Heavy particulate matter (PM) pollution and high energy consumption are the bottlenecks of hydrometallurgy, especially in the electrolysis process. Therefore, an urgent need is to explore PM reduction methods with pro...Heavy particulate matter (PM) pollution and high energy consumption are the bottlenecks of hydrometallurgy, especially in the electrolysis process. Therefore, an urgent need is to explore PM reduction methods with production performance co-benefits. This study presents three PM reduction methods based on controlling operating parameters, i.e., lowering electrolyte temperature, H2SO4 concentration, and current density of the cathode. The optimized conditions were also investigated using the response surface methodology to balance the PM reduction effect and Zn production. The results showed that lowering electrolyte temperature is the most efficient, with an 89.0% reduction in the PM generation flux (GFPM). Reducing H2SO4 concentration led to the minimum side effects on the current efficiency of Zn deposition (CEZn) or power consumption (PC). With the premise of non-deteriorating CEZn and PC, GFPM can be reduced by 86.3% at the optimal condition (electrolyte temperature = 295 K, H2SO4 = 110 g/L, current density = 373 A/m^(2)). In addition, the reduction mechanism was elucidated by comprehensively analyzing bubble characteristics, electrochemical reactions, and surface tension. Results showed that lower electrolyte temperature inhibited the oxygen evolution reaction (OER) and compressed gas volume. Lower H2SO4 concentration inhibited the hydrogen evolution reaction (HER) and reduced electrolyte surface tension. Lower current density inhibited both OER and HER by decreasing the reaction current. The inhibited gas evolutions reduced the microbubbles’ number and size, thereby reducing GFPM. These results may provide energy-efficient PM reduction methods and theoretical hints of exploring cleaner PM reduction approaches for industrial electrolysis.展开更多
China has established the largest clean coal-fired power generation system in the world by accomplishing the technological transformation of coal-fired power plants(CFPPs)to achieve ultra-low emission.The potential fo...China has established the largest clean coal-fired power generation system in the world by accomplishing the technological transformation of coal-fired power plants(CFPPs)to achieve ultra-low emission.The potential for further particulate matter(PM)emission reduction to achieve near-zero emission for CFPPs has become a hotspot issue.In this study,PM emission from some ultra-low emission CFPPs adopting advanced air pollutant control technologies in China was reviewed.The results revealed that the average filterable particulate matter(FPM)concentration,measured as the total particulate matter(TPM)according to the current national monitoring standard,was(1.67±0.86)mg/m^(3),which could fully achieve the ultra-low emission standard for key regions(5 mg/m^(3)),but that achieving the near-zero emission standard was difficult(1 mg/m^(3)).However,the condensable particulate matter(CPM),with an average concentration of(1.06±1.28)mg/m^(3),was generally ignored during monitoring,which led to about 38.7%underestimation of the TPM.Even considering both FPM and CPM,the TPM emission from current CFPPs would contribute to less than 5%of atmospheric PM_(2.5) concentrations in the key cities and regions in China.Therefore,further reduction in FPM emission proposed by the near-zero emission plan of CFPPs may have less environmental benefit than emission control of other anthropogenic sources.However,it is suggested that the management of CPM emission should be strengthened,and a national standard for CPM emission monitoring based on the indirect dilution method should be established for CFPPs.Those measurements are helpful for optimal operation of air pollutant control devices and continuously promoting further emission reduction.展开更多
A spectrometer combining electrical mobility sizing and aerodynamic sizing was developed to measure aerosol size distributions in the range of 3 nm to 10 μm. It includes three instruments which cover different size r...A spectrometer combining electrical mobility sizing and aerodynamic sizing was developed to measure aerosol size distributions in the range of 3 nm to 10 μm. It includes three instruments which cover different size ranges (a nano scanning mobility particle sizer (NSMPS, 3 - 60 nm), a regular scanning mobility particle sizer (RSMPS, 40 - 700nm), and an aerodynamic particle sizer (APS, 550nm- 10 μm)). High voltage and sheath flow of the NSMPS and RSMPS were supplied using two home-built control boxes. A LabVIEW program was developed for spectrometer automatic operation. A linear inversion method was applied to correct particle multiple charging effects and to integrate data from the three instruments into a wide-range size distribution. Experi- ments were conducted to compare distributions in the overlap size ranges measured by three instruments. Good agreement between the NSMPS and RSMPS was achieved after correcting for the difference in counting efficiencies of the two particle counters. Aerodynamic size distribu- tions reported by the APS were converted to mobility size distributions by applying an effective density method. Distributions measured by the RSMPS and APS were consistent in the overlap size range of 550 - 700 nm. A full spectrum in the size range of 3nm to 10~tm was demonstrated by measuring aerosol generated using a mixture of different sized polystyrene latex spheres.展开更多
The reaction of alkenes with ozone has great effect on atmospheric oxidation,its transient species can produce OH radicals and contribute to the formation of secondary organic aerosols(SOA).In the present study,the re...The reaction of alkenes with ozone has great effect on atmospheric oxidation,its transient species can produce OH radicals and contribute to the formation of secondary organic aerosols(SOA).In the present study,the reaction of tetramethylethene(TME) with ozone was investigated using self-assembled low temperature matrix isolation system.The TME and ozone were co-deposited on a salt plate at 15 K,and then slowly warmed up the plate.The first transient species primary ozonide(POZ) was detected,indicating that the reaction followed Criegee mechanism.Then POZ began to decompose at 180 K.However,secondary ozonide(SOZ) was not observed according to Criegee mechanism.Probably,Criegee Intermediate(CI) did not react with inert carbonyl of acetone,but with remaining TME formed tetra-methyl epoxide(EPO).展开更多
基金supported by the National Natural Science Foundation of China(No.22106081)the Natural Science of Foundation of Shandong Province,China(No.ZR202103040646)+2 种基金the special fund of State Key Joint Laboratory of Environment Simulation and Pollution Control(China)(No.20K09ESPCT)the Major Basic Research Projects of Natural Science Foundation of Shandong Province(China)(No.ZR2020KE025)the Fundamental Research Funds for the Central Universities(China)(No.22120220166).
文摘Heavy particulate matter (PM) pollution and high energy consumption are the bottlenecks of hydrometallurgy, especially in the electrolysis process. Therefore, an urgent need is to explore PM reduction methods with production performance co-benefits. This study presents three PM reduction methods based on controlling operating parameters, i.e., lowering electrolyte temperature, H2SO4 concentration, and current density of the cathode. The optimized conditions were also investigated using the response surface methodology to balance the PM reduction effect and Zn production. The results showed that lowering electrolyte temperature is the most efficient, with an 89.0% reduction in the PM generation flux (GFPM). Reducing H2SO4 concentration led to the minimum side effects on the current efficiency of Zn deposition (CEZn) or power consumption (PC). With the premise of non-deteriorating CEZn and PC, GFPM can be reduced by 86.3% at the optimal condition (electrolyte temperature = 295 K, H2SO4 = 110 g/L, current density = 373 A/m^(2)). In addition, the reduction mechanism was elucidated by comprehensively analyzing bubble characteristics, electrochemical reactions, and surface tension. Results showed that lower electrolyte temperature inhibited the oxygen evolution reaction (OER) and compressed gas volume. Lower H2SO4 concentration inhibited the hydrogen evolution reaction (HER) and reduced electrolyte surface tension. Lower current density inhibited both OER and HER by decreasing the reaction current. The inhibited gas evolutions reduced the microbubbles’ number and size, thereby reducing GFPM. These results may provide energy-efficient PM reduction methods and theoretical hints of exploring cleaner PM reduction approaches for industrial electrolysis.
基金supported by the National Key Research and Development Project(No.2019YFC0214800)the Science and Technology Innovation Project of China Energy Investment Corporation Limited(No.51609225)Tsinghua-Foshan Innovation Special Fund(No.2020THFS0102)。
文摘China has established the largest clean coal-fired power generation system in the world by accomplishing the technological transformation of coal-fired power plants(CFPPs)to achieve ultra-low emission.The potential for further particulate matter(PM)emission reduction to achieve near-zero emission for CFPPs has become a hotspot issue.In this study,PM emission from some ultra-low emission CFPPs adopting advanced air pollutant control technologies in China was reviewed.The results revealed that the average filterable particulate matter(FPM)concentration,measured as the total particulate matter(TPM)according to the current national monitoring standard,was(1.67±0.86)mg/m^(3),which could fully achieve the ultra-low emission standard for key regions(5 mg/m^(3)),but that achieving the near-zero emission standard was difficult(1 mg/m^(3)).However,the condensable particulate matter(CPM),with an average concentration of(1.06±1.28)mg/m^(3),was generally ignored during monitoring,which led to about 38.7%underestimation of the TPM.Even considering both FPM and CPM,the TPM emission from current CFPPs would contribute to less than 5%of atmospheric PM_(2.5) concentrations in the key cities and regions in China.Therefore,further reduction in FPM emission proposed by the near-zero emission plan of CFPPs may have less environmental benefit than emission control of other anthropogenic sources.However,it is suggested that the management of CPM emission should be strengthened,and a national standard for CPM emission monitoring based on the indirect dilution method should be established for CFPPs.Those measurements are helpful for optimal operation of air pollutant control devices and continuously promoting further emission reduction.
基金We thank Dr. James Smith for his assistance on designing the control box and Ms. Zhiying Xie for her help on setting up the spectrometer. Financial supports from the National Natural Science Foundation of China (Grant Nos: 41227805, 21107060, 21190054 and 21221004), National Key Basic Research and Development Program of China (Grant No: 2013CB228505), and Beijing Natural Science Foundation (8122025) are acknowledged.
文摘A spectrometer combining electrical mobility sizing and aerodynamic sizing was developed to measure aerosol size distributions in the range of 3 nm to 10 μm. It includes three instruments which cover different size ranges (a nano scanning mobility particle sizer (NSMPS, 3 - 60 nm), a regular scanning mobility particle sizer (RSMPS, 40 - 700nm), and an aerodynamic particle sizer (APS, 550nm- 10 μm)). High voltage and sheath flow of the NSMPS and RSMPS were supplied using two home-built control boxes. A LabVIEW program was developed for spectrometer automatic operation. A linear inversion method was applied to correct particle multiple charging effects and to integrate data from the three instruments into a wide-range size distribution. Experi- ments were conducted to compare distributions in the overlap size ranges measured by three instruments. Good agreement between the NSMPS and RSMPS was achieved after correcting for the difference in counting efficiencies of the two particle counters. Aerodynamic size distribu- tions reported by the APS were converted to mobility size distributions by applying an effective density method. Distributions measured by the RSMPS and APS were consistent in the overlap size range of 550 - 700 nm. A full spectrum in the size range of 3nm to 10~tm was demonstrated by measuring aerosol generated using a mixture of different sized polystyrene latex spheres.
基金primarily supported by National Key R&D Program of China(No.2019YFC0214200)National Environmental Protection Public Welfare Industry Research Project(No.201509010)+1 种基金National Basic Science Research Program of Chinese Research Academy of Environmental Sciences(No.JY-21277132-201309406)the National Natural Science Foundation of China(No.21277132)
文摘The reaction of alkenes with ozone has great effect on atmospheric oxidation,its transient species can produce OH radicals and contribute to the formation of secondary organic aerosols(SOA).In the present study,the reaction of tetramethylethene(TME) with ozone was investigated using self-assembled low temperature matrix isolation system.The TME and ozone were co-deposited on a salt plate at 15 K,and then slowly warmed up the plate.The first transient species primary ozonide(POZ) was detected,indicating that the reaction followed Criegee mechanism.Then POZ began to decompose at 180 K.However,secondary ozonide(SOZ) was not observed according to Criegee mechanism.Probably,Criegee Intermediate(CI) did not react with inert carbonyl of acetone,but with remaining TME formed tetra-methyl epoxide(EPO).