Journal of Environmental Chemical Engineering
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2022
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IF 7.968
Xihong Guo,Ying Li,Huan Huang,Dongmei Wang,Rongli Cui,Jialiang Li,Yidong Zhao,Dan Wang,Hui Yuan,Jinquan Dong,Baoyun Sun
Graphdiyne-based materials are promising candidates for the adsorption and detection of heavy metal ions (HMIs) as the acetylenic links in graphdiyne strongly interact with some metal ions. To improve the sensing performance of graphdiyne-based materials and further understand their detection mechanism, we prepared N-substituted graphdiyne (TGDY) through bottom-up method as electrode modified materials, which contained position-fixed and content-controlled alkynyl bonds and pyridine N atoms. By comparing with the H-substituted graphdiyne (HGDY), which was roughly the same in structure as TGDY except that the benzene ring without N atoms, we found that the introduction of N in TGDY greatly improves the electrochemical performance and the signal intensity is closely related to the number of detection sites. Furthermore, the performance of TGDY-based electrochemical sensor was also explored, which showed satisfactory selectivity , reproducibility, stability and applicability for the detection of Cd 2+ and Pb 2+ in water. Our work provided an important reference for rational design and synthesis of electrode materials through bottom-up method to improve the detection performance and explore the detection mechanism.
研究领域:
材料科学
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环境科学
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分析化学
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高影响因子
GEOCHIMICA ET COSMOCHIMICA ACTA
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2012
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IF 4.259
Hui Yin,Wenfeng Tan,Lirong Zheng,Haojie Cui,Guohong Qiu,Fan Liu,Xionghan Feng
Hexagonal birnessite is the most ubiquitous manganese oxide in geological environments. It is often highly enriched in trace metal ions such as Ni and plays an important role in metal(loids) geochemistry . Nanostructured birnessites containing different amounts of Ni were synthesized by addition of Ni 2+ to initial reactants. Powder X-ray diffraction (XRD), element analysis, field emission scanning electron microscopy (FE-SEM), X-ray photoelectron spectroscopy (XPS), thermogravimetric analysis (TGA), X-ray absorption spectroscopy (XAS) and isothermal adsorption and oxidation of metal(loids) were carried out to investigate the effects of Ni doping on the substructure and physicochemical properties of birnessite, and Ni crystal chemistry in birnessite. These Ni-rich birnessites have Ni contents as high as 2.99% (Ni5) and 6.08% (Ni10) in weight. EXAFS results show that Ni5 has 23.7% of the total Ni (0.71 wt.%) and Ni10 has 34.5% of the total Ni (2.10 wt.%) in Mn octahedral layer with the remaining Ni located at vacancies and edge sites. The Ni-rich birnessites have weaker crystallinity and thermal stability, fewer layers stacked along the c axis, ∼1.5–2.7 times larger surfaces areas, and a higher Mn average oxidation numbers (AONs) compared to the birnessite without Ni. Additionally, the doping of Ni during birnessite crystallization enhances the formation of vacancies in the layer; however, adsorption capacities for Pb 2+ and Zn 2+ by these Ni-rich birnessites are reduced, mainly because of vacancies and edge sites occupation by a large amount of Ni. The Ni-rich birnessites exhibit much higher oxidation capability and can completely oxidize As(III) in solution at rapid initial reaction rates under the experimental condition. The results indicate that incorporation of Ni into the natural birnessite in ferromanganese nodules may be achieved both by direct coprecipitation with Mn to build the layers and migration over time from adsorbed Ni on the surface into the layer structure. It is also implied that Ni doping in birnessite has great impact on the geochemical behaviors of heavy metals, either in adsorption or oxidation reactions.
研究领域:
地球化学
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环境科学
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JOURNAL OF MATERIALS SCIENCE-MATERIALS IN ELECTRONICS
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2023
·Vol. 34
·期 6
·1-11
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IF 2.8
Ni Yafei,Li Haimin,Li Ming,Liu Xingchong,Wang Hanyu,Lei Yue,Liu Shuqian,Tang Yanling
Perovskite solar cells (PSCs) have received extensive attention due to their excellent photovoltaic properties. However, existence of defects, such as Pb 2+ and I − vacancies, restricts its further improvement of power conversion efficiency (PCE) and affects the stability of PSCs devices. In this study, glycine methyl ester hydrochloride (GMEH) was introduced as interface modification material. As Lewis base, GMEH formed a chemical bonding of Pb–O with perovskite to decrease uncoordinated Pb 2+ defects, thus transfer of charge carriers was obviously facilitated, indicating that status of Pb 2+ in perovskite structure is one of key factors for carrier transportation. Meanwhile, amino group in GMEH combined with iodide to form hydrogen bond, thereby stabilized perovskite structure and decreased ion migration. Eventually, a champion efficiency of 21.94% was obtained with promoted short-circuit current ( J SC ) and fill factor (FF). Meanwhile, the stability of PSCs was significantly improved. The modified PSCs can maintain 90% of the initial efficiency after storing in a nitrogen filled glove box for 1700 h, while the control one can only maintain 55%. And the stability of the modified device in humid air was also greatly improved.
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SCIENCE OF THE TOTAL ENVIRONMENT
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2022
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IF 10.753
Yan Chen,Hong Liu,Mengsheng Xia,Miaomiao Cai,Zeguang Nie,Junkai Gao
To date, most existing engineering materials have difficulty simultaneously separating oil/water and removing heavy metals from complex oily wastewater. In response to this challenge, a novel multifunctional composite hydrogel membrane (named PVA-CS-LDHs) was fabricated by incorporating chitosan (CS) and nanohydrotalcite (LDHs) into a polyvinyl alcohol (PVA) hydrogel. This material was developed using an easy yet versatile strategy of freezing and salting-out, which can enable the formation of a PVA-CS-LDH hydrogel membrane in one step and endow the PVA-CS-LDHs with high strength, excellent stretchability, favourable shape recoverability , and an ideal 3D microstructure. The PVA-CS-LDH membrane can purify emulsified oil and metal ions simultaneously with a separation efficiency of 99.89 % for emulsified oil and a removal efficiency of 97.44 % for Pb2+ ions. Additionally, the high-efficiency, multifunctional, high-antifouling and eco-friendly properties of the PVA-CS-LDH membrane make it a promising hydrogel material for both emulsified oil separation and heavy metal ion removal. Thus, this material provides critical application potential that can address scientific and technological challenges in complex oily wastewater purification.
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PubMed
高影响因子
Frontiers in Materials
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2022
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IF 3.985
Chen Yu,Liu Miao
Application of amino-functionalized mesoporous silica-coated core-shell magnetic nanoparticles (Fe3O4@mSiO2-NH2 NPs) for adsorbing heavy metal ions has attracted intensive interest in recent years. Despite the cytotoxicity triggered by the co-exposure of nanoparticles (NPs) and metal ions in relatively high dosages being reported, the effect of the adsorbed heavy metal ions on the cytotoxicity to human cells remains unexplored. Herein, we demonstrated the effect of amino-functionalized Fe3O4@mSiO2 core-shell magnetic nanoparticles before and after adsorbing Pb2+ ions on the cytotoxicity of human kidney cells (HEK293). The surface morphology, viability, and oxidative stress (OS) induction of HEK293 cells incubated with Fe3O4@mSiO2-NH2 NPs and Pb2+ ion-adsorbed Fe3O4@mSiO2-NH2 NPs were assessed, respectively. Transmission electron microscopic (TEM) images of cell sections depicted that Fe3O4@mSiO2-NH2 NPs were internalized by HEK293 cells and gathered mainly in the cytoplasm. Cell viability (MTT) assays revealed the Fe3O4@mSiO2-NH2 NPs could enhance the cell viability to 119.9% and 108.2% compared to the control group, respectively. On contrast, the Pb2+ ion-adsorbed Fe3O4@mSiO2-NH2 NPs were toxic to the cell because when the Pb2+ ion contents were 5.0 and 7.5 μg mL−1, the viabilities of the samples decreased to 97.1% and 84.7%, respectively. Oxidative stress data proved that OS was negatively affected by both dissociative Pb2+ ions and the Pb2+ ion-adsorbed Fe3O4@mSiO2-NH2 NPs. Cytotoxicity may be attributed to the OS induced by Pb2+ ions leaked from the adsorbent. Under the same Pb2+ ion concentration, the cytotoxicity of the adsorbed Pb2+ ions was lower than that of the dissociative Pb2+ ions, indicating that the adsorption by NPs inhibited the cytotoxicity of Pb2+ ions. This work will provide new references for assessing the cytotoxicity of Pb2+-adsorbed nanoparticles.
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Materials Today Chemistry
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2022
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IF 7.613
S. Yang,Y. Cheng,T. E,Y. Wang,L. Liu,Y. Li,D. Wang,J. Qian
The inert substrate surface of MoS 2 leads to unsatisfactory adsorption performance. Herein, an inert substrate surface activation strategy is proposed, and the resulted MoS 2 /montmorillonite (MMT) prepared via the hydrothermal method is immersed with NaF (F–Mt). The intercalation of Na + contributes to inducing the transformation of MoS 2 from 2H phase to 1 T phase, thereby providing a large number of S vacancies and exposing available Mo 4+ . Meanwhile, the surface of MMT is activated due to the fact that partially [Si 4 O 10 ] 4- are etched by F - , which facilitates forming Si–O–Mo bonds to promote the charge transfer. The improved charge transfer rate can make S 2- in MoS 2 accumulate more negative charges, greatly enhancing the adsorption capacity to Pb 2+ . Moreover, the natural negative potential on the surface of MMT solves the problem of easy stacking for nanosheets , improving the availability of active sites on the edge, which are also benefit from the etching effect on MoS 2 nanosheets with NaF. The maximum adsorption capacity achieves 97.09 mg/g. Additionally, density functional theory (DFT) calculations confirm the resulted S vacancies in MoS 2 are in favor of removing Pb 2+ , which is also contributed by the electrostatic and chemical adsorption with MMT. Therefore, it suggests that F–Mt is an excellent adsorbent for Pb 2+ .
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MICROCHEMICAL JOURNAL
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2024
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IF 4.9
Juan Hou,Qinqin Chen,Xiangzhi Meng,Donghan Wang,Huiling Liu,Wei Feng
The increasing presence of heavy metals and amino acids in environmental and pharmaceutical samples necessitates the development of effective and sensitive detection methods. Traditional analytical techniques often lack the specificity and sensitivity required for simultaneous detection of multiple analytes, leading to a need for novel approaches. In this study, we developed a ratiometric fluorescence probe based on a physical mixture of red and blue carbon dots (R/BCDs) for the selective detection of lead ions (Pb 2+ ) and L-cysteine (L-Cys). The probe was synthesized through hydrothermal methods and characterized by various spectroscopic techniques. The R/BCDs probe exhibited a remarkable 11.6-fold fluorescence quenching in response to Pb 2+ , with a detection limit of 15 nM, while subsequent addition of L-Cys showed a 9.6-fold restored fluorescence signal, achieving a detection limit of 75 nM. Additionally, we demonstrated the feasibility of fabricating colorimetric test paper and hydrogels, enabling rapid on-site analysis. This dual-analyte detection capability was demonstrated through successful application in real water and pharmaceutical samples. The R/BCDs probe offers a novel, simple, and effective strategy for environmental monitoring and biological assessments, highlighting its potential for practical applications.
研究领域:
环境科学
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分析化学
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生物医学
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高影响因子
FOOD CHEMISTRY
·
2021
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IF 7.514
Gangfeng Li,Tarun Belwal,Zisheng Luo,Yintao Li,Li Li,Yanqun Xu,Xingyu Lin
Direct electrochemical detection in real food samples remains challenging due to the fouling and interference by abundant interference components. Herein, we report an electrochemical sensing platform based on binary assembly of silica nanochannels and polydimethylsiloxane that is able to detect Pb 2+ and Cd 2+ in real food samples without complex pretreatments. Using differential pulse anodic stripping voltammetry, the electrochemical detection consists of electro-deposition of metal species and subsequent anodic stripping in the modified silica-nanochannels. Under the optimized conditions, the linear ranges were obtained from 4 to 1500 μg L −1 for Pb 2+ and 30 to 900 μg L −1 for Cd 2+ . The relative standard deviations were 2.9% and 3.6% for Pb 2+ and Cd 2+ of 300 μg L −1 . Without tedious pretreatments, the quantitative detection of Pb 2+ and Cd 2+ in real juice and beverage samples was successfully performed, revealing that the developed sensor possesses excellent anti-interference and practicability properties for unprocessed food.
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PubMed
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JOURNAL OF MOLECULAR LIQUIDS
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2020
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IF 5.065
Hongling Zhang,Mingxing Shi,Jianzhe Ma,Mingzhu Xia,Fengyun Wang,Chuan Liao
The maximum adsorption capacities of threonine-montmorillonite (Thr–Mt) composite to Pb 2+ and Cu 2+ in aqueous solution were higher than that of original sodium-montmorillonite (Na–Mt). Molecular dynamics (MD) simulation and Multiwfn wavefunction program based on density functional theory (DFT) were exploited to probe the interaction and mechanism between threonine-montmorillonite composite and Pb 2+ or Cu 2+ . Moreover, for the first time, Independent Gradient Model (IGM) analysis was utilized to decode the interaction essence among Thr, Mt. and Pb 2+ or Cu 2+ to reveal the removal mechanism of Thr-Mt to Pb 2+ and Cu 2+ . MD results indicated that the arrangement of Thr + presented a preferred almost vertical orientation, which was consistent with the X-ray diffraction (XRD) result. There was hydrogen bonding between carboxyl group or hydroxy group of Thr + and Mt. surface. Multiwfn calculation implied that the minimum points of ESP and ALIE were located near the O atoms of hydroxyl group and carboxyl group, which were most likely providing the lone pair electron to form a complex with the metal ion ,which was accordance with the result of basin analysis. IGM analysis vividly revealed that O atoms of carboxyl group and hydroxyl group were binding sites, and the interaction between Pb 2+ and Na–Mt or Pb 2+ and Thr-Mt was stronger than that of Cu 2+ , which was well consistent with the experimental conclusion.
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SENSORS AND ACTUATORS B-CHEMICAL
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2020
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IF 7.1
Jiajia Han,Jingguo Yu,Yufei Guo,Li Wang,Yonghai Song
The indissolubility or poor dissolubility of covalent-organic frameworks (COFs) limits their wide applications. Here, the COF BTLP-1 which were prepared by the aminaldehyde condensation between 1,4-benzenedithiol-2,5-diamino-hydrochloride and 1,3,5-triformylbenzene was controllably grown on kenaf stem-derived macroporous carbon (3D-KSC). Compared with COF BTLP-1 powder, the COF BTLP-1 grown on 3D-KSC avoided their random orientation effectively. The results showed that the amount of COF BTLP-1 could be effectively controlled by adjusting the concentration of monomers and growing time. Each unit of COF BTLP-1 has 12 adsorption sites (6 sulfur atoms and 6 nitrogen atoms) for heavy metal ions (HMIs) and regular holes to facilitate the transfer of HMIs. A large number of adsorption sites of HMIs could identify and captured HMIs selectively, and accordingly Cd 2+ , Pb 2+ , Cu 2+ and Hg 2+ could be detected simultaneously by using the COF BTLP-1 /3D-KSC electrode. The detection limits for Cd 2+ , Pb 2+ , Cu 2+ and Hg 2+ are 12.3 nM, 11.8 nM, 18.6 nM and 21.4 nM, respectively. The sensitivities are up to 1337.4 μA/μM cm 2 , 1389.0 μA/μM cm 2 and 886.2 μA/μM cm 2 , 770.0 μA/μM cm 2 , respectively. The COF BTLP-1 /3D-KSC may be also applied in other fields of electroanalytical chemistry.
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Applied Water Science
·
2021
·Vol. 11
·期 9
·1-8
·
IF 3.874
Song Fuxiang,Wang Na,Hu Zezhou,Zhang Zhen,Mai Xiaoxue,Jie Weibo,Bin Liu
Oral medical wastewater with heavy metal ions (such as plumbum, Pb 2+ ) is regarded as the main pollutant produced in the oral cavity diagnosis, and the treatment process can pose a serious threat to human health. The removal of Pb 2+ from oral medical wastewater facing major difficulties and challenges. Therefore, it is of great significance to take effective measures to remove Pb 2+ by using effective methods. A new activated three-dimensional framework carbon (3D AFC), regarded as the main material to remove Pb 2+ in the oral medical wastewater, has been fabricated successfully. In this experiment, the effects of 3D AFC absorbing Pb 2+ under different conditions (including solid-to-liquid ratio, pH, ionic strength, contact time, and initial concentration, etc.) were discussed. And the result revealed that the adsorption kinetics process of Pb 2+ on 3D AFC conformed to the pseudo-second-order model and the adsorption isotherm conformed to the Freundlich model. Under the condition that pH = 5.5 and T = 298 k, the calculated maximum adsorption capacity of 3D AFC for Pb 2+ was 270.88 mg/g. In practical application, it has strong adsorption ability for Pb 2+ in oral medical wastewater. Thus, 3D AFC shows promise for Pb 2+ remove and recovery applications because of high adsorption capacity for Pb 2+ in oral medical wastewater due to its high specific surface area, outstanding three-dimensional network structure.
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CHEMOSPHERE
·
2021
·
IF 7.086
Hewei Song,Amit Kumar,Yuling Zhang
In the recent decades, due to rapid increase in industrialization, urbanization, anthropogenic activity in the catchments, removal of heavy metals contaminants in wastewater has become global challenges. Numerous advance technologies have been introduced to deal with these problems but failed in reducing adequate pollution load in the contaminated water and/or wastewater. In this study, sulfur-ferromagnetic nanoparticles (SFMNs) were synthesized by modification of nano-Fe 3 O 4 , which can be rapidly separated from the environment by an external magnetic field after in situ repair. Its structure and physical properties were characterized by conventional techniques included Transmission electron microscope (TEM), X-ray diffraction (XRD) and vibrating sample magnetometer (VSM). The ability of the SFMNs to remove Pb 2+ and Cd 2+ was studied at different temperatures and initial metal ions concentrations. The adsorption kinetics showed that the adsorption equilibrium time of Pb 2+ and Cd 2+ was 300 min consequently adsorption process of SFMNs fit well (R 2 > 0.99) with pseudo-second-order model. The adsorption thermodynamics showed that the adsorption of Pb 2+ and Cd 2+ on SFMNs is spontaneous (negative value of ΔG 0 ) endothermic process (positive value of ΔH 0 ) and fit well (R 2 > 0.98) with the Langmuir isothermal model. Density functional theory (DFT) calculations show that SFMNs can transfer electrons to Pb 2+ and Cd 2+ , and the metal ions form stable chelates on the ligand surface. This study implies that newly synthesized sulfur-ferromagnetic nanoparticles could play an instrumental role in metal ions removal from water and wastewater.
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