Zeolite catalysts have found extensive applications in the synthesis of various fine chemicals.However,the micropores of zeolites impose diffusion limitations on bulky molecules,greatly reducing the catalytic efficien...Zeolite catalysts have found extensive applications in the synthesis of various fine chemicals.However,the micropores of zeolites impose diffusion limitations on bulky molecules,greatly reducing the catalytic efficiency.Herein,we explore an economic and environmentally friendly method for synthesizing hierarchical NaX zeolite that exhibits improved catalytic performance in the Knoevenagel condensation reaction for producing the useful fine chemical 2-cyano-3-phenylacrylate.The synthesis was achieved via a low-temperature activation of kaolinite and subsequent in-situ transformation strategy without any template or seed.Systematic characterizations reveal that the synthesized NaX zeolite has both intercrystalline and intra-crystalline mesopores,smaller crystal size,and larger external specific surface area compared to commercial NaX zeolite.Detailed mechanism investigations show that the inter-crystalline mesopores are generated by stacking smaller crystals formed from in-situ crystallization of the depolymerized kaolinite,and the intra-crystalline mesopores are inherited from the pores in the depolymerized kaolinite.This synthesis strategy provides an energy-saving and effective way to construct hierarchical zeolites,which may gain wide applications in fine chemical manufacturing.展开更多
This study delves into the intricate relationship between iron(Fe)content in kaolinite and its impact on the adsorption behavior of sodium oleate.The effects of different iron concentrations on adsorption energy,hydro...This study delves into the intricate relationship between iron(Fe)content in kaolinite and its impact on the adsorption behavior of sodium oleate.The effects of different iron concentrations on adsorption energy,hydrogen bond kinetics and adsorption efficiency were studied through simulation and experimental verification.The results show that the presence of iron in the kaolinite structure significantly improves the adsorption capacity of sodium oleate.Kaolinite samples with high iron content have better adsorption properties,lower adsorption energy levels and shorter and stronger hydrogen bonds than pure kaolinite.The optimal concentration of oleic acid ions for achieving maximum adsorption efficiency was identified as 1.2 mmol/L across different kaolinite samples.At this concentration,the adsorption rates and capacities reach their peak,with Fe-enriched kaolinite samples exhibiting notably higher flotation recovery rates.This optimal concentration represents a balance between sufficient oleic acid ion availability for surface interactions and the prevention of self-aggregation phenomena that could hinder adsorption.This study offers promising avenues for optimizing the flotation process in mineral processing applications.展开更多
The flotation and adsorption behaviors of dodecyltrimethylammonium chloride（DTAC） and cetyltrimethylammonium chloride（CTAC） on diaspore and kaolinite were studied.Solution depletion methods were used to determine ...The flotation and adsorption behaviors of dodecyltrimethylammonium chloride（DTAC） and cetyltrimethylammonium chloride（CTAC） on diaspore and kaolinite were studied.Solution depletion methods were used to determine adsorption isotherms.Fluorescence probe test along with Zeta potential measurement was also conducted for further investigation into the adsorption of quaternary amines at the mineral-water interface.The results show that the flotation recovery of kaolinite decreases with an increase in pH when DTAC and CTAC are used as collectors,while diaspore is on the contrary.As the carbon chain length of the collectors increases,the flotation recoveries of minerals increase.However,the increment rate of kaolinite is significantly lower than that of diaspore.In the low surfactant concentration range,the cationic surfactants adsorb readily on diaspore surfaces just due to electrostatic interactions.As for kaolinite surfaces,ion exchange process also exists.With a further increase in surfactant concentration,the adsorption was ascribed to the hydrophobic association of chain-chain interactions.Micro-polarity of mineral surfaces study shows that CTAC has a better hydrophobic characteristic than DTAC.Larger aggregates are formed with CTAC on diaspore than on kaolinite in the same solution concentration.The results also indicate that the chain length of cationic surfactants has a greater influence on the adsorption of diaspore than on kaolinite,which is consistent with the flotation result.展开更多
The collecting power of tertiary amines（DRN,DEN and DPN） on kaolinite follows the order of DENDPNDRN.After reacting with DRN,DEN and DPN,the surface potentials of kaolinite increase remarkably,and the recruitments c...The collecting power of tertiary amines（DRN,DEN and DPN） on kaolinite follows the order of DENDPNDRN.After reacting with DRN,DEN and DPN,the surface potentials of kaolinite increase remarkably,and the recruitments caused by collectors also follow the order of DENDPNDRN.The results of dynamics simulation show that the geometries of substituent groups bonding to N are deflected and twisted,and some of bond angles are changed when tertiary amines cations adsorb on kaolinite（001） surface.Based on the results of dynamics simulations and quantum chemistry calculations,the electrostatic forces between three tertiary amines cations and 4×4×3（001） plane of kaolinite are 1.38×10？7 N（DRN12H＋）,1.44×10-6 N（DEN12H＋）,1.383×10-6 N（DPN12H＋）,respectively.展开更多
为全面了解土壤胶体影响重金属行为方向的研究现状和前沿动态,基于Web of Science(WoS)核心合集数据库,利用WoS自带分析工具、HistCite引文图谱分析软件、VOSviewer和Citespace可视化分析软件对1990—2021年间土壤胶体影响重金属行为的...为全面了解土壤胶体影响重金属行为方向的研究现状和前沿动态,基于Web of Science(WoS)核心合集数据库,利用WoS自带分析工具、HistCite引文图谱分析软件、VOSviewer和Citespace可视化分析软件对1990—2021年间土壤胶体影响重金属行为的文献进行了计量分析。结果表明,在世界范围内该方向的发文量逐年稳步增长,我国相关研究起步较晚,但近些年呈现迅猛发展的势头。目前土壤胶体影响重金属行为研究发文量最多的国家和研究机构分别是美国和中国科学院,发文量最高的期刊为Environmental Science&Technology,主要研究学科为环境科学与生态学的交叉学科。关键词聚类分析显示“土壤胶体颗粒粒径分级与重金属的形态分布”、“土壤胶体的释放、沉积及对重金属的吸附作用”和“土壤胶体颗粒的迁移机制与迁移模型研究”为主要的研究主题,人工纳米颗粒在土壤中的行为、迁移转化以及生物有效性是现阶段的研究热点。利用场流分离技术结合单粒子电感耦合等离子体质谱等技术,探讨土壤胶体与人工纳米颗粒之间发生的复杂相互作用及其对人工纳米颗粒迁移归趋与环境命运的影响,是未来的主要研究方向。展开更多
This report examined electrochemical remediation of copper contaminated kaolinite by controlling electrolytes′ pH for both of anolyte and catholyte simultaneously. Results showed that electrokinetic process and remed...This report examined electrochemical remediation of copper contaminated kaolinite by controlling electrolytes′ pH for both of anolyte and catholyte simultaneously. Results showed that electrokinetic process and remediation efficiency varied obviously when different buffer systems, including citric acid (test 1), nitric acid + EDTA (test 2) and nitric acid (test 3), were used to control catholyte pH and Na_2CO_3 was used at the same time to control all anolyte one. It was found that under such pH condition soil′s pH in soil column kept at 3.0—7.0 successfully, and correspondingly no copper precipitation and decrease of soil electroconductivity appeared, which are usually observed in electrokinetic process due to OH - introduction into soil column by electrochemical reaction occurred in cathode. Electroosmosis flow rates were almost equal for these three tests, indicating that these buffers did not affect Zeta-potential of kaolinite within the examined duration. More acid and basic solution was added into electrokinetic cell when nitric acid was used as buffer than when nitric acid + EDTA and then citric acid were used. Due to introduction of large amounts of ions into soil column, significant higher current was observed for test 3 than other two. Analysis of copper speciation and total quantity in kaolinite indicated that 22.5%, 23.74% and 55.65% Cu were removed from kaolinite for test 1, test 2 and test 3 respectively after only 10 days′ electrokinetic remediation.展开更多
基金The financial supports from the National Natural Science Foundation of China (22178059, 22208054 and 22072019)Natural Science Foundation of Fujian Province, China (2020J01513)+1 种基金Sinochem Quanzhou Energy Technology Co., Ltd. (ZHQZKJ-19-F-ZS0076)Qingyuan Innovation Laboratory (00121002)
文摘Zeolite catalysts have found extensive applications in the synthesis of various fine chemicals.However,the micropores of zeolites impose diffusion limitations on bulky molecules,greatly reducing the catalytic efficiency.Herein,we explore an economic and environmentally friendly method for synthesizing hierarchical NaX zeolite that exhibits improved catalytic performance in the Knoevenagel condensation reaction for producing the useful fine chemical 2-cyano-3-phenylacrylate.The synthesis was achieved via a low-temperature activation of kaolinite and subsequent in-situ transformation strategy without any template or seed.Systematic characterizations reveal that the synthesized NaX zeolite has both intercrystalline and intra-crystalline mesopores,smaller crystal size,and larger external specific surface area compared to commercial NaX zeolite.Detailed mechanism investigations show that the inter-crystalline mesopores are generated by stacking smaller crystals formed from in-situ crystallization of the depolymerized kaolinite,and the intra-crystalline mesopores are inherited from the pores in the depolymerized kaolinite.This synthesis strategy provides an energy-saving and effective way to construct hierarchical zeolites,which may gain wide applications in fine chemical manufacturing.
基金supported by the Natural Science Foundation of China(No.52174232)the Project was supported by Open Research Grant of Joint National-Local Engineering Research Centre for Safe and Precise Coal Mining(Nos.EC2022003 and EC2023005)+1 种基金Anhui University of Science and Technology 2023 Graduate Student Innovation Fund(No.2023cx2106)Open Research Grant of Anhui Engineering Research Center for Coal Clean Processing and Carbon Emission Reduction(No.CCCE-2023003).
文摘This study delves into the intricate relationship between iron(Fe)content in kaolinite and its impact on the adsorption behavior of sodium oleate.The effects of different iron concentrations on adsorption energy,hydrogen bond kinetics and adsorption efficiency were studied through simulation and experimental verification.The results show that the presence of iron in the kaolinite structure significantly improves the adsorption capacity of sodium oleate.Kaolinite samples with high iron content have better adsorption properties,lower adsorption energy levels and shorter and stronger hydrogen bonds than pure kaolinite.The optimal concentration of oleic acid ions for achieving maximum adsorption efficiency was identified as 1.2 mmol/L across different kaolinite samples.At this concentration,the adsorption rates and capacities reach their peak,with Fe-enriched kaolinite samples exhibiting notably higher flotation recovery rates.This optimal concentration represents a balance between sufficient oleic acid ion availability for surface interactions and the prevention of self-aggregation phenomena that could hinder adsorption.This study offers promising avenues for optimizing the flotation process in mineral processing applications.
基金Projects (50974134,50804055) supported by the National Natural Science Foundation of ChinaProject (2005CB623701) supported by the National Basic Research Program of China
文摘The flotation and adsorption behaviors of dodecyltrimethylammonium chloride（DTAC） and cetyltrimethylammonium chloride（CTAC） on diaspore and kaolinite were studied.Solution depletion methods were used to determine adsorption isotherms.Fluorescence probe test along with Zeta potential measurement was also conducted for further investigation into the adsorption of quaternary amines at the mineral-water interface.The results show that the flotation recovery of kaolinite decreases with an increase in pH when DTAC and CTAC are used as collectors,while diaspore is on the contrary.As the carbon chain length of the collectors increases,the flotation recoveries of minerals increase.However,the increment rate of kaolinite is significantly lower than that of diaspore.In the low surfactant concentration range,the cationic surfactants adsorb readily on diaspore surfaces just due to electrostatic interactions.As for kaolinite surfaces,ion exchange process also exists.With a further increase in surfactant concentration,the adsorption was ascribed to the hydrophobic association of chain-chain interactions.Micro-polarity of mineral surfaces study shows that CTAC has a better hydrophobic characteristic than DTAC.Larger aggregates are formed with CTAC on diaspore than on kaolinite in the same solution concentration.The results also indicate that the chain length of cationic surfactants has a greater influence on the adsorption of diaspore than on kaolinite,which is consistent with the flotation result.
基金Project (2005CB623701) supported by the National Basic Research Program of China Project (201011031) supported by National Department Public Benefit Research Foundation from Ministry of Land and Resources of China+1 种基金 Project (2935) supported by the Foundation for the Author of Zhengzhou Institute of Multipurpose Utilization of Mineral Resources CAGS, China Project (1212011120304) supported by the Geological Surrey Program
文摘The collecting power of tertiary amines（DRN,DEN and DPN） on kaolinite follows the order of DENDPNDRN.After reacting with DRN,DEN and DPN,the surface potentials of kaolinite increase remarkably,and the recruitments caused by collectors also follow the order of DENDPNDRN.The results of dynamics simulation show that the geometries of substituent groups bonding to N are deflected and twisted,and some of bond angles are changed when tertiary amines cations adsorb on kaolinite（001） surface.Based on the results of dynamics simulations and quantum chemistry calculations,the electrostatic forces between three tertiary amines cations and 4×4×3（001） plane of kaolinite are 1.38×10？7 N（DRN12H＋）,1.44×10-6 N（DEN12H＋）,1.383×10-6 N（DPN12H＋）,respectively.
文摘为全面了解土壤胶体影响重金属行为方向的研究现状和前沿动态,基于Web of Science(WoS)核心合集数据库,利用WoS自带分析工具、HistCite引文图谱分析软件、VOSviewer和Citespace可视化分析软件对1990—2021年间土壤胶体影响重金属行为的文献进行了计量分析。结果表明,在世界范围内该方向的发文量逐年稳步增长,我国相关研究起步较晚,但近些年呈现迅猛发展的势头。目前土壤胶体影响重金属行为研究发文量最多的国家和研究机构分别是美国和中国科学院,发文量最高的期刊为Environmental Science&Technology,主要研究学科为环境科学与生态学的交叉学科。关键词聚类分析显示“土壤胶体颗粒粒径分级与重金属的形态分布”、“土壤胶体的释放、沉积及对重金属的吸附作用”和“土壤胶体颗粒的迁移机制与迁移模型研究”为主要的研究主题,人工纳米颗粒在土壤中的行为、迁移转化以及生物有效性是现阶段的研究热点。利用场流分离技术结合单粒子电感耦合等离子体质谱等技术,探讨土壤胶体与人工纳米颗粒之间发生的复杂相互作用及其对人工纳米颗粒迁移归趋与环境命运的影响,是未来的主要研究方向。
文摘This report examined electrochemical remediation of copper contaminated kaolinite by controlling electrolytes′ pH for both of anolyte and catholyte simultaneously. Results showed that electrokinetic process and remediation efficiency varied obviously when different buffer systems, including citric acid (test 1), nitric acid + EDTA (test 2) and nitric acid (test 3), were used to control catholyte pH and Na_2CO_3 was used at the same time to control all anolyte one. It was found that under such pH condition soil′s pH in soil column kept at 3.0—7.0 successfully, and correspondingly no copper precipitation and decrease of soil electroconductivity appeared, which are usually observed in electrokinetic process due to OH - introduction into soil column by electrochemical reaction occurred in cathode. Electroosmosis flow rates were almost equal for these three tests, indicating that these buffers did not affect Zeta-potential of kaolinite within the examined duration. More acid and basic solution was added into electrokinetic cell when nitric acid was used as buffer than when nitric acid + EDTA and then citric acid were used. Due to introduction of large amounts of ions into soil column, significant higher current was observed for test 3 than other two. Analysis of copper speciation and total quantity in kaolinite indicated that 22.5%, 23.74% and 55.65% Cu were removed from kaolinite for test 1, test 2 and test 3 respectively after only 10 days′ electrokinetic remediation.
