increase significantly with Ni content and reaction temperature,but they level off at high temperatures when the Ni content is over 8 wt.%.The morphology of the CNMs strongly depended on the temperature.Multiwall carbon nanotubes were formed at higher temperature,while carbon nanofibers formed at the lower temperature.The catalytic activity of the Ni/ZSM-5 decreased with time.
基金Project(2016YFC0801608) supported by the National Key Research and Development Plan,ChinaProject(51574148) supported by the National Natural Science Foundation of China
文摘Caprocks play an important role in the trapping of coalbed methane(CBM)reservoirs.To study the sealing capacities of caprocks,five samples with different lithologies of Neogene clayrock,Paleogene redbeds,Permian sandstone,Permian mudstone and Permian siltstone were collected and tested using experimental methods of microstructure observation,pore structure measurement and diffusion properties determination.Results indicate that with denser structures,lower porosities,much more developed micropores/transition pores and higher pore/throat ratios,mudstone and siltstone have the more ideal sealing capacities for CBM preservation when comparing to other kinds of caprocks;the methane diffusion coefficients of mudstone/siltstone are about 6 times higher than sandstone and almost 90 times higher than clayrock/redbeds.To further estimate the CBM escape through caprocks,a one-dimensional CBM diffusion model is derived.Modeling calculation result demonstrates that under the same thickness,the CBM sealing abilities of mudstone/siltstone are almost 100 times higher than those of clayrock/redbeds,and nearly 17 times higher than sandstone,which indicates that the coal seam below caprocks like clayrock,redbeds or sandstone may suffer stronger CBM diffusion effect than that below mudstone or siltstone.Such conclusion is verified by the case study from III3 District,Xutuan Colliery,where the coal seam capped by Paleogene redbeds has a much lower CBM content than that capped by the Permian strata like mudstone,siltstone and sandstone.
基金The project was supported by the FAPESP(2014/09087-4,2014/50279-4).
文摘The main objective of this paper was to characterize the voltammetric profiles of the Pt/C,Pt/C-ATO,Pd/C and Pd/CATO electrocatalysts and study their catalytic activities for methane oxidation in an acidic electrolyte at 25 ℃ and in a direct methane proton exchange membrane fuel cell at 80 ℃. The electrocatalysts prepared also were characterized by X-ray diffraction( XRD) and transmission electron microscopy( TEM). The diffractograms of the Pt/C and Pt/C-ATO electrocatalysts show four peaks associated with Pt face-centered cubic( fcc) structure,and the diffractograms of Pd/C and Pd/C-ATO show four peaks associated with Pd face-centered cubic( fcc) structure. For Pt/C-ATO and Pd/C-ATO,characteristic peaks of cassiterite( SnO_2) phase are observed,which are associated with Sb-doped SnO_2( ATO) used as supports for electrocatalysts. Cyclic voltammograms( CV) of all electrocatalysts after adsorption of methane show that there is a current increase during the anodic scan. However,this effect is more pronounced for Pt/C-ATO and Pd/C-ATO. This process is related to the oxidation of the adsorbed species through the bifunctional mechanism,where ATO provides oxygenated species for the oxidation of CO or HCO intermediates adsorbed in Pt or Pd sites. From in situ ATR-FTIR( Attenuated Total Reflectance-Fourier Transform Infrared) experiments for all electrocatalysts prepared the formation of HCO or CO intermediates are observed,which indicates the production of carbon dioxide. Polarization curves at 80 ℃in a direct methane fuel cell( DMEFC) show that Pd/C and Pt/C electroacatalysts have superior performance to Pd/C-ATO and Pt/C-ATO in methane oxidation.
基金Project(2017XKQY012)supported by the Fundamental Research Funds for the Central Universities,China。
文摘Thermal shocking effect occurs when the coalbed methane(CBM)reservoirs meet liquid nitrogen(LN2)of extremely low temperature.In this study,3D via X-ray microcomputer tomography(μCT)and scanning electron microscope(SEM)are employed to visualize and quantify morphological evolution characteristics of fractures in coal after LN2 thermal shocking treatments.LN2 thermal shocking leads to a denser fracture network than its original state with coal porosity growth rate increasing up to 183.3%.The surface porosity of theμCT scanned layers inside the coal specimen is influenced by LN2 thermal shocking which rises from 18.76%to 215.11%,illustrating the deformation heterogeneity of coal after LN2 thermal shocking.The cracking effect of LN2 thermal shocking on the surface of low porosity is generally more effective than that of high surface porosity,indicating the applicability of LN2 thermal shocking on low-permeability CBM reservoir stimulation.The characteristics of SEM scanned coal matrix in the coal powder and the coal block after the LN2 thermal shocking presented a large amount of deep and shallow progressive scratch layers,fracture variation diversity(i.e.extension,propagation,connectivity,irregularity)on the surface of the coal block and these were the main reasons leading to the decrease of the uniaxial compressive strength of the coal specimen.
基金Project(1343-74236000005) supported by the Innovation Foundation for Postgraduates of Hunan Province, ChinaProject(ZKJ2008001) supported by the Open Fund for Valuable Instruments of Central South University, ChinaProject(2008112048) supported by the Open Fund of State Key Laboratory of Metallurgy, China
文摘Diamond films were deposited on high-speed steel substrates by hot filament chemical vapor deposition （HFCVD） method. To minimize the early formation of graphite and to enhance the diamond film adhesion, a WC-Co coating was used as an interlayer on the steel substrates by high velocity oxy-fuel spraying. The effects of methane content on nucleation, quality, residual stress and adhesion of diamond films were investigated. The results indicate that the increasing methane content leads to the increase in nucleation density, residual stress, the degradation of quality and adhesion of diamond films. Diamond films deposited on high-speed steel （HSS） substrate with a WC-Co interlayer exhibit high nucleation density and good adhesion under the condition of the methane content initially set to be a higher value （4%, volume fraction） for 30 min, and then reduced to 2% for subsequent growth at pressure of 3 kPa and substrate temperature of 800 ℃.
基金Project(2014BAC31B01)supported by the National Science&Technology Support during the 12th Five-Year Plan Period,ChinaProjects(2015GSF117016,2015GSF115037)supported by the Key Research&Development Project of Shandong Province,China
文摘The easy acidification and high hydrogen sulfide （H2S） production during anaerobic digestion of macroalgae limited its application in biomethane production. In order to investigate the effects of ceramsite on methane and HzS productions during anaerobic digestion of macroalgae, batch experiments ofMacrocystis pyrifera were carried out. Four groups named C0, C1, C2 and C3 added with 0, 1.5, 3.0 and 4.5 g/g substrate of ceramsite, respectively, were studied and compared. The highest cumulative methane yield of 286.3 mL/g substrate is obtained in C2, which is 40.11% higher than that of CO. The cumulative HzS yields of C1, C2 and C3 are 32.67%, 44.66% and 53.21% lower than that of CO, respectively. Results indicate that ceramsite addition permits higher methane yields, shorter lag-phase time and lower HzS yields during anaerobic digestion of Macrocystispyrifera.
基金Project(2010CB227103) supported by the National Basic Research Program of ChinaProjects(50930007,50836005) supported by the Key Program of the National Natural Science Foundation of ChinaProject(U1034005) supported by the National Natural Science Foundation of China
文摘The reaction of CO2 reforming of CH4 has been investigated with y-A1203-supported platinum and ruthenium bimetallic catalysts, with the specific purpose of thermochemical energy storage. The catalysts were prepared by using the wetness impregnation method. The prepared catalysts were characterized by a series of physico-chemical characterization techniques such as BET surface area, thermo-gravimetric （TG）, transmission electron microscope （TEM） and X-ray photoelectron spectroscopy （XPS）. In addition, the amount of carbon deposits on the surface of the catalysts and the type of the carbonaceous species were discussed by TG. It was found that the bimetallic Pt-Ru/7-A1203 catalysts exhibit both superior catalytic activity and remarkable stability by comparison of monometallic catalysts. During the 500 h stability test, the bimetallic catalyst showed a good performance at 800 ~C in CO2 reforming of CH4, exhibiting an excellent anti-carbon performance with the mass loss of less than 8.5%. The results also indicate that CO2 and CH4 have quite stable conversions of 96.0 % and 94.0 %, respectively. Also, the selectivity of the catalysts is excellent with the products ratio of CO/H2 maintaining at 1.02. Furthermore, it was found in TEM images that the active carbonaceous species were formed during the catalytic reaction, and well-distributed dot-shaped metallic particles with a relatively uniform size of about 3 nm as well as amorphous carbon structures were observed. Combined with BET, TG, TEM tests, it is concluded that the selected bimetallic catalysts can work continuously in a stable state at the high temperature, which has a potential to be utilized for the closed-loop cycle of the solar thermochemical energy storage in future industry applications.
文摘Recently,methane of possible abiogenic origin has been reported from many localities within the Earth’s crust.However,little is known about the mechanisms of abiogenic methane formation during such processes.The Fischer-Tropsch reaction as a well known process for converting CO<sub>2</sub> to hydrocarbon gas by reaction with H<sub>2</sub> may take place on a metallic iron or iron oxide catalyst and also may take place on
文摘Coalbed methane enrichment will be controlled by many good macro geological dynamical conditions; there is evident difference of enrichment grade in different area and different geological conditions.This paper has studied tectonic dynamical conditions, thermal dynamical conditions and hydraulic conditions, which affect coalbed methane enrichment in Qinshui basin.Coalbed methane enrichment units have been divided based on tectonic dynamical conditions of Qinshui basin,combined with thermal dynamical conditions and hydraulic conditions.
基金Supported by the National Natural Science Foundation of China(No. 29792070-9, 29876032).
文摘Highly active and stable nickel catalyst for dehydrogenation of methane and hydrogenation of benzene is prepared from a precursor with hydrotalcite-like anionic clam structure by coprecipitation. The nickel particles have a narrow size distribution in several nanometers, and have a strong interaction with other components such as Al2O3. This catalyst is highly sensitive to further modification by doping and to reaction condition. On a modified catalyst, benzene hydrogenation to cyclohexane proceeds to complete at 373 K. While on another catalyst, different structured nanocarbons are obtained at moderate temperatures. It is found that the thioresistance of the nickel catalyst in hydrogenation can be improved by doping.
