In this research,a methodology named whole-process pollution control(WPPC)is demonstrated that improves the effectiveness of process optimization.This methodology considers waste/emission treatment as a step of the wh...In this research,a methodology named whole-process pollution control(WPPC)is demonstrated that improves the effectiveness of process optimization.This methodology considers waste/emission treatment as a step of the whole production process with respect to the minimization of cost and environmental impact for the whole process.The following procedures are introduced in a WPPC process optimization:①a material and energy flow investigation and optimization based on a systematic understanding of the distribution and physiochemical properties of potential pollutants;②a process optimization to increase the utilization efficiency of different elements and minimize pollutant emissions;and③an evaluation to reveal the effectiveness of the optimization strategies.The production of ammonium paratungstate was chosen for the case study.Two factors of the different optimization schemes-namely the cost-effectiveness factor and the environmental impact indicator-were evaluated and compared.This research demonstrates that by considering the nature of potential pollutants,technological innovations,economic viability,environmental impacts,and regulation requirements,WPPC can efficiently optimize a metal production process.展开更多
Prevention of mechanical and finally electrochemical failures of lithium batteries is a critical aspect to be considered during their design and performance, especially for those with high specific capacities. Interna...Prevention of mechanical and finally electrochemical failures of lithium batteries is a critical aspect to be considered during their design and performance, especially for those with high specific capacities. Internal failure is observed as one of the most serious factors, including loss of electrode materials, structure deformation and dendrite growth. It usually incubates from atomic/molecular level and progressively aggravates along with lithiation. Understanding the internal failure is of great importance for developing solutions of failure prevention and advanced anode materials. In this research, different internal failure processes of anode materials for lithium batteries are discussed. The progress on observation technologies of the anode failure is further summarized in order to understand their mechanisms of internal failure. On top of them, this review aims to summarize innovative methods to investigate the anode failure mechanisms and to gain new insights to develop advanced and stable anodes for lithium batteries.展开更多
This work presented the results of tungstic precipitation from Na_2WO_4-Na_2SO_4-H_2O system at 293.15 K, with which the Pitzer parameters of β_(Na2WO4)^(0) and β(Na2WO4)^(1) were determined from Pitzer equation by...This work presented the results of tungstic precipitation from Na_2WO_4-Na_2SO_4-H_2O system at 293.15 K, with which the Pitzer parameters of β_(Na2WO4)^(0) and β(Na2WO4)^(1) were determined from Pitzer equation by regression. Thus the mean ionic activity coefficients of sodium tungstate were calculated. The obtained β_(Na2WO4)^(0) and β(Na2WO4)^(1) were substituted as fixed values in extraction modeling from Na_2WO_4-H_2SO_4-H_2O system by primary amine(N1923) in toluene as diluent. Meanwhile the activity coefficient expressions in organic phase were varied based on Pitzer theory that the interaction term for the solvent should not be included. The Pitzer parameters for organic phase were re-regressed in order to make the model more accurate. The average absolute relative deviation(AARD) for calculated and experimental molality of WO_4～(2-) in aqueous phase was 5.24%. The results showed that the model can not only correlate but also predict the liquid-liquid equilibrium(LLE) data.展开更多
The optimization-based design of solvent mixtures used for phenolic wastewater treatment was investigated in this work.A nonlinear programming(NLP)model was formulated based on the concepts of computer-aid molecule de...The optimization-based design of solvent mixtures used for phenolic wastewater treatment was investigated in this work.A nonlinear programming(NLP)model was formulated based on the concepts of computer-aid molecule design(Computer-Aided Molecular Design,CAMD)to select solvent mixtures with the best extraction performance considering the constraints of extraction process and the environmental impact.Due to the complexity of the NLP model,multi-start method was adopted to solve this problem in order to get near global optimal solution.The results of the calculations suggested that the optimal mixture consisted of 70.1%n-octanol and 29.9%2-octanone(molar fraction).The 119 sets of experimental results showed that the extraction ability of the optimal solvent mixture identified by CAMD technique was among the top 6 sets compared to the experiment results.The results suggested that the developed NLP model could be able to screen the optimal solvent mixture in phenolic wastewater treatment.展开更多
A series of Ni/HZSM-5 and Ni/HIM-5 bi-functional catalysts were synthesized and applied to the aqueous-phase hydrodeoxygenation(HDO)of phenol.The Ni dispersibility and particle sizes were shown to be directly related ...A series of Ni/HZSM-5 and Ni/HIM-5 bi-functional catalysts were synthesized and applied to the aqueous-phase hydrodeoxygenation(HDO)of phenol.The Ni dispersibility and particle sizes were shown to be directly related to the porosity and crystal sizes of the parent zeolites,which further influenced the catalytic performances.The large pores and small crystal sizes of the parent zeolites were beneficial for dispersing Ni and forming small Ni particles,and the corresponding Ni/zeolite catalyst exhibited a higher phenol conversion and selectivity towards hydrocarbons.Importantly,the Ni/HIM-5 bi-functional catalyst exhibited a high activity(98.3%)and high selectivity for hydrocarbons(98.8%)when heated at 220°C for 1 h and is thus a new potential catalyst for the HDO of phenolics to form hydrocarbons in the aqueous phase.展开更多
In this work,liquid-liquid extraction of phenol from aqueous solutions using primary amine Primene JMT(Primene®JM-T)was investigated.The extraction capability of Primene®JM-T with different diluents,includin...In this work,liquid-liquid extraction of phenol from aqueous solutions using primary amine Primene JMT(Primene®JM-T)was investigated.The extraction capability of Primene®JM-T with different diluents,including 3-heptanone,sulfonated kerosene,methyl isobutyl ketone,n-octanol,toluene and petroleum ether was studied.The experimental results indicated that the distribution coefficient of phenol extracted using Primene®JM-T that was diluted in 3-heptanone could reach 101.74 under the pH of 9.2.Moreover,the extraction reaction was exothermic(enthalpy change for the extraction reaction(DrHm)was21.03 kJ/mol).High temperature showed a negative effect on the extraction of phenol.The results also showed that adding mineral salt was conducive to the extraction process,and the extraction effi-ciency fell in the descending order of:(NH_(4))_(2)SO_(4)>NaCl>NH_(4)Cl.Two empirical correlations were put forward to quantitatively describe the salting effect.Furthermore,the equilibrium constants of phenol extraction using Primene®JM-T were calculated to be 78.2 L/mol.The phenol was extracted using Primene®JM-T with the possible stoichiometric formula of:[RNH_(3)^(+),PhOH]_(org),where R represents the alkyl group of the amine.展开更多
The aqueous metal species with similar chemical properties are usually extracted together,limiting deep separation for high-purity metal.However,rare attention has been paid to metal speciation characterization and tr...The aqueous metal species with similar chemical properties are usually extracted together,limiting deep separation for high-purity metal.However,rare attention has been paid to metal speciation characterization and transformation during separation.Herein,the hydrolysis evolution of polymeric metal species was investigated systematically by electrospray ionization time-of-flight mass spectrometry(ESI-TOF-MS).The transformation evolutions were visualized with respect to characteristic vanadium species(V_(1),V_(2),V_(3),V_(4) and V_(10)),chromium species(Cr_(1) and Cr_(2)),tungsten(W_(1),W_(2),W_(4),W_(6) and W_(10))and molybdenum(Mo_(1),Mo_(2) and Mo_(4))species.The key characteristics(such as specfic pHs and concentrations)for speciation variation were revealed.The polymerization behavior of several transition metals can be semiquantitative characterized by this strategy.The sufficient speciation transformation provides a solid base for metal speciation chemistry,and guides further development of high-purity metal recovery.展开更多
基金The authors acknowledge financial support for this research from the National Key Research and Development Program of China(2017YFB0403300 and 2017YFB043305)the National Natural Science Foundation of China(51425405 and 51874269),the National Science-Technology Support Plan Projects(2015BAB02B05)the Youth Innovation Promotion Association of Chinese Academy of Sciences(2014037).Zhi Sun acknowledges financial support from the National Youth Thousand Talents Program.The authors acknowledge constructive suggestions from Prof.Jianxin Yang.
文摘In this research,a methodology named whole-process pollution control(WPPC)is demonstrated that improves the effectiveness of process optimization.This methodology considers waste/emission treatment as a step of the whole production process with respect to the minimization of cost and environmental impact for the whole process.The following procedures are introduced in a WPPC process optimization:①a material and energy flow investigation and optimization based on a systematic understanding of the distribution and physiochemical properties of potential pollutants;②a process optimization to increase the utilization efficiency of different elements and minimize pollutant emissions;and③an evaluation to reveal the effectiveness of the optimization strategies.The production of ammonium paratungstate was chosen for the case study.Two factors of the different optimization schemes-namely the cost-effectiveness factor and the environmental impact indicator-were evaluated and compared.This research demonstrates that by considering the nature of potential pollutants,technological innovations,economic viability,environmental impacts,and regulation requirements,WPPC can efficiently optimize a metal production process.
基金the financial support on this research from National Key Research and Development Program of China (2017YFB0403300/2017YFB043305)National Natural Science Foundation of China under Grant No. 51425405+1 种基金Key Program of Chinese Academy of Sciences KFZD-SW-3151000 Talents Program of China (Z.S.)
文摘Prevention of mechanical and finally electrochemical failures of lithium batteries is a critical aspect to be considered during their design and performance, especially for those with high specific capacities. Internal failure is observed as one of the most serious factors, including loss of electrode materials, structure deformation and dendrite growth. It usually incubates from atomic/molecular level and progressively aggravates along with lithiation. Understanding the internal failure is of great importance for developing solutions of failure prevention and advanced anode materials. In this research, different internal failure processes of anode materials for lithium batteries are discussed. The progress on observation technologies of the anode failure is further summarized in order to understand their mechanisms of internal failure. On top of them, this review aims to summarize innovative methods to investigate the anode failure mechanisms and to gain new insights to develop advanced and stable anodes for lithium batteries.
基金supported by the National Natural Science Foundation of China(21206168,51178446)
文摘This work presented the results of tungstic precipitation from Na_2WO_4-Na_2SO_4-H_2O system at 293.15 K, with which the Pitzer parameters of β_(Na2WO4)^(0) and β(Na2WO4)^(1) were determined from Pitzer equation by regression. Thus the mean ionic activity coefficients of sodium tungstate were calculated. The obtained β_(Na2WO4)^(0) and β(Na2WO4)^(1) were substituted as fixed values in extraction modeling from Na_2WO_4-H_2SO_4-H_2O system by primary amine(N1923) in toluene as diluent. Meanwhile the activity coefficient expressions in organic phase were varied based on Pitzer theory that the interaction term for the solvent should not be included. The Pitzer parameters for organic phase were re-regressed in order to make the model more accurate. The average absolute relative deviation(AARD) for calculated and experimental molality of WO_4～(2-) in aqueous phase was 5.24%. The results showed that the model can not only correlate but also predict the liquid-liquid equilibrium(LLE) data.
基金the National Natural Science Foundation(Grant 51178446).
文摘The optimization-based design of solvent mixtures used for phenolic wastewater treatment was investigated in this work.A nonlinear programming(NLP)model was formulated based on the concepts of computer-aid molecule design(Computer-Aided Molecular Design,CAMD)to select solvent mixtures with the best extraction performance considering the constraints of extraction process and the environmental impact.Due to the complexity of the NLP model,multi-start method was adopted to solve this problem in order to get near global optimal solution.The results of the calculations suggested that the optimal mixture consisted of 70.1%n-octanol and 29.9%2-octanone(molar fraction).The 119 sets of experimental results showed that the extraction ability of the optimal solvent mixture identified by CAMD technique was among the top 6 sets compared to the experiment results.The results suggested that the developed NLP model could be able to screen the optimal solvent mixture in phenolic wastewater treatment.
基金This work was supported by the National Natural Science Foundation of China(Grant No.21908225)the National Key Research and Development Program of China(Grant No.2016YFB0600505)Youth Innovation Promotion Association,CAS(2014037).
文摘A series of Ni/HZSM-5 and Ni/HIM-5 bi-functional catalysts were synthesized and applied to the aqueous-phase hydrodeoxygenation(HDO)of phenol.The Ni dispersibility and particle sizes were shown to be directly related to the porosity and crystal sizes of the parent zeolites,which further influenced the catalytic performances.The large pores and small crystal sizes of the parent zeolites were beneficial for dispersing Ni and forming small Ni particles,and the corresponding Ni/zeolite catalyst exhibited a higher phenol conversion and selectivity towards hydrocarbons.Importantly,the Ni/HIM-5 bi-functional catalyst exhibited a high activity(98.3%)and high selectivity for hydrocarbons(98.8%)when heated at 220°C for 1 h and is thus a new potential catalyst for the HDO of phenolics to form hydrocarbons in the aqueous phase.
基金the Strategic Priority Research Program of the Chinese Academy of Sciences(XDA21021102).
文摘In this work,liquid-liquid extraction of phenol from aqueous solutions using primary amine Primene JMT(Primene®JM-T)was investigated.The extraction capability of Primene®JM-T with different diluents,including 3-heptanone,sulfonated kerosene,methyl isobutyl ketone,n-octanol,toluene and petroleum ether was studied.The experimental results indicated that the distribution coefficient of phenol extracted using Primene®JM-T that was diluted in 3-heptanone could reach 101.74 under the pH of 9.2.Moreover,the extraction reaction was exothermic(enthalpy change for the extraction reaction(DrHm)was21.03 kJ/mol).High temperature showed a negative effect on the extraction of phenol.The results also showed that adding mineral salt was conducive to the extraction process,and the extraction effi-ciency fell in the descending order of:(NH_(4))_(2)SO_(4)>NaCl>NH_(4)Cl.Two empirical correlations were put forward to quantitatively describe the salting effect.Furthermore,the equilibrium constants of phenol extraction using Primene®JM-T were calculated to be 78.2 L/mol.The phenol was extracted using Primene®JM-T with the possible stoichiometric formula of:[RNH_(3)^(+),PhOH]_(org),where R represents the alkyl group of the amine.
基金supported by China Postdoctoral Science Foundation(No.2020M670459,2020T130655)National Natural Science Foundation of China(No.22008248 and 51934006).
文摘The aqueous metal species with similar chemical properties are usually extracted together,limiting deep separation for high-purity metal.However,rare attention has been paid to metal speciation characterization and transformation during separation.Herein,the hydrolysis evolution of polymeric metal species was investigated systematically by electrospray ionization time-of-flight mass spectrometry(ESI-TOF-MS).The transformation evolutions were visualized with respect to characteristic vanadium species(V_(1),V_(2),V_(3),V_(4) and V_(10)),chromium species(Cr_(1) and Cr_(2)),tungsten(W_(1),W_(2),W_(4),W_(6) and W_(10))and molybdenum(Mo_(1),Mo_(2) and Mo_(4))species.The key characteristics(such as specfic pHs and concentrations)for speciation variation were revealed.The polymerization behavior of several transition metals can be semiquantitative characterized by this strategy.The sufficient speciation transformation provides a solid base for metal speciation chemistry,and guides further development of high-purity metal recovery.
