Phosphate removal is crucial for eutrophication control and water quality improvement.Electro-assisted adsorption,an eco-friendly elec-trosorption process,exhibited a promising potential for wastewater treatment.Howev...Phosphate removal is crucial for eutrophication control and water quality improvement.Electro-assisted adsorption,an eco-friendly elec-trosorption process,exhibited a promising potential for wastewater treatment.However,there are few works focused on phosphate electro-sorption,and reported electrodes cannot attach satisfactory removal capacities and rates.Herein,electro-assisted adsorption of phosphate via in-situ construction of La active centers on hierarchically porous carbon(LaPC)has been originally demonstrated.The resulted LaPC composite not only possessed a hierarchically porous structure with uniformly dispersed La active sites,but also provided good conductivity for interfacial electron transfer.The LaPC electrode achieved an ultrahigh phosphate electrosorption capability of 462.01 mg g^(-1) at 1 V,outperforming most existing electrodes.The superior phosphate removal performance originates from abundant active centers formed by the coupling of electricfield and capture sites.Besides,the stability and selectivity toward phosphate capture were maintained well even under comprehensive conditions.Moreover,a series of kinetics and isotherms models were employed to validate the electrosorption process.This work demonstrates a deep understanding and promotes a new level of phosphate electrosorption.展开更多
The objectives of this work were to evaluate the surgical activities carried out in the general surgery department of the Reference Health Center of Commune I of Bamako, to describe the sociodemographic characteristic...The objectives of this work were to evaluate the surgical activities carried out in the general surgery department of the Reference Health Center of Commune I of Bamako, to describe the sociodemographic characteristics of the operated patients, to determine the main pathologies encountered and to evaluate qualitatively the result of the treatment. In order to improve performance, and the quality of care, and to identify common pathologies in the surgical department, we undertook a retrospective study on surgical activities from January 2009 to December 2010. At the end of this study, out of 474 men and 187 women (equal sex ratio 2.53);we were able to determine the frequency of surgical pathologies. Farmers, housewives and pupils/students were the most represented with 25.9% respectively;20% and 13.3%. The most frequently observed pathologies were wall hernia (44.8%), prostate adenoma (12%) and acute appendicitis (10.5%). The average length of hospitalization was 3.43 days. Infectious complications affected 25 patients (3.8% of cases) and a death rate of 0.45% (i.e. 3 patients). The average cost of care was 53,500 FCFA. Indeed, the reality of surgical practice in health centers was not the same because of the level of skills of practicing surgeons.展开更多
With the further advancement of the“National Fitness”strategy and the continuous development of the information age,the National Fitness Activity Centers have become more comprehensive.The comprehensiveness is refle...With the further advancement of the“National Fitness”strategy and the continuous development of the information age,the National Fitness Activity Centers have become more comprehensive.The comprehensiveness is reflected in the design of diversified sports functions and spaces.The article serves to explore the comprehensive development trend of National Fitness Activity Centers.Through summarizing and sorting out domestic and foreign cases,the trend of the comprehensive development of National Fitness Activity Centers is predicted at three levels:industry,city,and individual functions.展开更多
Deactivation mechanism of Cr-Al2O3catalyst and the interaction of Cr-A1 in the dehydrogenation of isobutane, as well as the nature of the catalytic active center, were studied using XRD, SEM, XPS, H2-TPR, isobutane-TP...Deactivation mechanism of Cr-Al2O3catalyst and the interaction of Cr-A1 in the dehydrogenation of isobutane, as well as the nature of the catalytic active center, were studied using XRD, SEM, XPS, H2-TPR, isobutane-TPR and TPO techniques. The results revealed that the deactivation of Cr-Al2O3 catalyst was mainly caused by carbon deposition on its surface. The Cr3+ ion could not be reduced by hydrogen but could be reduced to Cr2+ by hydrocarbons and monoxide carbon. The active center for isobutane dehydrogenation could be Cr2+/Cr3+ produced from Cr6+ by the on line reduction of hydrocarbon and carbon monoxide. The binding energy of Al3+ was strongly affected by the state of chromium cations in the catalysts.展开更多
The composition distribution (CD) and microisotacticity distribution (ID) of propene/1-hexene copolymer synthesized by MgCl2/DIBP/TiCl4 (DIBP: diisobutyl phthalate) were determined by fractionating the copolymers acco...The composition distribution (CD) and microisotacticity distribution (ID) of propene/1-hexene copolymer synthesized by MgCl2/DIBP/TiCl4 (DIBP: diisobutyl phthalate) were determined by fractionating the copolymers according to crystallinity and characterizing the fractions by (CNMR)-C-13. The effects of two alkoxysilane donors, triethoxyphenylsilane (PTES) and dimethoxydi-tert-butylsilane (TBMS), on CD and ID of the copolymers were compared. Three main parts in the CD diagram of each copolymer were distinguished, which were correlated to active center distribution (ACD) based on three groups of different active centers. By studying the changes in l-hexene content, microisotacticity and reactivity ratio product of three typical fractions, the effects of external donor on ACD were better elucidated. It was found that TBMS shows much stronger effects on ACD than PTES. In the former system, most fractions were produced on active centers with relatively lower r(1)r(2), higher reactivity to I-hexene, and higher stereospecificity as compared to the system without external donor. It is concluded that the observed very extensive changes in ACD are mainly resulted by the formation of new types of active centers, possibly by coordination of external donor to certain positions on the catalyst.展开更多
We interpret seismic activity in the active spreading centers of the Salton Trough to indicate 1) a magmatic intrusion in the lower crust beneath the active Brawly, Cerro Prieto, Imperial, Elsinore, and San Jacinto fa...We interpret seismic activity in the active spreading centers of the Salton Trough to indicate 1) a magmatic intrusion in the lower crust beneath the active Brawly, Cerro Prieto, Imperial, Elsinore, and San Jacinto fault systems;and 2) fluids in the upper crust that have been released from that magmatic body. The absence of a magmatic body and fluids at the location of fossil spreading centers along the Sand Hill and Algodones faults ndicated by little or no seismic activity in those areas. We show several lines of evidence to point out that both melt and fluids related to the seismic activity. In particular, receiver function analysis, Vp/Vs ratios, and tomographic data reveal low velocity zones coincide with the location of the active spreading centers. High Vp/Vs ratios and low velocity zones in the lower crust and upper mantle attributed to melt inclusion, while low Vp/Vs ratios in the upper crust are attributed water inclusions. Frequency-mag- nitude distributions characterized by high b-values in southern California;high b-values have also been associated with crustal fluids. A crustal scale model developed from the receiver functions, gravity, and magnetic data supports the existence of a magmatic intrusion within about 20 km of the surface southwest of the Salton Sea, that intrusion extends for 70 km in a SW-NE direction.展开更多
La_(2)O_(3) catalyzed oxidative coupling of methane(OCM) is a promising process that converts methane directly to valuable C_(2)(ethylene and ethane) products. Our online MS transient study results indicate that prist...La_(2)O_(3) catalyzed oxidative coupling of methane(OCM) is a promising process that converts methane directly to valuable C_(2)(ethylene and ethane) products. Our online MS transient study results indicate that pristine surface without carbonate species demonstrates a higher selectivity to C_(2) products, and a lower light-off temperature as well. Further study is focused on carbonate-free La_(2)O_(3) catalyst surface for identification of active oxygen species associated with such products behavior. XPS reveals unique oxygen species with O 1 s binding energy of 531.5 e V correlated with OCM catalytic activity and carbonates removal. However, indicated thermal stability of this species is much higher than the surface peroxide or superoxide structures proposed by earlier computation models. Motivated by experimental results,DFT calculations reveal a new more stable peroxide structure, formed at the subsurface hexacoordinate lattice oxygen sites, with energy 2.18 e V lower than the previous models. The new model of subsurface peroxide provides a perspective for understanding of methyl radicals formation and C_(2) products selectivity in OCM over La_(2)O_(3) catalyst.展开更多
Novel MgCl2-supported Ziegler-Natta (Z-N) catalysts prepared using a new one-pot ball milling method can effectively control the amounts of Ti-loading in the catalysts. Complex GPC data on polypropylene synthesized by...Novel MgCl2-supported Ziegler-Natta (Z-N) catalysts prepared using a new one-pot ball milling method can effectively control the amounts of Ti-loading in the catalysts. Complex GPC data on polypropylene synthesized by these novel catalysts were analyzed using the method of fitting the molecular weight distribution (MWD) curves with a multiple Flory-Schulz function. It was found that multiple active centers exist in these novel catalysts. Detailed study of the effects of the Ti-loadings in the catalysts on the distribution of the active centers showed that the Ti-loadings in the novel MgCl2-supported Z-N catalysts might affect the proportion of each type of active centers; and might be the main factor responsible for the effect of the Ti-loadings on the microstructure, the molecular weight and molecular weight distribution width of the resultant polymer, the catalytic activity and polymerization kinetics.展开更多
There have been reports about Fe ions boosting oxygen evolution reaction(OER)activity of Ni-based catalysts in alkaline conditions,while the origin and reason for the enhancement remains elusive.Herein,we attempt to i...There have been reports about Fe ions boosting oxygen evolution reaction(OER)activity of Ni-based catalysts in alkaline conditions,while the origin and reason for the enhancement remains elusive.Herein,we attempt to identify the activity improvement and discover that Ni sites act as a host to attract Fe(Ⅲ)to form Fe(Ni)(Ⅲ)binary centres,which serve as the dynamic sites to promote OER activity and stability by cyclical formation of intermediates(Fe(Ⅲ)→Fe(Ni)(Ⅲ)→Fe(Ni)-OH→Fe(Ni)-O→Fe(Ni)OOH→Fe(Ⅲ))at the electrode/electrolyte interface to emit O_(2).Additionally,some ions(Co(Ⅱ),Ni(Ⅱ),and Cr(Ⅲ))can also be the active sites to catalyze the OER process on a variety of electrodes.The Fe(Ⅲ)-catalyzed overall water-splitting electrolyzer comprising bare Ni foam as the anode and Pt/Ni-Mo as the cathode demonstrates robust stability for 1600 h at 1000 mA cm^(-2)@~1.75 V.The results provide insights into the ioncatalyzed effects boosting OER performance.展开更多
The study of low-frequency oscillations is an important part of climate variability research. In view of insufficient efforts spent on multidecadal and ENSO-scale changes of the climate, the present paper undertakes s...The study of low-frequency oscillations is an important part of climate variability research. In view of insufficient efforts spent on multidecadal and ENSO-scale changes of the climate, the present paper undertakes study of > 30 year slowly-varying means, called climate base state (CBS), of northern winter AAC’s in the past 100 years and more, with the CBS variability and its temporal evolution investigated, indicating that Aleutian low and Icelandic low (North Pacific high and North American high) experience maximum (minimum) variation in the CBS. The CBS exhibits two modes for its variation. The positive (negative) phase of mode I presents a weak (strong) NAO (North Atlantic Oscillation), a weaker (stronger) NPO (North Pacific Oscillation), a robust (feeble) Siberian high and a quite weak (vigorous) Aleutian low whilst the positive (negative) phase of mode II reveals a feeble (strong) Aleutian low and a weak (robust) Siberian high. Also, the research shows that the recent CBS of northern circulations is in a remarkably negative phase of mode I and a noticeably positive phase of mode II, viz., in the background of slowly-varying circulations of an exceptionally weak Siberian high, an extremely vigorous Aleutian low and an intense NAO. The background field is likely to persist for a matter of 30 years such that northern winter temperature is expected to be in such a warm situation for a long period to follow.展开更多
The number of active centers (C_p)-t and k_p-t profiles of Solvay type TiCl_3 - AlR_3 (R=C_2H_5, i-C_4H_9) or Stauffer AA TiCl_3-Al (C_2H_5)_3 catalyzed 1-octene polymerization were determined by using an acetyl chlor...The number of active centers (C_p)-t and k_p-t profiles of Solvay type TiCl_3 - AlR_3 (R=C_2H_5, i-C_4H_9) or Stauffer AA TiCl_3-Al (C_2H_5)_3 catalyzed 1-octene polymerization were determined by using an acetyl chloride quenching method as well as kinetic data. The results show that in the studied systems k_p decreases when C_p increases, indicating the presence of two or more types of different active centers. The C_(p^(-t)) plots of the Solvay TiCl_3-AlR_3 systems show the presence of both stable active centers and unstable centers which decay in the polymerization process. The phenomena are explained based on a model of active center plurality. The increases of C_p in the induction periods are also discussed.展开更多
Distribution of active centers(ACD)of ethylene or 1-hexene homopolymerization and ethylene-1-hexene copolymerization with a MgCl_2/TiCl_4 type Z-N catalyst were studied by deconvolution of the polymer molecular weight...Distribution of active centers(ACD)of ethylene or 1-hexene homopolymerization and ethylene-1-hexene copolymerization with a MgCl_2/TiCl_4 type Z-N catalyst were studied by deconvolution of the polymer molecular weight distribution into multiple Flory components.Each Flory component is thought to be formed by a certain type of active center. ACD of ethylene-1-hexene copolymer with very low 1-hexene incorporation was compared with that of ethylene homopolymer to see the effect of introducingα-olefin on ethyle...展开更多
This paper attempts to understand the Pt-like catalytic activity of transition metal carbide Ta4C_(3) for IRR(I_(3)^(-)reduction reaction)based on the correlation of adsorption energy to d-band center(εd).Ta4C_(3) wa...This paper attempts to understand the Pt-like catalytic activity of transition metal carbide Ta4C_(3) for IRR(I_(3)^(-)reduction reaction)based on the correlation of adsorption energy to d-band center(εd).Ta4C_(3) was prepared by carbothermal reduction method with a template.Its photoelectrochemical properties were investigated as a CE(counter electrode)in DSSC(dye-sensitized solar cell).Its surface electronic structures,including DOS(density of state)andεd,and adsorption energy were computed by first-principle DFT(density functional theory).In TMC(transition metal carbide)Ta4C_(3),the interaction between Ta and C atoms makes the d-band of Ta broaden and results in the downward shift of itsεd.A moderate absorption energy corresponding to theεd is achieved,which is the nature of the Pt-like catalytic activity of Ta4C_(3).Appropriate change of adsorption energy by adjustingεd is a promising strategy to improve catalytic activity.This work is of great significance to the fundamental and application researches.展开更多
Efficient catalysis of functinnatized β-cyctodextrins bearing aninoatkytimino groups for atdot condensations of nitrobenzatdehydes and acetone has been effected and substantiated by preparative experiments
CuOx/CeO2 catalysts were prepared by adsorption-impregnation method, CO conversion was tested over the catalysts pretreated under different conditions for preferential CO oxidation in H2, and the catalysts were charac...CuOx/CeO2 catalysts were prepared by adsorption-impregnation method, CO conversion was tested over the catalysts pretreated under different conditions for preferential CO oxidation in H2, and the catalysts were characterized with X-ray photoelectron spectroscopy and temperature programmed reduction. Experimental results show that there are two kinds of copper, which are Cu^+ and Cu^2+ in calcined CuOx/CeO2, Among them, the Cu^+ is the key active component for CO oxidation. The main reason is as follows: CO is activated by copper for CO oxidation over CuOx/CeO2, while CO can not be activated by Cu^2+. Only when Cu^2+ is reduced to Cu ^+ or Cu^0, the copper may be active for CO oxidation, moreover, the experimental results show that the reduction of Cu^2+ does not lead to an increase of catalytic activity. So the active species is Cu^+ in CuOx/CeO2 catalysts.展开更多
Background: Prolonged sitting is a risk factor for low-back pain. The primary purpose of this study is to determine if prolonged active sitting will result in increased trunk motion. Methods: Fifteen healthy female ...Background: Prolonged sitting is a risk factor for low-back pain. The primary purpose of this study is to determine if prolonged active sitting will result in increased trunk motion. Methods: Fifteen healthy female participants volunteered to sit for 30 vain on each of three surfaces including an air-cushion, a stability ball, and a hard surface. Trunk motion was monitored using a Vicon motion capture system, and foot center of pressure was collected with two AMTI force plates. Results: Our findings indicated that the average speed of the trunk center of mass significantly increased with seating surface compliance. There were significant differences in fight and left foot centers of pressure in the antero-posterior direction between the ball and air-cushion conditions and the ball and chair conditions. Conclusion: Active sitting results in increased trunk motion and could have a positive effect on low-back health.展开更多
Cost-effective atomically dispersed Fe-N-P-C complex catalysts are promising to catalyze the oxygen reduction reaction(ORR)and replace Pt catalysts in fuel cells and metal-air batteries.However,it remains a challenge ...Cost-effective atomically dispersed Fe-N-P-C complex catalysts are promising to catalyze the oxygen reduction reaction(ORR)and replace Pt catalysts in fuel cells and metal-air batteries.However,it remains a challenge to increase the number of atomically dispersed active sites on these catalysts.Here we report a highly efficient impregnation-pyrolysis method to prepare effective ORR electrocatalysts with large amount of atomically dispersed Fe active sites from biomass.Two types of active catalyst centers were identified,namely atomically dispersed Fe sites and Fe_(x)P particles.The ORR rate of the atomically dispersed Fe sites is three orders of magnitude higher than it of Fe_(x)P particles.A linear correlation between the amount of the atomically dispersed Fe and the ORR activity was obtained,revealing the major contribution of the atomically dispersed Fe to the ORR activity.The number of atomically dispersed Fe increases as the Fe loading increased and reaching the maximum at 1.86 wt%Fe,resulting in the maximum ORR rate.Optimized Fe-N-P-C complex catalyst was used as the cathode catalyst in a homemade Zn-air battery and good performance of an energy density of 771 Wh kgZn^(-1),a power density of 92.9 m W cm^(-2) at 137 m A cm^(-2) and an excellent durability were exhibited.展开更多
Due to the rapid development of electronic countermeasures(ECMs),the corresponding means of electronic counter countermeasures(ECCMs)are urgently needed.In this paper,an act-ive anti-jamming method based on frequency ...Due to the rapid development of electronic countermeasures(ECMs),the corresponding means of electronic counter countermeasures(ECCMs)are urgently needed.In this paper,an act-ive anti-jamming method based on frequency diverse array radar is proposed.By deriving the closed form of the phase center in a uniform line array FDA,we establish a model of the FDA signal based on adaptive weights and derive the effect of active anti-jamming in this regime.The pro-posed active anti-jamming method makes it difficult for jammers to detect or locate our radar.Fur-thermore,the effectiveness of the two frequency increment schemes in terms of anti-jamming is ana-lyzed by comparing the deviation of phase center.Finally,the simulation results verify the effective-ness and superiority of the proposed method.展开更多
基金This work is financially supported by the National Science Foundation of Tianjin(17JCYBJC23300).
文摘Phosphate removal is crucial for eutrophication control and water quality improvement.Electro-assisted adsorption,an eco-friendly elec-trosorption process,exhibited a promising potential for wastewater treatment.However,there are few works focused on phosphate electro-sorption,and reported electrodes cannot attach satisfactory removal capacities and rates.Herein,electro-assisted adsorption of phosphate via in-situ construction of La active centers on hierarchically porous carbon(LaPC)has been originally demonstrated.The resulted LaPC composite not only possessed a hierarchically porous structure with uniformly dispersed La active sites,but also provided good conductivity for interfacial electron transfer.The LaPC electrode achieved an ultrahigh phosphate electrosorption capability of 462.01 mg g^(-1) at 1 V,outperforming most existing electrodes.The superior phosphate removal performance originates from abundant active centers formed by the coupling of electricfield and capture sites.Besides,the stability and selectivity toward phosphate capture were maintained well even under comprehensive conditions.Moreover,a series of kinetics and isotherms models were employed to validate the electrosorption process.This work demonstrates a deep understanding and promotes a new level of phosphate electrosorption.
文摘The objectives of this work were to evaluate the surgical activities carried out in the general surgery department of the Reference Health Center of Commune I of Bamako, to describe the sociodemographic characteristics of the operated patients, to determine the main pathologies encountered and to evaluate qualitatively the result of the treatment. In order to improve performance, and the quality of care, and to identify common pathologies in the surgical department, we undertook a retrospective study on surgical activities from January 2009 to December 2010. At the end of this study, out of 474 men and 187 women (equal sex ratio 2.53);we were able to determine the frequency of surgical pathologies. Farmers, housewives and pupils/students were the most represented with 25.9% respectively;20% and 13.3%. The most frequently observed pathologies were wall hernia (44.8%), prostate adenoma (12%) and acute appendicitis (10.5%). The average length of hospitalization was 3.43 days. Infectious complications affected 25 patients (3.8% of cases) and a death rate of 0.45% (i.e. 3 patients). The average cost of care was 53,500 FCFA. Indeed, the reality of surgical practice in health centers was not the same because of the level of skills of practicing surgeons.
文摘With the further advancement of the“National Fitness”strategy and the continuous development of the information age,the National Fitness Activity Centers have become more comprehensive.The comprehensiveness is reflected in the design of diversified sports functions and spaces.The article serves to explore the comprehensive development trend of National Fitness Activity Centers.Through summarizing and sorting out domestic and foreign cases,the trend of the comprehensive development of National Fitness Activity Centers is predicted at three levels:industry,city,and individual functions.
基金supported by the Natural Science Foundation of Shandong Provence of China(ZR2013BM008)
文摘Deactivation mechanism of Cr-Al2O3catalyst and the interaction of Cr-A1 in the dehydrogenation of isobutane, as well as the nature of the catalytic active center, were studied using XRD, SEM, XPS, H2-TPR, isobutane-TPR and TPO techniques. The results revealed that the deactivation of Cr-Al2O3 catalyst was mainly caused by carbon deposition on its surface. The Cr3+ ion could not be reduced by hydrogen but could be reduced to Cr2+ by hydrocarbons and monoxide carbon. The active center for isobutane dehydrogenation could be Cr2+/Cr3+ produced from Cr6+ by the on line reduction of hydrocarbon and carbon monoxide. The binding energy of Al3+ was strongly affected by the state of chromium cations in the catalysts.
文摘The composition distribution (CD) and microisotacticity distribution (ID) of propene/1-hexene copolymer synthesized by MgCl2/DIBP/TiCl4 (DIBP: diisobutyl phthalate) were determined by fractionating the copolymers according to crystallinity and characterizing the fractions by (CNMR)-C-13. The effects of two alkoxysilane donors, triethoxyphenylsilane (PTES) and dimethoxydi-tert-butylsilane (TBMS), on CD and ID of the copolymers were compared. Three main parts in the CD diagram of each copolymer were distinguished, which were correlated to active center distribution (ACD) based on three groups of different active centers. By studying the changes in l-hexene content, microisotacticity and reactivity ratio product of three typical fractions, the effects of external donor on ACD were better elucidated. It was found that TBMS shows much stronger effects on ACD than PTES. In the former system, most fractions were produced on active centers with relatively lower r(1)r(2), higher reactivity to I-hexene, and higher stereospecificity as compared to the system without external donor. It is concluded that the observed very extensive changes in ACD are mainly resulted by the formation of new types of active centers, possibly by coordination of external donor to certain positions on the catalyst.
文摘We interpret seismic activity in the active spreading centers of the Salton Trough to indicate 1) a magmatic intrusion in the lower crust beneath the active Brawly, Cerro Prieto, Imperial, Elsinore, and San Jacinto fault systems;and 2) fluids in the upper crust that have been released from that magmatic body. The absence of a magmatic body and fluids at the location of fossil spreading centers along the Sand Hill and Algodones faults ndicated by little or no seismic activity in those areas. We show several lines of evidence to point out that both melt and fluids related to the seismic activity. In particular, receiver function analysis, Vp/Vs ratios, and tomographic data reveal low velocity zones coincide with the location of the active spreading centers. High Vp/Vs ratios and low velocity zones in the lower crust and upper mantle attributed to melt inclusion, while low Vp/Vs ratios in the upper crust are attributed water inclusions. Frequency-mag- nitude distributions characterized by high b-values in southern California;high b-values have also been associated with crustal fluids. A crustal scale model developed from the receiver functions, gravity, and magnetic data supports the existence of a magmatic intrusion within about 20 km of the surface southwest of the Salton Sea, that intrusion extends for 70 km in a SW-NE direction.
基金the Key Projects of Shanghai Science and Technology Commission (18JC1412100)the National Natural Science Foundation of China (No. 91745105, 22072092, 92045301)+2 种基金the startup funding provided by Shanghai Tech University for funding their participation in this workfunding provided through The Shell Foundation Grants (No. PT66201)the support from Analytical Instrumentation Center (contract no. SPSTAIC10112914), SPST, Shanghai Tech University。
文摘La_(2)O_(3) catalyzed oxidative coupling of methane(OCM) is a promising process that converts methane directly to valuable C_(2)(ethylene and ethane) products. Our online MS transient study results indicate that pristine surface without carbonate species demonstrates a higher selectivity to C_(2) products, and a lower light-off temperature as well. Further study is focused on carbonate-free La_(2)O_(3) catalyst surface for identification of active oxygen species associated with such products behavior. XPS reveals unique oxygen species with O 1 s binding energy of 531.5 e V correlated with OCM catalytic activity and carbonates removal. However, indicated thermal stability of this species is much higher than the surface peroxide or superoxide structures proposed by earlier computation models. Motivated by experimental results,DFT calculations reveal a new more stable peroxide structure, formed at the subsurface hexacoordinate lattice oxygen sites, with energy 2.18 e V lower than the previous models. The new model of subsurface peroxide provides a perspective for understanding of methyl radicals formation and C_(2) products selectivity in OCM over La_(2)O_(3) catalyst.
基金Project supported by the National Natural Science Foundation ofChina (No. 20172045) Science and Technology Plan Fund of Zhe-jiang Province (No. 001101116) and Foundation for Doctors ofNingbo City (No. 2003A62012) China
文摘Novel MgCl2-supported Ziegler-Natta (Z-N) catalysts prepared using a new one-pot ball milling method can effectively control the amounts of Ti-loading in the catalysts. Complex GPC data on polypropylene synthesized by these novel catalysts were analyzed using the method of fitting the molecular weight distribution (MWD) curves with a multiple Flory-Schulz function. It was found that multiple active centers exist in these novel catalysts. Detailed study of the effects of the Ti-loadings in the catalysts on the distribution of the active centers showed that the Ti-loadings in the novel MgCl2-supported Z-N catalysts might affect the proportion of each type of active centers; and might be the main factor responsible for the effect of the Ti-loadings on the microstructure, the molecular weight and molecular weight distribution width of the resultant polymer, the catalytic activity and polymerization kinetics.
基金financially supported by the 2022 Special Fund Project for Science and Technology Innovation Strategy of Guangdong Province(STKJ202209077 and STKJ202209083)the Guangdong Province Universities and Colleges Pearl River Scholar Funded Scheme 2019(GDUPS2019)the City University of Hong Kong Strategic Research Grant(SRG)(7005505)。
文摘There have been reports about Fe ions boosting oxygen evolution reaction(OER)activity of Ni-based catalysts in alkaline conditions,while the origin and reason for the enhancement remains elusive.Herein,we attempt to identify the activity improvement and discover that Ni sites act as a host to attract Fe(Ⅲ)to form Fe(Ni)(Ⅲ)binary centres,which serve as the dynamic sites to promote OER activity and stability by cyclical formation of intermediates(Fe(Ⅲ)→Fe(Ni)(Ⅲ)→Fe(Ni)-OH→Fe(Ni)-O→Fe(Ni)OOH→Fe(Ⅲ))at the electrode/electrolyte interface to emit O_(2).Additionally,some ions(Co(Ⅱ),Ni(Ⅱ),and Cr(Ⅲ))can also be the active sites to catalyze the OER process on a variety of electrodes.The Fe(Ⅲ)-catalyzed overall water-splitting electrolyzer comprising bare Ni foam as the anode and Pt/Ni-Mo as the cathode demonstrates robust stability for 1600 h at 1000 mA cm^(-2)@~1.75 V.The results provide insights into the ioncatalyzed effects boosting OER performance.
基金grant from the China National Natural Science Foundation (No.49875019)
文摘The study of low-frequency oscillations is an important part of climate variability research. In view of insufficient efforts spent on multidecadal and ENSO-scale changes of the climate, the present paper undertakes study of > 30 year slowly-varying means, called climate base state (CBS), of northern winter AAC’s in the past 100 years and more, with the CBS variability and its temporal evolution investigated, indicating that Aleutian low and Icelandic low (North Pacific high and North American high) experience maximum (minimum) variation in the CBS. The CBS exhibits two modes for its variation. The positive (negative) phase of mode I presents a weak (strong) NAO (North Atlantic Oscillation), a weaker (stronger) NPO (North Pacific Oscillation), a robust (feeble) Siberian high and a quite weak (vigorous) Aleutian low whilst the positive (negative) phase of mode II reveals a feeble (strong) Aleutian low and a weak (robust) Siberian high. Also, the research shows that the recent CBS of northern circulations is in a remarkably negative phase of mode I and a noticeably positive phase of mode II, viz., in the background of slowly-varying circulations of an exceptionally weak Siberian high, an extremely vigorous Aleutian low and an intense NAO. The background field is likely to persist for a matter of 30 years such that northern winter temperature is expected to be in such a warm situation for a long period to follow.
文摘The number of active centers (C_p)-t and k_p-t profiles of Solvay type TiCl_3 - AlR_3 (R=C_2H_5, i-C_4H_9) or Stauffer AA TiCl_3-Al (C_2H_5)_3 catalyzed 1-octene polymerization were determined by using an acetyl chloride quenching method as well as kinetic data. The results show that in the studied systems k_p decreases when C_p increases, indicating the presence of two or more types of different active centers. The C_(p^(-t)) plots of the Solvay TiCl_3-AlR_3 systems show the presence of both stable active centers and unstable centers which decay in the polymerization process. The phenomena are explained based on a model of active center plurality. The increases of C_p in the induction periods are also discussed.
基金the Major State Basic Research Programs(No.2005CB623804).
文摘Distribution of active centers(ACD)of ethylene or 1-hexene homopolymerization and ethylene-1-hexene copolymerization with a MgCl_2/TiCl_4 type Z-N catalyst were studied by deconvolution of the polymer molecular weight distribution into multiple Flory components.Each Flory component is thought to be formed by a certain type of active center. ACD of ethylene-1-hexene copolymer with very low 1-hexene incorporation was compared with that of ethylene homopolymer to see the effect of introducingα-olefin on ethyle...
基金Financial support for this work was provided by Key Research and Development Projects of Shanxi Province(201703D121023).
文摘This paper attempts to understand the Pt-like catalytic activity of transition metal carbide Ta4C_(3) for IRR(I_(3)^(-)reduction reaction)based on the correlation of adsorption energy to d-band center(εd).Ta4C_(3) was prepared by carbothermal reduction method with a template.Its photoelectrochemical properties were investigated as a CE(counter electrode)in DSSC(dye-sensitized solar cell).Its surface electronic structures,including DOS(density of state)andεd,and adsorption energy were computed by first-principle DFT(density functional theory).In TMC(transition metal carbide)Ta4C_(3),the interaction between Ta and C atoms makes the d-band of Ta broaden and results in the downward shift of itsεd.A moderate absorption energy corresponding to theεd is achieved,which is the nature of the Pt-like catalytic activity of Ta4C_(3).Appropriate change of adsorption energy by adjustingεd is a promising strategy to improve catalytic activity.This work is of great significance to the fundamental and application researches.
文摘Efficient catalysis of functinnatized β-cyctodextrins bearing aninoatkytimino groups for atdot condensations of nitrobenzatdehydes and acetone has been effected and substantiated by preparative experiments
文摘CuOx/CeO2 catalysts were prepared by adsorption-impregnation method, CO conversion was tested over the catalysts pretreated under different conditions for preferential CO oxidation in H2, and the catalysts were characterized with X-ray photoelectron spectroscopy and temperature programmed reduction. Experimental results show that there are two kinds of copper, which are Cu^+ and Cu^2+ in calcined CuOx/CeO2, Among them, the Cu^+ is the key active component for CO oxidation. The main reason is as follows: CO is activated by copper for CO oxidation over CuOx/CeO2, while CO can not be activated by Cu^2+. Only when Cu^2+ is reduced to Cu ^+ or Cu^0, the copper may be active for CO oxidation, moreover, the experimental results show that the reduction of Cu^2+ does not lead to an increase of catalytic activity. So the active species is Cu^+ in CuOx/CeO2 catalysts.
文摘Background: Prolonged sitting is a risk factor for low-back pain. The primary purpose of this study is to determine if prolonged active sitting will result in increased trunk motion. Methods: Fifteen healthy female participants volunteered to sit for 30 vain on each of three surfaces including an air-cushion, a stability ball, and a hard surface. Trunk motion was monitored using a Vicon motion capture system, and foot center of pressure was collected with two AMTI force plates. Results: Our findings indicated that the average speed of the trunk center of mass significantly increased with seating surface compliance. There were significant differences in fight and left foot centers of pressure in the antero-posterior direction between the ball and air-cushion conditions and the ball and chair conditions. Conclusion: Active sitting results in increased trunk motion and could have a positive effect on low-back health.
基金The financial supports from Department of Chemical Engineeringthe support from China Scholarship Council(CSC)for his study at NTNU。
文摘Cost-effective atomically dispersed Fe-N-P-C complex catalysts are promising to catalyze the oxygen reduction reaction(ORR)and replace Pt catalysts in fuel cells and metal-air batteries.However,it remains a challenge to increase the number of atomically dispersed active sites on these catalysts.Here we report a highly efficient impregnation-pyrolysis method to prepare effective ORR electrocatalysts with large amount of atomically dispersed Fe active sites from biomass.Two types of active catalyst centers were identified,namely atomically dispersed Fe sites and Fe_(x)P particles.The ORR rate of the atomically dispersed Fe sites is three orders of magnitude higher than it of Fe_(x)P particles.A linear correlation between the amount of the atomically dispersed Fe and the ORR activity was obtained,revealing the major contribution of the atomically dispersed Fe to the ORR activity.The number of atomically dispersed Fe increases as the Fe loading increased and reaching the maximum at 1.86 wt%Fe,resulting in the maximum ORR rate.Optimized Fe-N-P-C complex catalyst was used as the cathode catalyst in a homemade Zn-air battery and good performance of an energy density of 771 Wh kgZn^(-1),a power density of 92.9 m W cm^(-2) at 137 m A cm^(-2) and an excellent durability were exhibited.
基金the National Natural Science Foundation of China(No.61971438)the Natural Science Founda-tion of Shaanxi Province(No.2019JM-155).
文摘Due to the rapid development of electronic countermeasures(ECMs),the corresponding means of electronic counter countermeasures(ECCMs)are urgently needed.In this paper,an act-ive anti-jamming method based on frequency diverse array radar is proposed.By deriving the closed form of the phase center in a uniform line array FDA,we establish a model of the FDA signal based on adaptive weights and derive the effect of active anti-jamming in this regime.The pro-posed active anti-jamming method makes it difficult for jammers to detect or locate our radar.Fur-thermore,the effectiveness of the two frequency increment schemes in terms of anti-jamming is ana-lyzed by comparing the deviation of phase center.Finally,the simulation results verify the effective-ness and superiority of the proposed method.