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
In this work, phenol and oxalic acid(OA) degradation in an ozone and photocatalysis integrated process was intensively conducted with Fe^(3+)/TiO_2 catalyst. The ferrioxalate complex formed between Fe^(3+) and oxalate...In this work, phenol and oxalic acid(OA) degradation in an ozone and photocatalysis integrated process was intensively conducted with Fe^(3+)/TiO_2 catalyst. The ferrioxalate complex formed between Fe^(3+) and oxalate accelerated the removal of OA in the ozonation, photolysis and photocatalytic ozonation process, for its high reactivity with ozone and UV. Phenol was degraded in ozonation and photolysis with limited TOC removal rates, but much higher TOC removal was achieved in photocatalytic ozonation due to the generation of ·OH. The sequence of UV light and ozone in the sequential process also influences the TOC removal, and ozone is very powerful to oxidize intermediates catechol and hydroquinone to maleic acid. Fenton or photo-Fenton reactions only played a small part in Fe^(3+)/TiO_2catalyzed processes, because Fe^(3+) was greatly reduced but not regenerated in many cases.The synergetic effect was found to be highly related with the property of the target pollutants. Fe^(3+)/TiO_2 catalyzed system showed the highest ability to destroy organics, but the TiO_2 catalyzed system showed little higher synergy.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
A database-based strategy of candidate generation was proposed for molecular design of new de-phenol extractants following the idea of finding new applications of existing commercial compounds. The strategy has the ad...A database-based strategy of candidate generation was proposed for molecular design of new de-phenol extractants following the idea of finding new applications of existing commercial compounds. The strategy has the advantage that the environmental, safety and health risks of candidate compounds are known and controllable. In this work, the Existing Commercial Compounds(ECC) database and special combined search strategy were developed as the base for the proposed CAMD method following such idea, and molecules for phenol extraction used in coking wastewater treatment were selected from the ECC database. The candidate solvents cover the following categories: ketones, esters, ethers, alcohols, anhydrides and benzene compounds, which are consistent with the de-phenol extractants commonly used in the industry or experiment. The compounds with higher partition coefficient and selectivity than widely used methyl isobutyl ketone(MIBK) are mainly ketones. 26 obtained molecules show higher partition coefficient and selectivity than MIBK, which are suggested to be further investigated by experiment. Furthermore, analysis of these potential molecules may present the effective functional groups as the initial group set to generate new molecular structures of de-phenol extractants. The results show that the proposed method enables us to efficiently generate chemicals with benefits of less time, less economical cost, and known environmental impact as well.展开更多
Nanocomposites with synergistic effect are of great interest for their enhanced properties in a given application. Herein, we reported the high catalytic activity of Pt-containing Ag2S-noble metal nanocomposites in fo...Nanocomposites with synergistic effect are of great interest for their enhanced properties in a given application. Herein, we reported the high catalytic activity of Pt-containing Ag2S-noble metal nanocomposites in formic acid oxidation, which is a key reaction in direct formic acid fuel cell. The electrochemical measurements including voltammograms and chronoamperograms are used to characterize the catalytic property of Pt-containing nanocomposites for the oxidation of formic acid. In view of the limited literatures on using nanocomposites consisting of semiconductor and noble metals for catalyzing the reactions of polymer electrolyte membrane-based fuel cells, this study provides a helpful exploration for expanding the application of semiconductor-noble metal nanocomposites.展开更多
In this work, a new immobilization method based on dopamine(DA) self-polymerization was developed for laccase immobilization on magnetic nanoparticles(Fe_3O_4 NPs). To optimize the immobilization condition including r...In this work, a new immobilization method based on dopamine(DA) self-polymerization was developed for laccase immobilization on magnetic nanoparticles(Fe_3O_4 NPs). To optimize the immobilization condition including reaction pH, DA concentration and enzyme concentration, a central composite response surface method was applied. The optimal condition was determined as p H value of 5.92, laccase concentration of 0.25 mg mL^(-1) and DA concentration of 12.74 mg mL^(-1), under which a high enzyme activity recovery of 88.17% was obtained.By comparing with free laccase, the stabilities of immobilized laccase towards p H, thermostability, storage were enhanced significantly.Approximately 60% of relative activity for immobilized laccase was remained after being incubated for 6 h at 50℃, but the free laccase only remained 25%. After 40 days of storage at 4℃, the laccase immobilized by DA kept about 89% of its original activity, but the free laccase only retained 48%. After recycled 10 times, the relative activity of immobilized laccase still retained 70%. The immobilized laccase was then applied to catalyze the degradation of 4-chlorophenol(4-CP), 86% percentage of 4-CP was removed within 2 h. After degraded 10 times, the relative activity of immobilized laccase still remained 64% of its initial activity, which exhibits an excellent reusability and operational stability.展开更多
N-doped reduced graphene oxide quantum dots(N-rGQDs) have attracted more and more attention in efficient catalytic degradation of aqueous organic pollutants.However,the synthesis of N-rGQDs is generally a complex and ...N-doped reduced graphene oxide quantum dots(N-rGQDs) have attracted more and more attention in efficient catalytic degradation of aqueous organic pollutants.However,the synthesis of N-rGQDs is generally a complex and high energy required process for the reduction and N-doping steps.In this study,a facile and green fabrication approach of N-rGQDs is established,based on a metal-free Fenton reaction without additional energy-input.The N structures of N-rGQDs play a significant role in the promotion of their catalytic performance.The N-rGQDs with relatively high percentage of aromatic nitrogen(NAr-rGQDs) perform excellent catalytic activities,with which the degradation efficiency of pollutant is enhanced by 25 times.Density functional theory(DFT) calculation also indicates aromatic nitrogen structures with electron-rich sites are prone to transfer electron,presenting a key role in the catalytic reaction.This metal-free Fenton process provides a green and costeffective strategy for one-step fabrication of N-rGQDs with controllable features and potential environmental catalytic applications.展开更多
The sustainability of the coking industry is supported by reasonable production profit and environmental quality requirements.The traditional measures substantially increased the related costs for enterprises to reach...The sustainability of the coking industry is supported by reasonable production profit and environmental quality requirements.The traditional measures substantially increased the related costs for enterprises to reach standards.This paper aims to develop a comprehensive cost combined environmental impact assessment method that is necessary for the analysis of wastewater treatment systems.Typical three coking wastewater treatment processes in China were evaluated.Results showed that eutrophication dominantly contributed to the overall environmental effect.Improving effluent quality could significantly reduce the total environmental impact.In terms of an economic perspective,the price of raw materials was the main factor that affected the operating cost of comprehensive treatment.Based on subsystem analysis,the pretreatment stage accounted for the majority of environmental and cost burdens,respectively reaching 64%-78%and 64%-86%.Optimizing the pretreatment process by enhancing the efficiency of high concentration raw material recovery and substituting toxic raw materials for extractant could reduce the environmental impact and economic cost by 43.8%and 57%,respectively,which was an effective way to improve the potential performance of coking wastewater treatment plants(WWTPs).展开更多
The development of low-cost and efficient new mineral adsorbents has been a hot topic in recent years. In this study, Friedel's salt (FS:3CaO·A12O3 ·CaCl2 ·10H2O), a hexagonal layered inorganic abso...The development of low-cost and efficient new mineral adsorbents has been a hot topic in recent years. In this study, Friedel's salt (FS:3CaO·A12O3 ·CaCl2 ·10H2O), a hexagonal layered inorganic absorbent, was synthesized to remove Cd2+ from water. The adsorption process was simulated by Langmuir and Freundlich models. The adsorption mechanism was further analyzed with TEM, XRD, FT-IR analysis and monitoring of metal cations released and solution pH variation. The results indicated the adsorbent FS had an outstanding ability for Cd(Ⅱ) adsorption. The maximum adsorption capacity of the FS for Cd(Ⅱ) removal can reach up to 671.14 mg/g. The nearly equal numbers of Cd2+ adsorbed and Ca2+ released demonstrated that ion-exchange (both surface and inner) of the FS for Cd(Ⅱ) played an important role during the adsorption process. Furthermore, the surface of the FS after adsorption was microscopically disintegrated while the inner lamellar structure was almost unchanged. The behavior of Cd(Ⅱ) adsorption by FS was significantly affected by surface reactions. The mechanisms of Cd2+ adsorption by the FS mainly included surface complexation and surface precipitation. In the present study, the adsorption process was fitted better by the Langmuir isotherm model (R2 = 0.9999) than the Freundlich isotherm model (R2 = 0.8122). Finally, due to the high capacity for ion-exchange on the FS surface, FS is a promising layered inorganic adsorbent for the removal of Cd(Ⅱ) from water.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Supported by the Natural Science Foundation of Beijing City(8172043)the National Science Fund for Distinguished Young Scholars(51425405)National Natural Science Foundation of China(51378487)
文摘In this work, phenol and oxalic acid(OA) degradation in an ozone and photocatalysis integrated process was intensively conducted with Fe^(3+)/TiO_2 catalyst. The ferrioxalate complex formed between Fe^(3+) and oxalate accelerated the removal of OA in the ozonation, photolysis and photocatalytic ozonation process, for its high reactivity with ozone and UV. Phenol was degraded in ozonation and photolysis with limited TOC removal rates, but much higher TOC removal was achieved in photocatalytic ozonation due to the generation of ·OH. The sequence of UV light and ozone in the sequential process also influences the TOC removal, and ozone is very powerful to oxidize intermediates catechol and hydroquinone to maleic acid. Fenton or photo-Fenton reactions only played a small part in Fe^(3+)/TiO_2catalyzed processes, because Fe^(3+) was greatly reduced but not regenerated in many cases.The synergetic effect was found to be highly related with the property of the target pollutants. Fe^(3+)/TiO_2 catalyzed system showed the highest ability to destroy organics, but the TiO_2 catalyzed system showed little higher synergy.
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(Grant No.2156112001)National Basic Science Data Sharing Service Project(DKA2017-12-02-05)
文摘A database-based strategy of candidate generation was proposed for molecular design of new de-phenol extractants following the idea of finding new applications of existing commercial compounds. The strategy has the advantage that the environmental, safety and health risks of candidate compounds are known and controllable. In this work, the Existing Commercial Compounds(ECC) database and special combined search strategy were developed as the base for the proposed CAMD method following such idea, and molecules for phenol extraction used in coking wastewater treatment were selected from the ECC database. The candidate solvents cover the following categories: ketones, esters, ethers, alcohols, anhydrides and benzene compounds, which are consistent with the de-phenol extractants commonly used in the industry or experiment. The compounds with higher partition coefficient and selectivity than widely used methyl isobutyl ketone(MIBK) are mainly ketones. 26 obtained molecules show higher partition coefficient and selectivity than MIBK, which are suggested to be further investigated by experiment. Furthermore, analysis of these potential molecules may present the effective functional groups as the initial group set to generate new molecular structures of de-phenol extractants. The results show that the proposed method enables us to efficiently generate chemicals with benefits of less time, less economical cost, and known environmental impact as well.
基金Financial support from the 100 Talents Program of the Chinese Academy of Sciences, National Natural Science Foundation of China (No.: 21173226, 21376247)State Key Laboratory of Multiphase Complex Systems, Institute of Process Engineering, Chinese Academy of Sciences (MPCS-2011-D-08, MPCS-2010C-02)
文摘Nanocomposites with synergistic effect are of great interest for their enhanced properties in a given application. Herein, we reported the high catalytic activity of Pt-containing Ag2S-noble metal nanocomposites in formic acid oxidation, which is a key reaction in direct formic acid fuel cell. The electrochemical measurements including voltammograms and chronoamperograms are used to characterize the catalytic property of Pt-containing nanocomposites for the oxidation of formic acid. In view of the limited literatures on using nanocomposites consisting of semiconductor and noble metals for catalyzing the reactions of polymer electrolyte membrane-based fuel cells, this study provides a helpful exploration for expanding the application of semiconductor-noble metal nanocomposites.
基金support from the National Natural Science Foundation of China(Grant Nos.51378487,51425405,21376249,21336010)Youth Innovation Promotion Association,CAS(2014037)973 Program(2013CB733604)
文摘In this work, a new immobilization method based on dopamine(DA) self-polymerization was developed for laccase immobilization on magnetic nanoparticles(Fe_3O_4 NPs). To optimize the immobilization condition including reaction pH, DA concentration and enzyme concentration, a central composite response surface method was applied. The optimal condition was determined as p H value of 5.92, laccase concentration of 0.25 mg mL^(-1) and DA concentration of 12.74 mg mL^(-1), under which a high enzyme activity recovery of 88.17% was obtained.By comparing with free laccase, the stabilities of immobilized laccase towards p H, thermostability, storage were enhanced significantly.Approximately 60% of relative activity for immobilized laccase was remained after being incubated for 6 h at 50℃, but the free laccase only remained 25%. After 40 days of storage at 4℃, the laccase immobilized by DA kept about 89% of its original activity, but the free laccase only retained 48%. After recycled 10 times, the relative activity of immobilized laccase still retained 70%. The immobilized laccase was then applied to catalyze the degradation of 4-chlorophenol(4-CP), 86% percentage of 4-CP was removed within 2 h. After degraded 10 times, the relative activity of immobilized laccase still remained 64% of its initial activity, which exhibits an excellent reusability and operational stability.
基金funding by National Natural Science Foundation of China (No. 51978643)Youth Innovation Promotion Association of CAS (Y201814)The National Youth Talent Support Program of China。
文摘N-doped reduced graphene oxide quantum dots(N-rGQDs) have attracted more and more attention in efficient catalytic degradation of aqueous organic pollutants.However,the synthesis of N-rGQDs is generally a complex and high energy required process for the reduction and N-doping steps.In this study,a facile and green fabrication approach of N-rGQDs is established,based on a metal-free Fenton reaction without additional energy-input.The N structures of N-rGQDs play a significant role in the promotion of their catalytic performance.The N-rGQDs with relatively high percentage of aromatic nitrogen(NAr-rGQDs) perform excellent catalytic activities,with which the degradation efficiency of pollutant is enhanced by 25 times.Density functional theory(DFT) calculation also indicates aromatic nitrogen structures with electron-rich sites are prone to transfer electron,presenting a key role in the catalytic reaction.This metal-free Fenton process provides a green and costeffective strategy for one-step fabrication of N-rGQDs with controllable features and potential environmental catalytic applications.
基金The authors acknowledge financial support on this research from the ＂1000 talents program＂ of China （Zhi Sun）, and the National Natural Science Foundation of China （51425405）. This research was also supported by the National Science-Technology Support Program （2015 BAB02B05）.
基金We are very grateful to the National Science Foundation （CBET- 0967536） and the National Natural Science Foundation of China （2156112001）, which have contributed significantly to the completion of this research.
基金funding by the National Natural Science Foundation of China(No.51978643)Strategic Priority Research Program of the Chinese Academy of Sciences(No.XDA21021102)+2 种基金14th Five-year Informatization Plan of Chinese Academy of Sciences,Construction of Scientific Data Center System(WX145XQ07-12)Youth Innovation Promotion Association,CAS(Y201814)the National Youth Talent Support Program of China
文摘The sustainability of the coking industry is supported by reasonable production profit and environmental quality requirements.The traditional measures substantially increased the related costs for enterprises to reach standards.This paper aims to develop a comprehensive cost combined environmental impact assessment method that is necessary for the analysis of wastewater treatment systems.Typical three coking wastewater treatment processes in China were evaluated.Results showed that eutrophication dominantly contributed to the overall environmental effect.Improving effluent quality could significantly reduce the total environmental impact.In terms of an economic perspective,the price of raw materials was the main factor that affected the operating cost of comprehensive treatment.Based on subsystem analysis,the pretreatment stage accounted for the majority of environmental and cost burdens,respectively reaching 64%-78%and 64%-86%.Optimizing the pretreatment process by enhancing the efficiency of high concentration raw material recovery and substituting toxic raw materials for extractant could reduce the environmental impact and economic cost by 43.8%and 57%,respectively,which was an effective way to improve the potential performance of coking wastewater treatment plants(WWTPs).
基金supported by the National Natural Science Foundation of China (No. 51108441, 51178446)
文摘The development of low-cost and efficient new mineral adsorbents has been a hot topic in recent years. In this study, Friedel's salt (FS:3CaO·A12O3 ·CaCl2 ·10H2O), a hexagonal layered inorganic absorbent, was synthesized to remove Cd2+ from water. The adsorption process was simulated by Langmuir and Freundlich models. The adsorption mechanism was further analyzed with TEM, XRD, FT-IR analysis and monitoring of metal cations released and solution pH variation. The results indicated the adsorbent FS had an outstanding ability for Cd(Ⅱ) adsorption. The maximum adsorption capacity of the FS for Cd(Ⅱ) removal can reach up to 671.14 mg/g. The nearly equal numbers of Cd2+ adsorbed and Ca2+ released demonstrated that ion-exchange (both surface and inner) of the FS for Cd(Ⅱ) played an important role during the adsorption process. Furthermore, the surface of the FS after adsorption was microscopically disintegrated while the inner lamellar structure was almost unchanged. The behavior of Cd(Ⅱ) adsorption by FS was significantly affected by surface reactions. The mechanisms of Cd2+ adsorption by the FS mainly included surface complexation and surface precipitation. In the present study, the adsorption process was fitted better by the Langmuir isotherm model (R2 = 0.9999) than the Freundlich isotherm model (R2 = 0.8122). Finally, due to the high capacity for ion-exchange on the FS surface, FS is a promising layered inorganic adsorbent for the removal of Cd(Ⅱ) from water.
