Amino-type adsorbents(ATAs) were prepared by radiation-induced graft copolymerization of 4-hydroxybutyl acry late glycidyl ether(HB) onto a polyethylene-coated polypropylene(PE/PP) duplex fiber of a non-woven fabric,a...Amino-type adsorbents(ATAs) were prepared by radiation-induced graft copolymerization of 4-hydroxybutyl acry late glycidyl ether(HB) onto a polyethylene-coated polypropylene(PE/PP) duplex fiber of a non-woven fabric,and modified with different amines of ethylenediamine(EDA),diethylenetriamine(DETA),triethylenetetramine(TETA) and diethylamine(DEA).The adsorption behavior of uranyl ions onto the ATAs was studied in batch experiments.The effects of the contact time,initial concentration of the ions,temperature,and pH value.The salinity were investigated along with the adsorption kinetics and the adsorption isotherms.The kinetic experimental data followed the pseudo second-order kinetic model,and the adsorption isotherms correlated well with the Langmuir model.The ATAs showed good efficiency in adsorbing uranyl ions,with the best saturation adsorption capacity being 64.26 mg g^(-1) for ATA-DETA within 120 min.The temperature dependence of ATADETA was quite abnormal and the quickest behavior was obtained at 25 ℃.ATAs showed good adsorption capacity over a wide pH range of 4.0-8.5,and HCl could be used in the elution process.Salinity of the solution had great effect on the adsorption capacity,3.5%salinity resulted in a 55%loss of capacity from ATA-DETA.The selectivity of ATA-DETA showed an order of:UO_2^(2+)≈Fe^(3+)> Zn^(2+) > VO_3^- > Co^(2+) > Ni^(2+).展开更多
Composite materials have elicited much interest because of their superior performance in the removal of toxic and radioactive uranyl ions from aqueous solutions.With polyethyleneimine as a functional group,carboxylate...Composite materials have elicited much interest because of their superior performance in the removal of toxic and radioactive uranyl ions from aqueous solutions.With polyethyleneimine as a functional group,carboxylated chitosan as a matrix,and oxidizing activated carbon as a nanofiller,this study synthesized a novel environment-friendly polyethylenimine-functionalized carboxylated chitosan/oxidized activated charcoal(PCO)biocomposite with a unique three-dimensional porous structure.PCO was synthesized through an easy chemical cross-linking method.Detailed characterization certified the formation of the unique three-dimensional porous structure.The obtained PCO was used to remove uranyl ions from an aqueous solution,demonstrating the maximum adsorption capacity of 450 mg·g^(−1).The adsorption capacity of PCO decreased by less than 7.51%after five adsorption-desorption cycles.PCO exhibited good adsorption selectivity(K_(d)=3.45×10^(4) mL·g^(−1))for uranyl ions.The adsorption mechanism of PCO was also discussed.The material showed good potential for application in the treatment of wastewater containing uranyl ions.展开更多
Under the public spotlight,uranyl(UO22+)ions has attracted considerable attention for the extreme radioactive and chemical toxicity to ourselves and our environment.Herein,we present a simple and effective ratiometric...Under the public spotlight,uranyl(UO22+)ions has attracted considerable attention for the extreme radioactive and chemical toxicity to ourselves and our environment.Herein,we present a simple and effective ratiometric fluorescence imaging method for the visualizing and quantitative detection UO22+ions by cellphone-based optical platform.The sensing solution was prepared by mixing label-free red carbon dots(r-CDs)and blue carbon dots(b-CDs)together with a fixed photoluminescence intensity ratio of 4:1.When UO22+ions were added,the fluorescence of r-CDs can be selectively quenched,while the fluorescence of b-CDs remains stable without spectral cha nges.With the gradually increase the amounts of UO22+ions,the different response of dual-color CDs resulted in a signification color evolution from deep red to dark purple under the ultraviolet(UV)light illumination.Then,a cellphone-based optical platform was constructed for directly imaging the color change of the samples,and the built-in Colorpicker APP quickly output the red,green and blue(RGB)channel values of these images within one second.Interesting,there was a linear relationship between the ratio of red and blue(R/B)channel values and UO22+ions concentration from 0μmol/L to 30.0μmol/L(R^2=0.92804)with the detection limit of^8.15μmol/L(signal-to-noise ratio of 3).In addition,the optical platform has also been applied to the quantification of UO22+ions in tap water and river water sample.With the advantage of low-cost,portable,easy to operation,we anticipate that this method would greatly improve the accessibility of UO22+ions detection even in resource-limited areas.展开更多
The uranyl ion(UO22+) poses high risks to human health and the environment, hence its detection and monitoring is of utmost significance. However, the development of an ultra-sensitive, high-efficiency and convenient ...The uranyl ion(UO22+) poses high risks to human health and the environment, hence its detection and monitoring is of utmost significance. However, the development of an ultra-sensitive, high-efficiency and convenient approach for on-site detection of UO22+ remains a challenge. Herein, a reliable and reusable surface-enhanced Raman spectroscopy(SERS)-based microfluidic biosensor was developed for rapid detection of UO22+ in real samples. The detection protocol involved the reaction of 5′-Rhodamine B(RhB)-labeled double-stranded DNA for UO22+-specific DNAzyme-cleavage reaction in a U-shaped microchannel. Then, the reaction products were delivered into three parallel samples for high-throughput tests by SERS biochips,where 3 D ZnO-Ag mesoporous nanosheet arrays(MNSs) were modified with a single-stranded DNA(ssDNA). The ssDNAwas sequence-complementary with the 5′-RhB-labeled cleaved-stranded DNA(csDNA) from the reaction products. By the hybridization of ssDNA and csDNA, the signal probe RhB was fixed close to the surface of the ZnO-Ag MNSs to enhance the Raman signal. The limit of detection for UO22+ with the microfluidic-SERS biosensor was 3.71×10-15 M. An over 20,000-fold selectivity towards UO22+ response was also achieved in the presence of 15 other metal ions. The high-throughput microfluidicSERS biosensor operated well for practical UO22+ detection, with excellent recoveries in contaminated river and tap water from95.2% to 106.3%(relative standard deviation(RSD)<6.0%, n=6). Although the SERS-based microfluidic biosensor developed in this study was deployed for the detection of UO22+, the reusable and high-efficiency system may be expanded to the detection of other analytes on-site.展开更多
-The i. r. spectra of Na4 [UO2 (CO3)3], Na [UO2 (OH)3] and the surface species of uranium on HTO underthe condition of flowing natural seawater and concentrated seawater (NaCl-NaHCO3-U) were recorded, with the bands o...-The i. r. spectra of Na4 [UO2 (CO3)3], Na [UO2 (OH)3] and the surface species of uranium on HTO underthe condition of flowing natural seawater and concentrated seawater (NaCl-NaHCO3-U) were recorded, with the bands of urany! of surface species obtained and the finding that iigands of surface species besides HTO are mainly water and OH, and there are some CO32- groups under the condition of natural seawater. Some relations between the complex properties and the j. r. spectroscopic characters for uranyl complexes were studied, and the transferred change quantity of surface complex was calculated.Structure models for surface species of adsorption are herein presented and the mechanism for uranium adsorption is deduced.展开更多
通过在阳离子结构中引入铀酰离子萃取剂磷酸三丁酯(TBP)的功能结构,设计合成了两种咪唑型离子液体,使该离子液体在硝酸介质中萃取铀酰离子时,既是稀释剂又具有萃取剂功能。利用傅里叶红外光谱(FTIR)、核磁共振(1 H NMR)和元素分析,对合...通过在阳离子结构中引入铀酰离子萃取剂磷酸三丁酯(TBP)的功能结构,设计合成了两种咪唑型离子液体,使该离子液体在硝酸介质中萃取铀酰离子时,既是稀释剂又具有萃取剂功能。利用傅里叶红外光谱(FTIR)、核磁共振(1 H NMR)和元素分析,对合成的离子液体结构进行了确认,并对硝酸介质中萃取铀酰离子进行了初步研究。结果表明:室温条件下,所合成的具有特定功能的离子液体可在硝酸介质中萃取铀酰离子,萃取率可达90%以上。展开更多
基金Supported by National Natural Science Foundation of China(Nos.11175234 and 11105210)the"Strategic Priority Research Program"of the Chinese Academy of Sciences(No.XDA02030200)+1 种基金the"Knowledge Innovation Program"of the Chinese Academy of Sciences(No.KJCX2YW-N49)Shanghai Municipal Commission for Science and Technology(Nos.11ZR1445400 and 12ZR1453300)
文摘Amino-type adsorbents(ATAs) were prepared by radiation-induced graft copolymerization of 4-hydroxybutyl acry late glycidyl ether(HB) onto a polyethylene-coated polypropylene(PE/PP) duplex fiber of a non-woven fabric,and modified with different amines of ethylenediamine(EDA),diethylenetriamine(DETA),triethylenetetramine(TETA) and diethylamine(DEA).The adsorption behavior of uranyl ions onto the ATAs was studied in batch experiments.The effects of the contact time,initial concentration of the ions,temperature,and pH value.The salinity were investigated along with the adsorption kinetics and the adsorption isotherms.The kinetic experimental data followed the pseudo second-order kinetic model,and the adsorption isotherms correlated well with the Langmuir model.The ATAs showed good efficiency in adsorbing uranyl ions,with the best saturation adsorption capacity being 64.26 mg g^(-1) for ATA-DETA within 120 min.The temperature dependence of ATADETA was quite abnormal and the quickest behavior was obtained at 25 ℃.ATAs showed good adsorption capacity over a wide pH range of 4.0-8.5,and HCl could be used in the elution process.Salinity of the solution had great effect on the adsorption capacity,3.5%salinity resulted in a 55%loss of capacity from ATA-DETA.The selectivity of ATA-DETA showed an order of:UO_2^(2+)≈Fe^(3+)> Zn^(2+) > VO_3^- > Co^(2+) > Ni^(2+).
基金This work was financially supported by the basic research project of Sichuan Province for Science and Technology Development(Grant No.2019YJ0355)Outstanding Youth Science and Technology Talents Program of Sichuan(Grant No.19JCQN0085)+1 种基金Key Projects of the Pre-research Fund of the General Armament Department(Grant No.6140720020101)National Defense Technology Foundation Project(Grant No.JSJL2016404B002).
文摘Composite materials have elicited much interest because of their superior performance in the removal of toxic and radioactive uranyl ions from aqueous solutions.With polyethyleneimine as a functional group,carboxylated chitosan as a matrix,and oxidizing activated carbon as a nanofiller,this study synthesized a novel environment-friendly polyethylenimine-functionalized carboxylated chitosan/oxidized activated charcoal(PCO)biocomposite with a unique three-dimensional porous structure.PCO was synthesized through an easy chemical cross-linking method.Detailed characterization certified the formation of the unique three-dimensional porous structure.The obtained PCO was used to remove uranyl ions from an aqueous solution,demonstrating the maximum adsorption capacity of 450 mg·g^(−1).The adsorption capacity of PCO decreased by less than 7.51%after five adsorption-desorption cycles.PCO exhibited good adsorption selectivity(K_(d)=3.45×10^(4) mL·g^(−1))for uranyl ions.The adsorption mechanism of PCO was also discussed.The material showed good potential for application in the treatment of wastewater containing uranyl ions.
基金the National Natural Science Foundation of China(Nos.21976002,21675158,21507134,61603001,61705239 and 81773684)Natural Science Foundation of Anhui Province(Nos.1908085MB41,1908085QB75)+2 种基金Guangdong Natural Science Funds for Distinguished Young Scholars(No.2018B030306033)Pearl River S&T Nova Program of Guangzhou(No.201806010060)Pearl River Talent Program(No.2017GC010363)。
文摘Under the public spotlight,uranyl(UO22+)ions has attracted considerable attention for the extreme radioactive and chemical toxicity to ourselves and our environment.Herein,we present a simple and effective ratiometric fluorescence imaging method for the visualizing and quantitative detection UO22+ions by cellphone-based optical platform.The sensing solution was prepared by mixing label-free red carbon dots(r-CDs)and blue carbon dots(b-CDs)together with a fixed photoluminescence intensity ratio of 4:1.When UO22+ions were added,the fluorescence of r-CDs can be selectively quenched,while the fluorescence of b-CDs remains stable without spectral cha nges.With the gradually increase the amounts of UO22+ions,the different response of dual-color CDs resulted in a signification color evolution from deep red to dark purple under the ultraviolet(UV)light illumination.Then,a cellphone-based optical platform was constructed for directly imaging the color change of the samples,and the built-in Colorpicker APP quickly output the red,green and blue(RGB)channel values of these images within one second.Interesting,there was a linear relationship between the ratio of red and blue(R/B)channel values and UO22+ions concentration from 0μmol/L to 30.0μmol/L(R^2=0.92804)with the detection limit of^8.15μmol/L(signal-to-noise ratio of 3).In addition,the optical platform has also been applied to the quantification of UO22+ions in tap water and river water sample.With the advantage of low-cost,portable,easy to operation,we anticipate that this method would greatly improve the accessibility of UO22+ions detection even in resource-limited areas.
基金supported by the Science Challenge Project (TZ2018004)the National Natural Science Foundation of China (21502179)
文摘The uranyl ion(UO22+) poses high risks to human health and the environment, hence its detection and monitoring is of utmost significance. However, the development of an ultra-sensitive, high-efficiency and convenient approach for on-site detection of UO22+ remains a challenge. Herein, a reliable and reusable surface-enhanced Raman spectroscopy(SERS)-based microfluidic biosensor was developed for rapid detection of UO22+ in real samples. The detection protocol involved the reaction of 5′-Rhodamine B(RhB)-labeled double-stranded DNA for UO22+-specific DNAzyme-cleavage reaction in a U-shaped microchannel. Then, the reaction products were delivered into three parallel samples for high-throughput tests by SERS biochips,where 3 D ZnO-Ag mesoporous nanosheet arrays(MNSs) were modified with a single-stranded DNA(ssDNA). The ssDNAwas sequence-complementary with the 5′-RhB-labeled cleaved-stranded DNA(csDNA) from the reaction products. By the hybridization of ssDNA and csDNA, the signal probe RhB was fixed close to the surface of the ZnO-Ag MNSs to enhance the Raman signal. The limit of detection for UO22+ with the microfluidic-SERS biosensor was 3.71×10-15 M. An over 20,000-fold selectivity towards UO22+ response was also achieved in the presence of 15 other metal ions. The high-throughput microfluidicSERS biosensor operated well for practical UO22+ detection, with excellent recoveries in contaminated river and tap water from95.2% to 106.3%(relative standard deviation(RSD)<6.0%, n=6). Although the SERS-based microfluidic biosensor developed in this study was deployed for the detection of UO22+, the reusable and high-efficiency system may be expanded to the detection of other analytes on-site.
文摘-The i. r. spectra of Na4 [UO2 (CO3)3], Na [UO2 (OH)3] and the surface species of uranium on HTO underthe condition of flowing natural seawater and concentrated seawater (NaCl-NaHCO3-U) were recorded, with the bands of urany! of surface species obtained and the finding that iigands of surface species besides HTO are mainly water and OH, and there are some CO32- groups under the condition of natural seawater. Some relations between the complex properties and the j. r. spectroscopic characters for uranyl complexes were studied, and the transferred change quantity of surface complex was calculated.Structure models for surface species of adsorption are herein presented and the mechanism for uranium adsorption is deduced.
文摘通过在阳离子结构中引入铀酰离子萃取剂磷酸三丁酯(TBP)的功能结构,设计合成了两种咪唑型离子液体,使该离子液体在硝酸介质中萃取铀酰离子时,既是稀释剂又具有萃取剂功能。利用傅里叶红外光谱(FTIR)、核磁共振(1 H NMR)和元素分析,对合成的离子液体结构进行了确认,并对硝酸介质中萃取铀酰离子进行了初步研究。结果表明:室温条件下,所合成的具有特定功能的离子液体可在硝酸介质中萃取铀酰离子,萃取率可达90%以上。