CO_(2)is one of the most important greenhouse gases(GHGs)in the earth’s atmosphere.Since the industrial era,anthropogenic activities have emitted excessive quantities of GHGs into the atmosphere,resulting in climate ...CO_(2)is one of the most important greenhouse gases(GHGs)in the earth’s atmosphere.Since the industrial era,anthropogenic activities have emitted excessive quantities of GHGs into the atmosphere,resulting in climate warming since the 1950s and leading to an increased frequency of extreme weather and climate events.In 2020,China committed to striving for carbon neutrality by 2060.This commitment and China’s consequent actions will result in significant changes in global and regional anthropogenic carbon emissions and therefore require timely,comprehensive,and objective monitoring and verification support(MVS)systems.The MVS approach relies on the top-down assimilation and inversion of atmospheric CO_(2)concentrations,as recommended by the Intergovernmental Panel on Climate Change(IPCC)Inventory Guidelines in 2019.However,the regional high-resolution assimilation and inversion method is still in its initial stage of development.Here,we have constructed an inverse system for carbon sources and sinks at the kilometer level by coupling proper orthogonal decomposition(POD)with four-dimensional variational(4DVar)data assimilation based on the weather research and forecasting-greenhouse gas(WRF-GHG)model.Our China Carbon Monito ring and Verification Support at the Regional level(CCMVS-R)system can continuously assimilate information on atmospheric CO_(2)and other related information and realize the inversion of regional and local anthropogenic carbon emissions and natural terrestrial ecosystem carbon exchange.Atmospheric CO_(2)data were collected from six ground-based monito ring sites in Shanxi Province,China to verify the inversion effect of regio nal anthropogenic carbon emissions by setting ideal and real experiments using a two-layer nesting method(at 27 and 9 km).The uncertainty of the simulated atmospheric CO_(2)decreased significantly,with a root-mean-square error of CO_(2)concentration values between the ideal value and the simulated after assimilation was close to 0.The total anthropogenic carbon emissions in Shanxi Province in 2019 from the assimilated inversions were approximately 28.6%(17%-38%)higher than the mean of five emission inventories using the bottomup method,showing that the top-down CCMVS-R system can obtain more comprehensive information on anthropogenic carbon emissions.展开更多
In this work, the zeolite-Y was ion-exchanged by introducing silver cations into the framework of microsized nano-porous sodium zeolite-Y using a liquid-phase ion exchanged method. The Ag+ion-exchanged zeolite, was th...In this work, the zeolite-Y was ion-exchanged by introducing silver cations into the framework of microsized nano-porous sodium zeolite-Y using a liquid-phase ion exchanged method. The Ag+ion-exchanged zeolite, was then embedded into the Matrimid5218 matrix to form novel mixed matrix membranes(MMMs). The particles and MMMs were characterized by ultraviolet-visible diffuse reflectance spectroscopy(UV–vis DRS), N2adsorption–desorption isotherm, X-ray diffraction(XRD), Fourier transform infrared(FTIR) and scanning electron microscopy(SEM). Furthermore, the effects of filler content(0–20wt%) on pure and mixed gas experiments, feed pressure(2–20 bar) and operating temperature(35–75 oC)on CO2/CH4transport properties of Matrimid/Ag Y MMMs were considered. Characterization results confirmed an appropriate ion-exchange treatment of the zeolites. The SEM results confirmed the superior interfacial adhesion between polymer and zeolites, particularly in the case of Matrimid/Ag Y membranes.This is due to the proper silverous zeolite/Matrimid functional groups’ interactions. The gas permeation results showed that the CO2permeability increased about 123%, from 8.34 Barrer for pure Matrimid to18.62 Barrer for Matrimid/Ag Y(15 wt%). The CO2/CH4selectivity was improved about 66%, from 36.3 for Matrimid to 60.1 for Matrimid/Ag Y(15 wt%). The privileged gas separation performance of Matrimid/Ag Y(15 wt%) was the result of a combined effect of facilitated transport mechanism of Ag+ions as well as the intrinsic surface diffusion mechanism of Y-type zeolite. In order to survey the possibility of using the developed MMMs in industry, the CO2-induced plasticization effect and mixed gas experiment were accomplished. It was deduced that the fabricated MMMs could maintain the superior performance in actual operating conditions.展开更多
Reactions between CH_4 and CO_2 under the action of continuous microwave discharge at atmospheric pressure were studied in a special homemade reactor. The main products were CO and H2, while acetylene and ethylene wer...Reactions between CH_4 and CO_2 under the action of continuous microwave discharge at atmospheric pressure were studied in a special homemade reactor. The main products were CO and H2, while acetylene and ethylene were also found in the products. Experimental results show that conversions of CH4 and CO2 could be higher than 90% without the presence of any catalyst. Effects of CO2/CH4 molar ratio and total flow rate of the feed gas on the reaction were also investigated.展开更多
Since hydrate resources play a part of the stratigraphic framework structure in sediments,establishing a safe and economic method for hydrates exploitation remains the primary challenge to this day.Among the proposed ...Since hydrate resources play a part of the stratigraphic framework structure in sediments,establishing a safe and economic method for hydrates exploitation remains the primary challenge to this day.Among the proposed methods,the spontaneous displacement of CH_(4) from hydrate cages by CO_(2) seems to be a perfect mechanism to address gas production and CO_(2) storage,especially in today's strong demand for carbon reduction and replacing clean energy.After extensive lab researches,in the past decade,injecting a mixture of CO_(2) and small molecule gas has become a key means to enhance displacement efficiency and has great potential for application.However,there is a lack of in-depth research on gas flow in the reservoir,while the injected gas always passes through low-saturated hydrate areas with high permeability and then occurs gas channel in a short term,finally resulting in the decreases in gas production efficiency and produced gas quality.Therefore,we explored a new injection-production mode of alternate injection of N2 and CO_(2) in order to fully coordinate the advantages of N_(2) in enhanced hydrate decomposition and CO_(2) in solid storage and heat compensation.These alternate"taking"and"storing"processes perfectly repair the problem of the gas channel,achieving self-regulation effect of CH_(4) recovery and CO_(2) storage.The 3-D experimental results show that compared to the mixed gas injection,CH_(4) recovery is increased by>50%and CO_(2) storage is increased by>70%.Additionally,this alternate injection mode presented a better performance in CH_(4) concentration of produced gas and showed outstanding N_(2) utilization efficiency.Further,we analyzed its self-adaptive gas flow mechanism and proposed an application model of"one injection and multiple production".We look forward to this study accelerating the application of CO_(2)-CH_(4) replacement technology.展开更多
Carbon emission reduction and clean energy development are urgent demands for mankind in the coming decades.Exploring an efficient CO_(2) storage method can significantly reduce CO_(2) emissions in the short term.In t...Carbon emission reduction and clean energy development are urgent demands for mankind in the coming decades.Exploring an efficient CO_(2) storage method can significantly reduce CO_(2) emissions in the short term.In this study,we attempted to construct sediment samples with different residual CH_(4) hydrate amounts and reservoir conditions,and then investigate the potentials of both CO_(2) storage and enhanced CH_(4) recovery in depleted gas hydrate deposits in the permafrost and ocean zones,respectively.The results demonstrate that CO_(2) hydrate formation rate can be significantly improved due to the presence of residual hydrate seeds;However,excessive residual hydrates in turn lead to the decrease in CO_(2) storage efficiency.Affected by the T-P conditions of the reservoir,the storage amount of liquid CO_(2) can reach 8 times that of gaseous CO_(2),and CO_(2) stored in hydrate form reaches 2-4 times.Additionally,we noticed two other advantages of this method.One is that CO_(2) injection can enhance CH_(4) recovery rate and increases CH_(4) recovery by 10%-20%.The second is that hydrate saturation in the reservoir can be restored to 20%-40%,which means that the solid volume of the reservoir avoids serious shrinkage.Obviously,this is crucial for protecting the goaf stability.In summary,this approach is greatly promising for high-efficient CO_(2) storage and safe exploitation of gas hydrate.展开更多
Biaxia lrotary tillage in dryland(DBRT)can complete biaxial rotary tillage with straw incorporation,secondary suppression,and ditching,and it has been previously studied in direct-seeded rice and wheat.However,the eff...Biaxia lrotary tillage in dryland(DBRT)can complete biaxial rotary tillage with straw incorporation,secondary suppression,and ditching,and it has been previously studied in direct-seeded rice and wheat.However,the effects of DBRT on the mechanically transplanted rice yield and greenhouse gas emissions remain unclear.To evaluate the effects of DBRT on improving the food security of mechanically transplanted rice and reducing the greenhouse gas emissions,we conducted an experiment for two years with wheat straw incorporation.Three tillage methods were set up:DBRT,uniaxial rotary tillage in dryland and paddy(DPURT),and uniaxial rotary tillage in paddy(PURT).The results showed that compared with DPURT and PURT,DBRT increased the yield of machine-transplanted rice by 7.5-11.0%and 13.3-26.7%,respectively,while the seasonal cumulative CH_(4) emissions were reduced by 13.9-21.2%and 30.2-37.0%,respectively,and the seasonal cumulative N_(2)O emissions were increased by 13.5-28.6%and 50.0-73.1%,respectively.Consequently,DBRT reduced the global warming potential by 10.7-15.5%and 23.7-28.6%,respectively,andtheyield-scaledglobalwarmingpotentialby18.2-21.8%and36.4-39.3%,respectively,compared to DPURT and PURT.These results were mainly related to the fact that DBRT significantly reduced soil bulk density and increased soil redox potential(Eh).Therefore,implementing DBRT in machine-transplanted rice fields is feasible,which cannot only increase the rice yield,but also reduce the greenhouse gas emissions.展开更多
Lithium-ion batteries(LIBs)featuring a Ni-rich cathode exhibit increased specific capacity,but the establishment of a stable interphase through the implementation of a functional electrolyte strategy remains challengi...Lithium-ion batteries(LIBs)featuring a Ni-rich cathode exhibit increased specific capacity,but the establishment of a stable interphase through the implementation of a functional electrolyte strategy remains challenging.Especially when the battery is operated under high temperature,the trace water present in the electrolyte will accelerate the hydrolysis of the electrolyte and the resulting HF will further erode the interphase.In order to enhance the long-term cycling performance of graphite/LiNi_(0.8)Co_(0.1)Mn_(0.1)O_(2)(NCM811)LIBs,herein,Tolylene-2,4-diisocyanate(TDI)additive containing lone-pair electrons is employed to formulate a novel bifunctional electrolyte aimed at eliminating H_(2)O/HF generated at elevated temperature.After 1000 cycles at 25℃,the battery incorporating the TDI-containing electrolyte exhibits an impressive capacity retention of 94%at 1 C.In contrast,the battery utilizing the blank electrolyte has a lower capacity retention of only 78%.Furthermore,after undergoing 550 cycles at 1 C under45℃,the inclusion of TDI results in a notable enhancement of capacity,increasing it from 68%to 80%.This indicates TDI has a favorable influence on the cycling performance of LIBs,especially at elevated temperatures.The analysis of the film formation mechanism suggests that the lone pair of electrons of the isocyanate group in TDI play a crucial role in inhibiting the generation of H_(2)O and HF,which leads to the formation of a thin and dense interphase.The existence of this interphase is thought to substantially enhance the cycling performance of the LIBs.This work not only improves the performance of graphite/NCM811 batteries at room temperature and high temperature by eliminating H_(2)O/HF but also presents a novel strategy for advancing functional electrolyte development.展开更多
Using the closed chamber technique, the in situ measurements of N2O and CH4 fluxes was conducted in a broad-leaved Korean pine mixed forest ecosystem in Changbai Mountain, China. from June 1994 to october 1995. The re...Using the closed chamber technique, the in situ measurements of N2O and CH4 fluxes was conducted in a broad-leaved Korean pine mixed forest ecosystem in Changbai Mountain, China. from June 1994 to october 1995. The relationships between fluxes (N2O and CH4) and some major environmental factors (temperature, soil water content and soil availabIe nitrogen) were studied. A significant positive correlation between Nzo emission and air/soil temperature was observed, but no significant correIation was found between N2O emission and soil water content (SWC). This result showed that temperature was an important controlling factor of N2O flux. There was a significant correlation between CH4 uptake and SWC, but no significant correlation was found between CH4 uptake and temperature. This suggested SWC was an important factor controlling CH4 uptake. The very significant negative correlation between logarithmic N2O flux and soil nitrate concentration, significant negative correlation between CH4 flux and soil ammonium content were also found.展开更多
Soil samples were taken from depth of 0-12cm in the virgin broad- leaved/Korean pine mixed forest in Changbai Mountain in April, 2000. 20 μL·L-1 and 200 μL·L-1 CH4 and N2O concentration were supplied for a...Soil samples were taken from depth of 0-12cm in the virgin broad- leaved/Korean pine mixed forest in Changbai Mountain in April, 2000. 20 μL·L-1 and 200 μL·L-1 CH4 and N2O concentration were supplied for analysis. Laboratory study on CH4 oxidation and N2O emission in forest soil showed that fresh soil sample could oxidize atmospheric methane and product N2O. Air-dried soil sample could not oxidize atmospheric methane, but could produCt N2O. However, it could oxidize the supplied methane quickly when its concentration was higher than 20 μL·L-1. The oxidation rate of methane was increased with its initial concentration. An addition of water to dry soil caused large pulse of N2O emissions within 2 hours. There were curvilinear correlations between N2O emission and temperature (r2=0.706, p <0.05), and between N2O emission andtwater content (r2=0.2968. p <0.05). These suggested temperature and water content were important factors controlling N2O emission. The correlation between CH4 oxidization and temperature was also found while CH4 was supplied 200 μL·L-1 (r2 =0.3573, p<0.05). Temperature was an important f8Ctor controlling CH4 oxidation. However, when 20 μL·L-1 CH4 was supplied, there was no correlation among CH4 oxidization, N2O emission, temperature and water content.展开更多
Regulating the selectivity toward a target hydrocarbon product is still the focus of CO_(2)electroreduction.Here,we discover that the original surface Cu species in Cu gas-diffusion electrodes plays a more important r...Regulating the selectivity toward a target hydrocarbon product is still the focus of CO_(2)electroreduction.Here,we discover that the original surface Cu species in Cu gas-diffusion electrodes plays a more important role than the surface roughness,local pH,and facet in governing the selectivity toward C_(1)or C_(2)hydrocarbons.The selectivity toward C_(2)H_(4) progressively increases,while CH_(4) decreases steadily upon lowering the Cu oxidation species fraction.At a relatively low electrodeposition voltage of 1.5 V,the Cu gas-diffusion electrode with the highest Cu^(δ+)/Cu^(0)ratio favors the pathways of∗CO hydrogenation to form CH_(4) with maximum Faradaic efficiency of 65.4%and partial current density of 228 mA cm^(−2)at−0.83 V vs RHE.At 2.0 V,the Cu gas-diffusion electrode with the lowest Cu^(δ+)/Cu^(0)ratio prefers C-C coupling to form C_(2)+products with Faradaic efficiency topping 80.1%at−0.75 V vs RHE,where the Faradaic efficiency of C_(2)H_(4) accounts for 46.4%and the partial current density of C_(2)H_(4) achieves 279 mA cm^(−2).This work demonstrates that the selectivity from CH_(4) to C_(2)H_(4) is switchable by tuning surface Cu species composition of Cu gas-diffusion electrodes.展开更多
The cobalt precursor affects the catalytic performance of Co/SiO_2 catalyst remarkably. The catalyst prepared from cobalt acetate exhibits excellent activity, stability and resistance to carbon deposition.
Controlled-release urea(CRU)is widely reported to supply crop nitrogen(N)demand with one basal application,thus effectively replacing split applications of urea without diminishing grain yield and N use efficiency(NUE...Controlled-release urea(CRU)is widely reported to supply crop nitrogen(N)demand with one basal application,thus effectively replacing split applications of urea without diminishing grain yield and N use efficiency(NUE).However,its use for replacement for high-yield split applications of urea(CK)for rice is untested.In addition,the degree to which greenhouse gas(GHG)emissions in rice systems are affected when CRU is substituted for CK remains unclear.During 2017 and 2018,we sampled plant growth and gas emissions in a rice paddy field treated with three CRU types(sulfur-coated urea[SCU],polymer-coated urea[PCU],and bulk blended CRU[BBU])applied via two methods(surface broadcasting on the soil and subsurface banding at 5 cm depth),with CK as a control.The three CRUs led to different soil NH_(4)^(+)-N dynamics,and the N supply pattern under BBU was more beneficial for rice seedling establishment than under SCU and PCU,resulting in grain yield and NUE comparable to those under CK.CRU type showed no significant effect on either CH_(4) emissions or N_(2)O emissions,and broadcast CRUs exhibited significantly higher total GHG emissions than CK.However,banded CRUs significantly reduced the total GHG emissions in comparison with broadcast CRUs,by 9.2%averaged across the two years.Reduced CH_(4) emissions,particularly during the period prior to the middle drainage,contributed largely to the GHG difference.With comparably high grain yield and low total GHG emissions,banded BBU showed a low yield-scaled GHG(GHG emissions divided by grain yield)comparable to that under CK in both years.Overall,our study suggested that N management synchronized with rice demand and contributing to a high NUE tended to minimize yield-scaled GHG.Broadcast CRU can hardly substitute for CK in terms of either grain yield or GHG emissions,but banded BBU is a promising N management strategy for sustaining rice production while minimizing environmental impacts.展开更多
Electrochemical CO_(2)reduction to C_(2)H_(4)can provide a sustainable route to reduce globally accelerating CO_(2)emissions and produce energy-rich chemical feedstocks.However,the poor selectivity in C_(2)H_(4)electr...Electrochemical CO_(2)reduction to C_(2)H_(4)can provide a sustainable route to reduce globally accelerating CO_(2)emissions and produce energy-rich chemical feedstocks.However,the poor selectivity in C_(2)H_(4)electrosynthesis limits its implementation in industrially interesting processes.Herein,we report a composite structured catalyst composed of Ag and Cu_(2)O with different crystal faces to achieve highly efficient reduction of CO_(2)to C_(2)H_(4).The catalyst composed of Ag and octahedral Cu_(2)O enclosed with(111)facet exhibits the best CO_(2)electroreduction performance,with the Faradaic efficiency(FE)and partial current density reaching 66.8%and 17.8 mA cm2 for C_(2)H_(4)product at-1.2 VRHE in 0.5 M KHCO_(3),respectively.Physical characterization and electrochemical test analysis indicate that the high selectivity for C_(2)H_(4)product stems from the synergistic effect of crystal faces control engineering and tandem catalysis.Specifically,Ag can provide optimal availability of CO intermediate by suppressing hydrogen evolution;subsequently,C-C coupling is promoted on the intimate surface of Cu_(2)O with facetdependent selectivity.The insights gained from this work may be beneficial for designing efficient multicomponent catalysts for improving the selectivity of electrochemical CO_(2)reduction reaction to generate C2þproducts.展开更多
基金supported by the General Project of Top-Design of Multi-Scale Nature-Social ModelsData Support and Decision Support System for NSFC Carbon Neutrality Major Project(42341202)the Basic Scientific Research Fund of the Chinese Academy of Meteorological Sciences(2021Z014)。
文摘CO_(2)is one of the most important greenhouse gases(GHGs)in the earth’s atmosphere.Since the industrial era,anthropogenic activities have emitted excessive quantities of GHGs into the atmosphere,resulting in climate warming since the 1950s and leading to an increased frequency of extreme weather and climate events.In 2020,China committed to striving for carbon neutrality by 2060.This commitment and China’s consequent actions will result in significant changes in global and regional anthropogenic carbon emissions and therefore require timely,comprehensive,and objective monitoring and verification support(MVS)systems.The MVS approach relies on the top-down assimilation and inversion of atmospheric CO_(2)concentrations,as recommended by the Intergovernmental Panel on Climate Change(IPCC)Inventory Guidelines in 2019.However,the regional high-resolution assimilation and inversion method is still in its initial stage of development.Here,we have constructed an inverse system for carbon sources and sinks at the kilometer level by coupling proper orthogonal decomposition(POD)with four-dimensional variational(4DVar)data assimilation based on the weather research and forecasting-greenhouse gas(WRF-GHG)model.Our China Carbon Monito ring and Verification Support at the Regional level(CCMVS-R)system can continuously assimilate information on atmospheric CO_(2)and other related information and realize the inversion of regional and local anthropogenic carbon emissions and natural terrestrial ecosystem carbon exchange.Atmospheric CO_(2)data were collected from six ground-based monito ring sites in Shanxi Province,China to verify the inversion effect of regio nal anthropogenic carbon emissions by setting ideal and real experiments using a two-layer nesting method(at 27 and 9 km).The uncertainty of the simulated atmospheric CO_(2)decreased significantly,with a root-mean-square error of CO_(2)concentration values between the ideal value and the simulated after assimilation was close to 0.The total anthropogenic carbon emissions in Shanxi Province in 2019 from the assimilated inversions were approximately 28.6%(17%-38%)higher than the mean of five emission inventories using the bottomup method,showing that the top-down CCMVS-R system can obtain more comprehensive information on anthropogenic carbon emissions.
文摘In this work, the zeolite-Y was ion-exchanged by introducing silver cations into the framework of microsized nano-porous sodium zeolite-Y using a liquid-phase ion exchanged method. The Ag+ion-exchanged zeolite, was then embedded into the Matrimid5218 matrix to form novel mixed matrix membranes(MMMs). The particles and MMMs were characterized by ultraviolet-visible diffuse reflectance spectroscopy(UV–vis DRS), N2adsorption–desorption isotherm, X-ray diffraction(XRD), Fourier transform infrared(FTIR) and scanning electron microscopy(SEM). Furthermore, the effects of filler content(0–20wt%) on pure and mixed gas experiments, feed pressure(2–20 bar) and operating temperature(35–75 oC)on CO2/CH4transport properties of Matrimid/Ag Y MMMs were considered. Characterization results confirmed an appropriate ion-exchange treatment of the zeolites. The SEM results confirmed the superior interfacial adhesion between polymer and zeolites, particularly in the case of Matrimid/Ag Y membranes.This is due to the proper silverous zeolite/Matrimid functional groups’ interactions. The gas permeation results showed that the CO2permeability increased about 123%, from 8.34 Barrer for pure Matrimid to18.62 Barrer for Matrimid/Ag Y(15 wt%). The CO2/CH4selectivity was improved about 66%, from 36.3 for Matrimid to 60.1 for Matrimid/Ag Y(15 wt%). The privileged gas separation performance of Matrimid/Ag Y(15 wt%) was the result of a combined effect of facilitated transport mechanism of Ag+ions as well as the intrinsic surface diffusion mechanism of Y-type zeolite. In order to survey the possibility of using the developed MMMs in industry, the CO2-induced plasticization effect and mixed gas experiment were accomplished. It was deduced that the fabricated MMMs could maintain the superior performance in actual operating conditions.
文摘Reactions between CH_4 and CO_2 under the action of continuous microwave discharge at atmospheric pressure were studied in a special homemade reactor. The main products were CO and H2, while acetylene and ethylene were also found in the products. Experimental results show that conversions of CH4 and CO2 could be higher than 90% without the presence of any catalyst. Effects of CO2/CH4 molar ratio and total flow rate of the feed gas on the reaction were also investigated.
基金financially supported by the National Natural Science Foundation of ChinaChina(Nos.22378424,22127812,U20B6005,52004136)+1 种基金the Science Foundation of China University of Petroleum,Beijing(No.2462023BJRC017)Hunan Provincial Department of Education Scientific Research Project(No.22B0310)。
文摘Since hydrate resources play a part of the stratigraphic framework structure in sediments,establishing a safe and economic method for hydrates exploitation remains the primary challenge to this day.Among the proposed methods,the spontaneous displacement of CH_(4) from hydrate cages by CO_(2) seems to be a perfect mechanism to address gas production and CO_(2) storage,especially in today's strong demand for carbon reduction and replacing clean energy.After extensive lab researches,in the past decade,injecting a mixture of CO_(2) and small molecule gas has become a key means to enhance displacement efficiency and has great potential for application.However,there is a lack of in-depth research on gas flow in the reservoir,while the injected gas always passes through low-saturated hydrate areas with high permeability and then occurs gas channel in a short term,finally resulting in the decreases in gas production efficiency and produced gas quality.Therefore,we explored a new injection-production mode of alternate injection of N2 and CO_(2) in order to fully coordinate the advantages of N_(2) in enhanced hydrate decomposition and CO_(2) in solid storage and heat compensation.These alternate"taking"and"storing"processes perfectly repair the problem of the gas channel,achieving self-regulation effect of CH_(4) recovery and CO_(2) storage.The 3-D experimental results show that compared to the mixed gas injection,CH_(4) recovery is increased by>50%and CO_(2) storage is increased by>70%.Additionally,this alternate injection mode presented a better performance in CH_(4) concentration of produced gas and showed outstanding N_(2) utilization efficiency.Further,we analyzed its self-adaptive gas flow mechanism and proposed an application model of"one injection and multiple production".We look forward to this study accelerating the application of CO_(2)-CH_(4) replacement technology.
基金financially supported by the National Natural Science Foundation of China,China(22378424,52004136,22127812,U20B6005)the Science Foundation of China University of Petroleum Beijing(2462023BJRC017)Hunan Provincial Department of Education Scientific Research Project(22B0310).
文摘Carbon emission reduction and clean energy development are urgent demands for mankind in the coming decades.Exploring an efficient CO_(2) storage method can significantly reduce CO_(2) emissions in the short term.In this study,we attempted to construct sediment samples with different residual CH_(4) hydrate amounts and reservoir conditions,and then investigate the potentials of both CO_(2) storage and enhanced CH_(4) recovery in depleted gas hydrate deposits in the permafrost and ocean zones,respectively.The results demonstrate that CO_(2) hydrate formation rate can be significantly improved due to the presence of residual hydrate seeds;However,excessive residual hydrates in turn lead to the decrease in CO_(2) storage efficiency.Affected by the T-P conditions of the reservoir,the storage amount of liquid CO_(2) can reach 8 times that of gaseous CO_(2),and CO_(2) stored in hydrate form reaches 2-4 times.Additionally,we noticed two other advantages of this method.One is that CO_(2) injection can enhance CH_(4) recovery rate and increases CH_(4) recovery by 10%-20%.The second is that hydrate saturation in the reservoir can be restored to 20%-40%,which means that the solid volume of the reservoir avoids serious shrinkage.Obviously,this is crucial for protecting the goaf stability.In summary,this approach is greatly promising for high-efficient CO_(2) storage and safe exploitation of gas hydrate.
基金jointly supported by the Key R&D Program of Jiangsu ProvinceChina(BE2022338)+3 种基金the Jiangsu Agriculture Science and Technology Innovation FundChina(CX(20)1012)the National Natural Science Foundation of China(31801293)a project funded by the Priority Academic Program Development of Jiangsu Higher Education Institutions(PAPD),China。
文摘Biaxia lrotary tillage in dryland(DBRT)can complete biaxial rotary tillage with straw incorporation,secondary suppression,and ditching,and it has been previously studied in direct-seeded rice and wheat.However,the effects of DBRT on the mechanically transplanted rice yield and greenhouse gas emissions remain unclear.To evaluate the effects of DBRT on improving the food security of mechanically transplanted rice and reducing the greenhouse gas emissions,we conducted an experiment for two years with wheat straw incorporation.Three tillage methods were set up:DBRT,uniaxial rotary tillage in dryland and paddy(DPURT),and uniaxial rotary tillage in paddy(PURT).The results showed that compared with DPURT and PURT,DBRT increased the yield of machine-transplanted rice by 7.5-11.0%and 13.3-26.7%,respectively,while the seasonal cumulative CH_(4) emissions were reduced by 13.9-21.2%and 30.2-37.0%,respectively,and the seasonal cumulative N_(2)O emissions were increased by 13.5-28.6%and 50.0-73.1%,respectively.Consequently,DBRT reduced the global warming potential by 10.7-15.5%and 23.7-28.6%,respectively,andtheyield-scaledglobalwarmingpotentialby18.2-21.8%and36.4-39.3%,respectively,compared to DPURT and PURT.These results were mainly related to the fact that DBRT significantly reduced soil bulk density and increased soil redox potential(Eh).Therefore,implementing DBRT in machine-transplanted rice fields is feasible,which cannot only increase the rice yield,but also reduce the greenhouse gas emissions.
基金financially supported by the Scientific and Technological Plan Projects of Guangzhou City(202103040001),P.R.Chinathe Project of Science and Technology Department of Henan Province(222102240074)the Key Research Programs of Higher Education Institutions of Henan Province(24B150009)。
文摘Lithium-ion batteries(LIBs)featuring a Ni-rich cathode exhibit increased specific capacity,but the establishment of a stable interphase through the implementation of a functional electrolyte strategy remains challenging.Especially when the battery is operated under high temperature,the trace water present in the electrolyte will accelerate the hydrolysis of the electrolyte and the resulting HF will further erode the interphase.In order to enhance the long-term cycling performance of graphite/LiNi_(0.8)Co_(0.1)Mn_(0.1)O_(2)(NCM811)LIBs,herein,Tolylene-2,4-diisocyanate(TDI)additive containing lone-pair electrons is employed to formulate a novel bifunctional electrolyte aimed at eliminating H_(2)O/HF generated at elevated temperature.After 1000 cycles at 25℃,the battery incorporating the TDI-containing electrolyte exhibits an impressive capacity retention of 94%at 1 C.In contrast,the battery utilizing the blank electrolyte has a lower capacity retention of only 78%.Furthermore,after undergoing 550 cycles at 1 C under45℃,the inclusion of TDI results in a notable enhancement of capacity,increasing it from 68%to 80%.This indicates TDI has a favorable influence on the cycling performance of LIBs,especially at elevated temperatures.The analysis of the film formation mechanism suggests that the lone pair of electrons of the isocyanate group in TDI play a crucial role in inhibiting the generation of H_(2)O and HF,which leads to the formation of a thin and dense interphase.The existence of this interphase is thought to substantially enhance the cycling performance of the LIBs.This work not only improves the performance of graphite/NCM811 batteries at room temperature and high temperature by eliminating H_(2)O/HF but also presents a novel strategy for advancing functional electrolyte development.
文摘Using the closed chamber technique, the in situ measurements of N2O and CH4 fluxes was conducted in a broad-leaved Korean pine mixed forest ecosystem in Changbai Mountain, China. from June 1994 to october 1995. The relationships between fluxes (N2O and CH4) and some major environmental factors (temperature, soil water content and soil availabIe nitrogen) were studied. A significant positive correlation between Nzo emission and air/soil temperature was observed, but no significant correIation was found between N2O emission and soil water content (SWC). This result showed that temperature was an important controlling factor of N2O flux. There was a significant correlation between CH4 uptake and SWC, but no significant correlation was found between CH4 uptake and temperature. This suggested SWC was an important factor controlling CH4 uptake. The very significant negative correlation between logarithmic N2O flux and soil nitrate concentration, significant negative correlation between CH4 flux and soil ammonium content were also found.
文摘Soil samples were taken from depth of 0-12cm in the virgin broad- leaved/Korean pine mixed forest in Changbai Mountain in April, 2000. 20 μL·L-1 and 200 μL·L-1 CH4 and N2O concentration were supplied for analysis. Laboratory study on CH4 oxidation and N2O emission in forest soil showed that fresh soil sample could oxidize atmospheric methane and product N2O. Air-dried soil sample could not oxidize atmospheric methane, but could produCt N2O. However, it could oxidize the supplied methane quickly when its concentration was higher than 20 μL·L-1. The oxidation rate of methane was increased with its initial concentration. An addition of water to dry soil caused large pulse of N2O emissions within 2 hours. There were curvilinear correlations between N2O emission and temperature (r2=0.706, p <0.05), and between N2O emission andtwater content (r2=0.2968. p <0.05). These suggested temperature and water content were important factors controlling N2O emission. The correlation between CH4 oxidization and temperature was also found while CH4 was supplied 200 μL·L-1 (r2 =0.3573, p<0.05). Temperature was an important f8Ctor controlling CH4 oxidation. However, when 20 μL·L-1 CH4 was supplied, there was no correlation among CH4 oxidization, N2O emission, temperature and water content.
基金partially financially supported by NSF CBET-2033343.J.Z.thanks the support from National Natural Science Foundation of China(52172293,51772072,and 51672065)the Fundamental Research Funds for the Central Universities(JZ2021HGQB0282 and PA2021GDSK0088)+3 种基金financial support from the Key R&D Projects of Anhui Province(202104b11020016)the 111 Project(B18018)the National Synchrotron Light Source II,a U.S.Department of Energy(DOE)Office of Science User Facility operated for the DOE Office of Science by Brookhaven National Laboratory under Contract No.DE-SC0012704the use of facilities within the Eyring Materials Center at Arizona State University supported in part by NNCI-ECCS-1542160.
文摘Regulating the selectivity toward a target hydrocarbon product is still the focus of CO_(2)electroreduction.Here,we discover that the original surface Cu species in Cu gas-diffusion electrodes plays a more important role than the surface roughness,local pH,and facet in governing the selectivity toward C_(1)or C_(2)hydrocarbons.The selectivity toward C_(2)H_(4) progressively increases,while CH_(4) decreases steadily upon lowering the Cu oxidation species fraction.At a relatively low electrodeposition voltage of 1.5 V,the Cu gas-diffusion electrode with the highest Cu^(δ+)/Cu^(0)ratio favors the pathways of∗CO hydrogenation to form CH_(4) with maximum Faradaic efficiency of 65.4%and partial current density of 228 mA cm^(−2)at−0.83 V vs RHE.At 2.0 V,the Cu gas-diffusion electrode with the lowest Cu^(δ+)/Cu^(0)ratio prefers C-C coupling to form C_(2)+products with Faradaic efficiency topping 80.1%at−0.75 V vs RHE,where the Faradaic efficiency of C_(2)H_(4) accounts for 46.4%and the partial current density of C_(2)H_(4) achieves 279 mA cm^(−2).This work demonstrates that the selectivity from CH_(4) to C_(2)H_(4) is switchable by tuning surface Cu species composition of Cu gas-diffusion electrodes.
文摘The cobalt precursor affects the catalytic performance of Co/SiO_2 catalyst remarkably. The catalyst prepared from cobalt acetate exhibits excellent activity, stability and resistance to carbon deposition.
基金supported by the Natural Science Foundation of Jiangsu Province(BK20200539)Postdoctoral Research Foundation of China(2019M661863)Jiangsu Provincial Key Research and Development Program(BE2019377,BE2019343)。
文摘Controlled-release urea(CRU)is widely reported to supply crop nitrogen(N)demand with one basal application,thus effectively replacing split applications of urea without diminishing grain yield and N use efficiency(NUE).However,its use for replacement for high-yield split applications of urea(CK)for rice is untested.In addition,the degree to which greenhouse gas(GHG)emissions in rice systems are affected when CRU is substituted for CK remains unclear.During 2017 and 2018,we sampled plant growth and gas emissions in a rice paddy field treated with three CRU types(sulfur-coated urea[SCU],polymer-coated urea[PCU],and bulk blended CRU[BBU])applied via two methods(surface broadcasting on the soil and subsurface banding at 5 cm depth),with CK as a control.The three CRUs led to different soil NH_(4)^(+)-N dynamics,and the N supply pattern under BBU was more beneficial for rice seedling establishment than under SCU and PCU,resulting in grain yield and NUE comparable to those under CK.CRU type showed no significant effect on either CH_(4) emissions or N_(2)O emissions,and broadcast CRUs exhibited significantly higher total GHG emissions than CK.However,banded CRUs significantly reduced the total GHG emissions in comparison with broadcast CRUs,by 9.2%averaged across the two years.Reduced CH_(4) emissions,particularly during the period prior to the middle drainage,contributed largely to the GHG difference.With comparably high grain yield and low total GHG emissions,banded BBU showed a low yield-scaled GHG(GHG emissions divided by grain yield)comparable to that under CK in both years.Overall,our study suggested that N management synchronized with rice demand and contributing to a high NUE tended to minimize yield-scaled GHG.Broadcast CRU can hardly substitute for CK in terms of either grain yield or GHG emissions,but banded BBU is a promising N management strategy for sustaining rice production while minimizing environmental impacts.
基金This work was supported by the University of Science and Technology Beijing.DG acknowledges the financial support from 111 Project(no.B170003)Foshan Science and Technology Innovation Project(no.2018IT100363).
文摘Electrochemical CO_(2)reduction to C_(2)H_(4)can provide a sustainable route to reduce globally accelerating CO_(2)emissions and produce energy-rich chemical feedstocks.However,the poor selectivity in C_(2)H_(4)electrosynthesis limits its implementation in industrially interesting processes.Herein,we report a composite structured catalyst composed of Ag and Cu_(2)O with different crystal faces to achieve highly efficient reduction of CO_(2)to C_(2)H_(4).The catalyst composed of Ag and octahedral Cu_(2)O enclosed with(111)facet exhibits the best CO_(2)electroreduction performance,with the Faradaic efficiency(FE)and partial current density reaching 66.8%and 17.8 mA cm2 for C_(2)H_(4)product at-1.2 VRHE in 0.5 M KHCO_(3),respectively.Physical characterization and electrochemical test analysis indicate that the high selectivity for C_(2)H_(4)product stems from the synergistic effect of crystal faces control engineering and tandem catalysis.Specifically,Ag can provide optimal availability of CO intermediate by suppressing hydrogen evolution;subsequently,C-C coupling is promoted on the intimate surface of Cu_(2)O with facetdependent selectivity.The insights gained from this work may be beneficial for designing efficient multicomponent catalysts for improving the selectivity of electrochemical CO_(2)reduction reaction to generate C2þproducts.