Coke powder is expected to be an excellent raw material to produce activated carbon because of its high carbon content. Potassium hydroxide(KOH), as an effective activation agent, was reported to be effective in activ...Coke powder is expected to be an excellent raw material to produce activated carbon because of its high carbon content. Potassium hydroxide(KOH), as an effective activation agent, was reported to be effective in activating coke powder. However, the microstructures development in the coke powder and its mechanisms when KOH was applied were still unclear. In this study, effects of KOH on the microstructure activation of coke powder were investigated using the surface area and pore structure analyzer, scanning electron microscope(SEM) and thermogravimetry-differential scanning calorimetry-mass spectrometry(TG-DSC-MS), etc. Results revealed that the addition KOH at its lower ratio(mass ratios of KOH and coke powder in a range of 0.5 and 1) decreased the specific surface area and average lateral sizes, but sharply increased of the specific surface area to 132 m^2·g^-1 and 355 m^2·g^-1 and decreased of the space size of aromatic crystallites upon the further increase of the KOH addition amounts(ratios of KOH and coke powder in a range of 3 and 7), generating a number of new micropores and mesopores. The mechanisms study implied surface reactions between KOH and aliphatic hydrocarbon side chain and other carbon functional groups of the coke powder to destruct aromatic crystallites in one dimension and broaden pores at lower KOH addition. In the activation process, KOH was decomposed to be more active components, which can be rapidly destruct the aromatic layers in spatial scope to form developed porous carbon structures within coke powder at higher KOH addition.展开更多
The utilization of coal fly ash derived from circulating fluidized bed combustion(CFBFA)still faces great challenges because of its unique characteristics.In this study,a zeolitic material with Na-P1 zeolite as the ma...The utilization of coal fly ash derived from circulating fluidized bed combustion(CFBFA)still faces great challenges because of its unique characteristics.In this study,a zeolitic material with Na-P1 zeolite as the main phase was successfully synthesized via a hydrothermal method by using CFBFA as the raw material.The effects of hydrothermal temperature,time,and added CTAB amount on the characterizations of synthesized materials were investigated by XRD,SEM,and XPS.The properties of the optimal zeolitic material and its adsorption performance for Pb^(2+)in aqueous solution were evaluated.The influences of pH,initial concentration,dosage,and temperature on Pb^(2+)adsorption were also examined.Results revealed the following optimal parameters for the synthesis of zeolitic material:NaOH concentration of 2 mol·L^(-1),solid-to-liquid ratio of 1:10 g·ml^(-1),hydrothermal temperature of 110℃,hydrothermal time of 9 h,and CTAB amount of 1 g(per 100 ml solution).The adsorption capacities of the zeolitic material reached 329.67,424.69,and 542.22 mg·g^(-1) when the pH values of aqueous solution were 5,6,and 7,respectively.The Pb^(2+)removal efficiency can reach more than 99%in aqueous solution with the initial concentrations of 100-300 mg·L^(-1) under pH 6 and suitable adsorbent dosage.The adsorption and kinetics of Pb^(2+)on the zeolitic material can be described by Langmuir isotherm and pseudo-second-order kinetic models,respectively.The ion exchange between Pb^(2+)and Na^(+)and chemisorption are the main adsorption mechanism.All these findings imply that the synthesis of low-cost adsorbent for Pb^(2+)removal from weak acid and neutral aqueous solution provides a highly effective method to utilize CFBFA.展开更多
Rare earth elements(REE)are strategic resources and the recycling of REE in alternative resources is urgent and gets increasingly attention.However,the separation of REE in these alternative resources is still a chall...Rare earth elements(REE)are strategic resources and the recycling of REE in alternative resources is urgent and gets increasingly attention.However,the separation of REE in these alternative resources is still a challenge due to the low concentration of REE and multi coexisted ions in acidic system.In this study,the species distribution of REE within the pH 0-8.0 was calculated.The SBA-15 originated from coal fly ash was modified by two steps with(3-aminopropyl)triethoxysilane(APTES)and diethylenetriaminepentaacetic dianhydride(DTPADA)to obtain DTPADA-SBA-15 adsorbent,which was applied to the selective adsorption of REE.The results showed that DTPADA-SBA-15 possessed excellent adsorption performance on the selective adsorption of REE,including Eu,Gd,Tb,Nd and Sm,in acidic solution(pH 2)with multi competing ions.The FT-IR and Zeta potential characterization verified that the chemical adsorption through the coordination of O in DTPADA-SBA-15 with REE was dominant at lower pH value.The study of adsorption kinetics indicated that the adsorption of rare earth metal ions followed pseudosecond-order kinetic,of which the adsorption process followed the Langmuir isotherm model.展开更多
Lithium(Li)is an important energy metal in the 21st century.However,the selective recovery of Li is still a big challenge,especially from acidic solutions with multiple metal ions existence.Herein we report a new ion ...Lithium(Li)is an important energy metal in the 21st century.However,the selective recovery of Li is still a big challenge,especially from acidic solutions with multiple metal ions existence.Herein we report a new ion pair induced mechanism for selectively extracting Li^(+)from acidic chloride solutions by tributyl phosphate(TBP).It is shown that the acidity and the chloride ions in the aqueous phase have great effects on the extraction of Li^(+).The FT-IR,UV-Vis and ESI-MS experiments provide solid evidence for the formation of ion-pair complex[Li(TBP)_n(H_(2)O)_(m)]^(+)[FeCl_(4)]^(-)(n-1,2,3;m-0,1)in the organic phase,which brings about the effective and efficient extraction of Li^(+).This mechanism can overcome the Hofmeister bias and allow for the selective extraction of Li^(+) from the extremely hydrophilic chlorides.It has also been proved that the loaded Li in TBP can be effectively stripped by concentrated HCl solution with a Li/Fe separation factor>500.The understanding of the ion-pair transport mechanism is helpful for optimizing the recovery process or further advancing more efficient recovery techniques for Li from acidic liquor.展开更多
基金Supported by the National Key R&D Plan(2016YFE0131100,2017YFB0603101)the Program for Sanjin Scholars of Shanxi Provincethe Talent Training Program of Shanxi Joint Postgraduate Training Base(2016JD07).
文摘Coke powder is expected to be an excellent raw material to produce activated carbon because of its high carbon content. Potassium hydroxide(KOH), as an effective activation agent, was reported to be effective in activating coke powder. However, the microstructures development in the coke powder and its mechanisms when KOH was applied were still unclear. In this study, effects of KOH on the microstructure activation of coke powder were investigated using the surface area and pore structure analyzer, scanning electron microscope(SEM) and thermogravimetry-differential scanning calorimetry-mass spectrometry(TG-DSC-MS), etc. Results revealed that the addition KOH at its lower ratio(mass ratios of KOH and coke powder in a range of 0.5 and 1) decreased the specific surface area and average lateral sizes, but sharply increased of the specific surface area to 132 m^2·g^-1 and 355 m^2·g^-1 and decreased of the space size of aromatic crystallites upon the further increase of the KOH addition amounts(ratios of KOH and coke powder in a range of 3 and 7), generating a number of new micropores and mesopores. The mechanisms study implied surface reactions between KOH and aliphatic hydrocarbon side chain and other carbon functional groups of the coke powder to destruct aromatic crystallites in one dimension and broaden pores at lower KOH addition. In the activation process, KOH was decomposed to be more active components, which can be rapidly destruct the aromatic layers in spatial scope to form developed porous carbon structures within coke powder at higher KOH addition.
基金supported by National Natural Science Foundation of China(22078181,U1810205)the Bidding Project of Shanxi Province(20191101007).
文摘The utilization of coal fly ash derived from circulating fluidized bed combustion(CFBFA)still faces great challenges because of its unique characteristics.In this study,a zeolitic material with Na-P1 zeolite as the main phase was successfully synthesized via a hydrothermal method by using CFBFA as the raw material.The effects of hydrothermal temperature,time,and added CTAB amount on the characterizations of synthesized materials were investigated by XRD,SEM,and XPS.The properties of the optimal zeolitic material and its adsorption performance for Pb^(2+)in aqueous solution were evaluated.The influences of pH,initial concentration,dosage,and temperature on Pb^(2+)adsorption were also examined.Results revealed the following optimal parameters for the synthesis of zeolitic material:NaOH concentration of 2 mol·L^(-1),solid-to-liquid ratio of 1:10 g·ml^(-1),hydrothermal temperature of 110℃,hydrothermal time of 9 h,and CTAB amount of 1 g(per 100 ml solution).The adsorption capacities of the zeolitic material reached 329.67,424.69,and 542.22 mg·g^(-1) when the pH values of aqueous solution were 5,6,and 7,respectively.The Pb^(2+)removal efficiency can reach more than 99%in aqueous solution with the initial concentrations of 100-300 mg·L^(-1) under pH 6 and suitable adsorbent dosage.The adsorption and kinetics of Pb^(2+)on the zeolitic material can be described by Langmuir isotherm and pseudo-second-order kinetic models,respectively.The ion exchange between Pb^(2+)and Na^(+)and chemisorption are the main adsorption mechanism.All these findings imply that the synthesis of low-cost adsorbent for Pb^(2+)removal from weak acid and neutral aqueous solution provides a highly effective method to utilize CFBFA.
基金the National Natural Science Foundation of China(U1810205)Scientific and Technological Innovation Programs of Higher Education Institutions in Shanxi Province(2020L0022)Key Research and Development Program of Shanxi Province(201903D311006).
文摘Rare earth elements(REE)are strategic resources and the recycling of REE in alternative resources is urgent and gets increasingly attention.However,the separation of REE in these alternative resources is still a challenge due to the low concentration of REE and multi coexisted ions in acidic system.In this study,the species distribution of REE within the pH 0-8.0 was calculated.The SBA-15 originated from coal fly ash was modified by two steps with(3-aminopropyl)triethoxysilane(APTES)and diethylenetriaminepentaacetic dianhydride(DTPADA)to obtain DTPADA-SBA-15 adsorbent,which was applied to the selective adsorption of REE.The results showed that DTPADA-SBA-15 possessed excellent adsorption performance on the selective adsorption of REE,including Eu,Gd,Tb,Nd and Sm,in acidic solution(pH 2)with multi competing ions.The FT-IR and Zeta potential characterization verified that the chemical adsorption through the coordination of O in DTPADA-SBA-15 with REE was dominant at lower pH value.The study of adsorption kinetics indicated that the adsorption of rare earth metal ions followed pseudosecond-order kinetic,of which the adsorption process followed the Langmuir isotherm model.
基金supported by the National Natural Science Foundation of China(21706257,21878180)the Shanxi Province Coal Based Low-carbon Technology Major Projects(MC2016-05)the Xiangyuan Key Technology Research Projects(2018XYSDYY-02)。
文摘Lithium(Li)is an important energy metal in the 21st century.However,the selective recovery of Li is still a big challenge,especially from acidic solutions with multiple metal ions existence.Herein we report a new ion pair induced mechanism for selectively extracting Li^(+)from acidic chloride solutions by tributyl phosphate(TBP).It is shown that the acidity and the chloride ions in the aqueous phase have great effects on the extraction of Li^(+).The FT-IR,UV-Vis and ESI-MS experiments provide solid evidence for the formation of ion-pair complex[Li(TBP)_n(H_(2)O)_(m)]^(+)[FeCl_(4)]^(-)(n-1,2,3;m-0,1)in the organic phase,which brings about the effective and efficient extraction of Li^(+).This mechanism can overcome the Hofmeister bias and allow for the selective extraction of Li^(+) from the extremely hydrophilic chlorides.It has also been proved that the loaded Li in TBP can be effectively stripped by concentrated HCl solution with a Li/Fe separation factor>500.The understanding of the ion-pair transport mechanism is helpful for optimizing the recovery process or further advancing more efficient recovery techniques for Li from acidic liquor.