Marine sediment microbial fuel cell(MSMFCs)can be utilized as a long lasting power source to drive small instruments to work for long time on ocean floor and its higher power has a significant meaning for practical ap...Marine sediment microbial fuel cell(MSMFCs)can be utilized as a long lasting power source to drive small instruments to work for long time on ocean floor and its higher power has a significant meaning for practical application.Anode modification can greatly improve the performance of MSMFCs.Herein,humic acid(HA)and humic acid-iron ion complex(HA-Fe)were used to modify the anode for constructing a better MSMFCs.The results indicated that HA-Fe modified anode,better than HA modification,significantly improved the MSMFCs cell power output.The maximum power density of HA-Fe modified MSMFCs is 165.3 mW m−2,which are 6.5-folds of blank MSMFCs.The number of microorganisms on anode,redox activity,and relative kinetic activity were 1.8-,6.1-,and 13.1-folds of blank MSMFCs,respectively.The MSMFCs improvement would be attributed to the electron transfer media of HA and the valence conversion of Fe ions.A synergistic interaction between the naturally occurring HA and Fe ions on the anodic surface in marine sediments would make the modified anodes have‘renewable’characteristics,which is beneficial for the MSMFCs to maintain its long-term higher power.展开更多
Iron is a vital micronutrient for growth of bloom-forming Microcystis aeruginosa and competition with other algae,and its availability is affected by humic acid.The effect of iron and humic acid on growth and competit...Iron is a vital micronutrient for growth of bloom-forming Microcystis aeruginosa and competition with other algae,and its availability is affected by humic acid.The effect of iron and humic acid on growth and competition between M.aeruginosa and Scenedesmus obliquus was assessed.The results showed the growth of M.aeruginosa and S.obliquus in mono-cultures was inhibited by humic acid at low iron concentrations(0.01 mg/L);the maximum inhibition ratios were 67.84%and 38.31%,respectively.The inhibition of humic acid on the two species was significantly alleviated when iron concentrations were 1.00 mg/L,with the maximum inhibition rate reduced to 5.82%for M.aeruginosa and to 23.06%for S.obliquus.S.obliquus was the dominant species in mixed cultures,and the mutual inhibition between M.aeruginosa and S.obliquus at low iron concentration was greater than that at high iron concentration.The inhibition of S.obliquus on M.aeruginosa was reduced at low iron concentrations;it increased at high iron concentrations,as concentrations of humic acid rose.展开更多
Dissimilatory iron reduction(DIR)coupled with carbon cycling is increasingly being recognized as an influential process in freshwater wetland soils and sediments.The role of DIR in organic matter(OM)mineralization,how...Dissimilatory iron reduction(DIR)coupled with carbon cycling is increasingly being recognized as an influential process in freshwater wetland soils and sediments.The role of DIR in organic matter(OM)mineralization,however,is still largely unknown in lake sediment environments.In this study,we clarified rates and pathways of OM mineralization in two shallow lakes with seasonal hydrological connectivity and different eutrophic situations.We found that in comparison with the domination of DIR(55%)for OM mineralization in Lake Xiaoxingkai,the contribution of methanogenesis was much higher(68%)in its connected lake(Lake Xingkai).The differences in rates and pathways of sediment OM mineralization between the two lakes were attributed to higher concentrations of carbonate associated iron oxides(Fecarb)in Lake Xiaoxingkai compared to Lake Xingkai(P=0.002),due to better deposition mixing,more contributions of terrigenous detrital materials,and higher OM content in Lake Xiaoxingkai.Results of structural equation modeling showed that Fecarb and total iron content(TFe)regulated 25%of DIR in Lake Xiaoxingkai and 76%in Lake Xingkai,accompanied by a negative effect of TFe on methanogenesis in Lake Xingkai.The relative abundance and diversity of Fe-reducing bacteria were significantly different between the two lakes,and showed a weak effect on sediment OM mineralization.Our findings emphasize the role of iron minerals and geochemical characterizations in regulating rates and pathways of OM mineralization,and deepen the understanding of carbon cycling in lake sediments.展开更多
Transformation of polychlorinated biphenyls (PCBs) by zero-valent iron represents one of the latest innovative technologies for environmental remediation. The dechlorination of 4-chlorobiphenyl (4-C1BP) by nanosca...Transformation of polychlorinated biphenyls (PCBs) by zero-valent iron represents one of the latest innovative technologies for environmental remediation. The dechlorination of 4-chlorobiphenyl (4-C1BP) by nanoscale zero-valent iron (NZVI) in the presence of humic acid or metal ions was investigated. The results showed that the dechlorination of 4-C1BP by NZVI increased with decreased solution pH. When the initial pH value was 4.0, 5.5, 6.8, and 9.0, the de.chlorination efficiencies of 4-CIBP after 48 hr were 53.8%, 47.8%, 35.7%, and 35.6%, respectively. The presence of humic acid inhibited the reduction of 4-CIBP in the first 4 hi', and then significantly accelerated the dechlorination by reaching 86.3% in 48 hr. Divalent metal ions, Co2+, Cu2+, and Ni2+, were reduced and formed bimetals with NZVI, thereby enhanced the dechlorination of 4-CIBP. The dechlorination percentages of 4-CIBP in the presence of 0.1 mmol/L Co2~, Cuz~ and Niz~ were 66.1%, 66.0% and 64.6% in 48 hr, and then increased to 67.9%, 71.3% and 73.5%, after 96 hr respectively. The dechlorination kinetics of 4-C1BP by the NZVI in all cases followed pseudo-first order model. The results provide a basis for better understanding of the dechlorination mechanisms of PCBs in real environment.展开更多
A method of size exclusion chromatography coupled with ultraviolet spectrophotometry and off-line graphite furnace atomic absorption spectrometry was developed to assess the complexation properties of iron(Fe) and h...A method of size exclusion chromatography coupled with ultraviolet spectrophotometry and off-line graphite furnace atomic absorption spectrometry was developed to assess the complexation properties of iron(Fe) and humic acid(HA) in a water environment. The factors affecting the complexation of Fe and HA, such as ionic strength, pH, temperature and UV radiation, were investigated. The Fe–HA complex residence time was also studied. Experimental results showed that pH could influence the deprotonation of HA and hydrolysis of Fe, and thus affected the complexation of Fe and HA. The complexation was greatly disrupted by the presence of NaCl. Temperature had some influence on the complexation. The yield of Fe–HA complexes showed a small decrease at high levels of UV radiation, but the effect of UV radiation on Fe–HA complex formation at natural levels could be neglected. It took about 10 hr for the complexation to reach equilibrium, and the Fe–HA complex residence time was about 20 hr.Complexation of Fe and HA reached a maximum level under the conditions of pH 6, very low ionic strength, in the dark and at a water temperature of about 25°C, for 10 hr. It was suggested that the Fe–HA complex could form mainly in freshwater bodies and reach high levels in the warm season with mild sunlight radiation. With changing environmental parameters, such as at lower temperature in winter or higher pH and ionic strength in an estuary, the concentration of the Fe–HA complex would decrease.展开更多
The phosphorus(P) fraction distribution and formation mechanism in the supernatant after P adsorption onto iron oxides and iron oxide-humic acid(HA) complexes were analyzed using the ultrafiltration method in this...The phosphorus(P) fraction distribution and formation mechanism in the supernatant after P adsorption onto iron oxides and iron oxide-humic acid(HA) complexes were analyzed using the ultrafiltration method in this study.With an initial P concentration of 20 mg/L(I =0.01 mol/L and pH = 7),it was shown that the colloid(1 kDa-0.45 μm) component of P accounted for 10.6%,11.6%,6.5%,and 4.0%of remaining total P concentration in the supernatant after P adsorption onto ferrihydrite(FH),goethite(GE),ferrihydrite-humic acid complex(FH-HA),goethite-humic acid complex(GE-HA),respectively.The 〈1 kDa component of P was still the predominant fraction in the supernatant,and underestimated colloidal P accounted for 2.2%,55.1%,45.5%,and 38.7%of P adsorption onto the solid surface of FH,FH-HA,GE and GE-HA,respectively.Thus,the colloid P could not be neglected.Notably,it could be interpreted that Fe3+ hydrolysis from the adsorbents followed by the formation of colloidal hydrous ferric oxide aggregates was the main mechanism for the formation of the colloid P in the supernatant.And colloidal adsorbent particles co-existing in the supernatant were another important reason for it.Additionally,dissolve organic matter dissolved from iron oxide-HA complexes could occupy large adsorption sites of colloidal iron causing less colloid P in the supernatant.Ultimately,we believe that the findings can provide a new way to deeply interpret the geochemical cycling of P,even when considering other contaminants such as organic pollutants,heavy metal ions,and arsenate at the sediment/soil-water interface in the real environment.展开更多
We reported solvent-free and recoverable heterogeneous iron functionalised imidazolium-based ionic liquid for the reduction of nitroarene derivatives in the presence of formic acid under greener conditions.Additionall...We reported solvent-free and recoverable heterogeneous iron functionalised imidazolium-based ionic liquid for the reduction of nitroarene derivatives in the presence of formic acid under greener conditions.Additionally,the experimental result shows that the iron complex could be an extremely resourceful,high rate and reusable catalyst for a different nitroarene substrate.展开更多
A modified humic acid(MHA) binder was tested as a substitute for bentonite to prepare qualified specularite pellets. The results show that there is stronger chemisorption between organic functional groups in MHA binde...A modified humic acid(MHA) binder was tested as a substitute for bentonite to prepare qualified specularite pellets. The results show that there is stronger chemisorption between organic functional groups in MHA binder molecular and specularite particles, improving the green pellet strength. MHA binder has obvious effect on the strength and microstructure of preheated pellets due to the thermal decomposition of organic matters in MHA binder. Appropriately increasing preheating temperature or time can eliminate the adverse impact of organic matters on the preheated pellet strength. Compared with the bentonite pellets, the roasted pellets with MHA binder have a more compact microstructure, and the recrystallization of the Fe2O3 crystal grains is better.Consequently, under optimal conditions, 0.75%(mass fraction) MHA binder pellets have equal or better pellet strengths and contain1.06% more total iron than 2 % bentonite pellets. The testing results indicate that MHA binder is a promising and effective alternative to bentonite for the specularite pellets.展开更多
基金supported by the National Natural Science Foundation of China(No.22075262).
文摘Marine sediment microbial fuel cell(MSMFCs)can be utilized as a long lasting power source to drive small instruments to work for long time on ocean floor and its higher power has a significant meaning for practical application.Anode modification can greatly improve the performance of MSMFCs.Herein,humic acid(HA)and humic acid-iron ion complex(HA-Fe)were used to modify the anode for constructing a better MSMFCs.The results indicated that HA-Fe modified anode,better than HA modification,significantly improved the MSMFCs cell power output.The maximum power density of HA-Fe modified MSMFCs is 165.3 mW m−2,which are 6.5-folds of blank MSMFCs.The number of microorganisms on anode,redox activity,and relative kinetic activity were 1.8-,6.1-,and 13.1-folds of blank MSMFCs,respectively.The MSMFCs improvement would be attributed to the electron transfer media of HA and the valence conversion of Fe ions.A synergistic interaction between the naturally occurring HA and Fe ions on the anodic surface in marine sediments would make the modified anodes have‘renewable’characteristics,which is beneficial for the MSMFCs to maintain its long-term higher power.
基金Supported by the Sichuan Science and Technology Program(No.2019YFH0127)the Joint Foundation of Shaanxi(No.2019JLM-59)the Scientific and Technological Innovation Team of Water Ecological Security for Water Source Region of Mid-line of South-to-North Diversion Project of Henan Province(No.17454)。
文摘Iron is a vital micronutrient for growth of bloom-forming Microcystis aeruginosa and competition with other algae,and its availability is affected by humic acid.The effect of iron and humic acid on growth and competition between M.aeruginosa and Scenedesmus obliquus was assessed.The results showed the growth of M.aeruginosa and S.obliquus in mono-cultures was inhibited by humic acid at low iron concentrations(0.01 mg/L);the maximum inhibition ratios were 67.84%and 38.31%,respectively.The inhibition of humic acid on the two species was significantly alleviated when iron concentrations were 1.00 mg/L,with the maximum inhibition rate reduced to 5.82%for M.aeruginosa and to 23.06%for S.obliquus.S.obliquus was the dominant species in mixed cultures,and the mutual inhibition between M.aeruginosa and S.obliquus at low iron concentration was greater than that at high iron concentration.The inhibition of S.obliquus on M.aeruginosa was reduced at low iron concentrations;it increased at high iron concentrations,as concentrations of humic acid rose.
基金the Key Program of the National Natural Science Foundation of China(42230516)National Natural Science Foundation of China(42271129,42101071,42171107)+2 种基金Natural Science Foundation of Jilin Province(YDZJ202201ZYTS480)Jilin Province Education Department Science and Technology Research Project(JJKH20210289KJ)International Wetlands Research League,Alliance of International Science Organizations(ANSO-PA-2020-14).
文摘Dissimilatory iron reduction(DIR)coupled with carbon cycling is increasingly being recognized as an influential process in freshwater wetland soils and sediments.The role of DIR in organic matter(OM)mineralization,however,is still largely unknown in lake sediment environments.In this study,we clarified rates and pathways of OM mineralization in two shallow lakes with seasonal hydrological connectivity and different eutrophic situations.We found that in comparison with the domination of DIR(55%)for OM mineralization in Lake Xiaoxingkai,the contribution of methanogenesis was much higher(68%)in its connected lake(Lake Xingkai).The differences in rates and pathways of sediment OM mineralization between the two lakes were attributed to higher concentrations of carbonate associated iron oxides(Fecarb)in Lake Xiaoxingkai compared to Lake Xingkai(P=0.002),due to better deposition mixing,more contributions of terrigenous detrital materials,and higher OM content in Lake Xiaoxingkai.Results of structural equation modeling showed that Fecarb and total iron content(TFe)regulated 25%of DIR in Lake Xiaoxingkai and 76%in Lake Xingkai,accompanied by a negative effect of TFe on methanogenesis in Lake Xingkai.The relative abundance and diversity of Fe-reducing bacteria were significantly different between the two lakes,and showed a weak effect on sediment OM mineralization.Our findings emphasize the role of iron minerals and geochemical characterizations in regulating rates and pathways of OM mineralization,and deepen the understanding of carbon cycling in lake sediments.
基金supported by the National Basic Research and Development Program (973) of China (No. 2007CB936604)
文摘Transformation of polychlorinated biphenyls (PCBs) by zero-valent iron represents one of the latest innovative technologies for environmental remediation. The dechlorination of 4-chlorobiphenyl (4-C1BP) by nanoscale zero-valent iron (NZVI) in the presence of humic acid or metal ions was investigated. The results showed that the dechlorination of 4-C1BP by NZVI increased with decreased solution pH. When the initial pH value was 4.0, 5.5, 6.8, and 9.0, the de.chlorination efficiencies of 4-CIBP after 48 hr were 53.8%, 47.8%, 35.7%, and 35.6%, respectively. The presence of humic acid inhibited the reduction of 4-CIBP in the first 4 hi', and then significantly accelerated the dechlorination by reaching 86.3% in 48 hr. Divalent metal ions, Co2+, Cu2+, and Ni2+, were reduced and formed bimetals with NZVI, thereby enhanced the dechlorination of 4-CIBP. The dechlorination percentages of 4-CIBP in the presence of 0.1 mmol/L Co2~, Cuz~ and Niz~ were 66.1%, 66.0% and 64.6% in 48 hr, and then increased to 67.9%, 71.3% and 73.5%, after 96 hr respectively. The dechlorination kinetics of 4-C1BP by the NZVI in all cases followed pseudo-first order model. The results provide a basis for better understanding of the dechlorination mechanisms of PCBs in real environment.
基金supported by the National Natural Science Foundation of China (No. 41176075)
文摘A method of size exclusion chromatography coupled with ultraviolet spectrophotometry and off-line graphite furnace atomic absorption spectrometry was developed to assess the complexation properties of iron(Fe) and humic acid(HA) in a water environment. The factors affecting the complexation of Fe and HA, such as ionic strength, pH, temperature and UV radiation, were investigated. The Fe–HA complex residence time was also studied. Experimental results showed that pH could influence the deprotonation of HA and hydrolysis of Fe, and thus affected the complexation of Fe and HA. The complexation was greatly disrupted by the presence of NaCl. Temperature had some influence on the complexation. The yield of Fe–HA complexes showed a small decrease at high levels of UV radiation, but the effect of UV radiation on Fe–HA complex formation at natural levels could be neglected. It took about 10 hr for the complexation to reach equilibrium, and the Fe–HA complex residence time was about 20 hr.Complexation of Fe and HA reached a maximum level under the conditions of pH 6, very low ionic strength, in the dark and at a water temperature of about 25°C, for 10 hr. It was suggested that the Fe–HA complex could form mainly in freshwater bodies and reach high levels in the warm season with mild sunlight radiation. With changing environmental parameters, such as at lower temperature in winter or higher pH and ionic strength in an estuary, the concentration of the Fe–HA complex would decrease.
基金supported by the National Natural Science Foundation of China(nos.41171198,41403079)the Chongqing Research Program of Basic Research and Frontier Technology(no.cstc2015jcyj A20021)the Fundamental Research Funds for the Central Universities of Ministry of Education of China(no.XDJK2015B035)
文摘The phosphorus(P) fraction distribution and formation mechanism in the supernatant after P adsorption onto iron oxides and iron oxide-humic acid(HA) complexes were analyzed using the ultrafiltration method in this study.With an initial P concentration of 20 mg/L(I =0.01 mol/L and pH = 7),it was shown that the colloid(1 kDa-0.45 μm) component of P accounted for 10.6%,11.6%,6.5%,and 4.0%of remaining total P concentration in the supernatant after P adsorption onto ferrihydrite(FH),goethite(GE),ferrihydrite-humic acid complex(FH-HA),goethite-humic acid complex(GE-HA),respectively.The 〈1 kDa component of P was still the predominant fraction in the supernatant,and underestimated colloidal P accounted for 2.2%,55.1%,45.5%,and 38.7%of P adsorption onto the solid surface of FH,FH-HA,GE and GE-HA,respectively.Thus,the colloid P could not be neglected.Notably,it could be interpreted that Fe3+ hydrolysis from the adsorbents followed by the formation of colloidal hydrous ferric oxide aggregates was the main mechanism for the formation of the colloid P in the supernatant.And colloidal adsorbent particles co-existing in the supernatant were another important reason for it.Additionally,dissolve organic matter dissolved from iron oxide-HA complexes could occupy large adsorption sites of colloidal iron causing less colloid P in the supernatant.Ultimately,we believe that the findings can provide a new way to deeply interpret the geochemical cycling of P,even when considering other contaminants such as organic pollutants,heavy metal ions,and arsenate at the sediment/soil-water interface in the real environment.
文摘We reported solvent-free and recoverable heterogeneous iron functionalised imidazolium-based ionic liquid for the reduction of nitroarene derivatives in the presence of formic acid under greener conditions.Additionally,the experimental result shows that the iron complex could be an extremely resourceful,high rate and reusable catalyst for a different nitroarene substrate.
基金Project(50804059)supported by the National Natural Science Foundation of ChinaProject(CX2012B121)supported by the Innovation Research Program for Graduate Student of Hunan Province,China
文摘A modified humic acid(MHA) binder was tested as a substitute for bentonite to prepare qualified specularite pellets. The results show that there is stronger chemisorption between organic functional groups in MHA binder molecular and specularite particles, improving the green pellet strength. MHA binder has obvious effect on the strength and microstructure of preheated pellets due to the thermal decomposition of organic matters in MHA binder. Appropriately increasing preheating temperature or time can eliminate the adverse impact of organic matters on the preheated pellet strength. Compared with the bentonite pellets, the roasted pellets with MHA binder have a more compact microstructure, and the recrystallization of the Fe2O3 crystal grains is better.Consequently, under optimal conditions, 0.75%(mass fraction) MHA binder pellets have equal or better pellet strengths and contain1.06% more total iron than 2 % bentonite pellets. The testing results indicate that MHA binder is a promising and effective alternative to bentonite for the specularite pellets.