Intraparticle charge delocalization occurs when metal nanoparticles are functionalized with organic capping ligands through conjugated rnetal-ligand interfacial bonds. In this study, metal nanoparticles of 5d metals ...Intraparticle charge delocalization occurs when metal nanoparticles are functionalized with organic capping ligands through conjugated rnetal-ligand interfacial bonds. In this study, metal nanoparticles of 5d metals （Ir, Pt, and Au） and 4d metals （Ru, Rh, and Pd） were prepared and capped with ethynylphenylacetylene and the impacts of the number of metal d electrons on the nanoparticle optoelectronic properties were examined. Both FTIR and photoluminescence measurements indicate that intraparticle charge delocalization was en- hanced with the increase of the number of d electrons in the same period with palladium being an exception.展开更多
A laser trapping-microspectroscopy technique combined with excitation energy transfer from a fluorescent cationic dye (Rhodamine B, RB+) to a non-fluorescent cationic dye (Malachite Green, MG+) was employed to study p...A laser trapping-microspectroscopy technique combined with excitation energy transfer from a fluorescent cationic dye (Rhodamine B, RB+) to a non-fluorescent cationic dye (Malachite Green, MG+) was employed to study pH effects on the diffusion coefficients of MG+ (D(MG+)) in single cation-exchange resin microparticles with the diameters of 16 μm. When RB+-pre-adsorbed resin particles were soaked in an aqueous MG+ solution, the RB+ fluorescence was quenched gradually with the soaking time. The time course of the quenching efficiency of RB+ by MG+ was then used to evaluate the D(MG+) value in the particle. The D(MG+) value increased from 1.1 × 10-11 to 4.3 × 10-11 cm2.s–1 on going the solu- tion pH value from 9 to 4. The results were explained reasonably by a Donnan electric potential model.展开更多
Intraparticle models of thermal processes are essential in the Discrete Element Method (DEM) when particles are thermally thick. Accurately solving the intraparticle conservation equations using the finite volume meth...Intraparticle models of thermal processes are essential in the Discrete Element Method (DEM) when particles are thermally thick. Accurately solving the intraparticle conservation equations using the finite volume method requires sufficient spatial and temporal resolution, increasing simulation cost. This short communication proposes to replace the finite volume method (FVM) by a novel tabulated model that reduces the computational effort without compromising accuracy. The look-up database is generated from a set of single-particle simulations under different boundary conditions using the FVM. To assess the capability of the tabulated model to reproduce the results of the finite volume method, another single particle case with periodic functions for the fluid temperature is simulated. Results showed that tabulation provides accurate predictions while reducing computational cost by a factor of 3–10.展开更多
Control of N-nitrosodimethylamine(NDMA)in drinking water could be achieved by removing its precursors as one practical way.Herein,superfine powdered activated carbons with a diameter of about 1μm(SPACs)were successfu...Control of N-nitrosodimethylamine(NDMA)in drinking water could be achieved by removing its precursors as one practical way.Herein,superfine powdered activated carbons with a diameter of about 1μm(SPACs)were successfully prepared by grinding powdered activated carbon(PAC,D50=24.3μm)and applied to remove model NDMA precursors,i.e.ranitidine(RAN)and nizatidine(NIZ).Results fromgrain diameter experiments demonstrated that the absorption velocity increased dramatically with decreasing particle size,and the maximum increase in k2 was 26.8-folds for RAN and 33.4-folds for NIZ.Moreover,kinetic experiments explained that rapid absorption could be attributed to the acceleration of intraparticle diffusion due to the shortening of the diffusion path.Furthermore,performance comparison experiments suggested that the removal of RAN and NIZ(C_(0)=0.5 mg/L)could reach 61.3%and 60%,respectively,within 5 min,when the dosage of SAPC-1.1(D_(50)=1.1μm)was merely 5 mg/L,while PAC-24.3 could only eliminate 17.5%and 18.6%.The adsorption isotherm was well defined by Langmuir isotherm model,indicating that the adsorption of RAN/NIZ was a monolayer coverage process.The adsorption of RAN or NIZ by SAPC-1.1 and PAC-24.3 was strongly pH dependent,and high adsorption capacity could be observed under the condition of pH>pk_(a)+1.The coexistence of humic acid(HA)had no significant effect on the adsorption performance because RAN/NIZ may be coupled with HA and removed simultaneously.The coexistence of anions had little effect on the adsorption also.This study is expected to provide an alternative strategy for drinking water safety triggered by NDMA.展开更多
Adsorption is one of the most widely applied techniques for environmental remediation. Its kinetics are of great significance to evaluate the performance of a given adsorbent and gain insight into the underlying mecha...Adsorption is one of the most widely applied techniques for environmental remediation. Its kinetics are of great significance to evaluate the performance of a given adsorbent and gain insight into the underlying mechanisms. There are lots of references available concerning adsorption kinetics, and several mathematic models have been developed to describe adsorption reaction and diffusion processes. However, these models were frequently employed to fit the kinetic data in an unsuitable or improper manner. This is mainly because the boundary conditions of the associated models were, to a considerable extent, ignored for data modeling. Here we reviewed several widely-used adsorption kinetic models and paid more attention to their boundary conditions. We believe that the review is of certain significance and improvement for adsorption kinetic modeling.展开更多
Over 70%of the treated contaminated water at the Fukushima Daiichi Nuclear Power Station contains radionuclides beyond the regulatory standard for discharge that need to be re-purified.Technetium-99(^(99)Tc),mainly in...Over 70%of the treated contaminated water at the Fukushima Daiichi Nuclear Power Station contains radionuclides beyond the regulatory standard for discharge that need to be re-purified.Technetium-99(^(99)Tc),mainly in the form of pertechnetate Tc(VII)O_(4)^(-),is one of the main sources of long-term radiotoxicity that jeopardizes the environment and human health.Herein,we used a series of dicationic pyridinium(DCP)derivative groups(–Py^(+)C_(n)H_(2n)N^(+)Me_(3),n=2,3,and 5)to modify commercial Reillex 425 resins containing tertiary pyridyl groups to improve the adsorption performance of rhenium(Re,an analog of radioactive Tc)and Tc.As the quaternary pyridinium and ammonium sites in one DCP group can adsorb ReO_(4)^(-) simultaneously,DCP-modified Reillex 425(Reillex-Cn)exhibited high maximum adsorption capacities for Re under neutral conditions.Adsorption capacities reached 344.8,416.7,and 588.2 mg g^(-)1 for Reillex 425-C2,Reillex 425-C3,and Reillex 425-C5,respectively.Intraparticle diffusion of ReO_(4)^(-)/TcO_(4)^(-) in Reillex 425-Cn was verified to be the rate-limiting step of adsorption.However,adsorption can be adjusted by the length of the alkyl spacers between the two positively charged N sites in DCP.–Py^(+)C_(2)H_(4)N^(+)Me_(3) significantly enhanced intraparticle diffusion compared to–Py^(+)C_(5)H_(10)N^(+)Me_(3).The two positive sites in–Py^(+)C_(2)H_(4)N^(+)Me_(3) would be laterally distributed,leading to a smaller steric hindrance for ReO_(4)–/TcO_(4)^(-) transport inside the microporous channels.Meanwhile,the longer alkyl spacers in–Py^(+)C_(5)H_(10)N^(+)Me_(3) formed hydrophobic microphases,repulsing the hydrated ReO_(4)–/TcO_(4)^(-) anions.Thus,the adsorptions of both ReO_(4)^(-) and TcO_(4)^(-) on Reillex 425-C2 were faster than those on Reillex 425-C5.Moreover,Reillex 425-Cn exhibited an exothermic nature,good selectivity,excellent reusability,and strong salinity tolerance.This study provides a simple strategy to enhance the Tc removal performance of adsorbents containing abundant micropores,which implies enormous environmental and economic benefits.展开更多
The influences of particle size,shape,and catalyst distribution on the reactivity and hydrocarbon product selectivity of a cobalt-based catalyst for Fischer-Tropsch synthesis were investigated in the present work.A se...The influences of particle size,shape,and catalyst distribution on the reactivity and hydrocarbon product selectivity of a cobalt-based catalyst for Fischer-Tropsch synthesis were investigated in the present work.A self-consistent kinetic model for Fischer-Tropsch reaction proposed here was found to correlate experimental data well and hence was used to describe the consumption rates of reactants and formation rates of hydrocarbon products.The perturbed-chain statistical associating fluid theory equation of state was used to describe vapor-liquid equilibrium behavior associated with Fischer-Tropsch reaction.Local interaction between intraparticle diffusion and Fischer-Tropsch reaction was investigated in detail.Results showed that in order to avoid the adverse influence of intraparticle diffusional limitations on catalyst reactivity and product selectivity,the use of small particles is necessary.Large eggshell spherical particles are shown to keep the original catalyst reactivity and enhance the selectivity of heavy hydrocarbon products.The suitable layer thickness for a spherical particle with a diameter of 2 mm is nearly 0.15 mm.With the same outer diameter of 2 mm,the catalyst reactivity and heavy product selectivity of hollow cylindrical particles with a layer thickness of 0.25 mm are found to be larger than eggshell spherical particles.From the viewpoint of catalytic performance,hollow cylindrical particles are a better choice for industrial applications.展开更多
In this study,the removal of monovalent and divalent cations,Nat,Kt,Mg2t,and Ca2t,in a diluted solution from Chott-El Jerid Lake,Tunisia,was investigated with the electrodialysis technique.The process was tested using...In this study,the removal of monovalent and divalent cations,Nat,Kt,Mg2t,and Ca2t,in a diluted solution from Chott-El Jerid Lake,Tunisia,was investigated with the electrodialysis technique.The process was tested using two cation-exchange membranes:sulfonated polyether sulfone cross-linked with 10%hexamethylenediamine(HEXCl)and sulfonated polyether sulfone grafted with octylamine(S-PESOS).The commercially available membrane Nafion®was used for comparison.The results showed that Nafion®and S-PESOS membranes had similar removal behaviors,and the investigated cations were ranked in the following descending order in terms of their demineralization rates:Nat>Ca2t>Mg2t>Kt.Divalent cations were more effectively removed by HEXCl than by monovalent cations.The plots based on the WebereMorris model showed a strong linearity.This reveals that intra-particle diffusion was not the removal rate-determining step,and the removal process was controlled by two or more concurrent mechanisms.The Boyd plots did not pass through their origin,and the sole controlling step was determined by film-diffusion resistance,especially after a long period of electrodialysis.Additionally,a semi-empirical model was established to simulate the temporal variation of the treatment process,and the physical significance and values of model parameters were compared for the three membranes.The findings of this study indicate that HEXCl and S-PESOS membranes can be efficiently utilized for water softening,especially when effluents are highly loaded with calcium and magnesium ions.展开更多
Continuous adsorption experiments are conducted using fixed-bed adsorption column to evaluate the performance of the adsorbent developed (from activated tamarind seeds) for the removal of Cr(VI) from aqueous solutions...Continuous adsorption experiments are conducted using fixed-bed adsorption column to evaluate the performance of the adsorbent developed (from activated tamarind seeds) for the removal of Cr(VI) from aqueous solutions and the results obtained are validated with a model developed in this study. The effects of significant parameters such as flow rate, mass of adsorbent, and initial Cr(VI) concentration are studied and breakthrough curves are obtained. As the flow rate increases from 10 to 20 mL min-1, the breakthrough time decreases from 210 to 80 min. As the mass of adsorbent increases, breakthrough time gets delayed. The breakthrough times are obtained as 110, 115 and 210 min for 15, 20 and 25 g of activated tamarind seeds. As the initial Cr(VI) concentration increases from 100 to 200 mgL-1, the break point time decreases from 210 to 45 min. The process parameters for fixed-bed adsorption such as breakthrough time, total percentage removal of Cr(VI), adsorption exhaustion rate and fraction of unused bed length are calculated and the performance of fixed-bed adsorption column is analyzed. The mechanism for Cr(VI) adsorption on activated tamarind seeds is proposed. At low value of solution pH (= 1), the increase in Cr(VI) adsorption is due to the electrostatic attraction between positively charged groups of activated tamarind seeds and the HCrO4-. A mathematical model for fixed-bed adsorption column is proposed by incorporating the effect of velocity variation along the bed length in the existing model. Pore and surface diffusion models are used to describe the intra-particle mechanism for Cr(VI) adsorption. The breakthrough curve obtained theoretically from pore diffusion model and surface diffusion model are compared with experimental results for different operating conditions. The standard deviation values obtained for pore diffusion model and solid diffusion model are 0.111 and 0.214 respectively.展开更多
Engineering single-photon states endowed with orbital angular momentum (OAM) is a powerful toolfor quantum information photonic implementations. Indeed, due to its unbounded nature, OAM is suitable forencoding qudits,...Engineering single-photon states endowed with orbital angular momentum (OAM) is a powerful toolfor quantum information photonic implementations. Indeed, due to its unbounded nature, OAM is suitable forencoding qudits, allowing a single carrier to transport a large amount of information. Most of the experimentalplatforms employ spontaneous parametric down-conversion processes to generate single photons, evenif this approach is intrinsically probabilistic, leading to scalability issues for an increasing number of qudits.Semiconductor quantum dots (QDs) have been used to get over these limitations by producing on-demand pure and indistinguishable single-photon states, although only recently they have been exploitedto create OAM modes. Our work employs a bright QD single-photon source to generate a complete set ofquantum states for information processing with OAM-endowed photons. We first study hybrid intraparticleentanglement between OAM and polarization degrees of freedom of a single photon whose preparationwas certified by means of Hong–Ou–Mandel visibility. Then, we investigate hybrid interparticle OAM-based entanglement by exploiting a probabilistic entangling gate. The performance of our approach isassessed by performing quantum state tomography and violating Bell inequalities. Our results pave theway for the use of deterministic sources for the on-demand generation of photonic high-dimensionalquantum states.展开更多
We show that through strong ligand mediated interfacial energy control between Au seeds and the deposited Au,the non-wetting growth of Au on Au seeds led to the formation homometallic core-satellite nanostructures.To ...We show that through strong ligand mediated interfacial energy control between Au seeds and the deposited Au,the non-wetting growth of Au on Au seeds led to the formation homometallic core-satellite nanostructures.To modulate the intraparticle plasmonic coupling between the core and the satellites,the number and size of the Au satellites,and their inter-island distances were continuously tuned by varying the growth kinetics.As a result of the precise structural control,the plasmonic absorptions of the core-satellite nanostructures were tuned from visible to near-infrared(NIR)spectral range,and the extent of spectral modulation(500-1300 nm)is among the best of the literature methods.This synthetic advance enriches the toolbox for nanosynthesis and points to a new direction in the exploration of sophisticated functional designs.展开更多
基金supported,in part,by the National Science Foundation(DMR-1409396 and CHE-1710408)carried out at the National Center for Electron Microscopy and Molecular Foundry of Lawrence Berkeley National Laboratory,which is supported by the US Department of Energy
文摘Intraparticle charge delocalization occurs when metal nanoparticles are functionalized with organic capping ligands through conjugated rnetal-ligand interfacial bonds. In this study, metal nanoparticles of 5d metals （Ir, Pt, and Au） and 4d metals （Ru, Rh, and Pd） were prepared and capped with ethynylphenylacetylene and the impacts of the number of metal d electrons on the nanoparticle optoelectronic properties were examined. Both FTIR and photoluminescence measurements indicate that intraparticle charge delocalization was en- hanced with the increase of the number of d electrons in the same period with palladium being an exception.
文摘A laser trapping-microspectroscopy technique combined with excitation energy transfer from a fluorescent cationic dye (Rhodamine B, RB+) to a non-fluorescent cationic dye (Malachite Green, MG+) was employed to study pH effects on the diffusion coefficients of MG+ (D(MG+)) in single cation-exchange resin microparticles with the diameters of 16 μm. When RB+-pre-adsorbed resin particles were soaked in an aqueous MG+ solution, the RB+ fluorescence was quenched gradually with the soaking time. The time course of the quenching efficiency of RB+ by MG+ was then used to evaluate the D(MG+) value in the particle. The D(MG+) value increased from 1.1 × 10-11 to 4.3 × 10-11 cm2.s–1 on going the solu- tion pH value from 9 to 4. The results were explained reasonably by a Donnan electric potential model.
基金funded by the Deutsche Forschungsgemeinschaft(DFG,German Research Foundation)–Project-ID 422037413–TRR 287.(Gefördert durch die Deutsche Forschungsgemeinschaft(DFG)–Projektnummer 422037413–TRR 287).
文摘Intraparticle models of thermal processes are essential in the Discrete Element Method (DEM) when particles are thermally thick. Accurately solving the intraparticle conservation equations using the finite volume method requires sufficient spatial and temporal resolution, increasing simulation cost. This short communication proposes to replace the finite volume method (FVM) by a novel tabulated model that reduces the computational effort without compromising accuracy. The look-up database is generated from a set of single-particle simulations under different boundary conditions using the FVM. To assess the capability of the tabulated model to reproduce the results of the finite volume method, another single particle case with periodic functions for the fluid temperature is simulated. Results showed that tabulation provides accurate predictions while reducing computational cost by a factor of 3–10.
基金supported by the Key Technology Research and Development Program of Shandong(No.2020CXGC011406)the National Natural Science Foundation of China(No.22076091)the State Key Joint Laboratory of Environment Simulation and Pollution Control,China(No.21L01ESPC).
文摘Control of N-nitrosodimethylamine(NDMA)in drinking water could be achieved by removing its precursors as one practical way.Herein,superfine powdered activated carbons with a diameter of about 1μm(SPACs)were successfully prepared by grinding powdered activated carbon(PAC,D50=24.3μm)and applied to remove model NDMA precursors,i.e.ranitidine(RAN)and nizatidine(NIZ).Results fromgrain diameter experiments demonstrated that the absorption velocity increased dramatically with decreasing particle size,and the maximum increase in k2 was 26.8-folds for RAN and 33.4-folds for NIZ.Moreover,kinetic experiments explained that rapid absorption could be attributed to the acceleration of intraparticle diffusion due to the shortening of the diffusion path.Furthermore,performance comparison experiments suggested that the removal of RAN and NIZ(C_(0)=0.5 mg/L)could reach 61.3%and 60%,respectively,within 5 min,when the dosage of SAPC-1.1(D_(50)=1.1μm)was merely 5 mg/L,while PAC-24.3 could only eliminate 17.5%and 18.6%.The adsorption isotherm was well defined by Langmuir isotherm model,indicating that the adsorption of RAN/NIZ was a monolayer coverage process.The adsorption of RAN or NIZ by SAPC-1.1 and PAC-24.3 was strongly pH dependent,and high adsorption capacity could be observed under the condition of pH>pk_(a)+1.The coexistence of humic acid(HA)had no significant effect on the adsorption performance because RAN/NIZ may be coupled with HA and removed simultaneously.The coexistence of anions had little effect on the adsorption also.This study is expected to provide an alternative strategy for drinking water safety triggered by NDMA.
基金supported by the National Natural Science Foundation of China (No. 20504012)the New Century Excellent Talents in University of China (No. NCET-07-0421)
文摘Adsorption is one of the most widely applied techniques for environmental remediation. Its kinetics are of great significance to evaluate the performance of a given adsorbent and gain insight into the underlying mechanisms. There are lots of references available concerning adsorption kinetics, and several mathematic models have been developed to describe adsorption reaction and diffusion processes. However, these models were frequently employed to fit the kinetic data in an unsuitable or improper manner. This is mainly because the boundary conditions of the associated models were, to a considerable extent, ignored for data modeling. Here we reviewed several widely-used adsorption kinetic models and paid more attention to their boundary conditions. We believe that the review is of certain significance and improvement for adsorption kinetic modeling.
基金supported by the National Natural Science Foundation of China(Nos.51803205,11775214,and 21790371)China Scholarship Council(No.201906345006).
文摘Over 70%of the treated contaminated water at the Fukushima Daiichi Nuclear Power Station contains radionuclides beyond the regulatory standard for discharge that need to be re-purified.Technetium-99(^(99)Tc),mainly in the form of pertechnetate Tc(VII)O_(4)^(-),is one of the main sources of long-term radiotoxicity that jeopardizes the environment and human health.Herein,we used a series of dicationic pyridinium(DCP)derivative groups(–Py^(+)C_(n)H_(2n)N^(+)Me_(3),n=2,3,and 5)to modify commercial Reillex 425 resins containing tertiary pyridyl groups to improve the adsorption performance of rhenium(Re,an analog of radioactive Tc)and Tc.As the quaternary pyridinium and ammonium sites in one DCP group can adsorb ReO_(4)^(-) simultaneously,DCP-modified Reillex 425(Reillex-Cn)exhibited high maximum adsorption capacities for Re under neutral conditions.Adsorption capacities reached 344.8,416.7,and 588.2 mg g^(-)1 for Reillex 425-C2,Reillex 425-C3,and Reillex 425-C5,respectively.Intraparticle diffusion of ReO_(4)^(-)/TcO_(4)^(-) in Reillex 425-Cn was verified to be the rate-limiting step of adsorption.However,adsorption can be adjusted by the length of the alkyl spacers between the two positively charged N sites in DCP.–Py^(+)C_(2)H_(4)N^(+)Me_(3) significantly enhanced intraparticle diffusion compared to–Py^(+)C_(5)H_(10)N^(+)Me_(3).The two positive sites in–Py^(+)C_(2)H_(4)N^(+)Me_(3) would be laterally distributed,leading to a smaller steric hindrance for ReO_(4)–/TcO_(4)^(-) transport inside the microporous channels.Meanwhile,the longer alkyl spacers in–Py^(+)C_(5)H_(10)N^(+)Me_(3) formed hydrophobic microphases,repulsing the hydrated ReO_(4)–/TcO_(4)^(-) anions.Thus,the adsorptions of both ReO_(4)^(-) and TcO_(4)^(-) on Reillex 425-C2 were faster than those on Reillex 425-C5.Moreover,Reillex 425-Cn exhibited an exothermic nature,good selectivity,excellent reusability,and strong salinity tolerance.This study provides a simple strategy to enhance the Tc removal performance of adsorbents containing abundant micropores,which implies enormous environmental and economic benefits.
基金supported by the National Natural Science Foundation of China(21908234)the National Key Research&Development Program of China(2020YFB0606404)+1 种基金the Inner Mongolia Science and Technology Agency Program(2019CG058)Shanxi Province Natural Science Foundation(202103021223063).
文摘The influences of particle size,shape,and catalyst distribution on the reactivity and hydrocarbon product selectivity of a cobalt-based catalyst for Fischer-Tropsch synthesis were investigated in the present work.A self-consistent kinetic model for Fischer-Tropsch reaction proposed here was found to correlate experimental data well and hence was used to describe the consumption rates of reactants and formation rates of hydrocarbon products.The perturbed-chain statistical associating fluid theory equation of state was used to describe vapor-liquid equilibrium behavior associated with Fischer-Tropsch reaction.Local interaction between intraparticle diffusion and Fischer-Tropsch reaction was investigated in detail.Results showed that in order to avoid the adverse influence of intraparticle diffusional limitations on catalyst reactivity and product selectivity,the use of small particles is necessary.Large eggshell spherical particles are shown to keep the original catalyst reactivity and enhance the selectivity of heavy hydrocarbon products.The suitable layer thickness for a spherical particle with a diameter of 2 mm is nearly 0.15 mm.With the same outer diameter of 2 mm,the catalyst reactivity and heavy product selectivity of hollow cylindrical particles with a layer thickness of 0.25 mm are found to be larger than eggshell spherical particles.From the viewpoint of catalytic performance,hollow cylindrical particles are a better choice for industrial applications.
文摘In this study,the removal of monovalent and divalent cations,Nat,Kt,Mg2t,and Ca2t,in a diluted solution from Chott-El Jerid Lake,Tunisia,was investigated with the electrodialysis technique.The process was tested using two cation-exchange membranes:sulfonated polyether sulfone cross-linked with 10%hexamethylenediamine(HEXCl)and sulfonated polyether sulfone grafted with octylamine(S-PESOS).The commercially available membrane Nafion®was used for comparison.The results showed that Nafion®and S-PESOS membranes had similar removal behaviors,and the investigated cations were ranked in the following descending order in terms of their demineralization rates:Nat>Ca2t>Mg2t>Kt.Divalent cations were more effectively removed by HEXCl than by monovalent cations.The plots based on the WebereMorris model showed a strong linearity.This reveals that intra-particle diffusion was not the removal rate-determining step,and the removal process was controlled by two or more concurrent mechanisms.The Boyd plots did not pass through their origin,and the sole controlling step was determined by film-diffusion resistance,especially after a long period of electrodialysis.Additionally,a semi-empirical model was established to simulate the temporal variation of the treatment process,and the physical significance and values of model parameters were compared for the three membranes.The findings of this study indicate that HEXCl and S-PESOS membranes can be efficiently utilized for water softening,especially when effluents are highly loaded with calcium and magnesium ions.
文摘Continuous adsorption experiments are conducted using fixed-bed adsorption column to evaluate the performance of the adsorbent developed (from activated tamarind seeds) for the removal of Cr(VI) from aqueous solutions and the results obtained are validated with a model developed in this study. The effects of significant parameters such as flow rate, mass of adsorbent, and initial Cr(VI) concentration are studied and breakthrough curves are obtained. As the flow rate increases from 10 to 20 mL min-1, the breakthrough time decreases from 210 to 80 min. As the mass of adsorbent increases, breakthrough time gets delayed. The breakthrough times are obtained as 110, 115 and 210 min for 15, 20 and 25 g of activated tamarind seeds. As the initial Cr(VI) concentration increases from 100 to 200 mgL-1, the break point time decreases from 210 to 45 min. The process parameters for fixed-bed adsorption such as breakthrough time, total percentage removal of Cr(VI), adsorption exhaustion rate and fraction of unused bed length are calculated and the performance of fixed-bed adsorption column is analyzed. The mechanism for Cr(VI) adsorption on activated tamarind seeds is proposed. At low value of solution pH (= 1), the increase in Cr(VI) adsorption is due to the electrostatic attraction between positively charged groups of activated tamarind seeds and the HCrO4-. A mathematical model for fixed-bed adsorption column is proposed by incorporating the effect of velocity variation along the bed length in the existing model. Pore and surface diffusion models are used to describe the intra-particle mechanism for Cr(VI) adsorption. The breakthrough curve obtained theoretically from pore diffusion model and surface diffusion model are compared with experimental results for different operating conditions. The standard deviation values obtained for pore diffusion model and solid diffusion model are 0.111 and 0.214 respectively.
基金This work was supported by the European Union’s Horizon 2020 Research and Innovation Programme under the PHOQUSING Project GA No.899544the European Union’s Horizon 2020 Research and Innovation Programme QUDOT-TECH under the Marie Sklodowska-Curie Grant Agreement No.86109.
文摘Engineering single-photon states endowed with orbital angular momentum (OAM) is a powerful toolfor quantum information photonic implementations. Indeed, due to its unbounded nature, OAM is suitable forencoding qudits, allowing a single carrier to transport a large amount of information. Most of the experimentalplatforms employ spontaneous parametric down-conversion processes to generate single photons, evenif this approach is intrinsically probabilistic, leading to scalability issues for an increasing number of qudits.Semiconductor quantum dots (QDs) have been used to get over these limitations by producing on-demand pure and indistinguishable single-photon states, although only recently they have been exploitedto create OAM modes. Our work employs a bright QD single-photon source to generate a complete set ofquantum states for information processing with OAM-endowed photons. We first study hybrid intraparticleentanglement between OAM and polarization degrees of freedom of a single photon whose preparationwas certified by means of Hong–Ou–Mandel visibility. Then, we investigate hybrid interparticle OAM-based entanglement by exploiting a probabilistic entangling gate. The performance of our approach isassessed by performing quantum state tomography and violating Bell inequalities. Our results pave theway for the use of deterministic sources for the on-demand generation of photonic high-dimensionalquantum states.
基金We gratefully acknowledge the financial support from the National Natural Science Foundation of China:General Program(No.21673117,HC)Major Program(No.91956109,HC)+2 种基金Zhejiang Provincial Natural Science Foundation of China:Major Program(No.2022XHSJJ002,HC)Jiangsu Science and Technology Plan(No.BK20211258,YF)Start-up Fund from Westlake University。
文摘We show that through strong ligand mediated interfacial energy control between Au seeds and the deposited Au,the non-wetting growth of Au on Au seeds led to the formation homometallic core-satellite nanostructures.To modulate the intraparticle plasmonic coupling between the core and the satellites,the number and size of the Au satellites,and their inter-island distances were continuously tuned by varying the growth kinetics.As a result of the precise structural control,the plasmonic absorptions of the core-satellite nanostructures were tuned from visible to near-infrared(NIR)spectral range,and the extent of spectral modulation(500-1300 nm)is among the best of the literature methods.This synthetic advance enriches the toolbox for nanosynthesis and points to a new direction in the exploration of sophisticated functional designs.
