The effect of temperature on the properties of boron adsorption-desorption in brown-red soil, yellowbrown soil and calcareous alluvial soil of Hubei Province was investigated with the mobile displacement technique. Th...The effect of temperature on the properties of boron adsorption-desorption in brown-red soil, yellowbrown soil and calcareous alluvial soil of Hubei Province was investigated with the mobile displacement technique. The experimental data of B adsorption-desorption amounts and reaction t line at 25 and 40℃ were fitted by the zero-order, first-order and parabolic diffusion kinetic equations. The adsorption process was in conformity with the parabolic diffusion law at both the temperatures, and the values of rate constant of the parabolic diffusion equation in B adsorption were 0.138, 0.124 and 0.105 mg kg-1 min-1/2 at 25℃, and 0.147, 0.146 and 0.135 mg kg-1 min-1/2 at 40℃ for the brown-red soil, yellow-brown soil, and calcareous alluvial soil, respectively. The relationship between amount of B desorption and reaction time could be well described by the first-order kinetic equation, and the corresponding values of rate constant were 0.0422, 0.0563 and 0.0384 min-1 at 25℃, and 0.0408, 0.042 3 and 0.0401 min-1 at 40℃ for the brown-red soil, the yellow-brown soil and the calcareous alluvial soil, respectively. Therefore, the desorption process of B might be related to the amount of B adsorbed in soil. The higher the temperature, the lower the amount of B adsorption for the same soil in the same reaction time. The values of the apparent activation energy of B adsorption in the three soils calculated with the rate constants of parabolic diffusion equation were 3.27, 8.44 and 12.99 kJ mol-1, respectively, based on the experimental data of B adsorption amounts and reaction time at 25 and 40℃.展开更多
Adsorption capacity of activated carbon prepared from spent tea leaves (STL-AC) for the removal of aspirin from aqueous solution was investigated in this study. Preliminary studies have shown that treatment with pho...Adsorption capacity of activated carbon prepared from spent tea leaves (STL-AC) for the removal of aspirin from aqueous solution was investigated in this study. Preliminary studies have shown that treatment with phosphoric acid (H3PO4) increased removal efficiency of STL-AC. Characterizations on STL-AC revealed excellent textural properties (1200 m2.g-1, 51% mesoporosity), as well as distinctive surface chemistry (1.08 mmol.g-1 and 0.54 mmol.g-1 for acidic and basic oxygenated groups, pHpzc = 2.02). Maximum removal efficiency of aspirin observed was 94.28% after 60 rain when the initial concentration was 100 mg.L-1, 0.5 g of adsorbent used, pH 3 and at a temperature of 30 ℃. The adsorption data were well fitted to the Freundlich isotherm model and obeyed the pseudo-second order kinetics model. The adsorption of aspirin onto STL-AC was exothermic in nature (△H = - 13.808 kJ.mol-1) and had a negative entropy change, △S (-41.444 J.mol-1). A negative Gibbs free energy, △G was obtained indicating feasibility and spontaneity of the adsorption process. The adsorp- tion capacity of △C-STL (178.57 mg.g-1) is considerably high compared to most adsorbents synthesized from various sources, due to the well-defined textural properties coupled with surface chemistry of STL-AC which fa- vors aspirin adsorption. The results demonstrate the potential of STL-AC as aspirin adsorbent.展开更多
High entropy alloys(HEAs)have been the star materials in electrocatalysis research in recent years.One of their key features is the greatly increased multiplicity of active sites compared to conventional catalytic mat...High entropy alloys(HEAs)have been the star materials in electrocatalysis research in recent years.One of their key features is the greatly increased multiplicity of active sites compared to conventional catalytic materials.This increased multiplicity stimulates a cocktail effect and a scaling-relation breaking effect,and results in improved activity.However,the multiplicity of active sites in HEAs also poses new problems for mechanistic studies.One apparent problem is the inapplicability to HEA catalysts of the currently most popular mechanistic study method,which uses the electrocatalytic theoretical framework(ETF)based on the computational hydrogen electrode(CHE).The ETF uses a single adsorption energy to represent the catalyst,i.e.,a catalyst is represented by a'point'in the volcanic relationship.It naturally does not involve the multiplicity of active sites of a catalyst,and hence loses brevity in expressing the cocktail effect and scaling-relation breaking effect in HEA catalysis.This paper attempts to solve this inapplicability.Based on the fact that the adsorption energy distribution of HEAs is close to a normal distribution,the mean and variance of the adsorption energy distribution are introduced as descriptors of the ETF,replacing the original single adsorption energy.A quantitative relationship between the variance and the cocktail and scaling-relation braking effects is established.We believe the method described in this work will make the ETF more effective in mechanistic studies of HEA electrocatalysis.展开更多
Gibbs free binding energy and adsorption energy between cations and charged soil particles were used to evaluate the interactions between ions and soil particles. The distribution of Gibbs free adsorption energies cou...Gibbs free binding energy and adsorption energy between cations and charged soil particles were used to evaluate the interactions between ions and soil particles. The distribution of Gibbs free adsorption energies could not be determined experimentally before the development of Wien effect measurements in dilute soil suspensions. In the current study, energy relationships between heavy metal ions and particles of Hapli-Udic Argosol (Alfisol) and Ferri-Udic Argosol were inferred from Wien effect measurements in dilute suspensions of homoionic soil particles (〈 2 μm) of the two soils, which were saturated with ions of five heavy metals, in deionized water. The mean Gibbs free binding energies of the heavy metal ions with Hapli-Udic Argosol and Ferri-Udic Argosol particles diminished in the order of Pb^2+ 〉 Cd^2+ 〉 Cu^2+ 〉 Zn^2+ 〉 Cr^3+, where the range of binding energies for Hapli-Udic Argosol (7.25-9.32 kJ mol^-1) was similar to that for Ferri-Udic Argosol (7.43-9.35 kJ mol^-1). The electrical field-dependent mean Gibbs free adsorption energies of these heavy metal ions for Hapli-Udic Argosol and for Ferri-Udic Argosol descended in the order: Cu^2+ 〉 Cd2^+ 〉 Pb^2+ 〉 Zn^2+ 〉 Cr^3+, and Cd^2+ 〉 Cu^2+ 〉 Pb^2+ 〉 Zn^2+ 〉 Cr^3+, respectively. The mean Gibbs free adsorption energies of Cu^2+, Zn^2+, Cd^2+, Pb^2+, and Cr^3+ at a field strength of 200 kV cm^-1, for example, were in the range of 0.8-3.2 kJ mo1^-1 for the two soils.展开更多
The objective of this research was to enhance adsorption capacity of Acacia nilotica (keekar) sawdust for the abatement of chromium bearing wastewater and to investigate the effect of process parameters on adsorptio...The objective of this research was to enhance adsorption capacity of Acacia nilotica (keekar) sawdust for the abatement of chromium bearing wastewater and to investigate the effect of process parameters on adsorption capacity. The sawdust was activated by acid wash and functionalized subsequently with formaldehyde. Functionalization of activated sawdust raised its chromium removal efficiency of almost 10% as compared to its adsorption removal efficiency of HCl treated sawdust in a batch adsorption study. Adsorption kinetic data provided better fitting with pseudo second order model. Maximum adsorption capacity calculated through the best fitting Langmuir model was 6.34 mg·g^-1 and 8.2 mg·g^-1 for HCl treated and formaldehyde functionalized sawdust adsorbents, respectively. The adsorption of Cr(VI) was endothermic when studied by varying temperature from 20℃ to 50℃ for both activated and functionalized adsorbents.展开更多
Adsorbents are important components in adsorption refrigeration. The diameter of an adsorbent can affect the heat and mass transfer of an adsorber. The effect of particle diameter on effective thermal conductivity was...Adsorbents are important components in adsorption refrigeration. The diameter of an adsorbent can affect the heat and mass transfer of an adsorber. The effect of particle diameter on effective thermal conductivity was investigated. The heat transfer coefficient of the refrigerant and the void rate of the adsorbent layer can also affect the effective thermal conductivity of adsorbents. The performance of mass transfer in the adsorber is better when pressure drop decreases. Pressure drop decreases with increasing permeability. The permeability of the adsorbent layer can be improved with increasing adsorbent diameter. The effect of adsorbent diameter on refrigeration output power was experimentally studied. Output power initially increases and then decreases with increasing diameter under different cycle time conditions. Output power increases with decreasing cycle time under similar diameters.展开更多
The diversities of hydrogen sorption properties of Mg2FeH6-based complexes with and without TiO2 were investigated. Mg2FeH6-based complexes with and without TiO2 were synthesized respectively by reactive mechanical al...The diversities of hydrogen sorption properties of Mg2FeH6-based complexes with and without TiO2 were investigated. Mg2FeH6-based complexes with and without TiO2 were synthesized respectively by reactive mechanical alloying,and hydrogen sorption properties of the complexes were examined by Sieverts-type apparatus. The results show that the sample without TiO2 releases 4.43 % (mass fraction) hydrogen in 1.5 ks at 653 K under 0.1 MPa H2 pressure and absorbs 90% of the total 4.43 % (mass fraction) hydrogen absorbed in 85 s at 623 K under 4.0 MPa H2 pressure. But for the sample with TiO2 addition under the same condition,it only needs 400 s to release all of the stored hydrogen and 60 s to absorb 90% of the total hydrogen absorbed. The activation energies for desorption process of the samples with and without TiO2 are determined to be 71.2 and 80.3 kJ/(mol.K),respectively. The improvement in hydrogen sorption rate and and reduction in activation energy can be attributed to the addition of TiO2.展开更多
The influence of water vapor on silica membrane with pore size of ,-4A has been investigated in terms of adsorption properties and percolation effect at 50 and 90 ℃. Two methods are employed: spectroscopic ellipsome...The influence of water vapor on silica membrane with pore size of ,-4A has been investigated in terms of adsorption properties and percolation effect at 50 and 90 ℃. Two methods are employed: spectroscopic ellipsometry for water vapor adsorption and gas permeation of binary mixture of helium and H2O The adsorption behaviors on the silica membrane comply with the first-order Langmuir isotherm. The investigation demonstrates that helium flux through the silica membrane decreases dramatically in presence of H20 molecules. The transport of gas molecules through such small pores is believed not to be continuous any more, whereas it is reasonably assumed that the gas molecules hop from one occupied site to another unoccupied one under the potential gradient. When the coverage of H20 molecules on the silica surface increases, the dramatic decrease of helium flux could be related to percolation effect, where the adsorbed H20 molecules on the silica surface block the hopping of helium molecules.展开更多
Bromine-based flow batteries(Br-FBs)are well suitable for stationary energy storage owing to their high energy density and low cost.However,their power density and lifespan are limited by relatively low reaction kinet...Bromine-based flow batteries(Br-FBs)are well suitable for stationary energy storage owing to their high energy density and low cost.However,their power density and lifespan are limited by relatively low reaction kinetics of Br_(2)/Br-couple and serious self-discharge caused by bromine migration.Herein,lamella-like porous carbon nitride nanosheets(PCNS)with adsorption and spatial confinement effects are used to modify cathodes for Br-FBs.The large specific surface area and plentiful N-containing groups enable PCNS with excellent adsorption capacity,which captures bromine species into the pores on PCNS layers.The captured bromine species is subsequently confined in PCNS interlayers due to the strong interaction between bromine species and N-containing groups,thus effectively depressing bromine diffusion/migration.Moreover,the strong bromine adsorption capacity significantly improves the electrochemical activity of PCNS.Consequently,a zinc-bromine flow battery(ZBFB)employing PCNS-modified cathode achieves a high current density of 180 m A cm^(-2),with an ultra-high coulombic efficiency of 99.22%.It also exhibits better self-discharge performance and a long cycle life of 500 cycles.Furthermore,a complexing agent-free ZBFB is successfully realized based on the superior bromineentrapping/retaining capacity of the PCNS-modified cathode.Consequently,this work provides a promising strategy toward electrode modifications for high-performance and long-lifespan Br-FBs.展开更多
Due to the good controllability and high energy efficiency in adsorption processes,photoresponsive adsorbents are intriguing for CO2 capture.Nevertheless,most reported photoresponsive adsorbents are designed based on ...Due to the good controllability and high energy efficiency in adsorption processes,photoresponsive adsorbents are intriguing for CO2 capture.Nevertheless,most reported photoresponsive adsorbents are designed based on weak adsorption sites,regulating CO2 adsorption through structural change or steric hindrance.In addition,ultraviolet(UV)light is commonly involved in the regulation of adsorption capacity.Here we report for the first time the smart adsorbents for CO2 capture,which makes strong adsorption sites respond to visible(Vis)light.The adsorbents were fabricated by introducing primary amine and Dispersed Red 1(DR1,a kind of push-pull azobenzene that responds to Vis light rapidly)units to mesoporous silica,which act as strong adsorption sites and triggers,respectively.The primary amine sites make the adsorbents highly selective in the adsorption of CO2 over CH4.Without light irradiation,azobenzene is in the form of trans configuration,which leads to decreased electrostatic potential of primary amines and subsequently,exposure of active sites and liberal adsorption of CO2.Upon Vis-light irradiation,cis isomers are formed,which results in increased electrostatic potential of primary amines and subsequently shelter of active sites.Even on such strong adsorption sites,the alteration of CO2 adsorption capacity can reach 40%for the adsorbent with and without Vis-light irradiation.Moreover,the trans/cis isomerization of DR1 units can be triggered reversibly by Vis light.The present smart system endows adsorbents with selective adsorption capacity and avoids the employment of UV light,which is unlikely to be achieved by conventional photoresponsive adsorbents.展开更多
文摘The effect of temperature on the properties of boron adsorption-desorption in brown-red soil, yellowbrown soil and calcareous alluvial soil of Hubei Province was investigated with the mobile displacement technique. The experimental data of B adsorption-desorption amounts and reaction t line at 25 and 40℃ were fitted by the zero-order, first-order and parabolic diffusion kinetic equations. The adsorption process was in conformity with the parabolic diffusion law at both the temperatures, and the values of rate constant of the parabolic diffusion equation in B adsorption were 0.138, 0.124 and 0.105 mg kg-1 min-1/2 at 25℃, and 0.147, 0.146 and 0.135 mg kg-1 min-1/2 at 40℃ for the brown-red soil, yellow-brown soil, and calcareous alluvial soil, respectively. The relationship between amount of B desorption and reaction time could be well described by the first-order kinetic equation, and the corresponding values of rate constant were 0.0422, 0.0563 and 0.0384 min-1 at 25℃, and 0.0408, 0.042 3 and 0.0401 min-1 at 40℃ for the brown-red soil, the yellow-brown soil and the calcareous alluvial soil, respectively. Therefore, the desorption process of B might be related to the amount of B adsorbed in soil. The higher the temperature, the lower the amount of B adsorption for the same soil in the same reaction time. The values of the apparent activation energy of B adsorption in the three soils calculated with the rate constants of parabolic diffusion equation were 3.27, 8.44 and 12.99 kJ mol-1, respectively, based on the experimental data of B adsorption amounts and reaction time at 25 and 40℃.
基金supported by Malaysia's Ministry of Higher Education's Fundamental Research Grant Scheme(FRGS,grant number4F872)Research University grant(GUP,grant number17H65)support from Universiti Teknologi Malaysia in the form of Post-Doctoral Fellowship Scheme for the Project:“Catalytic Cracking of Low Density Polyethylene Waste to Liquid Fuels in Fixed Bed Reactor”
文摘Adsorption capacity of activated carbon prepared from spent tea leaves (STL-AC) for the removal of aspirin from aqueous solution was investigated in this study. Preliminary studies have shown that treatment with phosphoric acid (H3PO4) increased removal efficiency of STL-AC. Characterizations on STL-AC revealed excellent textural properties (1200 m2.g-1, 51% mesoporosity), as well as distinctive surface chemistry (1.08 mmol.g-1 and 0.54 mmol.g-1 for acidic and basic oxygenated groups, pHpzc = 2.02). Maximum removal efficiency of aspirin observed was 94.28% after 60 rain when the initial concentration was 100 mg.L-1, 0.5 g of adsorbent used, pH 3 and at a temperature of 30 ℃. The adsorption data were well fitted to the Freundlich isotherm model and obeyed the pseudo-second order kinetics model. The adsorption of aspirin onto STL-AC was exothermic in nature (△H = - 13.808 kJ.mol-1) and had a negative entropy change, △S (-41.444 J.mol-1). A negative Gibbs free energy, △G was obtained indicating feasibility and spontaneity of the adsorption process. The adsorp- tion capacity of △C-STL (178.57 mg.g-1) is considerably high compared to most adsorbents synthesized from various sources, due to the well-defined textural properties coupled with surface chemistry of STL-AC which fa- vors aspirin adsorption. The results demonstrate the potential of STL-AC as aspirin adsorbent.
文摘High entropy alloys(HEAs)have been the star materials in electrocatalysis research in recent years.One of their key features is the greatly increased multiplicity of active sites compared to conventional catalytic materials.This increased multiplicity stimulates a cocktail effect and a scaling-relation breaking effect,and results in improved activity.However,the multiplicity of active sites in HEAs also poses new problems for mechanistic studies.One apparent problem is the inapplicability to HEA catalysts of the currently most popular mechanistic study method,which uses the electrocatalytic theoretical framework(ETF)based on the computational hydrogen electrode(CHE).The ETF uses a single adsorption energy to represent the catalyst,i.e.,a catalyst is represented by a'point'in the volcanic relationship.It naturally does not involve the multiplicity of active sites of a catalyst,and hence loses brevity in expressing the cocktail effect and scaling-relation breaking effect in HEA catalysis.This paper attempts to solve this inapplicability.Based on the fact that the adsorption energy distribution of HEAs is close to a normal distribution,the mean and variance of the adsorption energy distribution are introduced as descriptors of the ETF,replacing the original single adsorption energy.A quantitative relationship between the variance and the cocktail and scaling-relation braking effects is established.We believe the method described in this work will make the ETF more effective in mechanistic studies of HEA electrocatalysis.
基金Project supported by the National Natural Science Foundation of China(Nos.40401030 and 20577054).
文摘Gibbs free binding energy and adsorption energy between cations and charged soil particles were used to evaluate the interactions between ions and soil particles. The distribution of Gibbs free adsorption energies could not be determined experimentally before the development of Wien effect measurements in dilute soil suspensions. In the current study, energy relationships between heavy metal ions and particles of Hapli-Udic Argosol (Alfisol) and Ferri-Udic Argosol were inferred from Wien effect measurements in dilute suspensions of homoionic soil particles (〈 2 μm) of the two soils, which were saturated with ions of five heavy metals, in deionized water. The mean Gibbs free binding energies of the heavy metal ions with Hapli-Udic Argosol and Ferri-Udic Argosol particles diminished in the order of Pb^2+ 〉 Cd^2+ 〉 Cu^2+ 〉 Zn^2+ 〉 Cr^3+, where the range of binding energies for Hapli-Udic Argosol (7.25-9.32 kJ mol^-1) was similar to that for Ferri-Udic Argosol (7.43-9.35 kJ mol^-1). The electrical field-dependent mean Gibbs free adsorption energies of these heavy metal ions for Hapli-Udic Argosol and for Ferri-Udic Argosol descended in the order: Cu^2+ 〉 Cd2^+ 〉 Pb^2+ 〉 Zn^2+ 〉 Cr^3+, and Cd^2+ 〉 Cu^2+ 〉 Pb^2+ 〉 Zn^2+ 〉 Cr^3+, respectively. The mean Gibbs free adsorption energies of Cu^2+, Zn^2+, Cd^2+, Pb^2+, and Cr^3+ at a field strength of 200 kV cm^-1, for example, were in the range of 0.8-3.2 kJ mo1^-1 for the two soils.
文摘The objective of this research was to enhance adsorption capacity of Acacia nilotica (keekar) sawdust for the abatement of chromium bearing wastewater and to investigate the effect of process parameters on adsorption capacity. The sawdust was activated by acid wash and functionalized subsequently with formaldehyde. Functionalization of activated sawdust raised its chromium removal efficiency of almost 10% as compared to its adsorption removal efficiency of HCl treated sawdust in a batch adsorption study. Adsorption kinetic data provided better fitting with pseudo second order model. Maximum adsorption capacity calculated through the best fitting Langmuir model was 6.34 mg·g^-1 and 8.2 mg·g^-1 for HCl treated and formaldehyde functionalized sawdust adsorbents, respectively. The adsorption of Cr(VI) was endothermic when studied by varying temperature from 20℃ to 50℃ for both activated and functionalized adsorbents.
基金Supported by the Chinese Academy of Science Visiting Professorship for Senior International Scientists project(2009Z2-1973)
文摘Adsorbents are important components in adsorption refrigeration. The diameter of an adsorbent can affect the heat and mass transfer of an adsorber. The effect of particle diameter on effective thermal conductivity was investigated. The heat transfer coefficient of the refrigerant and the void rate of the adsorbent layer can also affect the effective thermal conductivity of adsorbents. The performance of mass transfer in the adsorber is better when pressure drop decreases. Pressure drop decreases with increasing permeability. The permeability of the adsorbent layer can be improved with increasing adsorbent diameter. The effect of adsorbent diameter on refrigeration output power was experimentally studied. Output power initially increases and then decreases with increasing diameter under different cycle time conditions. Output power increases with decreasing cycle time under similar diameters.
基金Project (50574105) supported by the National Natural Science Foundation of ChinaProject (NCET-06-0683) supported by the Program for the New Century Excellent Talents in University+1 种基金Project (08-030239) supported by the Program for 121 Excellent Talents in Hunan ProvinceProject (07MX21) supported by Mittal Student Innovation Foundation of Central South University
文摘The diversities of hydrogen sorption properties of Mg2FeH6-based complexes with and without TiO2 were investigated. Mg2FeH6-based complexes with and without TiO2 were synthesized respectively by reactive mechanical alloying,and hydrogen sorption properties of the complexes were examined by Sieverts-type apparatus. The results show that the sample without TiO2 releases 4.43 % (mass fraction) hydrogen in 1.5 ks at 653 K under 0.1 MPa H2 pressure and absorbs 90% of the total 4.43 % (mass fraction) hydrogen absorbed in 85 s at 623 K under 4.0 MPa H2 pressure. But for the sample with TiO2 addition under the same condition,it only needs 400 s to release all of the stored hydrogen and 60 s to absorb 90% of the total hydrogen absorbed. The activation energies for desorption process of the samples with and without TiO2 are determined to be 71.2 and 80.3 kJ/(mol.K),respectively. The improvement in hydrogen sorption rate and and reduction in activation energy can be attributed to the addition of TiO2.
基金This work was supported by the Fhndamental Research Funds for the Central Universities (No.XDJK2015C002) and the National Natural Science Foundation of China (No.51402243). Special thanks are given to Prof. H. J. M Bouwmeester and Dr. N.E. Benes from University of Twente for fruitful discussion.
文摘The influence of water vapor on silica membrane with pore size of ,-4A has been investigated in terms of adsorption properties and percolation effect at 50 and 90 ℃. Two methods are employed: spectroscopic ellipsometry for water vapor adsorption and gas permeation of binary mixture of helium and H2O The adsorption behaviors on the silica membrane comply with the first-order Langmuir isotherm. The investigation demonstrates that helium flux through the silica membrane decreases dramatically in presence of H20 molecules. The transport of gas molecules through such small pores is believed not to be continuous any more, whereas it is reasonably assumed that the gas molecules hop from one occupied site to another unoccupied one under the potential gradient. When the coverage of H20 molecules on the silica surface increases, the dramatic decrease of helium flux could be related to percolation effect, where the adsorbed H20 molecules on the silica surface block the hopping of helium molecules.
基金supported by CAS Strategic Leading Science&Technology Program(A)(XDA21070100)CAS Engineering Laboratory for Electrochemical Energy Storage(KFJ-PTXM-027)+1 种基金DICP funding(DICP I202026 DICP I201928)Liaoning Natural Science Foundation(2021-MS-024)。
文摘Bromine-based flow batteries(Br-FBs)are well suitable for stationary energy storage owing to their high energy density and low cost.However,their power density and lifespan are limited by relatively low reaction kinetics of Br_(2)/Br-couple and serious self-discharge caused by bromine migration.Herein,lamella-like porous carbon nitride nanosheets(PCNS)with adsorption and spatial confinement effects are used to modify cathodes for Br-FBs.The large specific surface area and plentiful N-containing groups enable PCNS with excellent adsorption capacity,which captures bromine species into the pores on PCNS layers.The captured bromine species is subsequently confined in PCNS interlayers due to the strong interaction between bromine species and N-containing groups,thus effectively depressing bromine diffusion/migration.Moreover,the strong bromine adsorption capacity significantly improves the electrochemical activity of PCNS.Consequently,a zinc-bromine flow battery(ZBFB)employing PCNS-modified cathode achieves a high current density of 180 m A cm^(-2),with an ultra-high coulombic efficiency of 99.22%.It also exhibits better self-discharge performance and a long cycle life of 500 cycles.Furthermore,a complexing agent-free ZBFB is successfully realized based on the superior bromineentrapping/retaining capacity of the PCNS-modified cathode.Consequently,this work provides a promising strategy toward electrode modifications for high-performance and long-lifespan Br-FBs.
基金the Excellent Young Scientists Fund from the National Natural Science Foundation of China(21722606)the National Natural Science Foundation of China(21676138,21878149 and 21808110)China Postdoctoral Science Foundation(2018M632295 and 2019T120419)。
文摘Due to the good controllability and high energy efficiency in adsorption processes,photoresponsive adsorbents are intriguing for CO2 capture.Nevertheless,most reported photoresponsive adsorbents are designed based on weak adsorption sites,regulating CO2 adsorption through structural change or steric hindrance.In addition,ultraviolet(UV)light is commonly involved in the regulation of adsorption capacity.Here we report for the first time the smart adsorbents for CO2 capture,which makes strong adsorption sites respond to visible(Vis)light.The adsorbents were fabricated by introducing primary amine and Dispersed Red 1(DR1,a kind of push-pull azobenzene that responds to Vis light rapidly)units to mesoporous silica,which act as strong adsorption sites and triggers,respectively.The primary amine sites make the adsorbents highly selective in the adsorption of CO2 over CH4.Without light irradiation,azobenzene is in the form of trans configuration,which leads to decreased electrostatic potential of primary amines and subsequently,exposure of active sites and liberal adsorption of CO2.Upon Vis-light irradiation,cis isomers are formed,which results in increased electrostatic potential of primary amines and subsequently shelter of active sites.Even on such strong adsorption sites,the alteration of CO2 adsorption capacity can reach 40%for the adsorbent with and without Vis-light irradiation.Moreover,the trans/cis isomerization of DR1 units can be triggered reversibly by Vis light.The present smart system endows adsorbents with selective adsorption capacity and avoids the employment of UV light,which is unlikely to be achieved by conventional photoresponsive adsorbents.