Excessive phosphorus and arsenic in water bodies not only destroy ecosystems but also pose a serious threat to human health.In this study,a series of Al-doped modified metal-organic frameworks(Zr-Al-MOF)were prepared ...Excessive phosphorus and arsenic in water bodies not only destroy ecosystems but also pose a serious threat to human health.In this study,a series of Al-doped modified metal-organic frameworks(Zr-Al-MOF)were prepared by solvothermal method,which achieved efficient removal of phosphate and arsenate in water.Due to the use of inexpensive Al salts,the material has a lower cost and is more economical.The molar ratio of metal salts,adsorption time,solution pH,initial concentration,temperature and coexisting anions were studied,and it was found that when the molar ratio of Zr:Al was 2,Zr-Al-MOF had the best adsorption performance for phosphate and arsenate,and the maximum adsorption capacity was 93.04 mg P/g and 173.83 mg As/g,respectively.It traps phosphate and arsenate at a fast reaction rate and can be recycled repeatedly.In addition,0.15 g/L of 2Zr-Al-MOF can effectively reduce the phosphate and arsenate content in the contaminated spring water samples of Yangzonghai Lake to the standard range of drinking water,which further confirms the application potential of 2Zr-Al-MOF.By FT-IR and XPS analysis,it was found that the adsorption mechanism was ligand exchange,electrostatic attraction and hydrogen bond formation.The theoretical calculation shows that the adsorption energy is negative,which indicates that 2Zr-Al-MOF is attractive to phosphate and arsenate,and the adsorption state is stable.The results show that 2Zr-Al-MOF is an effective phosphate and arsenate adsorbent and has broad application prospects in eutrophication water treatment.展开更多
Oily sludge,a hazardous by-product of the petroleum industry,poses significant environmental risks due to its elevated levels of hydrocarbons and heavy metals.As conventional disposal methods often lead to secondary p...Oily sludge,a hazardous by-product of the petroleum industry,poses significant environmental risks due to its elevated levels of hydrocarbons and heavy metals.As conventional disposal methods often lead to secondary pollution or inefficient resource recovery,this study investigates the synergistic pyrolysis of oily sludge with lignin to produce high-performance adsorbents for oily wastewater treatment.Thermogravimetric analyses demonstrated complementary properties and a synergistic copyrolysis effect between the two feedstocks.Kinetic analysis employing the Coats-Redfern method revealed that the co-pyrolysis of oily sludge and lignin significantly decreased the apparent activation energy while increasing the pre-exponential factor,confirming the lignin's catalytic role in enhancing pyrolysis efficiency.The optimal adsorbent,produced at an oily sludge-to-lignin mass ratio of 1:5,exhibited a specific surface area of 1324.5 m2/g,abundant micropores,and diverse surface functional groups,as confirmed by SEM and FT-IR analyses.Under optimized conditions—an adsorbent dosage of1.0 g/L,contact time of 40 min,and pH 7—this material effectively removed residual oil from synthetic oily wastewater and maintained over 70%removal efficiency after five regeneration cycles,highlighting its reusability.Finally,the chemical transformations of various components during the co-pyrolysis of oily sludge and biomass materials are elucidated.展开更多
A novel faujasite(FAU) type zeolitized ceramsite(FZC) was prepared via a novel three dimensional(3D) in-pore growth method.FZC is a centimeter sized spherical particle with a 3-dimensional radial morphology inside,wit...A novel faujasite(FAU) type zeolitized ceramsite(FZC) was prepared via a novel three dimensional(3D) in-pore growth method.FZC is a centimeter sized spherical particle with a 3-dimensional radial morphology inside,with a specific surface area and pore volume 6 and 30 times that of the original ceramsite,respectively.The unique structure was constructed through electrostatic and polymerization interactions between hexadecyl trimethyl ammonium bromide(CTAB) micelles,ceramic pore walls and silicate aluminate ions,which could simultaneously improve adsorption capacity and mass transfer,endowing FZC with excellent heavy metal adsorption properties.FZC-50 could remove the majority of Cu and Zn from solution within shorter periods(73.3 % and 80.0 %of original ceramsite,respectively) with larger adsorption capacities(340 % and 370 % of original ceramsite,respectively).Theoretical analysis and regeneration experiments both indicate that the adsorption of Cu(Ⅱ) and Zn(Ⅱ) on FZC-50 is dominated by ion exchange.And the spent sorbent can be effectively regenerated by NaCl,and the cycle number is expected to be 33 and 26 times for Cu(Ⅱ) and Zn(Ⅱ) adsorption,respectively.This work proposed a novel synthesis route to construct a 3D multi-stage porous zeolite inside ceramsite,and opened up new ideas for the further development of zeolitized ceramsite.展开更多
The development of efficient CO2 adsorbents is critical for achieving net-zero targets.MgO represents a promising solid adsorbent for CO2 capture,yet its limited specific surface area and insufficient active sit...The development of efficient CO2 adsorbents is critical for achieving net-zero targets.MgO represents a promising solid adsorbent for CO2 capture,yet its limited specific surface area and insufficient active sites restrict its adsorption capacity under moderate temperature conditions.A rod-like anhydrous MgCO3 precursor was hydrothermally synthesized and calcined at 500℃ for 3 h to obtain porous MgO(184.9 m2g-1,0.38 cm3/g),which was then modified with 20% NaNO2(by mole) via impregnation.This adsorbent achieved an adsorption capacity of 12.6 mmol g-1after 120 min under a pure CO2 atmosphere at 325℃.Comprehensive characterization reveals that NaNO2 modification leads to the NaNO3 and Na2 CO3 formation on the MgO surface during calcination.The introduced NaNO3 effectively promotes oxygen vacancy formation,while the generated Na2 CO3 serves as heterogeneous nucleation sites,collectively reducing the reaction energy barrier and enhancing interfacial mass transfer.This synergistic effect facilitates the MgCO3 formation followed by its conversion to the thermodynamically more stable Na2Mg(CO3)2.Kinetic studies elucidate that adsorption is dominated by surface chemical reactions and diffusion mechanisms at different stages.These fundamental insights into the adsorption mechanisms of nitrite-modified MgO provide valuable guidance for the rational design of advanced MgO-based CO2 adsorbents with enhanced performance.展开更多
基金supported by the NSFC-Yunnan Joint Fund(No.U2102210)the National Natural Science Foundation of China(No.22168044)+1 种基金Yunnan Provincial Department of Science and Technology(No.202201BF070001-013)the Research Innovation Fund for Graduate Students of Yunnan University(No.KC-23234004).
摘要Excessive phosphorus and arsenic in water bodies not only destroy ecosystems but also pose a serious threat to human health.In this study,a series of Al-doped modified metal-organic frameworks(Zr-Al-MOF)were prepared by solvothermal method,which achieved efficient removal of phosphate and arsenate in water.Due to the use of inexpensive Al salts,the material has a lower cost and is more economical.The molar ratio of metal salts,adsorption time,solution pH,initial concentration,temperature and coexisting anions were studied,and it was found that when the molar ratio of Zr:Al was 2,Zr-Al-MOF had the best adsorption performance for phosphate and arsenate,and the maximum adsorption capacity was 93.04 mg P/g and 173.83 mg As/g,respectively.It traps phosphate and arsenate at a fast reaction rate and can be recycled repeatedly.In addition,0.15 g/L of 2Zr-Al-MOF can effectively reduce the phosphate and arsenate content in the contaminated spring water samples of Yangzonghai Lake to the standard range of drinking water,which further confirms the application potential of 2Zr-Al-MOF.By FT-IR and XPS analysis,it was found that the adsorption mechanism was ligand exchange,electrostatic attraction and hydrogen bond formation.The theoretical calculation shows that the adsorption energy is negative,which indicates that 2Zr-Al-MOF is attractive to phosphate and arsenate,and the adsorption state is stable.The results show that 2Zr-Al-MOF is an effective phosphate and arsenate adsorbent and has broad application prospects in eutrophication water treatment.
基金financially supported by the Open Research Fund Program of the State Key Laboratory of Eco-hydraulics in Northwest Arid Region,Xi'an University of Technology(Grant No.2020KFKT-8)the Natural Science Foundation of China(No.52204046)+1 种基金the Natural Science Foundation of Shaanxi Province,China(No.2025 JC-YBMS-573)the Youth Innovation Team Research Program Project of Educational Commission of Shaanxi Province(No.23JP103)。
摘要Oily sludge,a hazardous by-product of the petroleum industry,poses significant environmental risks due to its elevated levels of hydrocarbons and heavy metals.As conventional disposal methods often lead to secondary pollution or inefficient resource recovery,this study investigates the synergistic pyrolysis of oily sludge with lignin to produce high-performance adsorbents for oily wastewater treatment.Thermogravimetric analyses demonstrated complementary properties and a synergistic copyrolysis effect between the two feedstocks.Kinetic analysis employing the Coats-Redfern method revealed that the co-pyrolysis of oily sludge and lignin significantly decreased the apparent activation energy while increasing the pre-exponential factor,confirming the lignin's catalytic role in enhancing pyrolysis efficiency.The optimal adsorbent,produced at an oily sludge-to-lignin mass ratio of 1:5,exhibited a specific surface area of 1324.5 m2/g,abundant micropores,and diverse surface functional groups,as confirmed by SEM and FT-IR analyses.Under optimized conditions—an adsorbent dosage of1.0 g/L,contact time of 40 min,and pH 7—this material effectively removed residual oil from synthetic oily wastewater and maintained over 70%removal efficiency after five regeneration cycles,highlighting its reusability.Finally,the chemical transformations of various components during the co-pyrolysis of oily sludge and biomass materials are elucidated.
基金supported by Yunnan Fundamental Research Projects(No.202301BE070001-056)Yunnan Major Scientific and Technological Projects(No.202202AG050019)+2 种基金the National Key Research and Development Program of China(No.2023YFC3906003)the Youth Innovation Promotion Association of the Chinese Academy of Sciences(No.2021044)Beijing Nova Program(No.2024072).
摘要A novel faujasite(FAU) type zeolitized ceramsite(FZC) was prepared via a novel three dimensional(3D) in-pore growth method.FZC is a centimeter sized spherical particle with a 3-dimensional radial morphology inside,with a specific surface area and pore volume 6 and 30 times that of the original ceramsite,respectively.The unique structure was constructed through electrostatic and polymerization interactions between hexadecyl trimethyl ammonium bromide(CTAB) micelles,ceramic pore walls and silicate aluminate ions,which could simultaneously improve adsorption capacity and mass transfer,endowing FZC with excellent heavy metal adsorption properties.FZC-50 could remove the majority of Cu and Zn from solution within shorter periods(73.3 % and 80.0 %of original ceramsite,respectively) with larger adsorption capacities(340 % and 370 % of original ceramsite,respectively).Theoretical analysis and regeneration experiments both indicate that the adsorption of Cu(Ⅱ) and Zn(Ⅱ) on FZC-50 is dominated by ion exchange.And the spent sorbent can be effectively regenerated by NaCl,and the cycle number is expected to be 33 and 26 times for Cu(Ⅱ) and Zn(Ⅱ) adsorption,respectively.This work proposed a novel synthesis route to construct a 3D multi-stage porous zeolite inside ceramsite,and opened up new ideas for the further development of zeolitized ceramsite.
基金financially supported by National Natural Science Foundation of China (Nos.52374271 and 52404290)Liaoning Province’ Xing Liao Ying Cai Program’ Outstanding Young Talents Project (No.XLYC2403010)+3 种基金Applied Basic Research Programs of Key Research and Development Program of Liaoning Province of China (No.2025JH2/101300041)Liaoning Provincial Engineering Research Center for High-Value Utilization of Magnesite (No.LMKK20240101)Research Fund Project of Liaoning Provincial Education Department (Nos.SYLUGXRC+12 and LJMKZ20220585)Program of China Scholarship Council (No.202506080127)。
摘要The development of efficient CO2 adsorbents is critical for achieving net-zero targets.MgO represents a promising solid adsorbent for CO2 capture,yet its limited specific surface area and insufficient active sites restrict its adsorption capacity under moderate temperature conditions.A rod-like anhydrous MgCO3 precursor was hydrothermally synthesized and calcined at 500℃ for 3 h to obtain porous MgO(184.9 m2g-1,0.38 cm3/g),which was then modified with 20% NaNO2(by mole) via impregnation.This adsorbent achieved an adsorption capacity of 12.6 mmol g-1after 120 min under a pure CO2 atmosphere at 325℃.Comprehensive characterization reveals that NaNO2 modification leads to the NaNO3 and Na2 CO3 formation on the MgO surface during calcination.The introduced NaNO3 effectively promotes oxygen vacancy formation,while the generated Na2 CO3 serves as heterogeneous nucleation sites,collectively reducing the reaction energy barrier and enhancing interfacial mass transfer.This synergistic effect facilitates the MgCO3 formation followed by its conversion to the thermodynamically more stable Na2Mg(CO3)2.Kinetic studies elucidate that adsorption is dominated by surface chemical reactions and diffusion mechanisms at different stages.These fundamental insights into the adsorption mechanisms of nitrite-modified MgO provide valuable guidance for the rational design of advanced MgO-based CO2 adsorbents with enhanced performance.