Deep eutectic solvents(DESs) are now considered a new class of ionic liquid analogs that have been generously used in various fields.Herein, vanadium phosphorus oxide(VPO) catalysts are synthesized in combination with...Deep eutectic solvents(DESs) are now considered a new class of ionic liquid analogs that have been generously used in various fields.Herein, vanadium phosphorus oxide(VPO) catalysts are synthesized in combination with a deep eutectic solvent containing rare earth metal(rE-DES), and their catalytic performance in n-butane selective oxidation to produce maleic anhydride(MA) is evaluated. The rE-DES is produced from the interaction of choline chloride(ChCl) and rare earth metal salts(Cerium, Europium, Lanthanum, and Samarium metal salt)(ChCl:rE = 1:0.5–1:3) under mild conditions. It was found that DESs served as structural modifiers and electronic promoters during VPO synthesis. It regulated the chemical state of the catalyst surface, such as the vanadium valence state, acid-base properties, and ratios of V^(4+)/V^(5+),Lat–O/Sur–O and P/V. Various characterization techniques, such as FT-IR, DSC, XRD, SEM, EDS, TEM, Raman, TGA, NH3-TPD, and XPS,were used to examine its physical and chemical characteristics. These characteristics were correlated with the catalytic performance. The VPO catalyst modified by rE-DES showed a significant enhancement of n-butane conversion and MA selectivity while suppressing the selectivity of CO and CO_(2)as well as the CO/CO_(2)ratio compared to the unpromoted VPO catalyst. Especially for Ce-DES-VPO, it increased the n-butane conversion and MA mass yield up to approximately 11% and 10%, respectively. In addition, we evaluated the catalytic performance under different activation atmospheres.展开更多
Lanthanum-containing(LaX)and cerium-containing X zeolites(CeX)were prepared by a doubleexchange,double-calcination method.By changing the calcination atmospheres between nitrogen and air,the Ce^(IV) contents in CeX ze...Lanthanum-containing(LaX)and cerium-containing X zeolites(CeX)were prepared by a doubleexchange,double-calcination method.By changing the calcination atmospheres between nitrogen and air,the Ce^(IV) contents in CeX zeolites were adjusted and their impacts on physicochemical properties and catalytic performance in isobutane alkylation were established.The crystallinity of CeX zeolite was found to be negatively correlated with the Ce^(IV) content.This i s believed to be due to the water formed during the oxidation of Ce^(III),which facilitates the framework dealumination.As a consequence,calcining in air resulted in a great elimination of strong Brønsted acid sites while under nitrogen protection,this phenomenon was mostly hindered and the sample’s acidity was preserved.When tested in a continuously flowed slurry reactor,the catalyst lifetime for isobutane alkylation was found to be linearly related to the strong Brønsted acid concentration.In addition,Ce^(3+)was found more benefit for the hydride transfer compared with La^(3+),which is ascribed to the stronger polarization effect on the CH bond of isobutane.Moreover,the decline of hydride transfer activity can be slowed down by the catalytic cracking of the bulky molecules.Based on the product distribution,a new catalytic cycle of dimethylhexanes(DMHs)involving a direct formation of isobutene rather than tert-butyl carbocation was proposed in isobutane alkylation.展开更多
The utilization of lighter alkanes into useful chemical products is essential for modern chemistry and reducing the CO_(2)emission.Particularly,n-butane has gained special attention across the globe due to the abundan...The utilization of lighter alkanes into useful chemical products is essential for modern chemistry and reducing the CO_(2)emission.Particularly,n-butane has gained special attention across the globe due to the abundant production of maleic anhydride(MA).Vanadium phosphorous oxide(VPO)is the most effective catalyst for selective oxidation of n-butane to MA so far.Interestingly,the VPO complex exists in more or less fifteen different structures,each one having distinct phase composition and exclusive surface morphology and physiochemical properties such as valence state,lattice oxygen,acidity etc.,which relies on precursor preparation method and the activation conditions of catalysts.The catalytic performance of VPO catalyst is improved by adding different promoters or co-catalyst such as various metals dopants,or either introducing template or structural-directing agents.Meanwhile,new preparation strategies such as electrospinning,ball milling,hydrothermal,barothermal,ultrasound,microwave irradiation,calcination,sol-gel method and solvothermal synthesis are also employed for introducing improvement in catalytic performance.Research in above-mentioned different aspects will be ascribed in current review in addition to summarizing overall catalysis activity and final yield.To analyze the performance of the catalytic precursor,the reaction mechanism and reaction kinetics both are discussed in this review to help clarify the key issues such as strong exothermic reaction,phosphorus supplement,water supplement,deactivation,and air/n-butane pretreatment etc.related to the various industrial applications of VPO.展开更多
A double-effect reactive distillation(DERD)process was proposed for the production of propylene glycol methyl ether from propylene oxide and methanol to overcome the shortcoming of low selectivity and high-energy cons...A double-effect reactive distillation(DERD)process was proposed for the production of propylene glycol methyl ether from propylene oxide and methanol to overcome the shortcoming of low selectivity and high-energy consumption in the tubular plug-flow reactor.A single-column reactive distillation(RD)process was conducted under optimized operating conditions based on sensitivity analysis as a reference.The results demonstrated that the proposed DERD process is able to achieve more than 95%selectivity of the desired product.After that,a design approach of the DERD process with an objective of the minimum operating cost was proposed to achieve further energy savings in the RD process.The proposed DERD configuration can provide a large energy-savings by totally utilization of the overhead vapor steam in the high-pressure RD column.A comparison of the single-column RD process revealed that the proposed DERD process can reduce the operating cost and the total annual cost of 25.3%and 30.7%,respectively,even though the total capital cost of DERD process is larger than that of the RD process.展开更多
Passive sampling technology has good application prospects for monitoring trace pollutants in aquatic environments.Further research on the sampling mechanism of this technology is essential to improve the measurement ...Passive sampling technology has good application prospects for monitoring trace pollutants in aquatic environments.Further research on the sampling mechanism of this technology is essential to improve the measurement accuracy and extend the application scope of this approach.In this study,adsorption and permeation experiments were performed to investigate the sorption and mass transfer properties of five chiral pharmaceuticals at the enantiomeric level on polyethersulfone(PES)and polytetrafluoroethylene(PTFE)membranes used in a polar organic chemical integrative sampler.Batch adsorption experiments showed that the PES membrane had an adsorption phenomenon for most selected pollutants and an insignificant sorption behavior was observed for all selected pharmaceuticals on the PTFE membrane except for R(S)-fluoxetine.The diffusion coefficients of selected pharmaceuticals onto the PTFE membrane were approximately one order of magnitude higher than those onto the PES membrane.The permeation experiment indicated that under different hydraulic conditions,the change of the relative pollutant concentration through the PTFE membrane for the composite pollutant system was more obvious than that for the single pollutant system,and mass transfer hysteresis exists for both contaminant systems through PES membranes.Using the first-order equation or 3-component model to estimate the overall mass transfer coefficients,the results showed that the overall mass transfer coefficient values of pollutants in the composite pollutant system onto both membranes were higher than those in the single pollutant system.This parameter was mainly influenced by the synergistic effects of the multi-analyte interaction and diminished water boundary layers during the mass transfer process.展开更多
Poly(ionic liquids)(PILs)combined with the macromolecular structure and unique properties of ionic liquids show unlimited potential in catalysis.In this work,a series of metal-based PIL with different ionic ratios wer...Poly(ionic liquids)(PILs)combined with the macromolecular structure and unique properties of ionic liquids show unlimited potential in catalysis.In this work,a series of metal-based PIL with different ionic ratios were prepared for the selective oxidation of cyclohexane.Characterization analysis reveals that different degrees of ionization could adjust the Co-N sites of the catalysts efficiently,leading to significant changes in their electronic structure,which strongly relate to catalytic performance in oxidation.20.07%cyclohexane conversion and 13.06%cyclohexanone and cyclohexanol(KA oil)yield can be achieved by metal-based PILs that are better than other commercial catalysts.Compared with CoCl_(2),metal-based PILs perform well,with superior conversion and KA oil yield.More interestingly,the catalyst created in this study features a malleable Co-N site,which may potentially have an impact on how oxygen species adsorb and desorb from the catalyst.Therefore,the catalyst studied in this work is used as molecular oxygen for the selective oxidation of cyclohexane to produce KA oil,and its application prospect is promising.展开更多
The sustainable synthesis of dimethyl maleate via diesterification through the utilization of ionic liquid(IL)is of great importance.However,the relationship between the ILs nature and the reactivity of diesterificati...The sustainable synthesis of dimethyl maleate via diesterification through the utilization of ionic liquid(IL)is of great importance.However,the relationship between the ILs nature and the reactivity of diesterification is still unclear.Herein,a series of ILs with different structures were selected for the comprehensive investigation of diesterification.The acidity(H_(0))and Kamlet-Taft solvent parameters(hydrogen bond donor ability(α),hydrogen bond acceptor ability(β),and polarizability(π^(*)))of ILs were measured by UV–Visible spectroscopy,and the effects of them on the diesterification of maleic anhydride were also studied in detail.The results indicated that not only H0of the IL-based catalysis system,but also itsα,β,andπ^(*)influenced the reaction activity of diesterification.Furthermore,a quantifiable correlation was fitted between the natural logarithm of the rate constant and multiple parameters of ILs,indicating that the diesterification rate had a positive correlation with the H0,α,andπ^(*),and inverse correlation with theβof the IL.A plausible synergetic reaction mechanism for the excellent performance of[(HSO_(3))PMim][HSO_(4)]has been proposed.Overall,this work thoroughly explored the relationship between the nature of ILs on diesterification in-depth,which will reveal the nature of diesterification in detail.展开更多
From the viewpoint of earth system science,this paper discusses the observation capability of the second-generation of Chinese polar-orbiting,sun-synchronous operational meteorological satellite observation systems,Fe...From the viewpoint of earth system science,this paper discusses the observation capability of the second-generation of Chinese polar-orbiting,sun-synchronous operational meteorological satellite observation systems,Fengyun-3(FY-3),based on the function and performance test results from the FY-3 D satellite observation system in orbit.The FY-3 series of satellites have numerous remote sensing instruments and a wide range of imaging and sounding electromagnetic spectrometers onboard.These instruments can obtain reflectivity data for land surface,soil,vegetation,water body,snow cover,ocean color,and sea ice on earth’s surface over a wide spectral range,as well as information on the absorption and scattering radiative transfer of molecules and particles(clouds and aerosols)in earth’s atmosphere.All of these data can be used to retrieve physical and chemical information about the land,ocean,and atmosphere of the earth system.Comprehensive observation of the earth system by the FY-3 meteorological satellites is preliminarily realized.展开更多
Dissolved organic matter(DOM)is an important constituent of wastewater treatment plant(WWTP)effluent.A novel combined tidal and subsurface flow constructed wetland(TF-SSFCW)of 90 L was constructed for a ten-month tria...Dissolved organic matter(DOM)is an important constituent of wastewater treatment plant(WWTP)effluent.A novel combined tidal and subsurface flow constructed wetland(TF-SSFCW)of 90 L was constructed for a ten-month trial of advanced treatment of the WWTP effluent.Excitation emission matrix(EEM)fluorescence spectroscopy,parallel factor(PARAFAC)analysis and a two end-member mixing model were employed to characterize the composition and removal process of the effluent DOM(EfOM)from the WWTP.The results showed that the TF-SSF-CW performed an efficient EfOM removal with dissolved organic carbon(DOC)removal rate of 88%and dissolved organic nitrogen(DON)removal rate of 91%.Further analysis demonstrated that the EfOM consisted mainly of two protein moieties and two humic-like groups;protein moieties(76%)constituted the main content of EfOM in raw water and humic-like groups(57%)became the dominating contributor after treatment.The EfOM from the WWTP was mainly of aquatic bacterial origin and evolved to a higher proportion of terrigenous origin with higher humification in the TF-SSF-CW effluent.A common controlling treatment-related factor for determining the concentrations of the same kind of substances(protein groups or humic-like groups)was revealed to exist,and the ratio of removal rates between the same substances in treatment was calculated.Our study demonstrates that the TF-SSF-CW can be a novel and effective treatment method for the EfOM from WWTPs,and is helpful for understanding of the character of EfOM in wetland treatment.展开更多
Ionic liquid coupled with strong acid systems presents considerable promise in some catalytic fields.In the present work,the multiple complex systems composed by 98 wt%concentrated sulfuric acid and[Bmim][SbF_6]were i...Ionic liquid coupled with strong acid systems presents considerable promise in some catalytic fields.In the present work,the multiple complex systems composed by 98 wt%concentrated sulfuric acid and[Bmim][SbF_6]were investigated in the terms of stability,acidity and interaction properties.It was found that acidolysis of[Bmim][SbF_6]occurred in the 98 wt%concentrated sulfuric acid accompanied by HF releasing and SbF_6~ degrading to[SbF_(6-y)XHSO_4]_y]^-.The species after acidolysis in the multiple complex systems were checked and confirmed by electrospray ionization mass spectrometry(ESI-MS),Fourier transform infrared spectroscopy(FT-IR),~1H NMR and ^(19)F NMR.Acidity increased slightly with less than 1 wt%[Bmim][SbF_6]addition,while decreased with more proportion,which was determined based on the Hammett acidity functions H_0,using ^(13)C NMR.The strong hydrogen bond S-O-H…F of interaction among the multiple complex systems was confirmed by molecular dynamic simulation.展开更多
The coexistence of wireless body sensor networks(WBSNs) is a very challenging problem, due to strong interference, which seriously affects energy consumption and spectral reuse. The energy efficiency and spectral effi...The coexistence of wireless body sensor networks(WBSNs) is a very challenging problem, due to strong interference, which seriously affects energy consumption and spectral reuse. The energy efficiency and spectral efficiency are two key performance evaluation metrics for wireless communication networks. In this paper, the fundamental tradeoff between energy efficiency and area spectral efficiency of WBSNs is first investigated under the Poisson point process(PPP) model and Matern hard-core point process(HCPP) model using stochastic geometry. The circuit power consumption is taken into consideration in energy efficiency calculation. The tradeoff judgement coefficient is developed and is shown to serve as a promising complementary measure. In addition, this paper proposes a new nearest neighbour distance power control strategy to improve energy efficiency. We show that there exists an optimal transmit power highly dependant on the density of WBSNs and the nearest neighbour distance. Some important properties are also addressed in the analysis of coexisting WBSNs based on the IEEE 802.15.4 standard, such as the impact of intensity nodes distribution,optimal guard zone, and outage probability. Simulation results show that the proposed power control design can reduce the outage probability and enhance energy efficiency. Energy efficiency and area spectral efficiency of the HCPP model are better than those of the PPP model. In addition, the optimal density of WBSNs coexistence is obtained.展开更多
Electroreduction of CO_(2) to target products with high activity and selectivity has techno-economic importance for renewable energy storage and CO_(2) utilization.Herein,we report a hierarchical CuS hollow polyhedron...Electroreduction of CO_(2) to target products with high activity and selectivity has techno-economic importance for renewable energy storage and CO_(2) utilization.Herein,we report a hierarchical CuS hollow polyhedron(CuS-HP)for electrocatalytic CO_(2) reduction(E-CO_(2)R)in neutral pH aqueous media.Under E-CO_(2)R conditions,CuS-HP undergoes structural reconstruction into sulfur-doped metallic Cu catalyst,which promotes formate production with Faradaic efficiency>90%in a wide potential range.展开更多
基金supported by the National Key Research and Development Program of China, China (2017YFA0206803)the Innovation Academy for Green Manufacture of Chinese Academy of Science (IAGM2020C17)+1 种基金K. C. Wong Education Foundation (No. GJTD-2018-04)Supported by the Joint Fund of the Yulin University and the Dalian National Laboratory for Clean Energy, China (Grant. YLU-DNL Fund2021016)。
文摘Deep eutectic solvents(DESs) are now considered a new class of ionic liquid analogs that have been generously used in various fields.Herein, vanadium phosphorus oxide(VPO) catalysts are synthesized in combination with a deep eutectic solvent containing rare earth metal(rE-DES), and their catalytic performance in n-butane selective oxidation to produce maleic anhydride(MA) is evaluated. The rE-DES is produced from the interaction of choline chloride(ChCl) and rare earth metal salts(Cerium, Europium, Lanthanum, and Samarium metal salt)(ChCl:rE = 1:0.5–1:3) under mild conditions. It was found that DESs served as structural modifiers and electronic promoters during VPO synthesis. It regulated the chemical state of the catalyst surface, such as the vanadium valence state, acid-base properties, and ratios of V^(4+)/V^(5+),Lat–O/Sur–O and P/V. Various characterization techniques, such as FT-IR, DSC, XRD, SEM, EDS, TEM, Raman, TGA, NH3-TPD, and XPS,were used to examine its physical and chemical characteristics. These characteristics were correlated with the catalytic performance. The VPO catalyst modified by rE-DES showed a significant enhancement of n-butane conversion and MA selectivity while suppressing the selectivity of CO and CO_(2)as well as the CO/CO_(2)ratio compared to the unpromoted VPO catalyst. Especially for Ce-DES-VPO, it increased the n-butane conversion and MA mass yield up to approximately 11% and 10%, respectively. In addition, we evaluated the catalytic performance under different activation atmospheres.
基金supported by the One Hundred Talent Program of CASthe National Natural Science Foundation of China Petroleum & Chemical Corporation Joint Fund(U1662129)+1 种基金the National Natural Science Foundation of China(91434203)the Key Research Program of Frontier Sciences,Chinese Academy of Sciences(QYZDY-SSW-JSC011)~~
基金This work was supported by the National Key Research and Development Program of China(2017YFA0206803)the National Natural Science Foundation of China(21878315)+3 种基金the Key Programs of the Chinese Academy of Sciences(KFZD-SW-413)the Key Programs of Innovation Academy for Green Manufacture,CAS(IAGM2020C17)K.C.Wong Education Foundation(No.GJTD-2018-04)the Major Program of National Natural Science Foundation of China(21890762).
文摘Lanthanum-containing(LaX)and cerium-containing X zeolites(CeX)were prepared by a doubleexchange,double-calcination method.By changing the calcination atmospheres between nitrogen and air,the Ce^(IV) contents in CeX zeolites were adjusted and their impacts on physicochemical properties and catalytic performance in isobutane alkylation were established.The crystallinity of CeX zeolite was found to be negatively correlated with the Ce^(IV) content.This i s believed to be due to the water formed during the oxidation of Ce^(III),which facilitates the framework dealumination.As a consequence,calcining in air resulted in a great elimination of strong Brønsted acid sites while under nitrogen protection,this phenomenon was mostly hindered and the sample’s acidity was preserved.When tested in a continuously flowed slurry reactor,the catalyst lifetime for isobutane alkylation was found to be linearly related to the strong Brønsted acid concentration.In addition,Ce^(3+)was found more benefit for the hydride transfer compared with La^(3+),which is ascribed to the stronger polarization effect on the CH bond of isobutane.Moreover,the decline of hydride transfer activity can be slowed down by the catalytic cracking of the bulky molecules.Based on the product distribution,a new catalytic cycle of dimethylhexanes(DMHs)involving a direct formation of isobutene rather than tert-butyl carbocation was proposed in isobutane alkylation.
基金supported by the National Key Research and Development Program of China(2017YFA0206803)the innovation Academy for Green Manufacture of Chinese Academy of Science(IAGM2020C17)+3 种基金the Key Programs of the Chinese Academy of Sciences(KFZD-SW-413)the National Nature Science Foundation of China(21808223)the Key Programs of Fujian Institute of Innovation,CAS(FJCXY18020203)Chinese Academy of Sciences,the One Hundred Talent Program of CAS。
文摘The utilization of lighter alkanes into useful chemical products is essential for modern chemistry and reducing the CO_(2)emission.Particularly,n-butane has gained special attention across the globe due to the abundant production of maleic anhydride(MA).Vanadium phosphorous oxide(VPO)is the most effective catalyst for selective oxidation of n-butane to MA so far.Interestingly,the VPO complex exists in more or less fifteen different structures,each one having distinct phase composition and exclusive surface morphology and physiochemical properties such as valence state,lattice oxygen,acidity etc.,which relies on precursor preparation method and the activation conditions of catalysts.The catalytic performance of VPO catalyst is improved by adding different promoters or co-catalyst such as various metals dopants,or either introducing template or structural-directing agents.Meanwhile,new preparation strategies such as electrospinning,ball milling,hydrothermal,barothermal,ultrasound,microwave irradiation,calcination,sol-gel method and solvothermal synthesis are also employed for introducing improvement in catalytic performance.Research in above-mentioned different aspects will be ascribed in current review in addition to summarizing overall catalysis activity and final yield.To analyze the performance of the catalytic precursor,the reaction mechanism and reaction kinetics both are discussed in this review to help clarify the key issues such as strong exothermic reaction,phosphorus supplement,water supplement,deactivation,and air/n-butane pretreatment etc.related to the various industrial applications of VPO.
基金Supported by the Second Tibetan Plateau Scientific Expedition and Research(STEP)program(grant no.2019QZKK0105)the National Key Research and Development Program of China(2018YFC1506603).
基金supported by the National Nature Science Foundation of China(21878315 and 21808223)National Key Research and Development Program of China(2017YFA0206803)+3 种基金Innovation Academy for Green ManufactureCAS(IAGM2020C17)K.C.Wong Education Foundation(GJTD-2018-04)。
文摘A double-effect reactive distillation(DERD)process was proposed for the production of propylene glycol methyl ether from propylene oxide and methanol to overcome the shortcoming of low selectivity and high-energy consumption in the tubular plug-flow reactor.A single-column reactive distillation(RD)process was conducted under optimized operating conditions based on sensitivity analysis as a reference.The results demonstrated that the proposed DERD process is able to achieve more than 95%selectivity of the desired product.After that,a design approach of the DERD process with an objective of the minimum operating cost was proposed to achieve further energy savings in the RD process.The proposed DERD configuration can provide a large energy-savings by totally utilization of the overhead vapor steam in the high-pressure RD column.A comparison of the single-column RD process revealed that the proposed DERD process can reduce the operating cost and the total annual cost of 25.3%and 30.7%,respectively,even though the total capital cost of DERD process is larger than that of the RD process.
基金supported by the National Natural Science Foundation of China (No.41977377)。
文摘Passive sampling technology has good application prospects for monitoring trace pollutants in aquatic environments.Further research on the sampling mechanism of this technology is essential to improve the measurement accuracy and extend the application scope of this approach.In this study,adsorption and permeation experiments were performed to investigate the sorption and mass transfer properties of five chiral pharmaceuticals at the enantiomeric level on polyethersulfone(PES)and polytetrafluoroethylene(PTFE)membranes used in a polar organic chemical integrative sampler.Batch adsorption experiments showed that the PES membrane had an adsorption phenomenon for most selected pollutants and an insignificant sorption behavior was observed for all selected pharmaceuticals on the PTFE membrane except for R(S)-fluoxetine.The diffusion coefficients of selected pharmaceuticals onto the PTFE membrane were approximately one order of magnitude higher than those onto the PES membrane.The permeation experiment indicated that under different hydraulic conditions,the change of the relative pollutant concentration through the PTFE membrane for the composite pollutant system was more obvious than that for the single pollutant system,and mass transfer hysteresis exists for both contaminant systems through PES membranes.Using the first-order equation or 3-component model to estimate the overall mass transfer coefficients,the results showed that the overall mass transfer coefficient values of pollutants in the composite pollutant system onto both membranes were higher than those in the single pollutant system.This parameter was mainly influenced by the synergistic effects of the multi-analyte interaction and diminished water boundary layers during the mass transfer process.
基金supported by the National Science Fund for Excellent Young Scholars(22222813)Key Scientific and Technological Projects in Huizhou(2021JBZ5.1)the Joint Fund of Yulin University,and the Dalian National Laboratory for Clean Energy(Grant No.YLU-DNL Fund 2021016)
文摘Poly(ionic liquids)(PILs)combined with the macromolecular structure and unique properties of ionic liquids show unlimited potential in catalysis.In this work,a series of metal-based PIL with different ionic ratios were prepared for the selective oxidation of cyclohexane.Characterization analysis reveals that different degrees of ionization could adjust the Co-N sites of the catalysts efficiently,leading to significant changes in their electronic structure,which strongly relate to catalytic performance in oxidation.20.07%cyclohexane conversion and 13.06%cyclohexanone and cyclohexanol(KA oil)yield can be achieved by metal-based PILs that are better than other commercial catalysts.Compared with CoCl_(2),metal-based PILs perform well,with superior conversion and KA oil yield.More interestingly,the catalyst created in this study features a malleable Co-N site,which may potentially have an impact on how oxygen species adsorb and desorb from the catalyst.Therefore,the catalyst studied in this work is used as molecular oxygen for the selective oxidation of cyclohexane to produce KA oil,and its application prospect is promising.
基金supported by the National Natural Science Foundation of China(21878315)the National Key Research and Development Program of China(2017YFA0206803)+1 种基金the Key Programs of the Chinese Academy of Sciences(KFZD-SW-413)the Key Programs of Innovation Academy for Green Manufacture,CAS(IAGM2020C17)。
文摘The sustainable synthesis of dimethyl maleate via diesterification through the utilization of ionic liquid(IL)is of great importance.However,the relationship between the ILs nature and the reactivity of diesterification is still unclear.Herein,a series of ILs with different structures were selected for the comprehensive investigation of diesterification.The acidity(H_(0))and Kamlet-Taft solvent parameters(hydrogen bond donor ability(α),hydrogen bond acceptor ability(β),and polarizability(π^(*)))of ILs were measured by UV–Visible spectroscopy,and the effects of them on the diesterification of maleic anhydride were also studied in detail.The results indicated that not only H0of the IL-based catalysis system,but also itsα,β,andπ^(*)influenced the reaction activity of diesterification.Furthermore,a quantifiable correlation was fitted between the natural logarithm of the rate constant and multiple parameters of ILs,indicating that the diesterification rate had a positive correlation with the H0,α,andπ^(*),and inverse correlation with theβof the IL.A plausible synergetic reaction mechanism for the excellent performance of[(HSO_(3))PMim][HSO_(4)]has been proposed.Overall,this work thoroughly explored the relationship between the nature of ILs on diesterification in-depth,which will reveal the nature of diesterification in detail.
基金Supported by the National Development and Reform Commission and Ministry of Finance of China.
文摘From the viewpoint of earth system science,this paper discusses the observation capability of the second-generation of Chinese polar-orbiting,sun-synchronous operational meteorological satellite observation systems,Fengyun-3(FY-3),based on the function and performance test results from the FY-3 D satellite observation system in orbit.The FY-3 series of satellites have numerous remote sensing instruments and a wide range of imaging and sounding electromagnetic spectrometers onboard.These instruments can obtain reflectivity data for land surface,soil,vegetation,water body,snow cover,ocean color,and sea ice on earth’s surface over a wide spectral range,as well as information on the absorption and scattering radiative transfer of molecules and particles(clouds and aerosols)in earth’s atmosphere.All of these data can be used to retrieve physical and chemical information about the land,ocean,and atmosphere of the earth system.Comprehensive observation of the earth system by the FY-3 meteorological satellites is preliminarily realized.
基金supported by the Evaluation and Management Project of Wetlands Purification in Henan Province (No.52352019013)。
文摘Dissolved organic matter(DOM)is an important constituent of wastewater treatment plant(WWTP)effluent.A novel combined tidal and subsurface flow constructed wetland(TF-SSFCW)of 90 L was constructed for a ten-month trial of advanced treatment of the WWTP effluent.Excitation emission matrix(EEM)fluorescence spectroscopy,parallel factor(PARAFAC)analysis and a two end-member mixing model were employed to characterize the composition and removal process of the effluent DOM(EfOM)from the WWTP.The results showed that the TF-SSF-CW performed an efficient EfOM removal with dissolved organic carbon(DOC)removal rate of 88%and dissolved organic nitrogen(DON)removal rate of 91%.Further analysis demonstrated that the EfOM consisted mainly of two protein moieties and two humic-like groups;protein moieties(76%)constituted the main content of EfOM in raw water and humic-like groups(57%)became the dominating contributor after treatment.The EfOM from the WWTP was mainly of aquatic bacterial origin and evolved to a higher proportion of terrigenous origin with higher humification in the TF-SSF-CW effluent.A common controlling treatment-related factor for determining the concentrations of the same kind of substances(protein groups or humic-like groups)was revealed to exist,and the ratio of removal rates between the same substances in treatment was calculated.Our study demonstrates that the TF-SSF-CW can be a novel and effective treatment method for the EfOM from WWTPs,and is helpful for understanding of the character of EfOM in wetland treatment.
基金supported by the One Hundred Talent Program of CASNational Natural Science Foundation of China Petroleum & Chemical Corporation Joint Fund(U1662129)+2 种基金Key Program of National Natural Science Foundation of China(91434203)Key Research Program ofFrontier Sciences,CAS(QYZDY-SSW-JSCO11)State Key Laboratory of Multiphase Complex Systems,IPE,CAS(MPCS-2015-A-05)
文摘Ionic liquid coupled with strong acid systems presents considerable promise in some catalytic fields.In the present work,the multiple complex systems composed by 98 wt%concentrated sulfuric acid and[Bmim][SbF_6]were investigated in the terms of stability,acidity and interaction properties.It was found that acidolysis of[Bmim][SbF_6]occurred in the 98 wt%concentrated sulfuric acid accompanied by HF releasing and SbF_6~ degrading to[SbF_(6-y)XHSO_4]_y]^-.The species after acidolysis in the multiple complex systems were checked and confirmed by electrospray ionization mass spectrometry(ESI-MS),Fourier transform infrared spectroscopy(FT-IR),~1H NMR and ^(19)F NMR.Acidity increased slightly with less than 1 wt%[Bmim][SbF_6]addition,while decreased with more proportion,which was determined based on the Hammett acidity functions H_0,using ^(13)C NMR.The strong hydrogen bond S-O-H…F of interaction among the multiple complex systems was confirmed by molecular dynamic simulation.
基金supported by EPSRC TOUCAN Project (Grant No. EP/L020009/1)EU FP7 QUICK Project (Grant No. PIRSES-GA-2013-612652)+3 种基金EU H2020 ITN 5G Wireless Project (Grant No. 641985)National Natural Science Foundation of China (Grant Nos. 61210002, 61401256)MOST 863 Project in 5G (Grant No. 2014AA01A701)International S&T Cooperation Program of China (Grant No. 2014DFA11640)
文摘The coexistence of wireless body sensor networks(WBSNs) is a very challenging problem, due to strong interference, which seriously affects energy consumption and spectral reuse. The energy efficiency and spectral efficiency are two key performance evaluation metrics for wireless communication networks. In this paper, the fundamental tradeoff between energy efficiency and area spectral efficiency of WBSNs is first investigated under the Poisson point process(PPP) model and Matern hard-core point process(HCPP) model using stochastic geometry. The circuit power consumption is taken into consideration in energy efficiency calculation. The tradeoff judgement coefficient is developed and is shown to serve as a promising complementary measure. In addition, this paper proposes a new nearest neighbour distance power control strategy to improve energy efficiency. We show that there exists an optimal transmit power highly dependant on the density of WBSNs and the nearest neighbour distance. Some important properties are also addressed in the analysis of coexisting WBSNs based on the IEEE 802.15.4 standard, such as the impact of intensity nodes distribution,optimal guard zone, and outage probability. Simulation results show that the proposed power control design can reduce the outage probability and enhance energy efficiency. Energy efficiency and area spectral efficiency of the HCPP model are better than those of the PPP model. In addition, the optimal density of WBSNs coexistence is obtained.
基金supported by the National Natural Science Foundation of China(nos.22002168,21975259,and 21673241)the Innovation Academy for Green Manufacture of the Chinese Academy of Sciences(no.IAGM2020C17)the Strategic Priority Research Program of the Chinese Academy of Sciences(no.XDB20000000).
文摘Electroreduction of CO_(2) to target products with high activity and selectivity has techno-economic importance for renewable energy storage and CO_(2) utilization.Herein,we report a hierarchical CuS hollow polyhedron(CuS-HP)for electrocatalytic CO_(2) reduction(E-CO_(2)R)in neutral pH aqueous media.Under E-CO_(2)R conditions,CuS-HP undergoes structural reconstruction into sulfur-doped metallic Cu catalyst,which promotes formate production with Faradaic efficiency>90%in a wide potential range.