We report a novel double-shelled nanoboxes photocatalyst architecture with tailored interfaces that accelerate quantum efficiency for photocatalytic CO_(2) reduction reaction(CO_(2)RR)via Mo–S bridging bonds sites in...We report a novel double-shelled nanoboxes photocatalyst architecture with tailored interfaces that accelerate quantum efficiency for photocatalytic CO_(2) reduction reaction(CO_(2)RR)via Mo–S bridging bonds sites in S_(v)–In_(2)S_(3)@2H–MoTe_(2).The X-ray absorption near-edge structure shows that the formation of S_(v)–In_(2)S_(3)@2H–MoTe_(2) adjusts the coordination environment via interface engineering and forms Mo–S polarized sites at the interface.The interfacial dynamics and catalytic behavior are clearly revealed by ultrafast femtosecond transient absorption,time-resolved,and in situ diffuse reflectance–Infrared Fourier transform spectroscopy.A tunable electronic structure through steric interaction of Mo–S bridging bonds induces a 1.7-fold enhancement in S_(v)–In_(2)S_(3)@2H–MoTe_(2)(5)photogenerated carrier concentration relative to pristine S_(v)–In_(2)S_(3).Benefiting from lower carrier transport activation energy,an internal quantum efficiency of 94.01%at 380 nm was used for photocatalytic CO_(2)RR.This study proposes a new strategy to design photocatalyst through bridging sites to adjust the selectivity of photocatalytic CO_(2)RR.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
Precipitation or dissolution due to geochemical reactions has been observed in the caprocks for CO_(2) geosequestration.Geochemical reactions modify the caprock sealing efficiency with self-limiting or self-enhancemen...Precipitation or dissolution due to geochemical reactions has been observed in the caprocks for CO_(2) geosequestration.Geochemical reactions modify the caprock sealing efficiency with self-limiting or self-enhancement.However,the effect of this modification on the caprock sealing efficiency has not been fully investigated through multiphysical-geochemical coupling analysis.In this study,a multiphysical-geochemical coupling model was proposed to analyze caprock sealing efficiency.This coupling model considered the full couplings of caprock deformation,two-phase flow,CO_(2) concentration diffusion,geochemical reaction,and CO_(2) sorption.The two-phase flow only occurs in the fracture network and the CO_(2) may partially dissolve into water and diffuse through the concentration difference.The dissolved CO_(2) has geochemical reactions with some critical minerals,thus altering flow channels.The CO_(2) in the fracture network diffuses into matrix,causing the matrix swelling.This fully coupling model was validated with a penetration experiment on a cement cube and compared with two other models for CO_(2) storage plumes.Finally,the effects of geochemical reactions on penetration depth and pore pressure were studied through parametric study.The numerical simulations reveal that the coupling of geochemical reactions and matrix diffusion significantly affect the caprock sealing efficiency.Geochemical reactions occur at a short time after the arrival of CO_(2) concentration and modify the fracture porosity.The CO_(2) diffusion into the matrix requires a much longer time and mainly induces matrix swelling.These effects may produce selfenhancement or self-limiting depending on the flow rate in the fracture network,thus significantly modifying caprock sealing efficiency.展开更多
This paper brings the comparison of performances of CO_(2)conversion by plasma and plasma-assisted catalysis based on the data collected from literature in this field,organised in an open access online database.This t...This paper brings the comparison of performances of CO_(2)conversion by plasma and plasma-assisted catalysis based on the data collected from literature in this field,organised in an open access online database.This tool is open to all users to carry out their own analyses,but also to contributors who wish to add their data to the database in order to improve the relevance of the comparisons made,and ultimately to improve the efficiency of CO_(2)conversion by plasma-catalysis.The creation of this database and database user interface is motivated by the fact that plasma-catalysis is a fast-growing field for all CO_(2)conversion processes,be it methanation,dry reforming of methane,methanolisation,or others.As a result of this rapid increase,there is a need for a set of standard procedures to rigorously compare performances of different systems.However,this is currently not possible because the fundamental mechanisms of plasma-catalysis are still too poorly understood to define these standard procedures.Fortunately however,the accumulated data within the CO_(2)plasma-catalysis community has become large enough to warrant so-called“big data”studies more familiar in the fields of medicine and the social sciences.To enable comparisons between multiple data sets and make future research more effective,this work proposes the first database on CO_(2)conversion performances by plasma-catalysis open to the whole community.This database has been initiated in the framework of a H_(2)0_(2)0 European project and is called the“PIONEER Data Base”.The database gathers a large amount of CO_(2)conversion performance data such as conversion rate,energy efficiency,and selectivity for numerous plasma sources coupled with or without a catalyst.Each data set is associated with metadata describing the gas mixture,the plasma source,the nature of the catalyst,and the form of coupling with the plasma.Beyond the database itself,a data extraction tool with direct visualisation features or advanced filtering functionalities has been developed and is available online to the public.The simple and fast visualisation of the state of the art puts new results into context,identifies literal gaps in data,and consequently points towards promising research routes.More advanced data extraction illustrates the impact that the database can have in the understanding of plasma-catalyst coupling.Lessons learned from the review of a large amount of literature during the setup of the database lead to best practice advice to increase comparability between future CO_(2)plasma-catalytic studies.Finally,the community is strongly encouraged to contribute to the database not only to increase the visibility of their data but also the relevance of the comparisons allowed by this tool.展开更多
基金the Natural Science Foundation of China(11922415,12274471)Guangdong Basic and Applied Basic Research Foundation(2022A1515011168,2019A1515011718,2019A1515011337)the Key Research and Development Program of Guangdong Province,China(2019B110209003).
文摘We report a novel double-shelled nanoboxes photocatalyst architecture with tailored interfaces that accelerate quantum efficiency for photocatalytic CO_(2) reduction reaction(CO_(2)RR)via Mo–S bridging bonds sites in S_(v)–In_(2)S_(3)@2H–MoTe_(2).The X-ray absorption near-edge structure shows that the formation of S_(v)–In_(2)S_(3)@2H–MoTe_(2) adjusts the coordination environment via interface engineering and forms Mo–S polarized sites at the interface.The interfacial dynamics and catalytic behavior are clearly revealed by ultrafast femtosecond transient absorption,time-resolved,and in situ diffuse reflectance–Infrared Fourier transform spectroscopy.A tunable electronic structure through steric interaction of Mo–S bridging bonds induces a 1.7-fold enhancement in S_(v)–In_(2)S_(3)@2H–MoTe_(2)(5)photogenerated carrier concentration relative to pristine S_(v)–In_(2)S_(3).Benefiting from lower carrier transport activation energy,an internal quantum efficiency of 94.01%at 380 nm was used for photocatalytic CO_(2)RR.This study proposes a new strategy to design photocatalyst through bridging sites to adjust the selectivity of photocatalytic CO_(2)RR.
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National Natural Science Foundation of China,Grant/Award Number:51674246Creative Research and Development Group Program of Jiangsu Province,Grant/Award Number:2014-27。
文摘Precipitation or dissolution due to geochemical reactions has been observed in the caprocks for CO_(2) geosequestration.Geochemical reactions modify the caprock sealing efficiency with self-limiting or self-enhancement.However,the effect of this modification on the caprock sealing efficiency has not been fully investigated through multiphysical-geochemical coupling analysis.In this study,a multiphysical-geochemical coupling model was proposed to analyze caprock sealing efficiency.This coupling model considered the full couplings of caprock deformation,two-phase flow,CO_(2) concentration diffusion,geochemical reaction,and CO_(2) sorption.The two-phase flow only occurs in the fracture network and the CO_(2) may partially dissolve into water and diffuse through the concentration difference.The dissolved CO_(2) has geochemical reactions with some critical minerals,thus altering flow channels.The CO_(2) in the fracture network diffuses into matrix,causing the matrix swelling.This fully coupling model was validated with a penetration experiment on a cement cube and compared with two other models for CO_(2) storage plumes.Finally,the effects of geochemical reactions on penetration depth and pore pressure were studied through parametric study.The numerical simulations reveal that the coupling of geochemical reactions and matrix diffusion significantly affect the caprock sealing efficiency.Geochemical reactions occur at a short time after the arrival of CO_(2) concentration and modify the fracture porosity.The CO_(2) diffusion into the matrix requires a much longer time and mainly induces matrix swelling.These effects may produce selfenhancement or self-limiting depending on the flow rate in the fracture network,thus significantly modifying caprock sealing efficiency.
基金funding from the European Union’s Horizon 2020 research and innovation programme under the Marie Sklodowska-Curie grant agreement No.813393partially funded by the Portuguese FCT-Funda??o para a Ciência e a Tecnologia,under projects UIDB/50010/2020,UIDP/50010/2020 and PTDC/FIS-PLA/1616/2021。
文摘This paper brings the comparison of performances of CO_(2)conversion by plasma and plasma-assisted catalysis based on the data collected from literature in this field,organised in an open access online database.This tool is open to all users to carry out their own analyses,but also to contributors who wish to add their data to the database in order to improve the relevance of the comparisons made,and ultimately to improve the efficiency of CO_(2)conversion by plasma-catalysis.The creation of this database and database user interface is motivated by the fact that plasma-catalysis is a fast-growing field for all CO_(2)conversion processes,be it methanation,dry reforming of methane,methanolisation,or others.As a result of this rapid increase,there is a need for a set of standard procedures to rigorously compare performances of different systems.However,this is currently not possible because the fundamental mechanisms of plasma-catalysis are still too poorly understood to define these standard procedures.Fortunately however,the accumulated data within the CO_(2)plasma-catalysis community has become large enough to warrant so-called“big data”studies more familiar in the fields of medicine and the social sciences.To enable comparisons between multiple data sets and make future research more effective,this work proposes the first database on CO_(2)conversion performances by plasma-catalysis open to the whole community.This database has been initiated in the framework of a H_(2)0_(2)0 European project and is called the“PIONEER Data Base”.The database gathers a large amount of CO_(2)conversion performance data such as conversion rate,energy efficiency,and selectivity for numerous plasma sources coupled with or without a catalyst.Each data set is associated with metadata describing the gas mixture,the plasma source,the nature of the catalyst,and the form of coupling with the plasma.Beyond the database itself,a data extraction tool with direct visualisation features or advanced filtering functionalities has been developed and is available online to the public.The simple and fast visualisation of the state of the art puts new results into context,identifies literal gaps in data,and consequently points towards promising research routes.More advanced data extraction illustrates the impact that the database can have in the understanding of plasma-catalyst coupling.Lessons learned from the review of a large amount of literature during the setup of the database lead to best practice advice to increase comparability between future CO_(2)plasma-catalytic studies.Finally,the community is strongly encouraged to contribute to the database not only to increase the visibility of their data but also the relevance of the comparisons allowed by this tool.
