Background,aim,and scope The tectonic uplift of the Cenozoic Tibetan Plateau has produced a chain effect,which is an excellent location for Earth system science research,and its uplift process,mechanism and environmen...Background,aim,and scope The tectonic uplift of the Cenozoic Tibetan Plateau has produced a chain effect,which is an excellent location for Earth system science research,and its uplift process,mechanism and environmental effects are the hot spot and frontier of the current research.The“Tibetan Plateau uplift-weathering-CO_(2) concentration-global climate change”model was put forward by Raymo and Ruddiman to interpret the Late Cenozoic climate change.However,there are still some questions suspended,such as does the weathering of the Tibetan Plateau have the ability to control the global climate?How to explain the modern-like global CO_(2) concentration starting at about 24 Ma?Here,a short space was taken to present a brainstorm about the above questions on account of existing geological pieces of evidence.Materials and methods In this paper,we integrate the formation and evolution of the Yangtze River and Pearl River,the origin and development of the Asian inland aridification-monsoon system,the Cenozoic tectonic uplift process of the Tibetan Plateau,and the westerly winds to discuss and analyze the relationship between the Cenozoic CO_(2) concentration changes and the uplift of the Tibetan Plateau and why the CO_(2) concentration similar to the present was formed at about 24 Ma.Results Similar correspondence of the surface uplift history of Xizang,other global mountains,and the declining CO_(2) concentration could support the theory Tibetan Plateau weathering inf luences CO_(2) concentration.Starting from 24 Ma,the most important character was the uplift and erosion of Xizang and Himalaya,collaborating with Ocean Iron Fertilization(OIF)together as an entity to control the atmospheric CO_(2) concentration because the great Asian rivers,Asian monsoons,and westerlies connected Xizang and surrounded seas together through materials transportation.Discussion Paleogeographic reconstructions from 40 Ma to 20 Ma illustrate that the main topographic change occurred in the Andes,Cordillera orogenic belt,and Xizang.We comprise a comprehensive set of evidence from independent data,which correspond temporally with the tipping point(about 24 Ma)of the atmospheric CO_(2) and we noticed that modern-like Asia monsoon,inland aridity,Asian great rivers,and climate zone formed at about 24 Ma and also there are tectonic activities for the Andes and Rockies.We raised the possibility that the modern-like atmospheric CO_(2) concentration at about 24 Ma was caused by the above geological factors.Here the rivers,monsoon,and westerlies are termed as“connectors”.In addition,these Asian rivers originated from Xizang,the monsoon,and inner Asian aridification are strongly a function of the uplift and growth of Xizang,thus,Xizang here is named as“trigger”.The distinct character of“trigger-connectors”model is that this not only takes the monsoon,westerlies,and the global great rivers into consideration but also expands the range which inf luences atmospheric CO_(2) concentration,from local points to a vast area since about 24 Ma,such as from Tibetan Plateau to Asia,including surrounded seas,after about 24 Ma.However,because the opening of the Late Oligocene-Early Miocene Antarctic periphery straits is highly coincident with the onset of modern-like global atmospheric CO_(2) concentration,we are forced to consider that they also had a significant impact on the reduction of atmospheric CO_(2) concentrations at this time.Conclusions“Trigger-connectors”was put forward to explain the Cenozoic CO_(2) variation,especially modern-like global CO_(2) concentration since about 24 Ma.Recommendations and perspectives Here we use the“trigger-connectors”model to explain the formation of modern-like CO_(2) concentrations starting at about 24 Ma,but there are still some problems.The most important premise for the“trigger-connectors”model is the constructed Cenozoic CO_(2) concentration record is reliable,which is the foundation of our hypothesis.In the future,potential improvements should focus on topographic reconstructions of Xizang and the global mountains.Here we have concentrated on Xizang in the considered timeslices but still,pay less attention to other global orogenic belts.Collaborations with geologist experts in those regions could provide valuable feedback to evaluate their potential role of them in CO_(2) evolution.What is more,considerable progress may be achieved with the addition and consideration of more and new geological data.展开更多
Ozone(O_(3))pollution has a profound impact on human health,vegetation development,and the ecological environment,making it a critical focus of global academic research.In recent years,O_(3)pollution in China has been...Ozone(O_(3))pollution has a profound impact on human health,vegetation development,and the ecological environment,making it a critical focus of global academic research.In recent years,O_(3)pollution in China has been on a steady rise,with ozone emerging as the sole conventional pollutant to consistently increase in concentration without any decline.This study conducted a quantitative analysis of O_(3)concentrations across 367 Chinese cities in 2019,examining spatial autocorrelation and local clustering of O_(3)levels,and investigated the diverse relationships between human activity factors and O_(3)concentration.The seasonal fluctuation of O_(3)exhibited the“M-type”pattern,with peak concentrations in winter and the lowest levels in summer.The center of O_(3)pollution migrated southeastward,with the area of highest concentration progressively shifting south along the eastern coast.Moreover,O_(3)concentration showed a strong positive correlation with population density,road freight volume,and industrial emissions,suggesting that human activities,vehicle emissions,and industrial operations are significant contributors to O_(3)production.The results provide comprehensive information on the characteristics,causes,and occurrence mechanism of O_(3)in Chinese cities that can be utilized by global government departments to formulate strategies to prevent and control O_(3)pollution.展开更多
Full concentration gradient lithium-rich layered oxides are catching lots of interest as the next generation cathode for lithium-ion batteries due to their high discharge voltage,reduced voltage decay and enhanced rat...Full concentration gradient lithium-rich layered oxides are catching lots of interest as the next generation cathode for lithium-ion batteries due to their high discharge voltage,reduced voltage decay and enhanced rate performance,whereas the high lithium residues on its surface impairs the structure stability and long-term cycle performance.Herein,a facile multifunctional surface modification method is implemented to eliminate surface lithium residues of full concentration gradient lithium-rich layered oxides by a wet chemistry reaction with tetrabutyl titanate and the post-annealing process.It realizes not only a stable Li_(2)TiO_(3)coating layer with 3D diffusion channels for fast Li^(+)ions transfer,but also dopes partial Ti^(4+)ions into the sub-surface region of full concentration gradient lithium-rich layered oxides to further strengthen its crystal structure.Consequently,the modified full concentration gradient lithium-rich layered oxides exhibit improved structure stability,elevated thermal stability with decomposition temperature from 289.57℃to 321.72℃,and enhanced cycle performance(205.1 mAh g^(-1)after 150 cycles)with slowed voltage drop(1.67 mV per cycle).This work proposes a facile and integrated modification method to enhance the comprehensive performance of full concentration gradient lithium-rich layered oxides,which can facilitate its practical application for developing higher energy density lithium-ion batteries.展开更多
A new method based on phononic crystals is presented to detect the concentration of heavy water(D_(2)O)in an H_(2)O-D_(2)O mixture.Results have been obtained and analyzed in the concentration range of 0%-10%and 90%-10...A new method based on phononic crystals is presented to detect the concentration of heavy water(D_(2)O)in an H_(2)O-D_(2)O mixture.Results have been obtained and analyzed in the concentration range of 0%-10%and 90%-100%D_(2)O.A proposed structure of tungsten scatterers in an aluminum host is studied.In order to detect the target material,a cavity region is considered as a sound wave resonator in which the target material with different concentrations of D_(2)O is embedded.By changing the concentration of D_(2)O in the H_(2)O-D_(2)O mixture,the resonance frequency undergoes a frequency shift.Each 1%change in D_(2)O concentration in the H_(2)O-D_(2)O mixture causes a frequency change of about 120 Hz.The finite element method is used as the numerical method to calculate and analyze the natural frequencies and transmission spectra of the proposed sensor.The performance evaluation index shows a high Q factor up to 1475758 and a high sensitivity up to 13075,which are acceptable values for sensing purposes.The other figures of merit related to the detection performance also indicate high-quality performance of the designed sensor.展开更多
For a highly efficient recycling of a wastewater containing a high concentration of MgCl_2,Al(Ⅲ)and P507 were scheduled to be removed in advance.In this study,the in-situ removal of Al(Ⅲ)and P507 from a high concent...For a highly efficient recycling of a wastewater containing a high concentration of MgCl_2,Al(Ⅲ)and P507 were scheduled to be removed in advance.In this study,the in-situ removal of Al(Ⅲ)and P507 from a high concentration MgCl_(2)solution at different pH values and Al/P molar ratios was investigated.The results showed that P507 formed organic complexes of Al_x(OH)_y~(Z+)-P507 at pH of 2.0-4.0.At pH of 4.0-5.0,Al(Ⅲ)precipitated and transferred into Al(OH)_(3)with a flocculent amorphous morphology.Active sites on the Al(OH)_(3)surface enhanced the removal efficiency of P507.At pH of 6.0-6.5,Al(Ⅲ)and Mg(Ⅱ)formed layered crystalline Al(OH)_(3)and MgAl_2(OH)_(8with)small pore channels and fewer active sites,resulting in a reduced removal efficiency of P507.When the Al/P molar ratio exceeded 13 and the pH was between 4.0 and 5.0,the removal rates of both Al(Ⅲ)and P507 were higher than98%,while the concentration loss of Mg(Ⅱ)was only 0.2%-0.9%.展开更多
Biogas is a renewable and clean energy source that plays an important role in the current environment of lowcarbon transition.If high-content CO_(2) in biogas can be separated,transformed,and utilized,it not only real...Biogas is a renewable and clean energy source that plays an important role in the current environment of lowcarbon transition.If high-content CO_(2) in biogas can be separated,transformed,and utilized,it not only realizes high-value utilization of biogas but also promotes carbon reduction in the biogas field.To improve the combustion stability of biogas,an inhomogeneous,partially premixed stratified(IPPS)combustion model was adopted in this study.The thermal flame structure and stability were investigated for a wide range of mixture inhomogeneities,turbulence levels,CO_(2) concentrations,air-to-fuel velocity ratios,and combustion energies in a concentric flow slot burner(CFSB).A fine-wire thermocouple is used to resolve the thermal flame structure.The flame size was reduced by increasing the CO_(2) concentration and the flames became lighter blue.The flame temperature also decreased with increase in CO_(2) concentration.Flame stability was reduced by increasing the CO_(2) concentration.However,at a certain level of mixture inhomogeneity,the concentration of CO_(2) in the IPPS mode did not affect the stability.Accordingly,the IPPS mode of combustion should be suitable for the combustion and stabilization of biogas.This should support the design of highly stabilized biogas turbulent flames independent of CO_(2) concentration.The data show that the lower stability conditions are partially due to the change in fuel combustion energy,which is characterized by the Wobbe index(WI).In addition,at a certain level of mixture inhomogeneity,the effect of the WI on flame stability becomes dominant.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
The increasing concentration of atmospheric CO_(2) since the Industrial Revolution has affected surface air temperature.However,the impact of the spatial distribution of atmospheric CO_(2) concentration on surface air...The increasing concentration of atmospheric CO_(2) since the Industrial Revolution has affected surface air temperature.However,the impact of the spatial distribution of atmospheric CO_(2) concentration on surface air temperature biases remains highly unclear.By incorporating the spatial distribution of satellite-derived atmospheric CO_(2) concentration in the Beijing Normal University Earth System Model,this study investigated the increase in surface air temperature since the Industrial Revolution in the Northern Hemisphere(NH) under historical conditions from 1976-2005.In comparison with the increase in surface temperature simulated using a uniform distribution of CO_(2),simulation with a nonuniform distribution of CO_(2)produced better agreement with the Climatic Research Unit(CRU) data in the NH under the historical condition relative to the baseline over the period 1901-30.Hemispheric June-July-August(JJA) surface air temperature increased by 1.28℃ ±0.29℃ in simulations with a uniform distribution of CO_(2),by 1.00℃±0.24℃ in simulations with a non-uniform distribution of CO_(2),and by 0.24℃ in the CRU data.The decrease in downward shortwave radiation in the non-uniform CO_(2) simulation was primarily attributable to reduced warming in Eurasia,combined with feedbacks resulting from increased leaf area index(LAI) and latent heat fluxes.These effects were more pronounced in the non-uniform CO_(2)simulation compared to the uniform CO_(2) simulation.Results indicate that consideration of the spatial distribution of CO_(2)concentration can reduce the overestimated increase in surface air temperature simulated by Earth system models.展开更多
文摘Background,aim,and scope The tectonic uplift of the Cenozoic Tibetan Plateau has produced a chain effect,which is an excellent location for Earth system science research,and its uplift process,mechanism and environmental effects are the hot spot and frontier of the current research.The“Tibetan Plateau uplift-weathering-CO_(2) concentration-global climate change”model was put forward by Raymo and Ruddiman to interpret the Late Cenozoic climate change.However,there are still some questions suspended,such as does the weathering of the Tibetan Plateau have the ability to control the global climate?How to explain the modern-like global CO_(2) concentration starting at about 24 Ma?Here,a short space was taken to present a brainstorm about the above questions on account of existing geological pieces of evidence.Materials and methods In this paper,we integrate the formation and evolution of the Yangtze River and Pearl River,the origin and development of the Asian inland aridification-monsoon system,the Cenozoic tectonic uplift process of the Tibetan Plateau,and the westerly winds to discuss and analyze the relationship between the Cenozoic CO_(2) concentration changes and the uplift of the Tibetan Plateau and why the CO_(2) concentration similar to the present was formed at about 24 Ma.Results Similar correspondence of the surface uplift history of Xizang,other global mountains,and the declining CO_(2) concentration could support the theory Tibetan Plateau weathering inf luences CO_(2) concentration.Starting from 24 Ma,the most important character was the uplift and erosion of Xizang and Himalaya,collaborating with Ocean Iron Fertilization(OIF)together as an entity to control the atmospheric CO_(2) concentration because the great Asian rivers,Asian monsoons,and westerlies connected Xizang and surrounded seas together through materials transportation.Discussion Paleogeographic reconstructions from 40 Ma to 20 Ma illustrate that the main topographic change occurred in the Andes,Cordillera orogenic belt,and Xizang.We comprise a comprehensive set of evidence from independent data,which correspond temporally with the tipping point(about 24 Ma)of the atmospheric CO_(2) and we noticed that modern-like Asia monsoon,inland aridity,Asian great rivers,and climate zone formed at about 24 Ma and also there are tectonic activities for the Andes and Rockies.We raised the possibility that the modern-like atmospheric CO_(2) concentration at about 24 Ma was caused by the above geological factors.Here the rivers,monsoon,and westerlies are termed as“connectors”.In addition,these Asian rivers originated from Xizang,the monsoon,and inner Asian aridification are strongly a function of the uplift and growth of Xizang,thus,Xizang here is named as“trigger”.The distinct character of“trigger-connectors”model is that this not only takes the monsoon,westerlies,and the global great rivers into consideration but also expands the range which inf luences atmospheric CO_(2) concentration,from local points to a vast area since about 24 Ma,such as from Tibetan Plateau to Asia,including surrounded seas,after about 24 Ma.However,because the opening of the Late Oligocene-Early Miocene Antarctic periphery straits is highly coincident with the onset of modern-like global atmospheric CO_(2) concentration,we are forced to consider that they also had a significant impact on the reduction of atmospheric CO_(2) concentrations at this time.Conclusions“Trigger-connectors”was put forward to explain the Cenozoic CO_(2) variation,especially modern-like global CO_(2) concentration since about 24 Ma.Recommendations and perspectives Here we use the“trigger-connectors”model to explain the formation of modern-like CO_(2) concentrations starting at about 24 Ma,but there are still some problems.The most important premise for the“trigger-connectors”model is the constructed Cenozoic CO_(2) concentration record is reliable,which is the foundation of our hypothesis.In the future,potential improvements should focus on topographic reconstructions of Xizang and the global mountains.Here we have concentrated on Xizang in the considered timeslices but still,pay less attention to other global orogenic belts.Collaborations with geologist experts in those regions could provide valuable feedback to evaluate their potential role of them in CO_(2) evolution.What is more,considerable progress may be achieved with the addition and consideration of more and new geological data.
基金supported by National Natural Science Foundation of China(grant number 42101318)the National Key R&D Program of China(grant number 2018YFD1100101)。
文摘Ozone(O_(3))pollution has a profound impact on human health,vegetation development,and the ecological environment,making it a critical focus of global academic research.In recent years,O_(3)pollution in China has been on a steady rise,with ozone emerging as the sole conventional pollutant to consistently increase in concentration without any decline.This study conducted a quantitative analysis of O_(3)concentrations across 367 Chinese cities in 2019,examining spatial autocorrelation and local clustering of O_(3)levels,and investigated the diverse relationships between human activity factors and O_(3)concentration.The seasonal fluctuation of O_(3)exhibited the“M-type”pattern,with peak concentrations in winter and the lowest levels in summer.The center of O_(3)pollution migrated southeastward,with the area of highest concentration progressively shifting south along the eastern coast.Moreover,O_(3)concentration showed a strong positive correlation with population density,road freight volume,and industrial emissions,suggesting that human activities,vehicle emissions,and industrial operations are significant contributors to O_(3)production.The results provide comprehensive information on the characteristics,causes,and occurrence mechanism of O_(3)in Chinese cities that can be utilized by global government departments to formulate strategies to prevent and control O_(3)pollution.
基金financially supported by the Natural Science Foundation of Shandong Province(ZR2022QB166,ZR2020KE032)the Strategic Priority Research Program of the Chinese Academy of Sciences(XDA22010600)+3 种基金the Youth Innovation Promotion Association of CAS(2021210)the Foundation of Qingdao Postdoctoral Application Program(Y63302190F)the Natural Science Foundation of Qingdao Institute ofBioenergy and Bioprocess Technology(QIBEBT SZ202101)support from the Max Planck-POSTECH-Hsinchu Center for Complex Phase Materials
文摘Full concentration gradient lithium-rich layered oxides are catching lots of interest as the next generation cathode for lithium-ion batteries due to their high discharge voltage,reduced voltage decay and enhanced rate performance,whereas the high lithium residues on its surface impairs the structure stability and long-term cycle performance.Herein,a facile multifunctional surface modification method is implemented to eliminate surface lithium residues of full concentration gradient lithium-rich layered oxides by a wet chemistry reaction with tetrabutyl titanate and the post-annealing process.It realizes not only a stable Li_(2)TiO_(3)coating layer with 3D diffusion channels for fast Li^(+)ions transfer,but also dopes partial Ti^(4+)ions into the sub-surface region of full concentration gradient lithium-rich layered oxides to further strengthen its crystal structure.Consequently,the modified full concentration gradient lithium-rich layered oxides exhibit improved structure stability,elevated thermal stability with decomposition temperature from 289.57℃to 321.72℃,and enhanced cycle performance(205.1 mAh g^(-1)after 150 cycles)with slowed voltage drop(1.67 mV per cycle).This work proposes a facile and integrated modification method to enhance the comprehensive performance of full concentration gradient lithium-rich layered oxides,which can facilitate its practical application for developing higher energy density lithium-ion batteries.
文摘A new method based on phononic crystals is presented to detect the concentration of heavy water(D_(2)O)in an H_(2)O-D_(2)O mixture.Results have been obtained and analyzed in the concentration range of 0%-10%and 90%-100%D_(2)O.A proposed structure of tungsten scatterers in an aluminum host is studied.In order to detect the target material,a cavity region is considered as a sound wave resonator in which the target material with different concentrations of D_(2)O is embedded.By changing the concentration of D_(2)O in the H_(2)O-D_(2)O mixture,the resonance frequency undergoes a frequency shift.Each 1%change in D_(2)O concentration in the H_(2)O-D_(2)O mixture causes a frequency change of about 120 Hz.The finite element method is used as the numerical method to calculate and analyze the natural frequencies and transmission spectra of the proposed sensor.The performance evaluation index shows a high Q factor up to 1475758 and a high sensitivity up to 13075,which are acceptable values for sensing purposes.The other figures of merit related to the detection performance also indicate high-quality performance of the designed sensor.
基金financial supports from the National Key Research and Development Program of China(No.2022YFB3504501)the National Natural Science Foundation of China(Nos.52274355,91962211)the Gansu Province Science and Technology Major Special Project,China(No.22ZD6GD061)。
文摘For a highly efficient recycling of a wastewater containing a high concentration of MgCl_2,Al(Ⅲ)and P507 were scheduled to be removed in advance.In this study,the in-situ removal of Al(Ⅲ)and P507 from a high concentration MgCl_(2)solution at different pH values and Al/P molar ratios was investigated.The results showed that P507 formed organic complexes of Al_x(OH)_y~(Z+)-P507 at pH of 2.0-4.0.At pH of 4.0-5.0,Al(Ⅲ)precipitated and transferred into Al(OH)_(3)with a flocculent amorphous morphology.Active sites on the Al(OH)_(3)surface enhanced the removal efficiency of P507.At pH of 6.0-6.5,Al(Ⅲ)and Mg(Ⅱ)formed layered crystalline Al(OH)_(3)and MgAl_2(OH)_(8with)small pore channels and fewer active sites,resulting in a reduced removal efficiency of P507.When the Al/P molar ratio exceeded 13 and the pH was between 4.0 and 5.0,the removal rates of both Al(Ⅲ)and P507 were higher than98%,while the concentration loss of Mg(Ⅱ)was only 0.2%-0.9%.
基金funded by the American University in Cairo research grants(Project number SSE-MENG-M.M.-FY18-FY19-FY20-RG(1-18)–2017-Nov-11-17-52-02).
文摘Biogas is a renewable and clean energy source that plays an important role in the current environment of lowcarbon transition.If high-content CO_(2) in biogas can be separated,transformed,and utilized,it not only realizes high-value utilization of biogas but also promotes carbon reduction in the biogas field.To improve the combustion stability of biogas,an inhomogeneous,partially premixed stratified(IPPS)combustion model was adopted in this study.The thermal flame structure and stability were investigated for a wide range of mixture inhomogeneities,turbulence levels,CO_(2) concentrations,air-to-fuel velocity ratios,and combustion energies in a concentric flow slot burner(CFSB).A fine-wire thermocouple is used to resolve the thermal flame structure.The flame size was reduced by increasing the CO_(2) concentration and the flames became lighter blue.The flame temperature also decreased with increase in CO_(2) concentration.Flame stability was reduced by increasing the CO_(2) concentration.However,at a certain level of mixture inhomogeneity,the concentration of CO_(2) in the IPPS mode did not affect the stability.Accordingly,the IPPS mode of combustion should be suitable for the combustion and stabilization of biogas.This should support the design of highly stabilized biogas turbulent flames independent of CO_(2) concentration.The data show that the lower stability conditions are partially due to the change in fuel combustion energy,which is characterized by the Wobbe index(WI).In addition,at a certain level of mixture inhomogeneity,the effect of the WI on flame stability becomes dominant.
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 (Grant Nos.42175142,42141017 and 41975112) for supporting our study。
文摘The increasing concentration of atmospheric CO_(2) since the Industrial Revolution has affected surface air temperature.However,the impact of the spatial distribution of atmospheric CO_(2) concentration on surface air temperature biases remains highly unclear.By incorporating the spatial distribution of satellite-derived atmospheric CO_(2) concentration in the Beijing Normal University Earth System Model,this study investigated the increase in surface air temperature since the Industrial Revolution in the Northern Hemisphere(NH) under historical conditions from 1976-2005.In comparison with the increase in surface temperature simulated using a uniform distribution of CO_(2),simulation with a nonuniform distribution of CO_(2)produced better agreement with the Climatic Research Unit(CRU) data in the NH under the historical condition relative to the baseline over the period 1901-30.Hemispheric June-July-August(JJA) surface air temperature increased by 1.28℃ ±0.29℃ in simulations with a uniform distribution of CO_(2),by 1.00℃±0.24℃ in simulations with a non-uniform distribution of CO_(2),and by 0.24℃ in the CRU data.The decrease in downward shortwave radiation in the non-uniform CO_(2) simulation was primarily attributable to reduced warming in Eurasia,combined with feedbacks resulting from increased leaf area index(LAI) and latent heat fluxes.These effects were more pronounced in the non-uniform CO_(2)simulation compared to the uniform CO_(2) simulation.Results indicate that consideration of the spatial distribution of CO_(2)concentration can reduce the overestimated increase in surface air temperature simulated by Earth system models.