Integrated CO_(2)capture and utilization(ICCU)technology requires dual functional materials(DFMs)to carry out the process in a single reaction system.The influence of the calcination atmosphere on efficiency of 4%Ru-8...Integrated CO_(2)capture and utilization(ICCU)technology requires dual functional materials(DFMs)to carry out the process in a single reaction system.The influence of the calcination atmosphere on efficiency of 4%Ru-8%Na_(2)CO_(3)-8%CaO/γ-Al_(2)O_(3)DFM is studied.The adsorbent precursors are first co-impregnated onto alumina and calcined in air.Then,Ru precursor is impregnated and four aliquotes are subjected to different calcination protocols:static air in muffle or under different mixtures(10%H_(2)/N_(2),50%H_(2)/N_(2)and N_(2))streams.Samples are characterized by XRD,N_(2)adsorption-desorption,H_(2)chemisorption,TEM,XPS,H_(2)-TPD,H_(2)-TPR,CO_(2)-TPD and TPSR.The catalytic behavior is evaluated,in cycles of CO_(2)adsorption and hydrogenation to CH_(4),and temporal evolution of reactants and products concentrations is analyzed.The calcination atmosphere influences the physicochemical properties and,ultimately,activity of DFMs.Characterization data and catalytic performance discover the acccomodation of Ru nanoparticles disposition and basic sites is mostly influencing the catalytic activity.DFM calcined under N_(2)flow(RuNaCa-N_(2))shows the highest CH_(4)production(449μmol/g at 370℃),because a well-controlled decomposition of precursors which favors the better accomodation of adsorbent and Ru phases,maximizing the specific surface area,the Ru-basic sites interface and the participation of different basic sites in the CO_(2)methanation reaction.Thus,the calcination in a N_(2)flow is revealed as the optimal calcination protocol to achieve highly efficient DFM for integrated CO_(2)adsorption and hydrogenation applications.展开更多
The ever-increasing atmospheric CO_(2) concentration is a key driver of modern global warming.However,the low heat capacity of atmosphere and strong convection processes in the troposphere both limit heat retention.Gi...The ever-increasing atmospheric CO_(2) concentration is a key driver of modern global warming.However,the low heat capacity of atmosphere and strong convection processes in the troposphere both limit heat retention.Given the higher heat capacity and CO_(2) concentration in soil compared to the atmosphere,the direct contributions of soil to the greenhouse effect may be significant.By experimentally manipulating CO_(2) concentrations both in the soil and the atmosphere,we demonstrated that the soil-retained heat and the slower soil heat transmission decrease the amount of heat energy leaking from the earth.Furthermore,the soil air temperature was affected by soil CO_(2) concentration,with the highest value recorded at 7500 ppm CO_(2).This study indicates that soil and soil CO_(2),together with atmospheric CO_(2),play a crucial role in the greenhouse effect.The spatial and temporal heterogeneity of soils and soil CO_(2) should be further investigated,given their potentially significant influence on global climate change.展开更多
基金supported by Ministry of Science and InnovationNational Research Agency(Project PID2019-105960RBC21)+1 种基金by the Basque Government(Project IT1509-2022)One of the authors(JAOC)acknowledges the post-doctoral research grant(DOCREC20/49)provided by the University of the Basque Country。
文摘Integrated CO_(2)capture and utilization(ICCU)technology requires dual functional materials(DFMs)to carry out the process in a single reaction system.The influence of the calcination atmosphere on efficiency of 4%Ru-8%Na_(2)CO_(3)-8%CaO/γ-Al_(2)O_(3)DFM is studied.The adsorbent precursors are first co-impregnated onto alumina and calcined in air.Then,Ru precursor is impregnated and four aliquotes are subjected to different calcination protocols:static air in muffle or under different mixtures(10%H_(2)/N_(2),50%H_(2)/N_(2)and N_(2))streams.Samples are characterized by XRD,N_(2)adsorption-desorption,H_(2)chemisorption,TEM,XPS,H_(2)-TPD,H_(2)-TPR,CO_(2)-TPD and TPSR.The catalytic behavior is evaluated,in cycles of CO_(2)adsorption and hydrogenation to CH_(4),and temporal evolution of reactants and products concentrations is analyzed.The calcination atmosphere influences the physicochemical properties and,ultimately,activity of DFMs.Characterization data and catalytic performance discover the acccomodation of Ru nanoparticles disposition and basic sites is mostly influencing the catalytic activity.DFM calcined under N_(2)flow(RuNaCa-N_(2))shows the highest CH_(4)production(449μmol/g at 370℃),because a well-controlled decomposition of precursors which favors the better accomodation of adsorbent and Ru phases,maximizing the specific surface area,the Ru-basic sites interface and the participation of different basic sites in the CO_(2)methanation reaction.Thus,the calcination in a N_(2)flow is revealed as the optimal calcination protocol to achieve highly efficient DFM for integrated CO_(2)adsorption and hydrogenation applications.
基金supported by the National Natural Science Foundation of China(41877054,31570516)the Zhongyuan Scholar Program(182101510005)the CAS/SAFEA International Partnership Program for Creative Research Teams.
文摘The ever-increasing atmospheric CO_(2) concentration is a key driver of modern global warming.However,the low heat capacity of atmosphere and strong convection processes in the troposphere both limit heat retention.Given the higher heat capacity and CO_(2) concentration in soil compared to the atmosphere,the direct contributions of soil to the greenhouse effect may be significant.By experimentally manipulating CO_(2) concentrations both in the soil and the atmosphere,we demonstrated that the soil-retained heat and the slower soil heat transmission decrease the amount of heat energy leaking from the earth.Furthermore,the soil air temperature was affected by soil CO_(2) concentration,with the highest value recorded at 7500 ppm CO_(2).This study indicates that soil and soil CO_(2),together with atmospheric CO_(2),play a crucial role in the greenhouse effect.The spatial and temporal heterogeneity of soils and soil CO_(2) should be further investigated,given their potentially significant influence on global climate change.
