To explain the influence mechanism of MgO on the consolidation and reduction characteristics of roasted iron pellets,the properties and structure of pellets were investigated from multi-dimensions.It indicated that th...To explain the influence mechanism of MgO on the consolidation and reduction characteristics of roasted iron pellets,the properties and structure of pellets were investigated from multi-dimensions.It indicated that the MgO addition decreased the reduction swelling index(RSI)and reduction degree of pellets in both CO and H_(2)atmospheres.During the stepwise reduction process of Fe2O3→Fe3O4→FeO,the reduction behaviour of pellets in CO and H_(2)was similar,while the reduction rate of pellets in H_(2)atmosphere was almost twice as high as that in CO atmosphere.During the stepwise reduction process of FeO→Fe,the RSI of pellets showed a logarithmic increase in CO atmosphere and a linear decrease in H_(2)atmosphere.As investigated by first-principles calculations,C and Fe mainly formed chemical bonds,and the CO reduction process released energy,promoting the formation of iron whiskers.However,H and Fe produced weak physical adsorption,and the H_(2)reduction process was endothermic,inhibiting the generation of iron whiskers.With Mg2+doping in FexO,the nucleation region of iron whiskers expanded in CO reduction process,and the morphology of iron whiskers transformed from“slender”to“stocky,”reducing RSI of the pellets.展开更多
Exploration of efficient and stable photocatalysts to mimic natural leaves for the conversion of atmospheric CO_(2)into hydrocarbons utilizing solar light is very important but remains a major challenge.Herein,we repo...Exploration of efficient and stable photocatalysts to mimic natural leaves for the conversion of atmospheric CO_(2)into hydrocarbons utilizing solar light is very important but remains a major challenge.Herein,we report the design of four novel metal-salen-incorporated conjugated microporous polymers as robust artificial leaves for photoreduction of atmospheric CO_(2)with gaseous water.Owing to the rich nitrogen and oxygen moieties in the polymeric frameworks,they show a maximum CO_(2)adsorption capacity of 46.1 cm3 g^(−1)and adsorption selectivity for CO_(2)/N_(2)of up to 82 at 273 K.Under air atmosphere and simulated solar light(100mWcm^(−2)),TEPT-Zn shows an excellent CO yield of 304.96μmol h^(−1)g^(−1)with a selectivity of approximately 100%,which represents one of the best results in terms of organic photocatalysts for gas-phase CO_(2)photoreduction so far.Furthermore,only small degradation in the CO yield is observed even after 120-h continuous illumination.More importantly,a good CO yield of 152.52μmol g^(−1)was achieved by directly exposing the photocatalytic reaction of TEPT-Zn in an outdoor environment for 3 h(25-28℃,52.3±7.9mWcm^(−2)).This work provides an avenue for the continued development of advanced polymers toward gas-phase photoconversion of CO_(2)from air.展开更多
China is the largest emitter of anthropogenic CO_(2) globally,with its cities recognized as significant emission hotspots.Consequently,evaluating anthropogenic CO_(2) emissions and the carbon neutral capability(CNC)of...China is the largest emitter of anthropogenic CO_(2) globally,with its cities recognized as significant emission hotspots.Consequently,evaluating anthropogenic CO_(2) emissions and the carbon neutral capability(CNC)of Chinese cities is critical for climate change mitigation.Despite this importance,no studies to date have assessed recent and future city-scale CNCs using the top-down atmospheric inversion approach,revealing substantial knowledge gaps regarding regional CO_(2) budgets.To address these issues,this research focused on Hangzhou,a megacity known for having the highest forest cover among China’s provincial capitals,as study region.Year-round atmospheric CO_(2) concentration measurements were conducted from December 2020 to November 2021 at two sites:one urban and one suburban.These observations,along with their difference,were utilized to derive city-scale posterior anthropogenic CO_(2) emissions and to evaluate recent and future CNCs.Our key findings are as follows:(1)The manufacturing industry,energy industry and oil refineries/transformation industry were identified as the largest contributors to urban-suburban CO_(2) difference,accounting for 36.5%,21.3%,and 16.6%,respectively.Additionally,82.5%,65.2%,81.2%and 86.3%of total anthropogenic CO_(2) enhancements were attributed to emissions within Hangzhou city in winter,spring,summer and autumn,respectively.(2)The posterior annual anthropogenic CO_(2) emission for Hangzhouwas estimated at 4.65(±0.72)×10^(10) kg/a,indicating significant biases among different prior CO_(2) emission inventories.The annual biological CO_(2) sink,derived from multiple products,was estimated at-0.48(±0.16)×10^(10) kg.(3)The calculated CNC for 2021was 10.3%±3.4%,highlighting a substantial gap towards achieving full carbon neutrality.Considering potential increases in ecosystem carbon sinks due to forest age and uncertainties from climate change,it was predicted that at least 65.2%-82.6%of anthropogenic CO_(2) emissions must be reduced to achieve the goal of full carbon neutrality by year of 2060.展开更多
Although atmospheric CO_(2) observations are becoming increasingly widespread in China,the identification of CO_(2) emission sources is still scarce,especially in undeveloped Central China.To effectively address this ...Although atmospheric CO_(2) observations are becoming increasingly widespread in China,the identification of CO_(2) emission sources is still scarce,especially in undeveloped Central China.To effectively address this issue,in a typical site in Central China,the simultaneous measurements of atmospheric CO_(2),CO,andδ^(13)C were conducted,and the characteristics of CO_(2) emission sources were systematically investigated based on the relationships among CO_(2),CO,andδ^(13)C.The average CO_(2)/CO ratio of winter increased from 52.4 ppm/ppm during 2018–2020 to 65.1 ppm/ppm during 2021–2022,which confirmed the improvement of energy consumption efficiency in China.Air-mass transportation from central China and Yangtze River Delta regions contributed largely to higher CO_(2)/CO ratios in 2021–2022.A highermean CO_(2)/CO ratio appeared during the morning rush hours(60.3 ppm/ppm)than in the afternoon rush hours(51.4 ppm/ppm)in winter.In addition,the meanδ^(13)C value of CO_(2) sources(δ^(13)Cs)also displayed more negative values during the morning rush hours(-28.3‰)than the afternoon rush hours(-22.2‰),suggesting the significant influence of vehicle and natural gas usage at themorning rush hours and the impact of straw burning in the afternoon rush hours.The meanδ^(13)Cs was-24.7‰for winter and-21.9‰for vegetation season,implying the main contribution of coal in winter and the impact of C4 plants during the vegetation season.The contribution of biogenic respiration CO_(2) was inferred to exceed 50%during the nighttime of summer according to the obtained meanδ^(13)C value of biogenic respiration CO_(2),which was calculated to be-21.4‰.展开更多
In this study,the impact of different reaction times on the preparation of powdered activated carbon(PAC)using a one-step rapid activation method under flue gas atmosphere is investigated,and the underlying reaction m...In this study,the impact of different reaction times on the preparation of powdered activated carbon(PAC)using a one-step rapid activation method under flue gas atmosphere is investigated,and the underlying reaction mechanism is summarized.Results indicate that the reaction process of this method can be divided into three stages:stage I is the rapid release of volatiles and the rapid consumption of O_(2),primarily occurring within a reaction time range of 0-0.5 s;stage II is mainly the continuous release and diffusion of volatiles,which is the carbonization and activation coupling reaction stage,and the carbonization process is the main in this stage.This stage mainly occurs at the reaction time range of 0.5 -2.0 s when SL-coal is used as material,and that is 0.5-3.0 s when JJ-coal is used as material;stage III is mainly the activation stage,during which activated components diffuse to both the surface and interior of particles.This stage mainly involves the reaction stage of CO_(2)and H2O(g)activation,and it mainly occurs at the reaction time range of 2.0-4.0 s when SL-coal is used as material,and that is 3.0-4.0 s when JJ-coal is used as material.Besides,the main function of the first two stages is to provide more diffusion channels and contact surfaces/activation sites for the diffusion and activation of the activated components in the third stage.Mastering the reaction mechanism would serve as a crucial reference and foundation for designing the structure,size of the reactor,and optimal positioning of the activator nozzle in PAC preparation.展开更多
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
A comparative study on the corrosion resistance of 17Ni/（NiFe2O4-10NiO） cermet inert anode prepared in differentsintering atmospheres was conducted in Na3AlF6-Al2O3 melt. The results indicate that the corrosion rate...A comparative study on the corrosion resistance of 17Ni/（NiFe2O4-10NiO） cermet inert anode prepared in differentsintering atmospheres was conducted in Na3AlF6-Al2O3 melt. The results indicate that the corrosion rates of NiFe2O4-based cermetanodes prepared in the vacuum and the atmosphere with oxygen content of 2×10^-3 （volume fraction） are 6.46 and 2.71 cm/a,respectively. Though there is a transition layer with lots of holes or pores, a densified layer is formed on the surface of anode due tosome reactions producing aluminates. For the anode prepared in the atmosphere with oxygen content of 2×10^-3, the thickness of thedensification layer （about 50 μm） is thicker than that （about 30 μm） formed on the surface of anode prepared in the vacuum. Thecontents of NiO and Fe（II） in NiFe2xO4-y-z increase with the decrease of oxygen content in sintering atmosphere, which reduces thecorrosion resistance of the material.展开更多
Base on the principle and method of B-P neural network,the prediction model of SO2 concentration in urban atmosphere was established by using the statistical data of a city in southwest China from 1991 to 2009,so as t...Base on the principle and method of B-P neural network,the prediction model of SO2 concentration in urban atmosphere was established by using the statistical data of a city in southwest China from 1991 to 2009,so as to forecast atmospheric SO2 concentration in a city of southwest China.The results showed that B-P neural network applied in the prediction of SO2 concentration in urban atmosphere was reasonable and efficient with high accuracy and wide adaptability,so it was worthy to be popularized.展开更多
[ Objective ] The paper was to study the effect of controlled atmosphere stress of carbon dioxide （ CO2 ） on Superoxide dismutase （SOD） activity of in- sect, so as to analyze the biological mechanism of the action...[ Objective ] The paper was to study the effect of controlled atmosphere stress of carbon dioxide （ CO2 ） on Superoxide dismutase （SOD） activity of in- sect, so as to analyze the biological mechanism of the action of controlled atmosphere stress on insect. [ Method] Using nitrotetrazolium blue chloride （NBT） light reduction method, SOD activity of drugstore beetle （ Stegobium panlceum ）, cigarette beetle （ Lasioderma serricorne） and coffee bean beetle （Araecerus fasciculatus） was studied, and the stress response of the enzyme under controlled atmosphere stress of CO2 was analyzed. [ Result ] SOD activity of drugstore beetle, cigarette beetle and coffee bean beetle exposed to controlled atmosphere stress of high concentrations of CO2 for 3 and 6 h had certain degree of increase, and the activity sig- nificantly increased from 2.011±0.954,2.664±0.218 and 1.458±0.718 to 3. 135±0. 105,3.050±0.673 and 2.975±0.229 U/（per pest · 30 min） after treat- ment for 6 h. [ Conclusion] Controlled atmosphere stress of high concentrations of CO2 had certain activation effect on SOD activity of storage pest in Chinese me- dicinal material within the context of sub-lethal events. The results could enrich the insecticidal mechanism of controlled atmosphere and theoretical system of analy- sis on insect resistance to controlled atmosphere.展开更多
To quantify the relative contributions of Arctic sea ice and unforced atmospheric internal variability to the “warm Arctic, cold East Asia”(WACE) teleconnection, this study analyses three sets of large-ensemble simu...To quantify the relative contributions of Arctic sea ice and unforced atmospheric internal variability to the “warm Arctic, cold East Asia”(WACE) teleconnection, this study analyses three sets of large-ensemble simulations carried out by the Norwegian Earth System Model with a coupled atmosphere–land surface model, forced by seasonal sea ice conditions from preindustrial, present-day, and future periods. Each ensemble member within the same set uses the same forcing but with small perturbations to the atmospheric initial state. Hence, the difference between the present-day(or future) ensemble mean and the preindustrial ensemble mean provides the ice-loss-induced response, while the difference of the individual members within the present-day(or future) set is the effect of atmospheric internal variability. Results indicate that both present-day and future sea ice loss can force a negative phase of the Arctic Oscillation with a WACE pattern in winter. The magnitude of ice-induced Arctic warming is over four(ten) times larger than the ice-induced East Asian cooling in the present-day(future) experiment;the latter having a magnitude that is about 30% of the observed cooling. Sea ice loss contributes about 60%(80%) to the Arctic winter warming in the present-day(future) experiment. Atmospheric internal variability can also induce a WACE pattern with comparable magnitudes between the Arctic and East Asia. Ice-lossinduced East Asian cooling can easily be masked by atmospheric internal variability effects because random atmospheric internal variability may induce a larger magnitude warming. The observed WACE pattern occurs as a result of both Arctic sea ice loss and atmospheric internal variability, with the former dominating Arctic warming and the latter dominating East Asian cooling.展开更多
COSMIC-2(constellation observing system for meteorology ionosphere and climate-2)作为COSMIC掩星星座的后续计划,得益于升级了支持多模GNSS信号的接收机和高增益定向波束掩星天线,其观测数据质量和数量得到显著提升。围绕掩星观...COSMIC-2(constellation observing system for meteorology ionosphere and climate-2)作为COSMIC掩星星座的后续计划,得益于升级了支持多模GNSS信号的接收机和高增益定向波束掩星天线,其观测数据质量和数量得到显著提升。围绕掩星观测数据和反演产品的定量评估,分析COSMIC-2定轨和掩星天线的原始观测数据质量,并以欧洲中期数值天气预报中心的再分析气象资料为基准,定量评估掩星反演大气廓线产品质量。结果显示,COSMIC-2定轨天线L1频段信噪比大多在45 dB以上,其对应伪距多路径效应中误差在0.2~0.4 m之间;掩星天线观测信噪比由第一代COSMIC的不足700 v/v大幅提升至1200 v/v,且GLONASS掩星廓线和GPS掩星廓线均与气象再分析资料表现出了很好的一致性。研究结果认为,升级后的COSMIC-2掩星载荷不仅大幅增加掩星观测数量,其高增益的掩星天线设计还有效地提升了掩星观测数据质量,为大气科学研究提供了重要气象观测资料。展开更多
The effects of atmospheres and precursors on MnOx/TiO2 catalysts were studied, which were prepared by the impregnation method and tested for their NOx conversion activity in ammonia selective catalytic reduction （NH3...The effects of atmospheres and precursors on MnOx/TiO2 catalysts were studied, which were prepared by the impregnation method and tested for their NOx conversion activity in ammonia selective catalytic reduction （NH3-SCR） reactions. Results showed that the manganese carbonate （MC） precursor caused mainly Mn2O3, while the manganese nitrate （MN） precursor resulted primarily in MnO2 and the manganese sulfate （MS） precursor was unchanged. The manganese acetate （MA） precursor leaded obtaining a mixture of Mn2O3 and Mn304. NOn conversion decreased in the following order： MA/TiO2 〉 MC/TiO2 〉 MN/TiO2 〉 MS/TiO2 〉 P25, with a calcination temperature of 773 K in air. Catalysts that were prepared by MA and calcined in oxygen performed strong interaction between Ti and Mn, while MnTiO3 was observed. Compared to the catalysts calcined in nitrogen, those calcined in oxygen had larger diameter and smaller surface area and pore. Catalysts that were prepared by MA and calcined in nitrogen tended to gain higher denitration rates than those in air, since they could be prepared with significant specific surface areas. NO., conversion decreased with calcination atmospheres： Nitrogen〉 Air〉 Oxygen. Meanwhile, amorphous Mn2O3 turned into crystalline Mn2O3, when the temperatures increased from 673 to 873 K.展开更多
The effects of sintering atmosphere on the properties of symmetric TiO2 membranes are studied with regard to sintering behavior, porosity, mean pore size, surface comPosition. and surface charge properties. The exerim...The effects of sintering atmosphere on the properties of symmetric TiO2 membranes are studied with regard to sintering behavior, porosity, mean pore size, surface comPosition. and surface charge properties. The exerimental results show that the symmetric TiO2 membranes display better sintering activity in the air than in argon, and the mean pore diameters and porosities of the membrane sintered in argon are higher than those of the membrane sintered in the air at the same temperature. The surface compositions of the symmetric TiO2 membrane sintered in the air and in argon at different temperatures, as studied by X-ray photoelectron spectroscopy, are discussed in terms of their chemical composition, with particular emphasis on the valence state of the titanium ions. The correlation between the valence state of the titanium ions at the surface and the surface charge properties is examined.It is found that the presence of Ti^3＋, introduced at the surface of the symmetric TiO2 membranes by sintering in a lower partial pressure of oxygen, is related to a significant decrease in the isoelectric point. TiO2 with Ti^4＋ at the interface has an isoelectric point of 5.1, but the non-stoichiometric TiO2-x with Ti^3＋ at the interface has a lower isoelectric point of 3.6.展开更多
CeO_2-ZrO_2 mixed oxides are widely used in the three-way catalysts due to their unique reversible oxygen storage and release capacity. Large surface area, high oxygen storage capacity and good thermal stability of ce...CeO_2-ZrO_2 mixed oxides are widely used in the three-way catalysts due to their unique reversible oxygen storage and release capacity. Large surface area, high oxygen storage capacity and good thermal stability of cerium zirconium mixed oxides are the key properties for the automotive catalysts so as to meet the strict emission regulations. In this work, alumina modified CeZrLaNd mixed oxides were prepared by a co-precipitation method. The effects of moisture in precursor and inert N2 atmosphere during calcinations on the structure and properties were investigated by Brunauer-Emmett-Teller(BET) surface area measurements, X-ray diffraction(XRD), scanning electron microscopy(SEM), transmission electron microscopy(TEM), hydrogen temperature-programmed reduction(H_2-TPR), oxygen storage capacity(OSC), Raman spectroscopy, and X-ray photoelectron spectroscopy(XPS). The results show that the moisture in precursor during calcinations increases the crystal grain size of the cerium zirconium mixed oxides, improving the thermal stability. And the aged surface area of sample after being calcined at1000 ℃ for 4 h reaches 68.8 m^2/g(5.7% increase compared with the common sample). The inert N2 atmosphere endows a great pore-enlarging effect, which leads to high fresh surface area of 148.9 m2/g(13.5% increase compared with the common sample) and big pore volume of 0.5705 mL/g. The redox and oxygen storage capacity are also improved by inert N2 atmosphere with high OSC value of 241.06μmolO_2/g(41.3% increase compared with the common calcination), due to the abundant formation of the crystal defects and oxygen vacancies.展开更多
The ozonolysis of 2,3,7,8-tetra-chlorodibenzo-p-dioxin （2,3,7,8-TCDD） is an efficient degradation way in the atmosphere. The ozonolysis process and possible reactions path of Criegee Intermediates with NO and H2O ar...The ozonolysis of 2,3,7,8-tetra-chlorodibenzo-p-dioxin （2,3,7,8-TCDD） is an efficient degradation way in the atmosphere. The ozonolysis process and possible reactions path of Criegee Intermediates with NO and H2O are introduced in detail at the method of MPWB1K/6-31＋G（d,p）//MPWB1K/6- 311＋G（3df,2p） level. In ozonolysis, H2O is an important source of OH radical formation and initiated the subsequent degradation reaction. The Rice-Ramsperger-Kassel-Marcus （RRKM） theory was applied to calculate rate constants with the temperature ranging from 200 to 600 K. The rate constant of reaction between 2,3,7,8-TCDD and 03 is 4.80 × 10^-20 cm3/（mole.sec） at 298 K and 760 Tort. The atmospheric lifetime of the reaction species was estimated according to rate constants, which is helpful for the atmospheric model study on the degradation and risk assessment of dioxin.展开更多
The atmospheric carbon dioxide(CO_(2))concentration has been increasing rapidly since the Industrial Revolution,which has led to unequivocal global warming and crucial environmental change.It is extremely important to...The atmospheric carbon dioxide(CO_(2))concentration has been increasing rapidly since the Industrial Revolution,which has led to unequivocal global warming and crucial environmental change.It is extremely important to investigate the interactions among atmospheric CO_(2),the physical climate system,and the carbon cycle of the underlying surface for a better understanding of the Earth system.Earth system models are widely used to investigate these interactions via coupled carbon-climate simulations.The Chinese Academy of Sciences Earth System Model version 2(CAS-ESM2.0)has successfully fixed a two-way coupling of atmospheric CO_(2)with the climate and carbon cycle on land and in the ocean.Using CAS-ESM2.0,we conducted a coupled carbon-climate simulation by following the CMIP6 proposal of a historical emissions-driven experiment.This paper examines the modeled CO_(2)by comparison with observed CO_(2)at the sites of Mauna Loa and Barrow,and the Greenhouse Gases Observing Satellite(GOSAT)CO_(2)product.The results showed that CAS-ESM2.0 agrees very well with observations in reproducing the increasing trend of annual CO_(2)during the period 1850-2014,and in capturing the seasonal cycle of CO_(2)at the two baseline sites,as well as over northern high latitudes.These agreements illustrate a good ability of CAS-ESM2.0 in simulating carbon-climate interactions,even though uncertainties remain in the processes involved.This paper reports an important stage of the development of CAS-ESM with the coupling of carbon and climate,which will provide significant scientific support for climate research and China’s goal of carbon neutrality.展开更多
基金support from the National Natural Science Foundation of China(52174290).
文摘To explain the influence mechanism of MgO on the consolidation and reduction characteristics of roasted iron pellets,the properties and structure of pellets were investigated from multi-dimensions.It indicated that the MgO addition decreased the reduction swelling index(RSI)and reduction degree of pellets in both CO and H_(2)atmospheres.During the stepwise reduction process of Fe2O3→Fe3O4→FeO,the reduction behaviour of pellets in CO and H_(2)was similar,while the reduction rate of pellets in H_(2)atmosphere was almost twice as high as that in CO atmosphere.During the stepwise reduction process of FeO→Fe,the RSI of pellets showed a logarithmic increase in CO atmosphere and a linear decrease in H_(2)atmosphere.As investigated by first-principles calculations,C and Fe mainly formed chemical bonds,and the CO reduction process released energy,promoting the formation of iron whiskers.However,H and Fe produced weak physical adsorption,and the H_(2)reduction process was endothermic,inhibiting the generation of iron whiskers.With Mg2+doping in FexO,the nucleation region of iron whiskers expanded in CO reduction process,and the morphology of iron whiskers transformed from“slender”to“stocky,”reducing RSI of the pellets.
基金Research Foundation for Advanced Talents of East China University of Technology,Grant/Award Number:DHBK201927Excellent Youth Foundation of Jiangxi Scientific Committee,Grant/Award Number:20232ACB213012+2 种基金National Science Foundation for Young Scientists of China,Grant/Award Number:21905122National Science Foundation for Young Scientists,Grant/Award Number:21905147Jiangxi Talent Program,Grant/Award Number:DHSQT32022005.
文摘Exploration of efficient and stable photocatalysts to mimic natural leaves for the conversion of atmospheric CO_(2)into hydrocarbons utilizing solar light is very important but remains a major challenge.Herein,we report the design of four novel metal-salen-incorporated conjugated microporous polymers as robust artificial leaves for photoreduction of atmospheric CO_(2)with gaseous water.Owing to the rich nitrogen and oxygen moieties in the polymeric frameworks,they show a maximum CO_(2)adsorption capacity of 46.1 cm3 g^(−1)and adsorption selectivity for CO_(2)/N_(2)of up to 82 at 273 K.Under air atmosphere and simulated solar light(100mWcm^(−2)),TEPT-Zn shows an excellent CO yield of 304.96μmol h^(−1)g^(−1)with a selectivity of approximately 100%,which represents one of the best results in terms of organic photocatalysts for gas-phase CO_(2)photoreduction so far.Furthermore,only small degradation in the CO yield is observed even after 120-h continuous illumination.More importantly,a good CO yield of 152.52μmol g^(−1)was achieved by directly exposing the photocatalytic reaction of TEPT-Zn in an outdoor environment for 3 h(25-28℃,52.3±7.9mWcm^(−2)).This work provides an avenue for the continued development of advanced polymers toward gas-phase photoconversion of CO_(2)from air.
基金supported by the National Natural Science Foundation of China(Nos.42475125,42105117,42021004 and 41975143)the National Key R&D Program of China(Nos.2019YFA0607202 and 2020YFA0607501)+4 种基金Jiangsu Science Foundation for Distinguished Young Scholar(No.BK20220055)the 333 Project of Jiangsu Province(No.BRA2017402)the R&D Foundation of Jiangsu Province,China(No.BK20220020)Zhejiang Provincial Basic Public Welfare Research Project(No.LGF22D050004)the Key Laboratory of Ecosystem Carbon Source and Sink,China Meteorological Administration(ECSSCMA).
文摘China is the largest emitter of anthropogenic CO_(2) globally,with its cities recognized as significant emission hotspots.Consequently,evaluating anthropogenic CO_(2) emissions and the carbon neutral capability(CNC)of Chinese cities is critical for climate change mitigation.Despite this importance,no studies to date have assessed recent and future city-scale CNCs using the top-down atmospheric inversion approach,revealing substantial knowledge gaps regarding regional CO_(2) budgets.To address these issues,this research focused on Hangzhou,a megacity known for having the highest forest cover among China’s provincial capitals,as study region.Year-round atmospheric CO_(2) concentration measurements were conducted from December 2020 to November 2021 at two sites:one urban and one suburban.These observations,along with their difference,were utilized to derive city-scale posterior anthropogenic CO_(2) emissions and to evaluate recent and future CNCs.Our key findings are as follows:(1)The manufacturing industry,energy industry and oil refineries/transformation industry were identified as the largest contributors to urban-suburban CO_(2) difference,accounting for 36.5%,21.3%,and 16.6%,respectively.Additionally,82.5%,65.2%,81.2%and 86.3%of total anthropogenic CO_(2) enhancements were attributed to emissions within Hangzhou city in winter,spring,summer and autumn,respectively.(2)The posterior annual anthropogenic CO_(2) emission for Hangzhouwas estimated at 4.65(±0.72)×10^(10) kg/a,indicating significant biases among different prior CO_(2) emission inventories.The annual biological CO_(2) sink,derived from multiple products,was estimated at-0.48(±0.16)×10^(10) kg.(3)The calculated CNC for 2021was 10.3%±3.4%,highlighting a substantial gap towards achieving full carbon neutrality.Considering potential increases in ecosystem carbon sinks due to forest age and uncertainties from climate change,it was predicted that at least 65.2%-82.6%of anthropogenic CO_(2) emissions must be reduced to achieve the goal of full carbon neutrality by year of 2060.
基金supported by the National Natural Science Foundation of China(No.42105159)the Key Technologies Research and Development Program(No.2022YFF0606400)+2 种基金China Meteorological Administration“Research on value realization of climate ecological products”Youth Innovation Team Project(No.CMA2024QN15)Jiangxi Meteorological Technology Project(Nos.JX2021Z06,JX2022Z03,and JX2023Z03)the Joint Open Fund of the Institute of Atmospheric Environment,China Meteorological Administration,Shenyang and Key Laboratory of Agro-Meteorological Disasters of Liaoning Province(No.2024SYIAEKFZD05)。
文摘Although atmospheric CO_(2) observations are becoming increasingly widespread in China,the identification of CO_(2) emission sources is still scarce,especially in undeveloped Central China.To effectively address this issue,in a typical site in Central China,the simultaneous measurements of atmospheric CO_(2),CO,andδ^(13)C were conducted,and the characteristics of CO_(2) emission sources were systematically investigated based on the relationships among CO_(2),CO,andδ^(13)C.The average CO_(2)/CO ratio of winter increased from 52.4 ppm/ppm during 2018–2020 to 65.1 ppm/ppm during 2021–2022,which confirmed the improvement of energy consumption efficiency in China.Air-mass transportation from central China and Yangtze River Delta regions contributed largely to higher CO_(2)/CO ratios in 2021–2022.A highermean CO_(2)/CO ratio appeared during the morning rush hours(60.3 ppm/ppm)than in the afternoon rush hours(51.4 ppm/ppm)in winter.In addition,the meanδ^(13)C value of CO_(2) sources(δ^(13)Cs)also displayed more negative values during the morning rush hours(-28.3‰)than the afternoon rush hours(-22.2‰),suggesting the significant influence of vehicle and natural gas usage at themorning rush hours and the impact of straw burning in the afternoon rush hours.The meanδ^(13)Cs was-24.7‰for winter and-21.9‰for vegetation season,implying the main contribution of coal in winter and the impact of C4 plants during the vegetation season.The contribution of biogenic respiration CO_(2) was inferred to exceed 50%during the nighttime of summer according to the obtained meanδ^(13)C value of biogenic respiration CO_(2),which was calculated to be-21.4‰.
基金supported by the Qingdao Postdoctoral Program Funding(QDBSH20220202045)Shandong provincial Natural Science Foundation(ZR2021ME049,ZR2022ME176)+1 种基金National Natural Science Foundation of China(22078176)Taishan Industrial Experts Program(TSCX202306135).
文摘In this study,the impact of different reaction times on the preparation of powdered activated carbon(PAC)using a one-step rapid activation method under flue gas atmosphere is investigated,and the underlying reaction mechanism is summarized.Results indicate that the reaction process of this method can be divided into three stages:stage I is the rapid release of volatiles and the rapid consumption of O_(2),primarily occurring within a reaction time range of 0-0.5 s;stage II is mainly the continuous release and diffusion of volatiles,which is the carbonization and activation coupling reaction stage,and the carbonization process is the main in this stage.This stage mainly occurs at the reaction time range of 0.5 -2.0 s when SL-coal is used as material,and that is 0.5-3.0 s when JJ-coal is used as material;stage III is mainly the activation stage,during which activated components diffuse to both the surface and interior of particles.This stage mainly involves the reaction stage of CO_(2)and H2O(g)activation,and it mainly occurs at the reaction time range of 2.0-4.0 s when SL-coal is used as material,and that is 3.0-4.0 s when JJ-coal is used as material.Besides,the main function of the first two stages is to provide more diffusion channels and contact surfaces/activation sites for the diffusion and activation of the activated components in the third stage.Mastering the reaction mechanism would serve as a crucial reference and foundation for designing the structure,size of the reactor,and optimal positioning of the activator nozzle in PAC preparation.
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Project(51474238)supported by the National Natural Science Foundation of China
文摘A comparative study on the corrosion resistance of 17Ni/（NiFe2O4-10NiO） cermet inert anode prepared in differentsintering atmospheres was conducted in Na3AlF6-Al2O3 melt. The results indicate that the corrosion rates of NiFe2O4-based cermetanodes prepared in the vacuum and the atmosphere with oxygen content of 2×10^-3 （volume fraction） are 6.46 and 2.71 cm/a,respectively. Though there is a transition layer with lots of holes or pores, a densified layer is formed on the surface of anode due tosome reactions producing aluminates. For the anode prepared in the atmosphere with oxygen content of 2×10^-3, the thickness of thedensification layer （about 50 μm） is thicker than that （about 30 μm） formed on the surface of anode prepared in the vacuum. Thecontents of NiO and Fe（II） in NiFe2xO4-y-z increase with the decrease of oxygen content in sintering atmosphere, which reduces thecorrosion resistance of the material.
文摘Base on the principle and method of B-P neural network,the prediction model of SO2 concentration in urban atmosphere was established by using the statistical data of a city in southwest China from 1991 to 2009,so as to forecast atmospheric SO2 concentration in a city of southwest China.The results showed that B-P neural network applied in the prediction of SO2 concentration in urban atmosphere was reasonable and efficient with high accuracy and wide adaptability,so it was worthy to be popularized.
基金Supported by Project of Guizhou Provincial Modernization of Chinese Medicine Material Project(QKHYZ[2011]5049Organization Department of CPCGuizhou Committee(TZJF-2009-02)Promotion Project of Key Scientific and Technological Achievements of Guiyang City([2010]1-T-4)~~
文摘[ Objective ] The paper was to study the effect of controlled atmosphere stress of carbon dioxide （ CO2 ） on Superoxide dismutase （SOD） activity of in- sect, so as to analyze the biological mechanism of the action of controlled atmosphere stress on insect. [ Method] Using nitrotetrazolium blue chloride （NBT） light reduction method, SOD activity of drugstore beetle （ Stegobium panlceum ）, cigarette beetle （ Lasioderma serricorne） and coffee bean beetle （Araecerus fasciculatus） was studied, and the stress response of the enzyme under controlled atmosphere stress of CO2 was analyzed. [ Result ] SOD activity of drugstore beetle, cigarette beetle and coffee bean beetle exposed to controlled atmosphere stress of high concentrations of CO2 for 3 and 6 h had certain degree of increase, and the activity sig- nificantly increased from 2.011±0.954,2.664±0.218 and 1.458±0.718 to 3. 135±0. 105,3.050±0.673 and 2.975±0.229 U/（per pest · 30 min） after treat- ment for 6 h. [ Conclusion] Controlled atmosphere stress of high concentrations of CO2 had certain activation effect on SOD activity of storage pest in Chinese me- dicinal material within the context of sub-lethal events. The results could enrich the insecticidal mechanism of controlled atmosphere and theoretical system of analy- sis on insect resistance to controlled atmosphere.
基金supported by the Chinese-Norwegian Collaboration Projects within Climate Systems jointly funded by the National Key Research and Development Program of China (Grant No.2022YFE0106800)the Research Council of Norway funded project MAPARC (Grant No.328943)+2 种基金the support from the Research Council of Norway funded project BASIC (Grant No.325440)the Horizon 2020 project APPLICATE (Grant No.727862)High-performance computing and storage resources were performed on resources provided by Sigma2 - the National Infrastructure for High-Performance Computing and Data Storage in Norway (through projects NS8121K,NN8121K,NN2345K,NS2345K,NS9560K,NS9252K,and NS9034K)。
文摘To quantify the relative contributions of Arctic sea ice and unforced atmospheric internal variability to the “warm Arctic, cold East Asia”(WACE) teleconnection, this study analyses three sets of large-ensemble simulations carried out by the Norwegian Earth System Model with a coupled atmosphere–land surface model, forced by seasonal sea ice conditions from preindustrial, present-day, and future periods. Each ensemble member within the same set uses the same forcing but with small perturbations to the atmospheric initial state. Hence, the difference between the present-day(or future) ensemble mean and the preindustrial ensemble mean provides the ice-loss-induced response, while the difference of the individual members within the present-day(or future) set is the effect of atmospheric internal variability. Results indicate that both present-day and future sea ice loss can force a negative phase of the Arctic Oscillation with a WACE pattern in winter. The magnitude of ice-induced Arctic warming is over four(ten) times larger than the ice-induced East Asian cooling in the present-day(future) experiment;the latter having a magnitude that is about 30% of the observed cooling. Sea ice loss contributes about 60%(80%) to the Arctic winter warming in the present-day(future) experiment. Atmospheric internal variability can also induce a WACE pattern with comparable magnitudes between the Arctic and East Asia. Ice-lossinduced East Asian cooling can easily be masked by atmospheric internal variability effects because random atmospheric internal variability may induce a larger magnitude warming. The observed WACE pattern occurs as a result of both Arctic sea ice loss and atmospheric internal variability, with the former dominating Arctic warming and the latter dominating East Asian cooling.
文摘COSMIC-2(constellation observing system for meteorology ionosphere and climate-2)作为COSMIC掩星星座的后续计划,得益于升级了支持多模GNSS信号的接收机和高增益定向波束掩星天线,其观测数据质量和数量得到显著提升。围绕掩星观测数据和反演产品的定量评估,分析COSMIC-2定轨和掩星天线的原始观测数据质量,并以欧洲中期数值天气预报中心的再分析气象资料为基准,定量评估掩星反演大气廓线产品质量。结果显示,COSMIC-2定轨天线L1频段信噪比大多在45 dB以上,其对应伪距多路径效应中误差在0.2~0.4 m之间;掩星天线观测信噪比由第一代COSMIC的不足700 v/v大幅提升至1200 v/v,且GLONASS掩星廓线和GPS掩星廓线均与气象再分析资料表现出了很好的一致性。研究结果认为,升级后的COSMIC-2掩星载荷不仅大幅增加掩星观测数量,其高增益的掩星天线设计还有效地提升了掩星观测数据质量,为大气科学研究提供了重要气象观测资料。
基金Funded by the National "Twelfth Five-Year" Plan for Science&Technology Support of China(No.2011BAE29B02))
文摘The effects of atmospheres and precursors on MnOx/TiO2 catalysts were studied, which were prepared by the impregnation method and tested for their NOx conversion activity in ammonia selective catalytic reduction （NH3-SCR） reactions. Results showed that the manganese carbonate （MC） precursor caused mainly Mn2O3, while the manganese nitrate （MN） precursor resulted primarily in MnO2 and the manganese sulfate （MS） precursor was unchanged. The manganese acetate （MA） precursor leaded obtaining a mixture of Mn2O3 and Mn304. NOn conversion decreased in the following order： MA/TiO2 〉 MC/TiO2 〉 MN/TiO2 〉 MS/TiO2 〉 P25, with a calcination temperature of 773 K in air. Catalysts that were prepared by MA and calcined in oxygen performed strong interaction between Ti and Mn, while MnTiO3 was observed. Compared to the catalysts calcined in nitrogen, those calcined in oxygen had larger diameter and smaller surface area and pore. Catalysts that were prepared by MA and calcined in nitrogen tended to gain higher denitration rates than those in air, since they could be prepared with significant specific surface areas. NO., conversion decreased with calcination atmospheres： Nitrogen〉 Air〉 Oxygen. Meanwhile, amorphous Mn2O3 turned into crystalline Mn2O3, when the temperatures increased from 673 to 873 K.
基金Supported by the National-Basic Research Program of China （2003CB615707） and the National Natural Science Foundation of China （20636020）.
文摘The effects of sintering atmosphere on the properties of symmetric TiO2 membranes are studied with regard to sintering behavior, porosity, mean pore size, surface comPosition. and surface charge properties. The exerimental results show that the symmetric TiO2 membranes display better sintering activity in the air than in argon, and the mean pore diameters and porosities of the membrane sintered in argon are higher than those of the membrane sintered in the air at the same temperature. The surface compositions of the symmetric TiO2 membrane sintered in the air and in argon at different temperatures, as studied by X-ray photoelectron spectroscopy, are discussed in terms of their chemical composition, with particular emphasis on the valence state of the titanium ions. The correlation between the valence state of the titanium ions at the surface and the surface charge properties is examined.It is found that the presence of Ti^3＋, introduced at the surface of the symmetric TiO2 membranes by sintering in a lower partial pressure of oxygen, is related to a significant decrease in the isoelectric point. TiO2 with Ti^4＋ at the interface has an isoelectric point of 5.1, but the non-stoichiometric TiO2-x with Ti^3＋ at the interface has a lower isoelectric point of 3.6.
基金Project supported by the China National Key Research and Development Program(2017YFC0211002)
文摘CeO_2-ZrO_2 mixed oxides are widely used in the three-way catalysts due to their unique reversible oxygen storage and release capacity. Large surface area, high oxygen storage capacity and good thermal stability of cerium zirconium mixed oxides are the key properties for the automotive catalysts so as to meet the strict emission regulations. In this work, alumina modified CeZrLaNd mixed oxides were prepared by a co-precipitation method. The effects of moisture in precursor and inert N2 atmosphere during calcinations on the structure and properties were investigated by Brunauer-Emmett-Teller(BET) surface area measurements, X-ray diffraction(XRD), scanning electron microscopy(SEM), transmission electron microscopy(TEM), hydrogen temperature-programmed reduction(H_2-TPR), oxygen storage capacity(OSC), Raman spectroscopy, and X-ray photoelectron spectroscopy(XPS). The results show that the moisture in precursor during calcinations increases the crystal grain size of the cerium zirconium mixed oxides, improving the thermal stability. And the aged surface area of sample after being calcined at1000 ℃ for 4 h reaches 68.8 m^2/g(5.7% increase compared with the common sample). The inert N2 atmosphere endows a great pore-enlarging effect, which leads to high fresh surface area of 148.9 m2/g(13.5% increase compared with the common sample) and big pore volume of 0.5705 mL/g. The redox and oxygen storage capacity are also improved by inert N2 atmosphere with high OSC value of 241.06μmolO_2/g(41.3% increase compared with the common calcination), due to the abundant formation of the crystal defects and oxygen vacancies.
基金supported by National Natural Science Foundation of China(No.21277082,21177076,71201093)the Promotive Research Fund for Excellent Young and Middle-aged Scientists of Shandong Province(No.BS2012HZ009,BS2012SF012)+2 种基金the Hi-Tech Research and Development Program(863)of China(No.2012AA06A301)the New Century Excellent Talents in University(NCET-13-0349)the Open Project from special fund of State Key Joint Laboratory of Environment Simulation and Pollution Control(No.13K05ESPCP)
文摘The ozonolysis of 2,3,7,8-tetra-chlorodibenzo-p-dioxin （2,3,7,8-TCDD） is an efficient degradation way in the atmosphere. The ozonolysis process and possible reactions path of Criegee Intermediates with NO and H2O are introduced in detail at the method of MPWB1K/6-31＋G（d,p）//MPWB1K/6- 311＋G（3df,2p） level. In ozonolysis, H2O is an important source of OH radical formation and initiated the subsequent degradation reaction. The Rice-Ramsperger-Kassel-Marcus （RRKM） theory was applied to calculate rate constants with the temperature ranging from 200 to 600 K. The rate constant of reaction between 2,3,7,8-TCDD and 03 is 4.80 × 10^-20 cm3/（mole.sec） at 298 K and 760 Tort. The atmospheric lifetime of the reaction species was estimated according to rate constants, which is helpful for the atmospheric model study on the degradation and risk assessment of dioxin.
基金the National Key Research and Development Program of China(Grant No.2022YFE0106500)the Youth Innovation Promotion Association of the Chinese Academy of Sciences(Grant No.2022076)+1 种基金the National Key Scientific and Technological Infrastructure project“Earth System Numerical Simulation Facility”(EarthLab2023-EL-ZD-00012)。
文摘The atmospheric carbon dioxide(CO_(2))concentration has been increasing rapidly since the Industrial Revolution,which has led to unequivocal global warming and crucial environmental change.It is extremely important to investigate the interactions among atmospheric CO_(2),the physical climate system,and the carbon cycle of the underlying surface for a better understanding of the Earth system.Earth system models are widely used to investigate these interactions via coupled carbon-climate simulations.The Chinese Academy of Sciences Earth System Model version 2(CAS-ESM2.0)has successfully fixed a two-way coupling of atmospheric CO_(2)with the climate and carbon cycle on land and in the ocean.Using CAS-ESM2.0,we conducted a coupled carbon-climate simulation by following the CMIP6 proposal of a historical emissions-driven experiment.This paper examines the modeled CO_(2)by comparison with observed CO_(2)at the sites of Mauna Loa and Barrow,and the Greenhouse Gases Observing Satellite(GOSAT)CO_(2)product.The results showed that CAS-ESM2.0 agrees very well with observations in reproducing the increasing trend of annual CO_(2)during the period 1850-2014,and in capturing the seasonal cycle of CO_(2)at the two baseline sites,as well as over northern high latitudes.These agreements illustrate a good ability of CAS-ESM2.0 in simulating carbon-climate interactions,even though uncertainties remain in the processes involved.This paper reports an important stage of the development of CAS-ESM with the coupling of carbon and climate,which will provide significant scientific support for climate research and China’s goal of carbon neutrality.
