Simultaneous recovery of Ni and Co from Fe(Ⅲ)and AI is a critical challenge in hydrometallurgical processes.Recognized solvent extraction systems often struggle with selectivity and effective performance in mixed met...Simultaneous recovery of Ni and Co from Fe(Ⅲ)and AI is a critical challenge in hydrometallurgical processes.Recognized solvent extraction systems often struggle with selectivity and effective performance in mixed metal ion environments.Herein,a new synergistic solvent extraction(SSX)system comprised of a novel pyridine analog,N,N-bis(pyridin-2-ylmethyl)dodecan-1-amine(BPMDA),and dinonylnaphthalene sulfonic acid(DNNSA)with tributyl phosphate as phase modifier is introduced.The SSX system demonstrates high extraction performance achieving>90%for Ni and>97%for Co in a singlestage extraction process,with high selectivity.Under optimal conditions,the selectivity sequence is observed as Co^(2+)(>97%)>Ni^(2+)(>90%)>Mn^(2+)(<20%)>Fe^(3+)(<10%)>Mg^(2+)(<5%)>Al^(3+)(<2%)>Ca^(2+)(<1%).Spectroscopic analysis evidences the preferential binding of BPMDA with Ni and Co in the presence of DNNSA,concurrently achieving a significant reduction in the co-extraction of Fe(Ⅲ)and Al.The selective complexation of Ni and Co using the SSX system offers a highly efficient and selective approach for their extraction,with promising potential for applications in recovery-based processes.展开更多
Solid phase extraction is widely used in sample pretreatment,concentration and analysis processes due to high selectivity and suitability for low concentration sample system.In this review,we systematically summarized...Solid phase extraction is widely used in sample pretreatment,concentration and analysis processes due to high selectivity and suitability for low concentration sample system.In this review,we systematically summarized and discussed the development trends of solid phase extraction by bibliometrics method.By analyzing papers output scale,the research and development direction of solid phase extraction technology is prospected.We also give an overview on current strategies of novel solid phase extraction from the separation medium and separation technology.The paper aims to describe the global research profile and the development trends of solid phase extraction,to help researchers to accurately grasp the research trend and to provide support for scientific research institutions to formulate scientific policies and strategic plans.Furthermore,the prospect of the development and application of solid phase extraction is also discussed.展开更多
Developing highly efficient,durable,and non-noble electrocatalysts for the sluggish anodic oxygen evolution reaction(OER)is the pivotal for meeting the practical demand in water splitting.However,the current transitio...Developing highly efficient,durable,and non-noble electrocatalysts for the sluggish anodic oxygen evolution reaction(OER)is the pivotal for meeting the practical demand in water splitting.However,the current transition-metal electrocatalysts still suffer from low activity and durability on account of poor interfacial reaction kinetics.In this work,a facile solid-state synthesis strategy is developed to construct transition-metal sulfides heterostructures(denoted as MS_(2)/NiS_(2),M=Mo or W)for boosting OER electrocatalysis.As a result,MoS2/NiS2 and WS2/NiS2 show lower overpotentials of 300 mV and 320 mV to achieve the current density of 10 mA·cm^(-2),and smaller Tafel slopes of 60 mV.dec^(-1) and 83 mV.dec^(-1)in 1 mol·L^(-1) KOH,respectively,in comparison with the single MoS2,WS2,NiS2,as well as even the benchmark RuO2.The experiments reveal that the designed heterostructures have strong electronic interactions and spontaneously develop a built-in electric field at the heterointerface with uneven charge distribution based on the difference of band structures,which promote interfacial charge transfer,improve absorptivity of OH-,and modulate the energy level more comparable to the OER.Thus,the designed transition-metal sulfides heterostructures exhibit a remarkably high electrocatalytic activity for OER.This study provides a simple strategy to manipulate the heterostructure interface via an energy level engineering method for OER and can be extended to fabricate other heterostructures for various energy-related applications.展开更多
A novel hybrid material consisted of carbon covered Fe_(3)O_(4)nanoparticles and MoS_(2)nanoflower(FCM)was designed and prepared by micelle-assisted hydrothermal methods.Multiple techniques,including X-Ray diffraction...A novel hybrid material consisted of carbon covered Fe_(3)O_(4)nanoparticles and MoS_(2)nanoflower(FCM)was designed and prepared by micelle-assisted hydrothermal methods.Multiple techniques,including X-Ray diffraction(XRD),high-resolution transmission electron microscopy(HRTEM)and X-ray photoelectron spectroscopy(XPS)were employed to characterize it.The results show that FCM has a flower-like morphology with a 330 nm Fe_(3)O_(4)core as well as 70 nm highly crystalline MoS_(2)shell.FCM is superparamagnetic with a saturation magnetization of 35 emu g-1.Then hydrocracking of Canadian bitumen residue(CBR)was applied to estimate its catalytic activity.The results show that FCM exhibits superior catalytic hydrocracking activity compared to bulk MoS_(2)and commercial oil-dispersed Mo(CO)6 by the same Mo loading.Further measurement by elemental analysis,XPS and XRD reveals that the MoS_(2)nanoflower with abundant catalytic active sites and covered carbon layer with anti-coke ability donate to the superior upgrading performance.Besides,the catalysts can be easily recovered by the external magnetic field.This work provides a novel kind magnetic nanocatalyst which is potential for slurry-phase hydrocracking applications.■2020,Institute of Process Engineering,Chinese Academy of Sciences.Publishing services by Elsevier B.V.on behalf of KeAi Communications Co.,Ltd.This is an open access article under the CC BY-NC-ND license(http://creativecommons.org/licenses/by-nc-nd/4.0/).展开更多
Mild stir-assisted membrane dispersion extraction(MDE) method was employed to enhance propionic acid(HA)extraction and compared to the mechanical stirred extraction(MSE) method. Triocylamine(TOA) and tributyl phosphat...Mild stir-assisted membrane dispersion extraction(MDE) method was employed to enhance propionic acid(HA)extraction and compared to the mechanical stirred extraction(MSE) method. Triocylamine(TOA) and tributyl phosphate(TBP) were chosen as model extractant to extract HA. Firstly, droplet size and the size distribution of organic phase were analyzed, and then the effects of phase ratio, extractant and HA concentration on extraction performance were investigated. Comparing the two extraction methods, the results show mild stir-assisted MDE method reduced the mass transfer equilibrium time compared to MSE method. The mass transfer mechanism was explored by analyzing mass transfer resistance. Mild stir-assisted MDE had less total mass transfer resistance than MSE. When the extractant concentration was 40%, the extraction process was controlled by organic phase mass transfer process with HA volume fraction was 1% and controlled by both of reaction process and organic phase mass transfer process when HA concentration increased to 5%. This work may provide a new type of extraction method for the recovery of organic carboxylic acid.展开更多
A synergistic solvent extraction system comprising trioctylamine(TOA)and ligands with hydroxyl and carboxyl groups can efficiently recover boric acid(H_(3)BO_(3))and separate boron isotopes.However,the structure of li...A synergistic solvent extraction system comprising trioctylamine(TOA)and ligands with hydroxyl and carboxyl groups can efficiently recover boric acid(H_(3)BO_(3))and separate boron isotopes.However,the structure of ligands might impact H_(3)BO_(3) extraction,boron isotope separation,and solvent loss,which has not been thoroughly investigated.This study initially evaluated the influence of ligand's type,pKa,and substituents on H_(3)BO_(3) extraction efficiency,as well as the impact of the B_((4))-O structure(boron is bound to four oxygen atoms)in the organic phase on isotope separation efficiency.Subsequently,by synthesizing the highly hydrophobic 2-hydroxydodecanoic acid(HYA),the extraction performance and mechanism of the TOA/HYA system were investigated.The findings highlight the superior extraction efficiency when employing di-phenolic hydroxyl,phenolic hydroxyl + carbinol hydroxyl,and alcoholic hydroxyl + carboxyl ligands compared to phenolic hydroxyl + carboxyl,phenolic hydroxyl + ethanol hydroxyl,diol hydroxyl,and dicarboxylic ligands.The organic phase anion complex,exclusively comprising the B_((4))-O structure,enhances isotope separation effectiveness.The TOA/HYA system achieves an 80%single-stage extraction efficiency for H_(3)BO_(3).H_(3)BO_(3) and HYA are extracted into the organic phase at a ratio of 1:2,with the anion complex solely containing the B_((4))-O structure.This study paves the way for the construction of novel boric acid extraction and boron isotope separation systems.展开更多
A bioadsorbent composed of magnetic silica nanoparticles encapsulated by chitosan microspheres was prepared by the emulsion cross-linking method, and it was then modified with quaternary ammonium groups by reaction wi...A bioadsorbent composed of magnetic silica nanoparticles encapsulated by chitosan microspheres was prepared by the emulsion cross-linking method, and it was then modified with quaternary ammonium groups by reaction with ethylenediamine and glycidyl trimethylammonium chloride. Characterization of the bioadsorbent indicated that it was highly acid resistant and magnetically responsive. The bioadsor- bent was then used to remove Cr（VI） from acidic aqueous solution. The results of batch experiments indicated that the optimal pH value was 2.5, and the adsorbent exhibited low pH dependence. The maximum adsorption capacity was 233.1mg/g at pH 2.5 and 25 ℃, and the equilibrium time was deter- mined to be 40-120 min depending on the initial Cr（VI） concentration. The adsorbent could be effectively regenerated using a mixture of 0.3 mol/L NaOH and 0.3 mol/L NaCI with a desorption efficiency of 95.6%, indicating high reusability. In conclusion, the bioadsorbent shows potential for Cr（VI） removal from acidic展开更多
A novel Heck reaction catalyst consisting of a palladium（ll） complex of meso-tetra（p- hydroxyphenyl）porphyrin （MTP） and cross-linked chloromethylated polystyrene microspheres （PMs） was successfully prepared vi...A novel Heck reaction catalyst consisting of a palladium（ll） complex of meso-tetra（p- hydroxyphenyl）porphyrin （MTP） and cross-linked chloromethylated polystyrene microspheres （PMs） was successfully prepared via covalent ether bonds between the chloride groups in the PMs and the hydroxyl groups in MTP. The catalyst was characterized using scanning electron microscopy, Fourier-transform infrared spectroscopy, and inductively coupled plasma atomic emission spectroscopy （ICP-AES）. This polystyrene-supported palladium-complex was an efficient heterogeneous catalyst for cross-coupling of aryl iodides with ethyl acrylate. The reaction of iodobenzene and ethyl acrylate under N2 at 100 °C and a catalyst concentration of 0.1% gave a gas chromatography product yield of 99.8%, which is much higher than that achieved using a free palladium（II） complex of MTP as the catalyst （41.3%）. The catalyst was recycled up to six times without significant loss of catalytic activity. These results suggest that the immobilized palladium（II） MTP catalyst has potential applications in synthetic and industrial chemistry.展开更多
In this paper, gas-assisted magnetic separation （GAMS）, a technique that combines magnetic separation with flotation, was investigated for the potential large-scale separation of proteins, The GAMS process includes ...In this paper, gas-assisted magnetic separation （GAMS）, a technique that combines magnetic separation with flotation, was investigated for the potential large-scale separation of proteins, The GAMS process includes adsorption of target proteins and magnetic separation to recover protein-loaded magnetic particles from the dilute biosuspension with the assistance of bubbles, Microsized ethylenediamine- functionalized poly（glycidyl methacrylate） superparamagnetic microspheres （MPMs） and bovine serum albumin （BSA） were used as a model system. The feasibility of GAMS for capturing BSA-loaded MPMs from an appropriate medium was shown, High recovery of BSA-loaded MPMs was obtained by simple adjustment of the initial solution pH without extra detergents and antifoaming agents. The GAMS con- ditions were consistent with the adsorption conditions, and no proteins were desorbed from the MPMs during this process. Under the optimal conditions, the separation rate and recovery percentage reached 410 mL/min and 98% in 0.61 min, respectively. Conformational changes of BSA during the GAMS process were investigated by fluorescence spectroscopy and circular dichroism spectrometry,展开更多
基金supported by the National Natural Science Foundation of China(22278407,22001147,21922814,22138012,22178349)CAS Project for Young Scientists in Basic Research(YSBR-038)+2 种基金the Ministry of Science and Technology of China(2021YFC2901500)Excellent Member in Youth Innovation Promotion Association,Chinese Academy of Sciences(Y202014)Shandong Energy Institute(SEI U202306).
文摘Simultaneous recovery of Ni and Co from Fe(Ⅲ)and AI is a critical challenge in hydrometallurgical processes.Recognized solvent extraction systems often struggle with selectivity and effective performance in mixed metal ion environments.Herein,a new synergistic solvent extraction(SSX)system comprised of a novel pyridine analog,N,N-bis(pyridin-2-ylmethyl)dodecan-1-amine(BPMDA),and dinonylnaphthalene sulfonic acid(DNNSA)with tributyl phosphate as phase modifier is introduced.The SSX system demonstrates high extraction performance achieving>90%for Ni and>97%for Co in a singlestage extraction process,with high selectivity.Under optimal conditions,the selectivity sequence is observed as Co^(2+)(>97%)>Ni^(2+)(>90%)>Mn^(2+)(<20%)>Fe^(3+)(<10%)>Mg^(2+)(<5%)>Al^(3+)(<2%)>Ca^(2+)(<1%).Spectroscopic analysis evidences the preferential binding of BPMDA with Ni and Co in the presence of DNNSA,concurrently achieving a significant reduction in the co-extraction of Fe(Ⅲ)and Al.The selective complexation of Ni and Co using the SSX system offers a highly efficient and selective approach for their extraction,with promising potential for applications in recovery-based processes.
基金financial support of the Natural Science Foundation of Beijing (2194086)the National Natural Science Foundation of China (Nos. 21922814, 21676273, 21961160745, 31961133019 and 21921005)
文摘Solid phase extraction is widely used in sample pretreatment,concentration and analysis processes due to high selectivity and suitability for low concentration sample system.In this review,we systematically summarized and discussed the development trends of solid phase extraction by bibliometrics method.By analyzing papers output scale,the research and development direction of solid phase extraction technology is prospected.We also give an overview on current strategies of novel solid phase extraction from the separation medium and separation technology.The paper aims to describe the global research profile and the development trends of solid phase extraction,to help researchers to accurately grasp the research trend and to provide support for scientific research institutions to formulate scientific policies and strategic plans.Furthermore,the prospect of the development and application of solid phase extraction is also discussed.
基金supported by the National Natural Science Foun-dation of China(21922814,22138012,21961160745,21921005,22178349,22078333,22108281 and 31961133019)Excellent Member in Youth Innovation Promotion Association,Chinese Academy of Sciences(Y202014)Shandong Energy Institute(Grant Number SEI 1202133).
文摘Developing highly efficient,durable,and non-noble electrocatalysts for the sluggish anodic oxygen evolution reaction(OER)is the pivotal for meeting the practical demand in water splitting.However,the current transition-metal electrocatalysts still suffer from low activity and durability on account of poor interfacial reaction kinetics.In this work,a facile solid-state synthesis strategy is developed to construct transition-metal sulfides heterostructures(denoted as MS_(2)/NiS_(2),M=Mo or W)for boosting OER electrocatalysis.As a result,MoS2/NiS2 and WS2/NiS2 show lower overpotentials of 300 mV and 320 mV to achieve the current density of 10 mA·cm^(-2),and smaller Tafel slopes of 60 mV.dec^(-1) and 83 mV.dec^(-1)in 1 mol·L^(-1) KOH,respectively,in comparison with the single MoS2,WS2,NiS2,as well as even the benchmark RuO2.The experiments reveal that the designed heterostructures have strong electronic interactions and spontaneously develop a built-in electric field at the heterointerface with uneven charge distribution based on the difference of band structures,which promote interfacial charge transfer,improve absorptivity of OH-,and modulate the energy level more comparable to the OER.Thus,the designed transition-metal sulfides heterostructures exhibit a remarkably high electrocatalytic activity for OER.This study provides a simple strategy to manipulate the heterostructure interface via an energy level engineering method for OER and can be extended to fabricate other heterostructures for various energy-related applications.
基金financial support:The National Natural Science Foundation of China(21922814,21921005,21676273,21961160745,U1507203,31961133019)the Youth Innovation Promotion Association,CAS(Grant Nos.2016043)+1 种基金Beijing Natural Science Foundation(20194086)China Petroleum Enterprise Cooperation Project(PRIKY17094)。
文摘A novel hybrid material consisted of carbon covered Fe_(3)O_(4)nanoparticles and MoS_(2)nanoflower(FCM)was designed and prepared by micelle-assisted hydrothermal methods.Multiple techniques,including X-Ray diffraction(XRD),high-resolution transmission electron microscopy(HRTEM)and X-ray photoelectron spectroscopy(XPS)were employed to characterize it.The results show that FCM has a flower-like morphology with a 330 nm Fe_(3)O_(4)core as well as 70 nm highly crystalline MoS_(2)shell.FCM is superparamagnetic with a saturation magnetization of 35 emu g-1.Then hydrocracking of Canadian bitumen residue(CBR)was applied to estimate its catalytic activity.The results show that FCM exhibits superior catalytic hydrocracking activity compared to bulk MoS_(2)and commercial oil-dispersed Mo(CO)6 by the same Mo loading.Further measurement by elemental analysis,XPS and XRD reveals that the MoS_(2)nanoflower with abundant catalytic active sites and covered carbon layer with anti-coke ability donate to the superior upgrading performance.Besides,the catalysts can be easily recovered by the external magnetic field.This work provides a novel kind magnetic nanocatalyst which is potential for slurry-phase hydrocracking applications.■2020,Institute of Process Engineering,Chinese Academy of Sciences.Publishing services by Elsevier B.V.on behalf of KeAi Communications Co.,Ltd.This is an open access article under the CC BY-NC-ND license(http://creativecommons.org/licenses/by-nc-nd/4.0/).
基金Supported by the Chinese High Technology Research and Development Program(2015CB251402,17-163-12-ZD-001-013-01)the National Natural Science Foundation of China(21676215,21676273,U1507203)+3 种基金China Petroleum Enterprise Cooperation Project(PRIKY17094)China Postdoctoral Science Foundation(2018M633556)the Youth Innovation Promotion Association,CAS(2016043)the Shaanxi Provincial Science Foundation(2017SF-201,2018JQ2052).
文摘Mild stir-assisted membrane dispersion extraction(MDE) method was employed to enhance propionic acid(HA)extraction and compared to the mechanical stirred extraction(MSE) method. Triocylamine(TOA) and tributyl phosphate(TBP) were chosen as model extractant to extract HA. Firstly, droplet size and the size distribution of organic phase were analyzed, and then the effects of phase ratio, extractant and HA concentration on extraction performance were investigated. Comparing the two extraction methods, the results show mild stir-assisted MDE method reduced the mass transfer equilibrium time compared to MSE method. The mass transfer mechanism was explored by analyzing mass transfer resistance. Mild stir-assisted MDE had less total mass transfer resistance than MSE. When the extractant concentration was 40%, the extraction process was controlled by organic phase mass transfer process with HA volume fraction was 1% and controlled by both of reaction process and organic phase mass transfer process when HA concentration increased to 5%. This work may provide a new type of extraction method for the recovery of organic carboxylic acid.
基金supported by the National Natural Science Foundation of China(22278407,21922814,22138012,22178349)CAS Project for Young Scientists in Basic Research(YSBR-038)+1 种基金National Key Research and Development Program of China(2021YFC2901500,2022YFC2105302)Shandong Energy Institute(SEI U202306).
文摘A synergistic solvent extraction system comprising trioctylamine(TOA)and ligands with hydroxyl and carboxyl groups can efficiently recover boric acid(H_(3)BO_(3))and separate boron isotopes.However,the structure of ligands might impact H_(3)BO_(3) extraction,boron isotope separation,and solvent loss,which has not been thoroughly investigated.This study initially evaluated the influence of ligand's type,pKa,and substituents on H_(3)BO_(3) extraction efficiency,as well as the impact of the B_((4))-O structure(boron is bound to four oxygen atoms)in the organic phase on isotope separation efficiency.Subsequently,by synthesizing the highly hydrophobic 2-hydroxydodecanoic acid(HYA),the extraction performance and mechanism of the TOA/HYA system were investigated.The findings highlight the superior extraction efficiency when employing di-phenolic hydroxyl,phenolic hydroxyl + carbinol hydroxyl,and alcoholic hydroxyl + carboxyl ligands compared to phenolic hydroxyl + carboxyl,phenolic hydroxyl + ethanol hydroxyl,diol hydroxyl,and dicarboxylic ligands.The organic phase anion complex,exclusively comprising the B_((4))-O structure,enhances isotope separation effectiveness.The TOA/HYA system achieves an 80%single-stage extraction efficiency for H_(3)BO_(3).H_(3)BO_(3) and HYA are extracted into the organic phase at a ratio of 1:2,with the anion complex solely containing the B_((4))-O structure.This study paves the way for the construction of novel boric acid extraction and boron isotope separation systems.
基金This work was supported by the National Natural Science Foun- dation of China （No. 21106162）, the National Key Natural Science Foundation of China （No. 21136009）, and the Major Project of the National Natural Science Foundation of China （No. 51090382）, the General Research Project of Liaoning Education Department （L2015045）, and the Youth Foundation of Dalian Polytechnic Uni- versity （67007908）.
文摘A bioadsorbent composed of magnetic silica nanoparticles encapsulated by chitosan microspheres was prepared by the emulsion cross-linking method, and it was then modified with quaternary ammonium groups by reaction with ethylenediamine and glycidyl trimethylammonium chloride. Characterization of the bioadsorbent indicated that it was highly acid resistant and magnetically responsive. The bioadsor- bent was then used to remove Cr（VI） from acidic aqueous solution. The results of batch experiments indicated that the optimal pH value was 2.5, and the adsorbent exhibited low pH dependence. The maximum adsorption capacity was 233.1mg/g at pH 2.5 and 25 ℃, and the equilibrium time was deter- mined to be 40-120 min depending on the initial Cr（VI） concentration. The adsorbent could be effectively regenerated using a mixture of 0.3 mol/L NaOH and 0.3 mol/L NaCI with a desorption efficiency of 95.6%, indicating high reusability. In conclusion, the bioadsorbent shows potential for Cr（VI） removal from acidic
基金financially supported by the National Natural Science Foundation of China(21106162)the National Key Natural Science Foundation of China(21136009)+1 种基金the National High Technology Research and Development Program of China (2009CB219904)the State Key Laboratory of Chemical Engineering(SKL-ChE-11A04)
文摘A novel Heck reaction catalyst consisting of a palladium（ll） complex of meso-tetra（p- hydroxyphenyl）porphyrin （MTP） and cross-linked chloromethylated polystyrene microspheres （PMs） was successfully prepared via covalent ether bonds between the chloride groups in the PMs and the hydroxyl groups in MTP. The catalyst was characterized using scanning electron microscopy, Fourier-transform infrared spectroscopy, and inductively coupled plasma atomic emission spectroscopy （ICP-AES）. This polystyrene-supported palladium-complex was an efficient heterogeneous catalyst for cross-coupling of aryl iodides with ethyl acrylate. The reaction of iodobenzene and ethyl acrylate under N2 at 100 °C and a catalyst concentration of 0.1% gave a gas chromatography product yield of 99.8%, which is much higher than that achieved using a free palladium（II） complex of MTP as the catalyst （41.3%）. The catalyst was recycled up to six times without significant loss of catalytic activity. These results suggest that the immobilized palladium（II） MTP catalyst has potential applications in synthetic and industrial chemistry.
文摘In this paper, gas-assisted magnetic separation （GAMS）, a technique that combines magnetic separation with flotation, was investigated for the potential large-scale separation of proteins, The GAMS process includes adsorption of target proteins and magnetic separation to recover protein-loaded magnetic particles from the dilute biosuspension with the assistance of bubbles, Microsized ethylenediamine- functionalized poly（glycidyl methacrylate） superparamagnetic microspheres （MPMs） and bovine serum albumin （BSA） were used as a model system. The feasibility of GAMS for capturing BSA-loaded MPMs from an appropriate medium was shown, High recovery of BSA-loaded MPMs was obtained by simple adjustment of the initial solution pH without extra detergents and antifoaming agents. The GAMS con- ditions were consistent with the adsorption conditions, and no proteins were desorbed from the MPMs during this process. Under the optimal conditions, the separation rate and recovery percentage reached 410 mL/min and 98% in 0.61 min, respectively. Conformational changes of BSA during the GAMS process were investigated by fluorescence spectroscopy and circular dichroism spectrometry,
