水气分散体系驱油技术是针对低渗透油田采出程度低研发的新型提高采收率技术,目前已在长庆油田取得明显增油效果,但分散体系中微气泡与孔隙作用复杂,对其微观驱油机理的研究正逐步深入。根据低渗透、非均质岩心的特点,制作边长为1.5 cm...水气分散体系驱油技术是针对低渗透油田采出程度低研发的新型提高采收率技术,目前已在长庆油田取得明显增油效果,但分散体系中微气泡与孔隙作用复杂,对其微观驱油机理的研究正逐步深入。根据低渗透、非均质岩心的特点,制作边长为1.5 cm的玻璃刻蚀模型,在油藏温压条件下,进行CO_(2)-水分散体系渗流实验。通过观察微气泡与油、水、岩石相互作用过程,获取气泡吸附能力、推动油膜能力、气泡弹性能量等数据,进而定量表征分析驱油效果。实验结果表明:微气泡与油界面结合,具有特殊的吸附油膜现象,与水驱、气驱等作用机理显著不同。驱替过程相邻气泡间的合并也促进了油膜汇聚,同时微气泡的合并有助于气泡的流动,使吸附在气泡表面的油膜随气泡运移。微气泡运移时,气泡体积因压力降低而膨胀,所释放的弹性能量能够推动吸附在壁面的油膜运移。此外,采用Volume of Fluid多相流模型,对水气分散体系中微气泡推动油膜的运移过程进行模拟及分析,得到驱替油膜的主要因素是微气泡形变产生的弹性能量和微气泡自身的能量。气泡的能量作用在气泡前缘,通过与油膜表面接触产生推动作用。展开更多
文章模拟了CO_(2)与绿氢合成甲醇的过程,提出了CO_(2)储能密度指标,研究了多个参数对甲醇储能性能的影响。研究结果表明:系统能效和甲醇能量产率随着电解水效率、单程CO_(2)转化率、电解水压力和CO_(2)初始压力的升高而升高,随着甲醇合...文章模拟了CO_(2)与绿氢合成甲醇的过程,提出了CO_(2)储能密度指标,研究了多个参数对甲醇储能性能的影响。研究结果表明:系统能效和甲醇能量产率随着电解水效率、单程CO_(2)转化率、电解水压力和CO_(2)初始压力的升高而升高,随着甲醇合成压力的升高而降低;CO_(2)储能密度随以上参数的变化趋势与系统能效和甲醇能量产率相反;电解水效率和单程CO_(2)转化率是敏感关键的参数;在最优组合工况下,基于甲醇高位和低位热值的系统能效分别为68.0%和59.6%,CO_(2)储能密度为6.07 k W·h/kg,能量产率为0.108 kg/(k W·h),表明以CO_(2)为原料的电制甲醇的系统能效不够理想,但储能密度优势显著。展开更多
The excessive use of nonrenewable energy has brought about serious greenhouse effect.Converting CO_(2) into high-value-added chemicals is undoubtedly the best choice to solve energy problems.Due to the excellent cost-...The excessive use of nonrenewable energy has brought about serious greenhouse effect.Converting CO_(2) into high-value-added chemicals is undoubtedly the best choice to solve energy problems.Due to the excellent cost-effectiveness and dramatic catalytic performance,nickel-based catalysts have been considered as the most promising candidates for the electrocatalytic CO_(2) reduction reaction(eCO_(2)RR).In this work,the electrocatalytic reduction mechanism of CO_(2) over Ni-based materials is reviewed.The strategies to improve the eCO_(2)RR performance are emphasized.Moreover,the research on Ni-based materials for syngas generation is briefly summarized.Finally,the prospects of nickel-based materials in the eCO_(2)RR are provided with the hope of improving transition-metal-based electrocatalysts for eCO_(2)RR in the future.展开更多
Although the internal electric field(IEF)of photocatalysts is acknowledged as a potent driving force for photocharge separation,modulating the IEF intensity to achieve enhanced photocatalytic performances remains a ch...Although the internal electric field(IEF)of photocatalysts is acknowledged as a potent driving force for photocharge separation,modulating the IEF intensity to achieve enhanced photocatalytic performances remains a challenge.Herein,cuprous sulfide nanosheets with different Cu vacancy concentration were employed to study IEF modulation and corresponding direct charge transfer.Among the samples,Cu_(1.8)S nanosheets possessed intensified IEF intensity compared with those of Cu_(2)S and Cu_(1.95)S nanosheets,suggesting that an enhanced IEF intensity could be achieved by introducing more Cu vacancies.This intensified IEF of Cu_(1.8)S nanosheets induced numerous photogenerated electrons to migrate to its surface,and the dissociative electrons were then captured by Cu vacancies,resulting in efficient charge separation spatially.In addition,the Cu vacancies on Cu_(1.8)S nanosheets accumulated electrons as active sites to lower the energy barrier of rate-determining step of CO_(2)photoreduction,leading to the selective conversion of CO_(2)to CO.Herein,the manipulation of IEF intensity through Cu vacancy concentration regulation of cuprous sulfide photocatalysts for efficient charge separation has been discussed,providing a scientific strategy to rationally improve photocata lytic performances for solar energy conversion.展开更多
Electrochemical carbon dioxide reduction reaction(CO_(2)RR)involves a variety of intermediates with highly correlated reaction and ad-desorption energies,hindering optimization of the catalytic activity.For example,in...Electrochemical carbon dioxide reduction reaction(CO_(2)RR)involves a variety of intermediates with highly correlated reaction and ad-desorption energies,hindering optimization of the catalytic activity.For example,increasing the binding of the*COOH to the active site will generally increase the*CO desorption energy.Breaking this relationship may be expected to dramatically improve the intrinsic activity of CO_(2)RR,but remains an unsolved challenge.Herein,we addressed this conundrum by constructing a unique atomic dispersed hetero-pair consisting of Mo-Fe di-atoms anchored on N-doped carbon carrier.This system shows an unprecedented CO_(2)RR intrinsic activity with TOF of 3336 h−1,high selectivity toward CO production,Faradaic efficiency of 95.96%at−0.60 V and excellent stability.Theoretical calculations show that the Mo-Fe diatomic sites increased the*COOH intermediate adsorption energy by bridging adsorption of*COOH intermediates.At the same time,d-d orbital coupling in the Mo-Fe di-atom results in electron delocalization and facilitates desorption of*CO intermediates.Thus,the undesirable correlation between these steps is broken.This work provides a promising approach,specifically the use of di-atoms,for breaking unfavorable relationships based on understanding of the catalytic mechanisms at the atomic scale.展开更多
Subsurface geothermal energy storage has greater potential than other energy storage strategies in terms of capacity scale and time duration.Carbon dioxide(CO_(2))is regarded as a potential medium for energy storage d...Subsurface geothermal energy storage has greater potential than other energy storage strategies in terms of capacity scale and time duration.Carbon dioxide(CO_(2))is regarded as a potential medium for energy storage due to its superior thermal properties.Moreover,the use of CO_(2)plumes for geothermal energy storage mitigates the greenhouse effect by storing CO_(2)in geological bodies.In this work,an integrated framework is proposed for synergistic geothermal energy storage and CO_(2)sequestration and utilization.Within this framework,CO_(2)is first injected into geothermal layers for energy accumulation.The resultant high-energy CO_(2)is then introduced into a target oil reservoir for CO_(2)utilization and geothermal energy storage.As a result,CO_(2)is sequestrated in the geological oil reservoir body.The results show that,as high-energy CO_(2)is injected,the average temperature of the whole target reservoir is greatly increased.With the assistance of geothermal energy,the geological utilization efficiency of CO_(2)is higher,resulting in a 10.1%increase in oil displacement efficiency.According to a storage-potential assessment of the simulated CO_(2)site,110 years after the CO_(2)injection,the utilization efficiency of the geological body will be as high as 91.2%,and the final injection quantity of the CO_(2)in the site will be as high as 9.529×10^(8)t.After 1000 years sequestration,the supercritical phase dominates in CO_(2)sequestration,followed by the liquid phase and then the mineralized phase.In addition,CO_(2)sequestration accounting for dissolution trapping increases significantly due to the presence of residual oil.More importantly,CO_(2)exhibits excellent performance in storing geothermal energy on a large scale;for example,the total energy stored in the studied geological body can provide the yearly energy supply for over 3.5×10^(7) normal households.Application of this integrated approach holds great significance for large-scale geothermal energy storage and the achievement of carbon neutrality.展开更多
文摘水气分散体系驱油技术是针对低渗透油田采出程度低研发的新型提高采收率技术,目前已在长庆油田取得明显增油效果,但分散体系中微气泡与孔隙作用复杂,对其微观驱油机理的研究正逐步深入。根据低渗透、非均质岩心的特点,制作边长为1.5 cm的玻璃刻蚀模型,在油藏温压条件下,进行CO_(2)-水分散体系渗流实验。通过观察微气泡与油、水、岩石相互作用过程,获取气泡吸附能力、推动油膜能力、气泡弹性能量等数据,进而定量表征分析驱油效果。实验结果表明:微气泡与油界面结合,具有特殊的吸附油膜现象,与水驱、气驱等作用机理显著不同。驱替过程相邻气泡间的合并也促进了油膜汇聚,同时微气泡的合并有助于气泡的流动,使吸附在气泡表面的油膜随气泡运移。微气泡运移时,气泡体积因压力降低而膨胀,所释放的弹性能量能够推动吸附在壁面的油膜运移。此外,采用Volume of Fluid多相流模型,对水气分散体系中微气泡推动油膜的运移过程进行模拟及分析,得到驱替油膜的主要因素是微气泡形变产生的弹性能量和微气泡自身的能量。气泡的能量作用在气泡前缘,通过与油膜表面接触产生推动作用。
文摘文章模拟了CO_(2)与绿氢合成甲醇的过程,提出了CO_(2)储能密度指标,研究了多个参数对甲醇储能性能的影响。研究结果表明:系统能效和甲醇能量产率随着电解水效率、单程CO_(2)转化率、电解水压力和CO_(2)初始压力的升高而升高,随着甲醇合成压力的升高而降低;CO_(2)储能密度随以上参数的变化趋势与系统能效和甲醇能量产率相反;电解水效率和单程CO_(2)转化率是敏感关键的参数;在最优组合工况下,基于甲醇高位和低位热值的系统能效分别为68.0%和59.6%,CO_(2)储能密度为6.07 k W·h/kg,能量产率为0.108 kg/(k W·h),表明以CO_(2)为原料的电制甲醇的系统能效不够理想,但储能密度优势显著。
基金support from the National Natural Science Foundation of China(52072389,52311530113)the Science and Technology Commission of Shanghai Municipality(22DZ1205600,20520760900)+2 种基金the Program of Shanghai Academic Research Leader(20XD1424300)for financial support.The authors also would like to express their gratitude to Tangshan Basic Research Funding Projects(23130210E),Hebei Province High-level Talent(Postdoctor)Funding Project(B2022003025)Key R&D projects of North China University of Science and Technology(ZD-ST-202301)Tangshan Talent Funding Project(A202202007)for their financial support.
文摘The excessive use of nonrenewable energy has brought about serious greenhouse effect.Converting CO_(2) into high-value-added chemicals is undoubtedly the best choice to solve energy problems.Due to the excellent cost-effectiveness and dramatic catalytic performance,nickel-based catalysts have been considered as the most promising candidates for the electrocatalytic CO_(2) reduction reaction(eCO_(2)RR).In this work,the electrocatalytic reduction mechanism of CO_(2) over Ni-based materials is reviewed.The strategies to improve the eCO_(2)RR performance are emphasized.Moreover,the research on Ni-based materials for syngas generation is briefly summarized.Finally,the prospects of nickel-based materials in the eCO_(2)RR are provided with the hope of improving transition-metal-based electrocatalysts for eCO_(2)RR in the future.
基金supported by the National Natural Science Foundation of China(52200123)the Open Project of Key Laboratory of Green Chemical Engineering Process of Ministry of Education(GCP2022007)the Scientific Research and Innovation Team Program of Sichuan University of Science and Engineering(SUSE652A014)。
文摘Although the internal electric field(IEF)of photocatalysts is acknowledged as a potent driving force for photocharge separation,modulating the IEF intensity to achieve enhanced photocatalytic performances remains a challenge.Herein,cuprous sulfide nanosheets with different Cu vacancy concentration were employed to study IEF modulation and corresponding direct charge transfer.Among the samples,Cu_(1.8)S nanosheets possessed intensified IEF intensity compared with those of Cu_(2)S and Cu_(1.95)S nanosheets,suggesting that an enhanced IEF intensity could be achieved by introducing more Cu vacancies.This intensified IEF of Cu_(1.8)S nanosheets induced numerous photogenerated electrons to migrate to its surface,and the dissociative electrons were then captured by Cu vacancies,resulting in efficient charge separation spatially.In addition,the Cu vacancies on Cu_(1.8)S nanosheets accumulated electrons as active sites to lower the energy barrier of rate-determining step of CO_(2)photoreduction,leading to the selective conversion of CO_(2)to CO.Herein,the manipulation of IEF intensity through Cu vacancy concentration regulation of cuprous sulfide photocatalysts for efficient charge separation has been discussed,providing a scientific strategy to rationally improve photocata lytic performances for solar energy conversion.
基金the National Natural Science Foundation of China(22279044,12034002,and 22202080)the Project for Self-Innovation Capability Construction of Jilin Province Development and Reform Commission(2021C026)+1 种基金Jilin Province Science and Technology Development Program(20210301009GX)the Fundamental Research Funds for the Central Universities.
文摘Electrochemical carbon dioxide reduction reaction(CO_(2)RR)involves a variety of intermediates with highly correlated reaction and ad-desorption energies,hindering optimization of the catalytic activity.For example,increasing the binding of the*COOH to the active site will generally increase the*CO desorption energy.Breaking this relationship may be expected to dramatically improve the intrinsic activity of CO_(2)RR,but remains an unsolved challenge.Herein,we addressed this conundrum by constructing a unique atomic dispersed hetero-pair consisting of Mo-Fe di-atoms anchored on N-doped carbon carrier.This system shows an unprecedented CO_(2)RR intrinsic activity with TOF of 3336 h−1,high selectivity toward CO production,Faradaic efficiency of 95.96%at−0.60 V and excellent stability.Theoretical calculations show that the Mo-Fe diatomic sites increased the*COOH intermediate adsorption energy by bridging adsorption of*COOH intermediates.At the same time,d-d orbital coupling in the Mo-Fe di-atom results in electron delocalization and facilitates desorption of*CO intermediates.Thus,the undesirable correlation between these steps is broken.This work provides a promising approach,specifically the use of di-atoms,for breaking unfavorable relationships based on understanding of the catalytic mechanisms at the atomic scale.
基金supported by the National Key Research and Development Program of China under grant(2022YFE0206700)the financial support by the National Natural Science Foundation of China(52004320)the Science Foundation of China University of Petroleum,Beijing(2462021QNXZ012 and 2462021YJRC012)。
文摘Subsurface geothermal energy storage has greater potential than other energy storage strategies in terms of capacity scale and time duration.Carbon dioxide(CO_(2))is regarded as a potential medium for energy storage due to its superior thermal properties.Moreover,the use of CO_(2)plumes for geothermal energy storage mitigates the greenhouse effect by storing CO_(2)in geological bodies.In this work,an integrated framework is proposed for synergistic geothermal energy storage and CO_(2)sequestration and utilization.Within this framework,CO_(2)is first injected into geothermal layers for energy accumulation.The resultant high-energy CO_(2)is then introduced into a target oil reservoir for CO_(2)utilization and geothermal energy storage.As a result,CO_(2)is sequestrated in the geological oil reservoir body.The results show that,as high-energy CO_(2)is injected,the average temperature of the whole target reservoir is greatly increased.With the assistance of geothermal energy,the geological utilization efficiency of CO_(2)is higher,resulting in a 10.1%increase in oil displacement efficiency.According to a storage-potential assessment of the simulated CO_(2)site,110 years after the CO_(2)injection,the utilization efficiency of the geological body will be as high as 91.2%,and the final injection quantity of the CO_(2)in the site will be as high as 9.529×10^(8)t.After 1000 years sequestration,the supercritical phase dominates in CO_(2)sequestration,followed by the liquid phase and then the mineralized phase.In addition,CO_(2)sequestration accounting for dissolution trapping increases significantly due to the presence of residual oil.More importantly,CO_(2)exhibits excellent performance in storing geothermal energy on a large scale;for example,the total energy stored in the studied geological body can provide the yearly energy supply for over 3.5×10^(7) normal households.Application of this integrated approach holds great significance for large-scale geothermal energy storage and the achievement of carbon neutrality.
