Electrocatalyst designs based on oxophilic foreign atoms are considered a promising approach for developing efficient pH-universal hydrogen evolution reaction(HER)electrocatalysts by overcoming the sluggish alkaline H...Electrocatalyst designs based on oxophilic foreign atoms are considered a promising approach for developing efficient pH-universal hydrogen evolution reaction(HER)electrocatalysts by overcoming the sluggish alkaline HER kinetics.Here,we design ternary transition metals-based nickel telluride(Mo WNi Te)catalysts consisting of high valence non-3d Mo and W metals and oxophilic Te as a first demonstration of non-precious heterogeneous electrocatalysts following the bifunctional mechanism.The Mo WNi Te showed excellent HER catalytic performance with overpotentials of 72,125,and 182 mV to reach the current densities of 10,100,and 1000 mA cm^(-2),respectively,and the corresponding Tafel slope of 47,52,and 58 mV dec-1in alkaline media,which is much superior to commercial Pt/C.Additionally,the HER performance of Mo WNi Te is well maintained up to 3000 h at the current density of 100 mA cm^(-2).It is further demonstrated that the Mo WNi Te exhibits remarkable HER activities with an overpotential of 45 mV(31 mV)and Tafel slope of 60 mV dec-1(34 mV dec-1)at 10 mA cm^(-2)in neutral(acid)media.The superior HER performance of Mo WNi Te is attributed to the electronic structure modulation,inducing highly active low valence states by the incorporation of high valence non-3d transition metals.It is also attributed to the oxophilic effect of Te,accelerating water dissociation kinetics through a bifunctional catalytic mechanism in alkaline media.Density functional theory calculations further reveal that such synergistic effects lead to reduced free energy for an efficient water dissociation process,resulting in remarkable HER catalytic performances within universal pH environments.展开更多
Intensive farming is a primary cause of increased sediment and associated nitrogen(N)and phosphorus(P)loads in surface water systems.Determining their contributing sources,pathways and loads present major challenges i...Intensive farming is a primary cause of increased sediment and associated nitrogen(N)and phosphorus(P)loads in surface water systems.Determining their contributing sources,pathways and loads present major challenges in the high-intensity agricultural catchments.Herein,we quantify the sediment sources and magnitude of sediment total N and total P from different sources using a novel application of compound-specific stable isotope(CSSI)and fallout radionuclides(FRNs)of^(137)cs and^(210)pbex in an intensive agricultural catchment in North China.Sediment sources from surface and sub-surface soils were estimated from FRNs fingerprint and accounted for 62±7%and 38±7%respectively,while surface soil from land uses that originated from hillslope were identified by CssI fingerprint.Using a novel application of FRNs and CSSI sediment fingerprinting techniques,the dominant sediment source was derived from maize farmland(44±0.1%),followed by channel bank(38±7%).The sedimentation rate(13.55±0.30 t ha^(-1)yr^(-1))was quantifed by the^(137)cs cores(0-60 cm)at the outlet of this catchment.The total N and total P in sediment were both mostly derived from maize farmland and least from channel banks.The channel banks are significant sediment sources but contribute little to the input of sediment N and P for eutrophication.It implies that chemically-applied farmlands are the main hotspots for catchment erosion control and pollution prevention.The novel application of FRNs and CSSI techniques cost-effectively quantified sediment N and P loads from different sources with a single visit to the catchment,enabling rapid assessment for optimizing soil conservation strategies and land management practices.展开更多
As the introduction of triple-frequency signals in GNSS,the multi-frequency ionosphere correction technology has been fast developing.References indicate that the triple-frequency second order ionosphere correction is...As the introduction of triple-frequency signals in GNSS,the multi-frequency ionosphere correction technology has been fast developing.References indicate that the triple-frequency second order ionosphere correction is worse than the dual-frequency first order ionosphere correction because of the larger noise amplification factor.On the assumption that the variances of three frequency pseudoranges were equal,other references presented the triple-frequency first order ionosphere correction,which proved worse or better than the dual-frequency first order correction in different situations.In practice,the PN code rate,carrier-to-noise ratio,parameters of DLL and multipath effect of each frequency are not the same,so three frequency pseudorange variances are unequal.Under this consideration,a new unequal-weighted triple-frequency first order ionosphere correction algorithm,which minimizes the variance of the pseudorange ionosphere-free combination,is proposed in this paper.It is found that conventional dual-frequency first-order correction algorithms and the equal-weighted triple-frequency first order correction algorithm are special cases of the new algorithm.A new pseudorange variance estimation method based on the three carrier combination is also introduced.Theoretical analysis shows that the new algorithm is optimal.The experiment with COMPASS G3 satellite observations demonstrates that the ionosphere-free pseudorange combination variance of the new algorithm is smaller than traditional multi-frequency correction algorithms.展开更多
Radionuclide fallout during nuclear accidents on the land may impair the atmosphere, contaminate farmland soils and crops, and can even reach the groundwater. Previous research focused on the field distribution of dep...Radionuclide fallout during nuclear accidents on the land may impair the atmosphere, contaminate farmland soils and crops, and can even reach the groundwater. Previous research focused on the field distribution of deposited radionuclides in farmland soils, but details of the amounts of radionuclides in the plough layer and the changes in their proportional distribution in the soil profile with time are still inadequate. In this study, a lysimeter experiment was conducted to determine the vertical migration of 137Cs and 60Co in brown and aeolian sandy soils, collected from the farmlands adjoining Shidaowan Nuclear Power Plant(NPP) in eastern China, and to identify the factors influencing their migration depths in soil. At the end of the experiment(800 d), >96% of added 137Cs and 60Co were retained in the top 0–20 cm soil layer of both soils;very little 137Cs or 60Co initially migrated to 20–30 cm, but their amounts at this depth increased with time. The migration depth of 137Cs was greater in the aeolian sandy soil than in the brown soil during 0–577 d, but at the end of the experiment, 137Cs migrated to the same depth(25 cm) in both soils. Three phases on the vertical migration rate(v) of 60Co in the aeolian sandy soil can be identified: an initial rapid movement(0–355 d, v = 219 ± 17 mm year-1), followed by a steady movement(355–577 d, v = 150 ± 24 mm year-1) and a very slow movement(577–800 d, v = 107 ± 7 mm year-1). In contrast, its migration rate in the brown soil(v = 133 ± 17 mm year-1) was steady throughout the 800-d experimental period. The migration of both 137Cs and 60Co in the two soils appears to be regulated by soil clay and silt fractions that provide most of the soil surface area, soil organic carbon(SOC), and soil pH, which were manifested by the solid-liquid distribution coefficient of 137Cs and 60Co. The results of this study suggest that most 137Cs and 60Co remained within the top layer(0–20 cm depth) of farmland soils following a simulated NPP accident, and little reached the subsurface(20–30 cm depth). Fixation of radionuclides onto clay minerals may limit their migration in soil, but some could be laterally distributed by soil erosion and taken up by crops, and migrate into groundwater in a high water table level area after several decades.Remediation measures, therefore, should focus on reducing their impact on the farmland soils, crops, and water.展开更多
基金supported through the National Research Foundation of Korea(NRF)funded by the Ministry of Science and ICT(2022M3H4A1A04096478)the support from the Supercomputing Center of Wuhan University。
文摘Electrocatalyst designs based on oxophilic foreign atoms are considered a promising approach for developing efficient pH-universal hydrogen evolution reaction(HER)electrocatalysts by overcoming the sluggish alkaline HER kinetics.Here,we design ternary transition metals-based nickel telluride(Mo WNi Te)catalysts consisting of high valence non-3d Mo and W metals and oxophilic Te as a first demonstration of non-precious heterogeneous electrocatalysts following the bifunctional mechanism.The Mo WNi Te showed excellent HER catalytic performance with overpotentials of 72,125,and 182 mV to reach the current densities of 10,100,and 1000 mA cm^(-2),respectively,and the corresponding Tafel slope of 47,52,and 58 mV dec-1in alkaline media,which is much superior to commercial Pt/C.Additionally,the HER performance of Mo WNi Te is well maintained up to 3000 h at the current density of 100 mA cm^(-2).It is further demonstrated that the Mo WNi Te exhibits remarkable HER activities with an overpotential of 45 mV(31 mV)and Tafel slope of 60 mV dec-1(34 mV dec-1)at 10 mA cm^(-2)in neutral(acid)media.The superior HER performance of Mo WNi Te is attributed to the electronic structure modulation,inducing highly active low valence states by the incorporation of high valence non-3d transition metals.It is also attributed to the oxophilic effect of Te,accelerating water dissociation kinetics through a bifunctional catalytic mechanism in alkaline media.Density functional theory calculations further reveal that such synergistic effects lead to reduced free energy for an efficient water dissociation process,resulting in remarkable HER catalytic performances within universal pH environments.
基金supported by the International Atomic Energy Agency through coordination research projects(CRP)under Research Contract No.23008 and technical cooperation project(TCP)RAS 5084,and the Central Public-interest Scientific Institution Basal Research Fund(No.BSRF202004)Funding for AC to collaborate on this work was provided by the High-end Foreign Experts Recruitment Program from State of Administration of Foreign Experts Affairs of ChinaThis work was partly supported by the Science and Technology Major Project of Guangxi(Guike AA17204078).
文摘Intensive farming is a primary cause of increased sediment and associated nitrogen(N)and phosphorus(P)loads in surface water systems.Determining their contributing sources,pathways and loads present major challenges in the high-intensity agricultural catchments.Herein,we quantify the sediment sources and magnitude of sediment total N and total P from different sources using a novel application of compound-specific stable isotope(CSSI)and fallout radionuclides(FRNs)of^(137)cs and^(210)pbex in an intensive agricultural catchment in North China.Sediment sources from surface and sub-surface soils were estimated from FRNs fingerprint and accounted for 62±7%and 38±7%respectively,while surface soil from land uses that originated from hillslope were identified by CssI fingerprint.Using a novel application of FRNs and CSSI sediment fingerprinting techniques,the dominant sediment source was derived from maize farmland(44±0.1%),followed by channel bank(38±7%).The sedimentation rate(13.55±0.30 t ha^(-1)yr^(-1))was quantifed by the^(137)cs cores(0-60 cm)at the outlet of this catchment.The total N and total P in sediment were both mostly derived from maize farmland and least from channel banks.The channel banks are significant sediment sources but contribute little to the input of sediment N and P for eutrophication.It implies that chemically-applied farmlands are the main hotspots for catchment erosion control and pollution prevention.The novel application of FRNs and CSSI techniques cost-effectively quantified sediment N and P loads from different sources with a single visit to the catchment,enabling rapid assessment for optimizing soil conservation strategies and land management practices.
文摘As the introduction of triple-frequency signals in GNSS,the multi-frequency ionosphere correction technology has been fast developing.References indicate that the triple-frequency second order ionosphere correction is worse than the dual-frequency first order ionosphere correction because of the larger noise amplification factor.On the assumption that the variances of three frequency pseudoranges were equal,other references presented the triple-frequency first order ionosphere correction,which proved worse or better than the dual-frequency first order correction in different situations.In practice,the PN code rate,carrier-to-noise ratio,parameters of DLL and multipath effect of each frequency are not the same,so three frequency pseudorange variances are unequal.Under this consideration,a new unequal-weighted triple-frequency first order ionosphere correction algorithm,which minimizes the variance of the pseudorange ionosphere-free combination,is proposed in this paper.It is found that conventional dual-frequency first-order correction algorithms and the equal-weighted triple-frequency first order correction algorithm are special cases of the new algorithm.A new pseudorange variance estimation method based on the three carrier combination is also introduced.Theoretical analysis shows that the new algorithm is optimal.The experiment with COMPASS G3 satellite observations demonstrates that the ionosphere-free pseudorange combination variance of the new algorithm is smaller than traditional multi-frequency correction algorithms.
基金the IAEA Project (No. 18176)the National Science and Technology Major Projects of China (No. 2013ZX06002001) that supported this workpart of the project supported by the National Key Research and Development Program of China (No. 2017YFC0505402)。
文摘Radionuclide fallout during nuclear accidents on the land may impair the atmosphere, contaminate farmland soils and crops, and can even reach the groundwater. Previous research focused on the field distribution of deposited radionuclides in farmland soils, but details of the amounts of radionuclides in the plough layer and the changes in their proportional distribution in the soil profile with time are still inadequate. In this study, a lysimeter experiment was conducted to determine the vertical migration of 137Cs and 60Co in brown and aeolian sandy soils, collected from the farmlands adjoining Shidaowan Nuclear Power Plant(NPP) in eastern China, and to identify the factors influencing their migration depths in soil. At the end of the experiment(800 d), >96% of added 137Cs and 60Co were retained in the top 0–20 cm soil layer of both soils;very little 137Cs or 60Co initially migrated to 20–30 cm, but their amounts at this depth increased with time. The migration depth of 137Cs was greater in the aeolian sandy soil than in the brown soil during 0–577 d, but at the end of the experiment, 137Cs migrated to the same depth(25 cm) in both soils. Three phases on the vertical migration rate(v) of 60Co in the aeolian sandy soil can be identified: an initial rapid movement(0–355 d, v = 219 ± 17 mm year-1), followed by a steady movement(355–577 d, v = 150 ± 24 mm year-1) and a very slow movement(577–800 d, v = 107 ± 7 mm year-1). In contrast, its migration rate in the brown soil(v = 133 ± 17 mm year-1) was steady throughout the 800-d experimental period. The migration of both 137Cs and 60Co in the two soils appears to be regulated by soil clay and silt fractions that provide most of the soil surface area, soil organic carbon(SOC), and soil pH, which were manifested by the solid-liquid distribution coefficient of 137Cs and 60Co. The results of this study suggest that most 137Cs and 60Co remained within the top layer(0–20 cm depth) of farmland soils following a simulated NPP accident, and little reached the subsurface(20–30 cm depth). Fixation of radionuclides onto clay minerals may limit their migration in soil, but some could be laterally distributed by soil erosion and taken up by crops, and migrate into groundwater in a high water table level area after several decades.Remediation measures, therefore, should focus on reducing their impact on the farmland soils, crops, and water.