The calculation method about infrared multi-sites passive system location is introduced based on the principle of the weighted least square method, and the variance matrix of estimated error is offered. Through deduct...The calculation method about infrared multi-sites passive system location is introduced based on the principle of the weighted least square method, and the variance matrix of estimated error is offered. Through deduction, it can be found out that treated appraise precision can be directly analyzed and deduced without carrying out real measure and reaching estimation value. The simulation result shows that the system performance based on the weighted least square method is much better than the traditional passive location method, and it can be also used for reference to the research of the location algorithm of similar system.展开更多
The special electronic characteristics and high atom usage efficiency of metal-nitrogen-carbon(M-N-C)materials have made them extremely attractive for oxygen reduction reactions(ORRs).However,it is inevitable that hyd...The special electronic characteristics and high atom usage efficiency of metal-nitrogen-carbon(M-N-C)materials have made them extremely attractive for oxygen reduction reactions(ORRs).However,it is inevitable that hydrogen peroxide(H_(2)O_(2))will be formed via the two-electron pathway in ORRs.Herein,the Cu nanoparticles(NPs)have been encapsulated into Ni doped hollow mesoporous carbon spheres(Ni-HMCS)to reduce the generation of H_(2)O_(2)in ORR.Electrochemical tests confirm that the introduction of Cu NPs improves the ORR performance greatly.The obtained Cu/Ni-HMCS exhibits a half-wave potential of 0.82 V vs.reversible hydrogen electrode and a limited current density of 5.5 mA cm^(-2),which is comparable with the commercial Pt/C.Moreover,Cu/Ni-HMCS has been used in Zn-air battery,demonstrating a high power density of 161 mW cm^(-2)and a long-term recharge capability(50 h at 5 mA cm^(-2)).The theoretical calculation proposes a tandem catalysis pathway for Cu/Ni multi-sites catalysis,that is,H_(2)O_(2)released from the Ni-N_(4)and Cu-N_(4)sites migrates to the Cu(111)face,on which the captive H_(2)O_(2)is further reduced to H_(2)O.This work demonstrates an interesting tandem catalytic pathway of dual-metal multi-sites for ORR,which provides an insight into the development of effective fuel cell electrocatalysts.展开更多
Hydrogen,as a cheap,clean,and cost-effective secondary energy source,performs an essential role in optimizing today’s energy structure.Magnesium hydride(Mg H_(2))represents an attractive hydrogen carrier for storage ...Hydrogen,as a cheap,clean,and cost-effective secondary energy source,performs an essential role in optimizing today’s energy structure.Magnesium hydride(Mg H_(2))represents an attractive hydrogen carrier for storage and transportation,however,the kinetic behavior and operating temperature remain undesirable.In this work,a dual-phase multi-site alloy(Ms A)anchored on carbon substrates was designed,and its superior catalytic effects on the hydrogen storage properties of MgH_(2) were reported.Mechanism analysis identified that multi-site Fe Ni_(3)/Ni Cu nanoalloys synergistically served as intrinsic drivers for the striking de/hydrogenation performance of the MgH_(2)-Ms A systems.Concretely,the unique multi-metallic site structure attached to the surface of MgH_(2)provided substantial reversible channels and accessible active sites conducive to the adsorption,activation,and nucleation of H atoms.In addition,the coupling system formed by FeNi_(3) and NiCu dual-phase alloys further enhanced the reactivity between Mg/MgH_(2) and H atoms.Hence,the onset dehydrogenation temperature of Mg H_(2)+5 wt%Ms A was reduced to 195℃ and the hydrogen desorption apparent activation energy was reduced to 83.6 k J/mol.5.08 wt%H_(2) could be released at 250℃ in 20 min,reaching a high dehydrogenation rate of 0.254 wt%H_(2)/min,yet that for MgH_(2) at a higher temperature of 335℃ was only 0.145 wt%H_(2)/min.Then,the dehydrogenated Mg H_(2)-Ms A sample could absorb hydrogen from room temperature(30℃)and charge 3.93 wt%H_(2) at 100℃ within20 min under 3.0 MPa H_(2) pressure.Benefiting from carbon substrates,the 5 wt%Ms A doped-MgH_(2) could still maintain 6.36 wt%hydrogen capacity after 20 cycles.In conclusion,this work provides experimental rationale and new insights for the design of efficient catalysts for magnesium-based solid-state hydrogen storage materials.展开更多
In contrast to the predominant mono or difunctionalization of alkenes,the multi-site functionalization of alkenes involving the synergistic formation of more than two new C–C or C–X bonds is much challenging,especia...In contrast to the predominant mono or difunctionalization of alkenes,the multi-site functionalization of alkenes involving the synergistic formation of more than two new C–C or C–X bonds is much challenging,especially for developing new reaction pathway to afford the functional heterocycle compounds with aggregation-induced emission(AIE)property has been rarely reported.In present work,the multi-site functionalization of in situ generated alkenes with indoles has been developed for the synthesis of diversely functionalized carbazoles through the synergistic construction of multiple C–C bonds and C=O bond.A proposed reaction sequence involving C–H alkenylation/radical oxygen atom transfer/Diels-Alder cycloaddition/dehydrogenative aromatization was supported by experiments and density functional theory calculations.Further derivative carbazole-linked-quinoxaline skeletons represent a class of AIEgens with acceptor-donor-acceptor configuration,which generated the desired twisted intramolecular charge transfer(TICT)AIE properties and could be used as fluorescent probes for detecting the micrometer-sized phase separation of polymer blends.The protocol provides a concise route for the synthesis and application of carbazole-based AIE luminogens.展开更多
A long-term(2007-2016) particulate matter dataset measured at multiple sites in Chengdu,an expanding megacity in southwest China, was analyzed. The trends of particulate chemical compositions and source apportionment ...A long-term(2007-2016) particulate matter dataset measured at multiple sites in Chengdu,an expanding megacity in southwest China, was analyzed. The trends of particulate chemical compositions and source apportionment were used to evaluate and review the effectiveness of source-specific control policies and measures in Atmospheric Pollution Prevention and Control Action Plan(APPCAP). The concentration of particulate matter decreased significantly, and most aerosol components changed synchronously with particulate matter. The results of advanced three-way factor analysis model suggested that six sources were resolved at three sites: coal combustion, vehicle, crustal dust, cement, sulfate, nitrate and secondary organic matter. Secondary source, including secondary organic carbon(SOC),sulfate, nitrate, and ammonium(SNA), was always the main pollution source in this region.Dust, including cement and crustal dust, was important primary source. Encouragingly, coal combustion had been significantly controlled after APPCAP. The central site represented the higher contribution of vehicles, nitrates and SOC, while north and eastern sites showed the higher contribution of sulfate, coal combustion and dust. Many evidence points to substantial alterations in the physicochemical attributes of Chengdu's atmosphere. The rising proportion of nitrate and the transition of the atmospheric environment from ammoniapoor to ammonia-rich conditions highlight the necessity for the next phase of particulate matter control to focus intensively on the management of NH3and NOx. China's APPCAP could provide useful experience for vast developing countries and other urbanizing and industrializing regions to strike a balance between social development and environmental protection.展开更多
Removing H_(2)S and CO_(2)is of great significance for natural gas purification.With excellent gas affinity and tunable structure,ionic liquids(ILs) have been regarded as nontrivial candidates for fabricating polymer-...Removing H_(2)S and CO_(2)is of great significance for natural gas purification.With excellent gas affinity and tunable structure,ionic liquids(ILs) have been regarded as nontrivial candidates for fabricating polymer-based membranes.Herein,we firstly reported the incorporation of protic ILs (PILs) having ether-rich and carboxylate sites (ECPILs) into poly(ether-block-amide)(Pebax) matrix for efficient separation H_(2)S and CO_(2)from CH_(4).Notably,the optimal permeability of H_(2)S reaches up to 4310 Barrer (40C,0.50 bar) in Pebax/ECPIL membranes,along with H_(2)S/CH_(4)and (H_(2)StCO_(2))/CH_(4)selectivity of 97.7 and 112.3,respectively.These values are increased by 1125%,160.8%and 145.9%compared to those in neat Pebax membrane.Additionally,the solubility and diffusion coefficients of the gases were measured,demonstrating that ECPIL can simultaneously strengthen the dissolution and diffusion of H_(2)S and CO_(2),thus elevating the permeability and permselectivity.By using quantum chemical calculations and FT-IR spectroscopy,the highly reversible multi-site hydrogen bonding interaction between ECPILs and H_(2)S was revealed,which is responsible for the fast permeation of H_(2)S and good selectivity.Furthermore,H_(2)S/CO_(2)/CH_(4)(3/3/94 mol/mol) ternary mixed gas can be efficiently and stably separated by Pebax/ECPIL membrane for at least 100 h.Overall,this work not only illustrates that PILs with ether-rich and carboxylate hydrogen bonding sites are outstanding materials for simultaneous removal of H_(2)S and CO_(2),but may also provide a novel insight into the design of membrane materials for natural gas upgrading.展开更多
Accurate multi-step PM_(2.5)(particulate matter with diameters≤2.5 um)concentration prediction is critical for humankinds’health and air populationmanagement because it could provide strong evidence for decisionmaki...Accurate multi-step PM_(2.5)(particulate matter with diameters≤2.5 um)concentration prediction is critical for humankinds’health and air populationmanagement because it could provide strong evidence for decisionmaking.However,it is very challenging due to its randomness and variability.This paper proposed a novel method based on convolutional neural network(CNN)and long-short-term memory(LSTM)with a space-shared mechanism,named space-shared CNN-LSTM(SCNN-LSTM)for multi-site dailyahead multi-step PM_(2.5)forecasting with self-historical series.The proposed SCNN-LSTM contains multi-channel inputs,each channel corresponding to one-site historical PM_(2.5)concentration series.In which,CNN and LSTM are used to extract each site’s rich hidden feature representations in a stack mode.Especially,CNN is to extract the hidden short-time gap PM_(2.5)concentration patterns;LSTM is to mine the hidden features with long-time dependency.Each channel extracted features aremerged as the comprehensive features for future multi-step PM_(2.5)concentration forecasting.Besides,the space-shared mechanism is implemented by multi-loss functions to achieve space information sharing.Therefore,the final features are the fusion of short-time gap,long-time dependency,and space information,which enables forecasting more accurately.To validate the proposed method’s effectiveness,the authors designed,trained,and compared it with various leading methods in terms of RMSE,MAE,MAPE,and R^(2)on four real-word PM_(2.5)data sets in Seoul,South Korea.The massive experiments proved that the proposed method could accurately forecast multi-site multi-step PM_(2.5)concentration only using self-historical PM_(2.5)concentration time series and running once.Specifically,the proposed method obtained averaged RMSE of 8.05,MAE of 5.04,MAPE of 23.96%,and R^(2)of 0.7 for four-site daily ahead 10-hourPM_(2.5)concentration forecasting.展开更多
A highly effective and mild protocol for ring opening of epoxides with NH4SCN in the presence of catalytic amount of a multi- site phase-transfer catalyst, α,α＇,α＂-N-hexakis（triethylammoniummethylene chloride）-...A highly effective and mild protocol for ring opening of epoxides with NH4SCN in the presence of catalytic amount of a multi- site phase-transfer catalyst, α,α＇,α＂-N-hexakis（triethylammoniummethylene chloride）-melamine, is developed. A variety of ^-hydroxy thiocyanates as important intermediates in agricultural and pharmaceutical chemistry were obtained in high yields with excellent regioselectivity and in short reaction times. 2009 Ali Reza Kiasat. Published by Elsevier B.V. on behalf of Chinese Chemical Society. All rights reserved.展开更多
Background:We aimed to characterise the geographical distribution of Sørensen-based multi-site dissimilarity(β_(sor))and its underlying true turnover(β_(sim))and nestedness(βsne)components for Chinese Lauracea...Background:We aimed to characterise the geographical distribution of Sørensen-based multi-site dissimilarity(β_(sor))and its underlying true turnover(β_(sim))and nestedness(βsne)components for Chinese Lauraceae and to analyse their relationships to current climate and past climate change.Methods:We used ensembles of small models(ESMs)to map the current distributions of 353 Lauraceae species in China and calculated β_(sor) and its β_(sim) and β_(sne) components.We tested the relationship between β_(sor),β_(sne) and β_(sim) with current climate and past climate change related predictors using a series of simultaneous autoregressive(SAR_(err))models.Results:Spatial distribution of β_(sor)of Lauraceae is positively correlated with latitude,showing an inverse rela-tionship to the latitudinalα-diversity(species richness)gradient.High β_(sor) occurs at the boundaries of the warm temperate and subtropical zones and at the Qinghai-Tibet Plateau due to high β_(sne).The optimized SAR_(err) model explainsβ_(sor) andβ_(sne) well,but notβ_(sim).Current mean annual temperature determinesβ_(sor) and β_(sne) of Lauraceae more than anomalies and velocities of temperature or precipitation since the Last Glacial Maximum.Conclusions:Current low temperatures and high climatic heterogeneity are the main factors explaining the high multi-siteβ-diversity of Lauraceae.In contrast to analyses of the β-diversity of entire species assemblages,studies of single plant families can provide complementary insights into the drivers of β-diversity of evolutionarily more narrowly defined entities.展开更多
Cellulose nanofibrils(CNFs)are promising sustainable materials that can be applied to nanocomposites,as well as medical and life-sciences devices.However,methods for the preparation of these important materials are en...Cellulose nanofibrils(CNFs)are promising sustainable materials that can be applied to nanocomposites,as well as medical and life-sciences devices.However,methods for the preparation of these important materials are energy intensive because heating and mechanical disintegration are required to produce cellulose fibers below 100 nm in size.In this study,CNFs were prepared through the multi-site regioselective oxidation of cellulose with 2,2,6,6-tetramethylpiperidine-1-oxyl(TEMPO)and periodate at room temperature(20–25°C),without any mechanical-disintegration treatment.Transmission electron microscopy(TEM)revealed that the CNFs had the average widths of 14.1,55.4,and 81.9 nm for three different treatments.Fourier-transform infrared spectroscopy revealed that carboxyl groups were created on the surfaces of the microfibrils,while X-ray diffraction studies showed that the cellulose I structure was maintained after oxidation,and that the cellulose nanofibril crystallinity index exceeded 70%.These results demonstrate that CNFs can be prepared by multi-site regioselective oxidation at room temperature in the absence of mechanical disintegration.In addition,a model was developed to calculate the total content of carboxylate and aldehyde groups of CNFs prepared by the TEMPO mediate oxidation,the periodate oxidation,and the multi-site regioselective oxidation methods based on the particle width determined by TEM.The calculated values of the model were in good agreement with the total content(experimental value)of carboxylate and aldehyde groups of CNFs prepared by the TEMPO-mediated oxidation and the multi-site regioselective oxidation methods.However,the model was not valid for CNFs prepared by the periodate oxidation method.展开更多
With the advent of spinal cord epidural stimulation techniques,i.e.,electrically enabled motor control（e Emc）in combination with activity dependent locomotor training,humans with traumatic complete sensori-motor par...With the advent of spinal cord epidural stimulation techniques,i.e.,electrically enabled motor control（e Emc）in combination with activity dependent locomotor training,humans with traumatic complete sensori-motor paralysis are able to initiate voluntary leg movements and achieve gains in postural control,and bladder and sexual function（Angeli et al.,2014）.展开更多
Recent years have seen a surge in assessment of potential impacts of climate change. As one of the most important tools for generating synthetic hydrological model inputs, weather generators have played an important r...Recent years have seen a surge in assessment of potential impacts of climate change. As one of the most important tools for generating synthetic hydrological model inputs, weather generators have played an important role in climate change impact analysis of water management. However, most weather generators like statistical downscaling model （SDSM） and long Ashton research station weather generator （LARS-WG） are designed for single site data generation. Considering the significance of spatial correlations of hydro-meteorological data, multi-site weather data generation becomes a necessity. In this study we aim to evaluate the performance of a new multi-site stochastic model, geo-spatial temporal weather generator （GIST）, in simulating precipitation in the Qiantang River Basin, East China. The correlation matrix, precipitation amount and occurrence of observed and GiST-generated data are first compared for the evaluation process. Then we use the GiST model combined with the change factor method （CFM） to investigate future changes of precipitation （2071 2100） in the study area using one global climate model, Hadgem2 ES, and an extreme emission scenario RCP 8.5, The final results show that the simulated precipitation amount and occurrence by GiST matched their historical counterparts reasonably. The correlation coefficients between simulated and his- torical precipitations show good consistence as well. Compared with the baseline period （1961 1990）, precipitation in the future time period （2071-2100） at high elevation stations will probably increase while at other stations decreases will occur. This study implies potential application of the GiST stochastic model in investigating the impact of climate change on hydrology and water resources.展开更多
The multi-sited practices (MSP) policy in China is expected to exert found implications upon uneven distribution of high-quality medical resources,coupled with the widespread phenomenon of physician's informal pra...The multi-sited practices (MSP) policy in China is expected to exert found implications upon uneven distribution of high-quality medical resources,coupled with the widespread phenomenon of physician's informal practices on multiple sites.Since 2009,the Chinese government has upheld a policy that allows medical doctors to take on secondary jobs for the purpose of encouraging talented physicians to work in medical institutions and underdeveloped areas where their expertise is badly needed.This paper focuses on the MSP policy in China by examining how it has been implemented at the national and provincial levels through a review of government documents,statistical information,academic papers,and newspaper accounts.Despite the MSP policy is to offer incentive to physicians at first-tier public hospitals to work in primary care centers or areas where their expertise,the evidence is hard to find.This paper identifies several outstanding challenges to the MSP policy:(1) The importance of the MSP policy which is made by the central government is perceived differently at the provincial level by health officials and hospital administrators;(2) Interest in implementing the policy varies among physicians and hospitals;(3) Concerns about quality control and legal responsibilities for medical doctors to take on secondary jobs are widespread.China's MSP policy differs from the 'dual practice' policy in many countries because of its top-down approach,with its emphasis on government's role and administrative intervention.This paper's findings may be useful for other developing countries where medical expertise is unevenly distributed due to market forces.On the special occasion of the Alma Ata Declaration's 40th anniversary and for the sake of promoting Universal Health Coverage,this paper also aims at sharing with other countries China's experience in trying to develop an adequate force of primary care professionals.At the end of this paper,a four-point proposal is made for policy makers in China.展开更多
Photocatalytic urea production from nitrogen(N_(2))and carbon dioxide(CO_(2))is a sustainable and ecofriendly alternative to the Bosch-Meiser route.However,it remains a significant challenge in developing highly effic...Photocatalytic urea production from nitrogen(N_(2))and carbon dioxide(CO_(2))is a sustainable and ecofriendly alternative to the Bosch-Meiser route.However,it remains a significant challenge in developing highly efficient photocatalysts for enhancing C-N coupling to high-yield urea synthesis.Herein,we propose a multi-site photocatalyst concept to address the concern of low yield by simultaneously improving photogenerated carrier separation and reactant activation.As a proof of concept,a well-defined multisite photocatalyst,Ru nanoparticles and Cu single atoms decorated CeO_(2)nanorods(Ru-Cu/CeO_(2)),is developed for efficient urea production.The incorporation of Ru and Cu sites is crucial not only to generate high-density photogenerated electrons,but also to facilitate N_(2)and CO_(2)adsorption and conversion.The in situ formed local nitrogen-rich area at Ru sites increases the encounter possibility with the carbon-containing species generated from Cu sites,substantially promoting C-N coupling.The Ru-Cu/CeO_(2)photocatalyst exhibits an impressive urea yield rate of 16.7μmol g^(-1)h^(-1),which ranks among the best performance reported to date.This work emphasizes the importance of multi-site catalyst design concept in guaranteeing rapid C-N coupling in photocatalytic urea synthesis and beyond.展开更多
Heteroatom-doping of carbocatalysts has been a powerful strategy to remarkably enhance the catalytic performance.Herein,the underlying nature of N promotional effects on peroxymonosulfate(PMS)activation for phenol rem...Heteroatom-doping of carbocatalysts has been a powerful strategy to remarkably enhance the catalytic performance.Herein,the underlying nature of N promotional effects on peroxymonosulfate(PMS)activation for phenol removal is understood by combining kinetics analysis with multiple techniques.A strategy using mixed acid oxidation of carbon nanotube(CNT)followed by NH3 treatment is employed to yield a series of catalysts with different N-doping contents but similar fraction of sp^(2)-hybridized carbon and defective degree,endowing with a chance to discriminate the dominant N-containing active sites.The multi-sites kinetics analysis suggests the graphitic N-containing sites as the dominant active sites.The mechanism of the surface-bound reactive species is also discriminated as the dominant reaction mechanism.The insights reported here could provide the methodology to fundamentally understand the heteroatom-doping effects of carbocatalysis.展开更多
Larix gmelinii var.principis-rupprechtii(Mayr.)Pilger is an important native tree species in North China with advantages of fast growth,straight trunk,and good wood properties.The multi-year and multi-site breeding re...Larix gmelinii var.principis-rupprechtii(Mayr.)Pilger is an important native tree species in North China with advantages of fast growth,straight trunk,and good wood properties.The multi-year and multi-site breeding research of families of the species has not been reported previously.Based on diameter at breast height(DBH),height and volume of 25 families on four experimental sites,we calculated variance components,genetic parameters,juvenile and mature trait correlations and made genotype main effect plus genotype×environment interaction effect(GGE)biplot based on the breeding values estimated using the method of best linear unbiased prediction(BLUP).Compared with height,DBH and volume had higher heritability and larger variation coefficients,making them the more suitable traits for family selection and evaluation.Based on these,GGE biplots containing 20 combinations of site×age were drawn using data at 13 to 17 years when the interactions between family and location were strong.Test sites classifications based on DBH,and volume were inconsistent,with two categories for DBH and one for volume.The Guyuan site was the most suitable with strong discriminating ability,high representativeness and stability among tree ages.Integrating the ranking results of DBH and volume,families 66,76,82 and 111 were high-yielding and stable,families 78 and96 were high-yielding with above average stability,families72 and 79 were high-yielding with below average stability,whereas stability of family 100 was inconsistent between DBH and volume.Early selection based on DBH was convenient and reliable,and can be made at seven years.This study provides support for the selection of Larix gmelinii var.principis-rupprechtii families in Hebei province and an example for the application of stem analysis data from multiple sites in tree breeding.展开更多
基金Supported by the Research Fund for the Department of Science and Technology of Xi'an (No.GG9907)
文摘The calculation method about infrared multi-sites passive system location is introduced based on the principle of the weighted least square method, and the variance matrix of estimated error is offered. Through deduction, it can be found out that treated appraise precision can be directly analyzed and deduced without carrying out real measure and reaching estimation value. The simulation result shows that the system performance based on the weighted least square method is much better than the traditional passive location method, and it can be also used for reference to the research of the location algorithm of similar system.
基金supported by the National Key Research and Development Program of China(2021YFA1501500 and 2018YFA0704502)the National Natural Science Foundation of China(22171265,22201286,22033008 and 22220102005)+2 种基金Fujian Science&Technology Innovation Laboratory for Optoelectronic Information of China(2021ZZ103)the Open Research Fund of CNMGE Platform&NSCC-TJthe Open Science Promotion Plan 2023 of CSTCloud。
文摘The special electronic characteristics and high atom usage efficiency of metal-nitrogen-carbon(M-N-C)materials have made them extremely attractive for oxygen reduction reactions(ORRs).However,it is inevitable that hydrogen peroxide(H_(2)O_(2))will be formed via the two-electron pathway in ORRs.Herein,the Cu nanoparticles(NPs)have been encapsulated into Ni doped hollow mesoporous carbon spheres(Ni-HMCS)to reduce the generation of H_(2)O_(2)in ORR.Electrochemical tests confirm that the introduction of Cu NPs improves the ORR performance greatly.The obtained Cu/Ni-HMCS exhibits a half-wave potential of 0.82 V vs.reversible hydrogen electrode and a limited current density of 5.5 mA cm^(-2),which is comparable with the commercial Pt/C.Moreover,Cu/Ni-HMCS has been used in Zn-air battery,demonstrating a high power density of 161 mW cm^(-2)and a long-term recharge capability(50 h at 5 mA cm^(-2)).The theoretical calculation proposes a tandem catalysis pathway for Cu/Ni multi-sites catalysis,that is,H_(2)O_(2)released from the Ni-N_(4)and Cu-N_(4)sites migrates to the Cu(111)face,on which the captive H_(2)O_(2)is further reduced to H_(2)O.This work demonstrates an interesting tandem catalytic pathway of dual-metal multi-sites for ORR,which provides an insight into the development of effective fuel cell electrocatalysts.
基金financial supports from the National Key R&D Program of China(No.2020YFA0406204)the National Natural Science Foundation of China(No.51801078)。
文摘Hydrogen,as a cheap,clean,and cost-effective secondary energy source,performs an essential role in optimizing today’s energy structure.Magnesium hydride(Mg H_(2))represents an attractive hydrogen carrier for storage and transportation,however,the kinetic behavior and operating temperature remain undesirable.In this work,a dual-phase multi-site alloy(Ms A)anchored on carbon substrates was designed,and its superior catalytic effects on the hydrogen storage properties of MgH_(2) were reported.Mechanism analysis identified that multi-site Fe Ni_(3)/Ni Cu nanoalloys synergistically served as intrinsic drivers for the striking de/hydrogenation performance of the MgH_(2)-Ms A systems.Concretely,the unique multi-metallic site structure attached to the surface of MgH_(2)provided substantial reversible channels and accessible active sites conducive to the adsorption,activation,and nucleation of H atoms.In addition,the coupling system formed by FeNi_(3) and NiCu dual-phase alloys further enhanced the reactivity between Mg/MgH_(2) and H atoms.Hence,the onset dehydrogenation temperature of Mg H_(2)+5 wt%Ms A was reduced to 195℃ and the hydrogen desorption apparent activation energy was reduced to 83.6 k J/mol.5.08 wt%H_(2) could be released at 250℃ in 20 min,reaching a high dehydrogenation rate of 0.254 wt%H_(2)/min,yet that for MgH_(2) at a higher temperature of 335℃ was only 0.145 wt%H_(2)/min.Then,the dehydrogenated Mg H_(2)-Ms A sample could absorb hydrogen from room temperature(30℃)and charge 3.93 wt%H_(2) at 100℃ within20 min under 3.0 MPa H_(2) pressure.Benefiting from carbon substrates,the 5 wt%Ms A doped-MgH_(2) could still maintain 6.36 wt%hydrogen capacity after 20 cycles.In conclusion,this work provides experimental rationale and new insights for the design of efficient catalysts for magnesium-based solid-state hydrogen storage materials.
文摘In contrast to the predominant mono or difunctionalization of alkenes,the multi-site functionalization of alkenes involving the synergistic formation of more than two new C–C or C–X bonds is much challenging,especially for developing new reaction pathway to afford the functional heterocycle compounds with aggregation-induced emission(AIE)property has been rarely reported.In present work,the multi-site functionalization of in situ generated alkenes with indoles has been developed for the synthesis of diversely functionalized carbazoles through the synergistic construction of multiple C–C bonds and C=O bond.A proposed reaction sequence involving C–H alkenylation/radical oxygen atom transfer/Diels-Alder cycloaddition/dehydrogenative aromatization was supported by experiments and density functional theory calculations.Further derivative carbazole-linked-quinoxaline skeletons represent a class of AIEgens with acceptor-donor-acceptor configuration,which generated the desired twisted intramolecular charge transfer(TICT)AIE properties and could be used as fluorescent probes for detecting the micrometer-sized phase separation of polymer blends.The protocol provides a concise route for the synthesis and application of carbazole-based AIE luminogens.
基金supported by the National Natural Science Foundation of China (No.42177085)。
文摘A long-term(2007-2016) particulate matter dataset measured at multiple sites in Chengdu,an expanding megacity in southwest China, was analyzed. The trends of particulate chemical compositions and source apportionment were used to evaluate and review the effectiveness of source-specific control policies and measures in Atmospheric Pollution Prevention and Control Action Plan(APPCAP). The concentration of particulate matter decreased significantly, and most aerosol components changed synchronously with particulate matter. The results of advanced three-way factor analysis model suggested that six sources were resolved at three sites: coal combustion, vehicle, crustal dust, cement, sulfate, nitrate and secondary organic matter. Secondary source, including secondary organic carbon(SOC),sulfate, nitrate, and ammonium(SNA), was always the main pollution source in this region.Dust, including cement and crustal dust, was important primary source. Encouragingly, coal combustion had been significantly controlled after APPCAP. The central site represented the higher contribution of vehicles, nitrates and SOC, while north and eastern sites showed the higher contribution of sulfate, coal combustion and dust. Many evidence points to substantial alterations in the physicochemical attributes of Chengdu's atmosphere. The rising proportion of nitrate and the transition of the atmospheric environment from ammoniapoor to ammonia-rich conditions highlight the necessity for the next phase of particulate matter control to focus intensively on the management of NH3and NOx. China's APPCAP could provide useful experience for vast developing countries and other urbanizing and industrializing regions to strike a balance between social development and environmental protection.
基金sponsored by the National Natural Science Foundation of China (Nos. 22308145, 22208140, 22178159, 22078145)Natural Science Foundation of Jiangsu Province (BK20230791)Postgraduate Research Innovation Program of Jiangsu Province (KYCX24_0165)。
文摘Removing H_(2)S and CO_(2)is of great significance for natural gas purification.With excellent gas affinity and tunable structure,ionic liquids(ILs) have been regarded as nontrivial candidates for fabricating polymer-based membranes.Herein,we firstly reported the incorporation of protic ILs (PILs) having ether-rich and carboxylate sites (ECPILs) into poly(ether-block-amide)(Pebax) matrix for efficient separation H_(2)S and CO_(2)from CH_(4).Notably,the optimal permeability of H_(2)S reaches up to 4310 Barrer (40C,0.50 bar) in Pebax/ECPIL membranes,along with H_(2)S/CH_(4)and (H_(2)StCO_(2))/CH_(4)selectivity of 97.7 and 112.3,respectively.These values are increased by 1125%,160.8%and 145.9%compared to those in neat Pebax membrane.Additionally,the solubility and diffusion coefficients of the gases were measured,demonstrating that ECPIL can simultaneously strengthen the dissolution and diffusion of H_(2)S and CO_(2),thus elevating the permeability and permselectivity.By using quantum chemical calculations and FT-IR spectroscopy,the highly reversible multi-site hydrogen bonding interaction between ECPILs and H_(2)S was revealed,which is responsible for the fast permeation of H_(2)S and good selectivity.Furthermore,H_(2)S/CO_(2)/CH_(4)(3/3/94 mol/mol) ternary mixed gas can be efficiently and stably separated by Pebax/ECPIL membrane for at least 100 h.Overall,this work not only illustrates that PILs with ether-rich and carboxylate hydrogen bonding sites are outstanding materials for simultaneous removal of H_(2)S and CO_(2),but may also provide a novel insight into the design of membrane materials for natural gas upgrading.
基金This work was supported by a Research Grant from Pukyong National University(2021).
文摘Accurate multi-step PM_(2.5)(particulate matter with diameters≤2.5 um)concentration prediction is critical for humankinds’health and air populationmanagement because it could provide strong evidence for decisionmaking.However,it is very challenging due to its randomness and variability.This paper proposed a novel method based on convolutional neural network(CNN)and long-short-term memory(LSTM)with a space-shared mechanism,named space-shared CNN-LSTM(SCNN-LSTM)for multi-site dailyahead multi-step PM_(2.5)forecasting with self-historical series.The proposed SCNN-LSTM contains multi-channel inputs,each channel corresponding to one-site historical PM_(2.5)concentration series.In which,CNN and LSTM are used to extract each site’s rich hidden feature representations in a stack mode.Especially,CNN is to extract the hidden short-time gap PM_(2.5)concentration patterns;LSTM is to mine the hidden features with long-time dependency.Each channel extracted features aremerged as the comprehensive features for future multi-step PM_(2.5)concentration forecasting.Besides,the space-shared mechanism is implemented by multi-loss functions to achieve space information sharing.Therefore,the final features are the fusion of short-time gap,long-time dependency,and space information,which enables forecasting more accurately.To validate the proposed method’s effectiveness,the authors designed,trained,and compared it with various leading methods in terms of RMSE,MAE,MAPE,and R^(2)on four real-word PM_(2.5)data sets in Seoul,South Korea.The massive experiments proved that the proposed method could accurately forecast multi-site multi-step PM_(2.5)concentration only using self-historical PM_(2.5)concentration time series and running once.Specifically,the proposed method obtained averaged RMSE of 8.05,MAE of 5.04,MAPE of 23.96%,and R^(2)of 0.7 for four-site daily ahead 10-hourPM_(2.5)concentration forecasting.
基金the partial support of this work by Shahid Chamran Research Council
文摘A highly effective and mild protocol for ring opening of epoxides with NH4SCN in the presence of catalytic amount of a multi- site phase-transfer catalyst, α,α＇,α＂-N-hexakis（triethylammoniummethylene chloride）-melamine, is developed. A variety of ^-hydroxy thiocyanates as important intermediates in agricultural and pharmaceutical chemistry were obtained in high yields with excellent regioselectivity and in short reaction times. 2009 Ali Reza Kiasat. Published by Elsevier B.V. on behalf of Chinese Chemical Society. All rights reserved.
基金This work was financially supported by the National Key Research and Development Program of China(Grant No.2016YFC0502101)the Second Tibetan Plateau Scientific Expedition and Research Program(STEP)(Grant No.SQ2019QZKK1603)a Visiting Scholarship funded by the China Scholarship Council(Grant No.202004910612).
文摘Background:We aimed to characterise the geographical distribution of Sørensen-based multi-site dissimilarity(β_(sor))and its underlying true turnover(β_(sim))and nestedness(βsne)components for Chinese Lauraceae and to analyse their relationships to current climate and past climate change.Methods:We used ensembles of small models(ESMs)to map the current distributions of 353 Lauraceae species in China and calculated β_(sor) and its β_(sim) and β_(sne) components.We tested the relationship between β_(sor),β_(sne) and β_(sim) with current climate and past climate change related predictors using a series of simultaneous autoregressive(SAR_(err))models.Results:Spatial distribution of β_(sor)of Lauraceae is positively correlated with latitude,showing an inverse rela-tionship to the latitudinalα-diversity(species richness)gradient.High β_(sor) occurs at the boundaries of the warm temperate and subtropical zones and at the Qinghai-Tibet Plateau due to high β_(sne).The optimized SAR_(err) model explainsβ_(sor) andβ_(sne) well,but notβ_(sim).Current mean annual temperature determinesβ_(sor) and β_(sne) of Lauraceae more than anomalies and velocities of temperature or precipitation since the Last Glacial Maximum.Conclusions:Current low temperatures and high climatic heterogeneity are the main factors explaining the high multi-siteβ-diversity of Lauraceae.In contrast to analyses of the β-diversity of entire species assemblages,studies of single plant families can provide complementary insights into the drivers of β-diversity of evolutionarily more narrowly defined entities.
基金This research was funded by The Talents Project for Harbin Science and Technology Innovation,grant number 2016RAXXJ006China Postdoctoral Science Foundation,grant number 2017M611341.
文摘Cellulose nanofibrils(CNFs)are promising sustainable materials that can be applied to nanocomposites,as well as medical and life-sciences devices.However,methods for the preparation of these important materials are energy intensive because heating and mechanical disintegration are required to produce cellulose fibers below 100 nm in size.In this study,CNFs were prepared through the multi-site regioselective oxidation of cellulose with 2,2,6,6-tetramethylpiperidine-1-oxyl(TEMPO)and periodate at room temperature(20–25°C),without any mechanical-disintegration treatment.Transmission electron microscopy(TEM)revealed that the CNFs had the average widths of 14.1,55.4,and 81.9 nm for three different treatments.Fourier-transform infrared spectroscopy revealed that carboxyl groups were created on the surfaces of the microfibrils,while X-ray diffraction studies showed that the cellulose I structure was maintained after oxidation,and that the cellulose nanofibril crystallinity index exceeded 70%.These results demonstrate that CNFs can be prepared by multi-site regioselective oxidation at room temperature in the absence of mechanical disintegration.In addition,a model was developed to calculate the total content of carboxylate and aldehyde groups of CNFs prepared by the TEMPO mediate oxidation,the periodate oxidation,and the multi-site regioselective oxidation methods based on the particle width determined by TEM.The calculated values of the model were in good agreement with the total content(experimental value)of carboxylate and aldehyde groups of CNFs prepared by the TEMPO-mediated oxidation and the multi-site regioselective oxidation methods.However,the model was not valid for CNFs prepared by the periodate oxidation method.
基金supported by Russian Foundation for Fundamental Research No.16-29-08173-ofi-m(YG)Partial support for data analysis and interpretation of the results was provided from the Russian Science Foundation No.14-45-00024(YG)the Craig H.Neilsen Foundation#72940(PKS)
文摘With the advent of spinal cord epidural stimulation techniques,i.e.,electrically enabled motor control（e Emc）in combination with activity dependent locomotor training,humans with traumatic complete sensori-motor paralysis are able to initiate voluntary leg movements and achieve gains in postural control,and bladder and sexual function（Angeli et al.,2014）.
基金Projcct supportcd by the International Scicncc ＆ Technology Co- operation Program of China （No. 2010DFA24320）, and the National Natural Science Foundation of China （Nos. 51379183 and 50809058） ~ Zhcjiang Univcrsity and Springcr-Vcrlag Bcrlin Hcidclberg 2014
文摘Recent years have seen a surge in assessment of potential impacts of climate change. As one of the most important tools for generating synthetic hydrological model inputs, weather generators have played an important role in climate change impact analysis of water management. However, most weather generators like statistical downscaling model （SDSM） and long Ashton research station weather generator （LARS-WG） are designed for single site data generation. Considering the significance of spatial correlations of hydro-meteorological data, multi-site weather data generation becomes a necessity. In this study we aim to evaluate the performance of a new multi-site stochastic model, geo-spatial temporal weather generator （GIST）, in simulating precipitation in the Qiantang River Basin, East China. The correlation matrix, precipitation amount and occurrence of observed and GiST-generated data are first compared for the evaluation process. Then we use the GiST model combined with the change factor method （CFM） to investigate future changes of precipitation （2071 2100） in the study area using one global climate model, Hadgem2 ES, and an extreme emission scenario RCP 8.5, The final results show that the simulated precipitation amount and occurrence by GiST matched their historical counterparts reasonably. The correlation coefficients between simulated and his- torical precipitations show good consistence as well. Compared with the baseline period （1961 1990）, precipitation in the future time period （2071-2100） at high elevation stations will probably increase while at other stations decreases will occur. This study implies potential application of the GiST stochastic model in investigating the impact of climate change on hydrology and water resources.
文摘The multi-sited practices (MSP) policy in China is expected to exert found implications upon uneven distribution of high-quality medical resources,coupled with the widespread phenomenon of physician's informal practices on multiple sites.Since 2009,the Chinese government has upheld a policy that allows medical doctors to take on secondary jobs for the purpose of encouraging talented physicians to work in medical institutions and underdeveloped areas where their expertise is badly needed.This paper focuses on the MSP policy in China by examining how it has been implemented at the national and provincial levels through a review of government documents,statistical information,academic papers,and newspaper accounts.Despite the MSP policy is to offer incentive to physicians at first-tier public hospitals to work in primary care centers or areas where their expertise,the evidence is hard to find.This paper identifies several outstanding challenges to the MSP policy:(1) The importance of the MSP policy which is made by the central government is perceived differently at the provincial level by health officials and hospital administrators;(2) Interest in implementing the policy varies among physicians and hospitals;(3) Concerns about quality control and legal responsibilities for medical doctors to take on secondary jobs are widespread.China's MSP policy differs from the 'dual practice' policy in many countries because of its top-down approach,with its emphasis on government's role and administrative intervention.This paper's findings may be useful for other developing countries where medical expertise is unevenly distributed due to market forces.On the special occasion of the Alma Ata Declaration's 40th anniversary and for the sake of promoting Universal Health Coverage,this paper also aims at sharing with other countries China's experience in trying to develop an adequate force of primary care professionals.At the end of this paper,a four-point proposal is made for policy makers in China.
基金support by the National Natural Science Foundation of China(12222508,12475325,and 22209061)the Youth Innovation Promotion Association CAS(2020454)+2 种基金the National Key R&D Program of China(2019YFA0405601 and2023YFA1506304)the Fundamental Research Funds for the Universities of Inner Mongolia Autonomous Region(JY20250030)the Start-up Fund for Senior Talents in Jiangsu University(21JDG060)。
文摘Photocatalytic urea production from nitrogen(N_(2))and carbon dioxide(CO_(2))is a sustainable and ecofriendly alternative to the Bosch-Meiser route.However,it remains a significant challenge in developing highly efficient photocatalysts for enhancing C-N coupling to high-yield urea synthesis.Herein,we propose a multi-site photocatalyst concept to address the concern of low yield by simultaneously improving photogenerated carrier separation and reactant activation.As a proof of concept,a well-defined multisite photocatalyst,Ru nanoparticles and Cu single atoms decorated CeO_(2)nanorods(Ru-Cu/CeO_(2)),is developed for efficient urea production.The incorporation of Ru and Cu sites is crucial not only to generate high-density photogenerated electrons,but also to facilitate N_(2)and CO_(2)adsorption and conversion.The in situ formed local nitrogen-rich area at Ru sites increases the encounter possibility with the carbon-containing species generated from Cu sites,substantially promoting C-N coupling.The Ru-Cu/CeO_(2)photocatalyst exhibits an impressive urea yield rate of 16.7μmol g^(-1)h^(-1),which ranks among the best performance reported to date.This work emphasizes the importance of multi-site catalyst design concept in guaranteeing rapid C-N coupling in photocatalytic urea synthesis and beyond.
基金supported by the Natural Science Foundation of China(21922803 and 21776077)the Shanghai Natural Science Foundation(17ZR1407300 and 17ZR1407500)+3 种基金the China Postdoctoral Science Foundation(BX20190116)the Program for Professor of Special Appointment(Eastern Scholar)at Shanghai Institutions of Higher Learning,the Shanghai Rising-Star Program(17QA1401200)the State Key Laboratory of Organic-Inorganic Composites(oic-201801007)the Open Project of State Key Laboratory of Chemical Engineering(SKLChe-15C03 and SKL-ChE-16C05).
文摘Heteroatom-doping of carbocatalysts has been a powerful strategy to remarkably enhance the catalytic performance.Herein,the underlying nature of N promotional effects on peroxymonosulfate(PMS)activation for phenol removal is understood by combining kinetics analysis with multiple techniques.A strategy using mixed acid oxidation of carbon nanotube(CNT)followed by NH3 treatment is employed to yield a series of catalysts with different N-doping contents but similar fraction of sp^(2)-hybridized carbon and defective degree,endowing with a chance to discriminate the dominant N-containing active sites.The multi-sites kinetics analysis suggests the graphitic N-containing sites as the dominant active sites.The mechanism of the surface-bound reactive species is also discriminated as the dominant reaction mechanism.The insights reported here could provide the methodology to fundamentally understand the heteroatom-doping effects of carbocatalysis.
基金supported by the Key Research and Development Program of Hebei Province[20326333D]Science and Technology Promotion Demonstration Project of forestry and grassland in Hebei Province[Hebei TG[2019]001]Science and Technology Promotion Demonstration Project of forestry and grassland in Hebei Province[Hebei TG[2020]013]。
文摘Larix gmelinii var.principis-rupprechtii(Mayr.)Pilger is an important native tree species in North China with advantages of fast growth,straight trunk,and good wood properties.The multi-year and multi-site breeding research of families of the species has not been reported previously.Based on diameter at breast height(DBH),height and volume of 25 families on four experimental sites,we calculated variance components,genetic parameters,juvenile and mature trait correlations and made genotype main effect plus genotype×environment interaction effect(GGE)biplot based on the breeding values estimated using the method of best linear unbiased prediction(BLUP).Compared with height,DBH and volume had higher heritability and larger variation coefficients,making them the more suitable traits for family selection and evaluation.Based on these,GGE biplots containing 20 combinations of site×age were drawn using data at 13 to 17 years when the interactions between family and location were strong.Test sites classifications based on DBH,and volume were inconsistent,with two categories for DBH and one for volume.The Guyuan site was the most suitable with strong discriminating ability,high representativeness and stability among tree ages.Integrating the ranking results of DBH and volume,families 66,76,82 and 111 were high-yielding and stable,families 78 and96 were high-yielding with above average stability,families72 and 79 were high-yielding with below average stability,whereas stability of family 100 was inconsistent between DBH and volume.Early selection based on DBH was convenient and reliable,and can be made at seven years.This study provides support for the selection of Larix gmelinii var.principis-rupprechtii families in Hebei province and an example for the application of stem analysis data from multiple sites in tree breeding.
