Radiant syngas cooler(RSC)is widely used as a waste heat recovery equipment in industrial gasification.In this work,an RSC with radiation screens is established and the impact of gaseous radiative property models,gas ...Radiant syngas cooler(RSC)is widely used as a waste heat recovery equipment in industrial gasification.In this work,an RSC with radiation screens is established and the impact of gaseous radiative property models,gas components,and ash particles on heat transfer is investigated by the numerical simulation method.Considering the syngas components and the pressure environment of the RSC,a modified weighted-sum-of-gray-gases model was developed.The modified model shows high accuracy in validation.In computational fluid dynamics simulation,the calculated steam production is only 0.63%in error with the industrial data.Compared with Smith's model,the temperature decay along the axial direction calculated by the modified model is faster.Syngas components are of great significance to heat recovery capacity,especially when the absorbing gas fraction is less than 10%.After considering the influence of particles,the outlet temperature and the proportion of radiative heat transfer are less affected,but the difference in steam output reaches 2.7 t·h^(-1).The particle deposition on the wall greatly reduces the heat recovery performance of an RSC.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
Perovskite oxides has been attracted much attention as high-performance oxygen carriers for chemical looping reforming of methane,but they are easily inactivated by the presence of trace H_(2)S.Here,we propose to modu...Perovskite oxides has been attracted much attention as high-performance oxygen carriers for chemical looping reforming of methane,but they are easily inactivated by the presence of trace H_(2)S.Here,we propose to modulate both the activity and resistance to sulfur poisoning by dual substitution of Mo and Ni ions with the Fe-sites of LaFeO_(3)perovskite.It is found that partial substitution of Ni for Fe substantially improves the activity of LaFeO_(3)perovskite,while Ni particles prefer to grow and react with H_(2)S during the long-term successive redox process,resulting in the deactivation of oxygen carriers.With the presence of Mo in LaNi_(0.05)Fe_(0.95)O_(3−σ)perovskite,H_(2)S preferentially reacts with Mo to generate MoS_(2),and then the CO_(2)oxidation can regenerate Mo via removing sulfur.In addition,Mo can inhibit the accumulation and growth of Ni,which helps to improve the redox stability of oxygen carriers.The LaNi_(0.05)Mo_(0.07)Fe_(0.88)O_(3−σ)oxygen carrier exhibits stable and excellent performance,with the CH_(4)conversion higher than 90%during the 50 redox cycles in the presence of 50 ppm H_(2)S at 800℃.This work highlights a synergistic effect in the perovskite oxides induced by dual substitution of different cations for the development of high-performance oxygen carriers with excellent sulfur tolerance.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
The energy industry faces a significant challenge in extracting natural gas from offshore natural gas hydrate(NGH)reservoirs,primarily due to the low productivity of wells and the high operational costs involved.The p...The energy industry faces a significant challenge in extracting natural gas from offshore natural gas hydrate(NGH)reservoirs,primarily due to the low productivity of wells and the high operational costs involved.The present study offers an assessment of the feasibility of utilizing geothermal energy to augment the production of natural gas from offshore gas hydrate reservoirs through the implementation of the methane-CO_(2)swapping technique.The present study expands the research scope of the authors beyond their previous publication,which exclusively examined the generation of methane from marine gas hydrates.Specifically,the current investigation explores the feasibility of utilizing the void spaces created by the extracted methane in the hydrate reservoir for carbon dioxide storage.Analytical models were employed to forecast the heat transfer from a geothermal zone to an NGH reservoir.A study was conducted utilizing data obtained from a reservoir situated in the Shenhu region of the Northern South China Sea.The findings of the model indicate that the implementation of geothermal heating can lead to a substantial enhancement in the productivity of wells located in heated reservoirs during CO_(2)swapping procedures.The non-linear relationship between the temperature of the heated reservoir and the rate of fold increase has been observed.It is anticipated that the fold of increase will surpass 5 when the gas hydrate reservoir undergoes a temperature rise from 6℃ to 16℃.The mathematical models utilized in this study did not incorporate the impact of heat convection resulting from CO_(2)flow into the gas reservoir.This factor has the potential to enhance well productivity.The mathematical models’deviation assumptions may cause over-prediction of well productivity in geothermal-stimulated reservoirs.Additional research is required to examine the impacts of temperature drawdown,heat convection resulting from depressurization,heat-induced gas pressure increment,and the presence of free gas in the formation containing hydrates.The process of CH4-CO_(2)swapping,which has been investigated,involves the utilization of geothermal stimulation.This method is highly encouraging as it enables the efficient injection of CO_(2)into gas hydrate reservoirs,resulting in the permanent sequestration of CO_(2)in a solid state.Additional research is warranted to examine the rate of mass transfer of CO_(2)within reservoirs of gas hydrates.展开更多
基金supported by the National Natural Science Foundation of China(21878082).
文摘Radiant syngas cooler(RSC)is widely used as a waste heat recovery equipment in industrial gasification.In this work,an RSC with radiation screens is established and the impact of gaseous radiative property models,gas components,and ash particles on heat transfer is investigated by the numerical simulation method.Considering the syngas components and the pressure environment of the RSC,a modified weighted-sum-of-gray-gases model was developed.The modified model shows high accuracy in validation.In computational fluid dynamics simulation,the calculated steam production is only 0.63%in error with the industrial data.Compared with Smith's model,the temperature decay along the axial direction calculated by the modified model is faster.Syngas components are of great significance to heat recovery capacity,especially when the absorbing gas fraction is less than 10%.After considering the influence of particles,the outlet temperature and the proportion of radiative heat transfer are less affected,but the difference in steam output reaches 2.7 t·h^(-1).The particle deposition on the wall greatly reduces the heat recovery performance of an RSC.
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financially supported by the National Natural Science Foundation of China (Nos. 52174279, U2202251, and 52266008)Applied Basic Research Program of Yunnan Province for Distinguished Young Scholars (No. 202201AV070004)+1 种基金Central Guiding Local Science and Technology Development Fund (No. 202207AA110001)the Yunnan Fundamental Research Projects (No. 202301AU070027, 202401AT070388)
文摘Perovskite oxides has been attracted much attention as high-performance oxygen carriers for chemical looping reforming of methane,but they are easily inactivated by the presence of trace H_(2)S.Here,we propose to modulate both the activity and resistance to sulfur poisoning by dual substitution of Mo and Ni ions with the Fe-sites of LaFeO_(3)perovskite.It is found that partial substitution of Ni for Fe substantially improves the activity of LaFeO_(3)perovskite,while Ni particles prefer to grow and react with H_(2)S during the long-term successive redox process,resulting in the deactivation of oxygen carriers.With the presence of Mo in LaNi_(0.05)Fe_(0.95)O_(3−σ)perovskite,H_(2)S preferentially reacts with Mo to generate MoS_(2),and then the CO_(2)oxidation can regenerate Mo via removing sulfur.In addition,Mo can inhibit the accumulation and growth of Ni,which helps to improve the redox stability of oxygen carriers.The LaNi_(0.05)Mo_(0.07)Fe_(0.88)O_(3−σ)oxygen carrier exhibits stable and excellent performance,with the CH_(4)conversion higher than 90%during the 50 redox cycles in the presence of 50 ppm H_(2)S at 800℃.This work highlights a synergistic effect in the perovskite oxides induced by dual substitution of different cations for the development of high-performance oxygen carriers with excellent sulfur tolerance.
基金supported by the National Natural Science Foundation of China(No.22038011,No.22078257,No.22108213,No.52176142)the China Postdoctoral Science Foundation(2021M692548)+1 种基金the Joint Fund of the Yulin University and the Dalian National Laboratory for Clean Energy(Grant YLU-DNL Fund 2022001)the Young Talent Support Plan of Shaanxi Province。
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funding the project“Safe,Sustainable,and Resilient Development of Offshore Reservoirs and Natural Gas Upgrading through Innovative Science and Technology:Gulf of Mexico–Mediterranean,”through Contract No.EC-19 Fossil Energy。
文摘The energy industry faces a significant challenge in extracting natural gas from offshore natural gas hydrate(NGH)reservoirs,primarily due to the low productivity of wells and the high operational costs involved.The present study offers an assessment of the feasibility of utilizing geothermal energy to augment the production of natural gas from offshore gas hydrate reservoirs through the implementation of the methane-CO_(2)swapping technique.The present study expands the research scope of the authors beyond their previous publication,which exclusively examined the generation of methane from marine gas hydrates.Specifically,the current investigation explores the feasibility of utilizing the void spaces created by the extracted methane in the hydrate reservoir for carbon dioxide storage.Analytical models were employed to forecast the heat transfer from a geothermal zone to an NGH reservoir.A study was conducted utilizing data obtained from a reservoir situated in the Shenhu region of the Northern South China Sea.The findings of the model indicate that the implementation of geothermal heating can lead to a substantial enhancement in the productivity of wells located in heated reservoirs during CO_(2)swapping procedures.The non-linear relationship between the temperature of the heated reservoir and the rate of fold increase has been observed.It is anticipated that the fold of increase will surpass 5 when the gas hydrate reservoir undergoes a temperature rise from 6℃ to 16℃.The mathematical models utilized in this study did not incorporate the impact of heat convection resulting from CO_(2)flow into the gas reservoir.This factor has the potential to enhance well productivity.The mathematical models’deviation assumptions may cause over-prediction of well productivity in geothermal-stimulated reservoirs.Additional research is required to examine the impacts of temperature drawdown,heat convection resulting from depressurization,heat-induced gas pressure increment,and the presence of free gas in the formation containing hydrates.The process of CH4-CO_(2)swapping,which has been investigated,involves the utilization of geothermal stimulation.This method is highly encouraging as it enables the efficient injection of CO_(2)into gas hydrate reservoirs,resulting in the permanent sequestration of CO_(2)in a solid state.Additional research is warranted to examine the rate of mass transfer of CO_(2)within reservoirs of gas hydrates.
