CHEMICAL ENGINEERING JOURNAL
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2020
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IF 10.652
Cong Liu,Xu Cui,Yanhui Li,Qian Duan
A novel hybrid Cu 2 O@TiO 2 - g -zinc-tetraamino-phthalocyanine (CT- g -ZnTAPc) hollow sphere as “ day-night ” photocatalyst with spatially separated structures was prepared successfully. Firstly, three layers SiO 2 @Cu 2 O@TiO 2 (SCT) was synthesized with core–shell structure. Then zinc-tetraamino-phthalocyanine (ZnTAPc) immobilized on the surface of maleic anhydride (MAH) modified SCT with amide linkages. Finally, hollow CT- g -ZnTAPc spheres were obtained by NaOH etching. In this structure, ZnTAPc was grafted on the outer surface of TiO 2 as the main visible light absorber, while the inner surface was adhered with Cu 2 O as a secondary absorption of the scattered light. Both of Cu 2 O and ZnTAPc sensitized TiO 2 synergistically to broaden light response from ultraviolet to visible region and enhance photocatalytic activity. Meanwhile, TiO 2 - g -ZnTAPc and Cu 2 O@TiO 2 p–n heterojunctions based on the close match band structures, so they were expected to facilitate electron-hole separation more effectively. Moreover, TiO 2 would capture electrons from Cu 2 O and ZnTAPc under visible light and delayed releasing electrons without illumination to perform photocatalyzing in dark as “ day-night ” photocatalysts. K 2 Cr 2 O 7 (Cr (VI)), Rhodamine B (RhB) and tetracycline hydrochloride (TC•HCl) were employed as model pollutants as well as Cr (VI)-RhB coexistence system. Almost 95.2% of Cr (VI) could be reduced by CT- g -ZnTAPc, which was about 1.57 times of Cu 2 O@TiO 2 and 1.64 times of TiO 2 - g -ZnTAPc. Furthermore, CT- g -ZnTAPc had a high specific surface area (219.3 m 2 /g) as an efficient pollutant adsorbent, and was investigated by Langmuir, Freundlich and Temkin isotherm models. The maximum quantity of Cr (VI) adsorbed by CT- g -ZnTAPc was 48.8 mg/g. As a result, CT- g -ZnTAPc would be a potential effective and energy-saving multifunctional photocatalyst.
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APPLIED SURFACE SCIENCE
·
2024
·
IF 6.3
Xinyu Zhang,Kui Du,Liping Deng,Ziyou Zhang,Zhiqiang Chen,Hongliang Dong
In this paper, we reported an innovative one-pot fabrication approach of a bifunctional nanohybrid through scaffolding of nanoscale zero-valent iron onto the inter-layer structure of graphitic carbon nitride in sequestering U(VI) and Cr(VI) in wastewater. The microstructures, morphologies and chemical compositions of the as–fabricated g-C 3 N 4 /NZVI nanohybrid before and after U(VI)/Cr(VI) sequestration were exploited in detail by applying various physicochemical and spectroscopic methods. Batch experimental results demonstrated that sequestration of targeted U(VI)/Cr(VI) by g-C 3 N 4 /NZVI was higher than those of pure NZVI or g-C 3 N 4 due to the pronounced boost performance, which was ascribed from the introduction of g-C 3 N 4 as matrix inhibited the oxidation of NZVI and improved its reactivity. The pH effect was also elucidated and it was found that lower pH facilitated the sequestration of the negatively–charged Cr(VI), while higher pH benefited the sequestration of the positively–charged U(VI). Moreover, the characterization insights into intrinsic mechanism manifested that sequestration of U(VI)/Cr(VI) was fulfilled through a synergistic effect of adsorption, reduction and coprecipitation. This work is of great significance for understanding the combined sequestration mechanism of U(VI) and Cr(VI), and usage of g-C 3 N 4 /NZVI in sequestration of severe dangerous metal ions, especially efficient detoxification of toxic cations and anions in wastewater.
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ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH
·
2025
·
IF 0
Maqinana Siphosethu,Kowenje Chrispin B. O.,Ojwach Stephen O.
Reactions of N 1 ,N 3 -bis(2-mercaptoethyl)isophthalamide with (3-aminopropyl)triethoxysilane (3-APTES) afforded the the corresponding Schiff base chelating ligand, (1Z,3Z)-N 1 ,N 3 -bis(2-mercaptoethyl)-N' 1 ,N' 3 bis(3(triethoxysilyl)propyl) isophthalimidamide ( L1 ) in high yields. Subsequent immobilization of L1 on mesoporous silica supports (SBA-15 and MCM-41) following a divergent method produced the respective fabricated L1@SBA-15 and L1@MCM-41 materials. Characterization of the fabricated chelating agents was accomplished using SEM, TEM, EDX, BET, PXRD, FT-IR, and TGA-DTA/DSC techniques. The fabricated materials were used as adsorbents for the removal of Cd(II), Pb(II) and Cr(VI) metal ions from water. Both the L1@SBA-15 and L1@MCM-41 materials demonstrated high extraction efficiencies for Cd(II) and Pb(II) cations, achieving over 98% and 97% removal, respectively, across a broad pH range (3–9). For Cr(VI) anions, relatively lower optimal extraction efficiencies of 67% and 77% were recorded between pH 3–12, for L1@SBA-15 and L1@MCM-41 , adsorbents, respectively. Faster extraction kinetics were observed for Cd(II) and Pb(II) cations, with over 94% removal achieved within 30 min, even at low initial metal concentrations (5 ppm) and adsorbent dosages (10 mg). Kinetic modelling showed that the adsorption process followed a pseudo -second-order kinetics, with high correlation coefficients (R 2 ) for Cd(II), Pb(II), and Cr(VI) of 0.97573, 0.97348, and 0.91017 using L1@MCM-41 , and 0.9754, 0.97089, and 0.89411 using L1@SBA-15 , respectively. Equilibrium data best fitted the Freundlich isotherm model, with R 2 values of 0.97952, 0.99892, and 0.97374 for L1@SBA-15 and 0.99879, 0.99999, and 0.90923 for L1@MCM-41 , corresponding to Cd(II), Pb(II), and Cr(VI), respectively. In competitive metal ion systems, the extraction selectivity followed the order Cd(II) > Pb(II) > Cr(VI), with L1@SBA-15 exhibiting superior overall performance compared to L1@MCM-41 . The extraction mechanism was postulated to occur through the coordination of the metal ions to the nitrogen/sulfur donor atoms in the chelating agents, consistent with the hard and soft acid and base (HSAB) principle. Furthermore, L1@MCM-41 demonstrated notable regeneration potential, retaining Cr(VI) extraction efficiencies over four successive cycles. Graphical
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TALANTA
·
2024
·
IF 5.6
Xueyun Wei,Zhuomin Zhang,Gongke Li
Aromatic disinfection by-products (DBPs) have garnered considerable interest in recent years for their potential carcinogenicity. However, efficient separation and enrichment of DBPs in complex samples is a challenge due to the extremely low content of aromatic DBPs and the complexity of sample matrices. In this study, a MIL-101(Cr)–NH 2 @TAPB-DVA-COF hybrid material was prepared as the enrichment medium of membrane solid-phase extraction (M-SPE) to efficiently determine trace emerging aromatic DBPs. This medium exhibited excellent enrichment capacity and selectivity for aromatic DBPs because of the strong hydrogen bonding, π-π stacking and hydrophobic interactions. An efficient analytical method for five aromatic DBPs in juice drinks was successfully established by use of this hybrid material as the enrichment medium for M-SPE in combination with liquid chromatography tandem mass spectrometry (LC-MS/MS). The limits of detection of the established method were from 0.50 to 3.00 ng/L. Moreover, the method had been successfully used in real juice drinks to determine trace five aromatic DBPs with the spiked recoveries ranging from 84.1% to 125%. The method possessed high analytical sensitivity and accuracy for these five aromatic DBPs in juice drinks with the aid of the efficient M-SPE technology proposed.
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JOURNAL OF HAZARDOUS MATERIALS
·
2026
·
IF 10.6
Yongji He,Jiamin Zhang,Wei Li,Xiangtao Huo,Haokun Li,Min Guo,Mei Zhang
In order to achieve the harmless and resource-efficient treatment of hazardous elements in vanadium extraction tailings, a one-step reductive smelting separation process was developed to transfer the toxic elements Cr and V into a high valuable vanadium containing ferrochrome alloy. Under the optimal parameter of basicity 1.2, C/O molar ratio 1.2, holding temperature 1550 °C and holding time 50 min, the reduction rate of Fe, V and Cr from vanadium extraction tailings reached 96.14%, 95.98%, 93.60%, respectively, with the simultaneous production of Fe-Cr-V alloy and Ti-rich slag. The hardness of the alloy was 42.27 ± 0.65 HRC and the average friction coefficient was 0.678 ± 0.001, indicating that it basically meets the standards for wear-resistant materials. Toxicity leaching test results demonstrate that the leaching concentrations of Cr and V were 0.030 and 0.013 mg/L, respectively, which were 1/32 and 1/2825 of those in the original slag. These results confirm that the tailings have been effectively rendered harmless and detoxified. Hence, this one-step reductive smelting separation method synchronously realizes metal recovery, wear-resistant alloy preparation and Ti-rich residue co-production, achieving the complete utilization of hazardous vanadium extraction tailings, and provides an effective technical approach for the resource treatment of other toxic waste residues.
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Analytical Methods
·
2023
·
IF 3.1
Yan Wu,Chengwei Zuo,Yujie Mou,Hao Wang,Yongrui Hou,Xiaodong Su,Zhenfu Jia,Huidong Qiu
In this study, a new type of red light-emitting carbon dots (R-CDs) that can selectively recognize Cr(VI) was prepared by using the strategy of 2,4-diaminophenol to enhance the fluorescence of O-phenylenediamine based carbon dots. The results showed that 2,4-diaminophenol increased the quantum yield (QY) of carbon quantum dots (CDs), and the QY of CDs increased from the original 8.7% to 20.1%(R-CDs). R-CDs show sensitivity to acidic conditions and maintain good linearity between pH = 1.00-4.00, making them useful for pH probes. Furthermore, the prepared R-CDs possess good solubility in water. They are responsive to changes in Cr(VI) concentrations in aqueous environments. R-CDs' quenching was linearly correlated with the Cr(VI) concentration within a range of 0-20 μM, with a lower detection limit of 66 nM. The detection mechanism is attributed to the formation of hydrogen bonds between Cr(VI) and R-CDs, resulting in the fluorescence quenching of R-CDs. R-CDs could be considered effective multifunctional fluorescent probes for pH and Cr(VI) in aqueous environments. This study will provide new R-CD design strategies that selectively identify specific target substances.
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SCIENCE OF THE TOTAL ENVIRONMENT
·
2023
·
IF 9.8
Kunlun Yang,Yanxiao Chi,Yuxuan Yang,Zimo Lou,Tonghui Wang,Dengyang Wang,Hengfeng Miao,Xinhua Xu
To avoid severe aggregation and synergistically utilize the intrinsic and photocatalytic reducibility, pyrite (FeS 2 ) was loaded onto N-doped reduced graphene oxides (N-rGO) to fabricate a novel FeS 2 /N-rGO heterojunction catalyst for enhanced chromium (Cr(VI)) reduction in oxic condition to simultaneously investigate the specific effect and role of dissolved oxygen (DO). Characterization results showed that strong interaction and combination of FeS 2 and N-rGO not only achieved the uniform distribution of FeS 2 , but also increased the defects, and exposed more functional groups. Meanwhile, the Type II heterojunction was formed in FeS 2 /N-rGO, which facilitated the separation efficiency of photo-generated carriers and electrons, endowing FeS 2 /N-rGO a superior photocatalytic activity. Cr(VI) was almost completely reduced via FeS 2 /N-rGO within 60 min under irradiation (Cr(VI) = 10 mg/L, dosage = 0.2 g/L), 3 times that of pristine FeS 2 (18.7 %). Trapping and Electron Spin Resonance (ESR) experiments indicated that photo-generated e − and derived O 2 − species from photoactivation of dioxygen (DO) were the key reactive species for the enhancement of photo-assisted Cr(VI) reduction, rather than reductive Fe 2+ and S 2 2− species. Although the photocatalysis of FeS 2 /N-rGO cannot directly generate hydroxyl radicals ( OH), the oxidative OH ascribed to superoxide radicals ( O 2 − ), photo-induced holes and free DO preferentially consumed by Fe 2+ and S 2 2− with stronger reducibility. Hence, as compared to the anoxic condition , the reduction rate of Cr(VI) was slightly decreased, but still could be totally removed within 60 min in the oxic conditions. Due to the excessive amount of FeS 2 /N-rGO, Cr(III) after reduction would not be influenced by oxidative species and maintain stability under oxic condition. This study provided a facile modification strategy for FeS 2 based composites and uncovered its working mechanism for Cr(VI) decontamination .
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CRYSTAL GROWTH & DESIGN
·
2018
·
IF 3.972
Wei Zhang,Run-Zhi Zhang,Yong-Qing Huang,Ji-Min Yang
Herein, we report that the surface charge status and size of the metal–organic framework (MOF) MIL-101(Cr) can be tailored by varying the concentration of tetramethylammonium hydroxide. The adsorption capacity of MIL-101(Cr)-2 toward the anionic dye Congo red (CR) was found to be significantly higher than that of other MIL-101(Cr) adsorbents, although MIL-101(Cr)-3 microcrystals exhibited the highest adsorption capacity toward the anionic dye methyl orange (MO) due to the different adsorption mechanisms involved. This is the first demonstration of the synergetic interplay between the electrostatic and π–π interactions, adsorption spaces and sites, and size of the dye molecules, in terms of the uptake capacity of an adsorbent. In addition, the obtained results shed new light on the adsorption mechanism toward organic dyes over MOFs. Moreover, the MIL-101(Cr) microparticles exhibited excellent adsorption capabilities toward CR, achieving a maximum capacity of 1367.1 mg g–1, which is higher than the majority of reported values for other materials. Therefore, these results indicate that the MIL-101(Cr) nanostructure exhibits potential for application in the treatment of anionic dye-containing wastewater.
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ANALYST
·
2018
·Vol. 143
·期 8
·1906-1915
·
IF 3.864
Baogang Wang,Yan Lin,Hui Tan,Mina Luo,Shanshan Dai,Hongsheng Lu,Zhiyu Huang
N-Doped carbon dots (CDs) were directly synthesized with a high yield of 21.85% by one-pot pyrolysis of a gel composed of ethanolamine and 1-carboxyethyl-3-methylimidazolium chloride at 220 °C for 2 h. The as-synthesized CDs with a mean particle size of 7.8 nm were uniform, amorphous, and abundant in nitrogen content (23.15 wt%) and surface groups such as amide and hydroxyl. Thus, the CDs exhibited good water-solubility, bright blue excitation- and pH-dependent fluorescence with a quantum yield of 17.93%, and high ionic strength tolerance. In addition, a CD-based fluorescent sensor towards Cr(VI) ions with favorable sensitivity and selectivity was constructed based on the inner filter effect. Two good linear relationships between the concentration of Cr(VI) ions and the PL quenching efficiency were obtained in the ranges from 0.2 to 2 (R2 = 0.9965) and 2–40 μM (R2 = 0.9918), and the limits of detection (LOD = 3σ/S) were calculated as 0.018 and 0.25 μM, respectively. Importantly, this sensor was solid and capable of rapidly detecting Cr(VI) ions in tap water with detection ranges of 0.2–2 (R2 = 0.9817) and 2–60 μM (R2 = 0.9902), LODs of 0.048 and 0.40 μM, and recoveries of 102.1–106%.
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TALANTA
·
2016
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IF 4.035
Xinpeng Dai,Xiuna Jia,Pan Zhao,Ting Wang,Jian Wang,Peiting Huang,Lu He,Xiaohong Hou
As a novel kind of materials, metal-organic frameworks (MOFs) have great potential for the preconcentration of trace analytes. In our work, MIL-101(Cr) was prepared and applied as a solid phase extraction (SPE) sorbent for the pretreatment of sulfadiazine (SDA), sulfamethazine (SMZ), sulfachloropyridazine (SCP) and sulfamethoxazole (SMX) in different environmental water samples coupling with ultra-high performance liquid chromatography-tandem mass spectrometry (UPLC-MS/MS) detection. Experimental parameters, such as SPE materials, pH of water sample, volume of sample, flow rate , and type and volume of elution solvent, were properly optimized. Under the optimum conditions, good sensitivity levels were achieved with the detection limits of 0.03–0.08 μg/L and the quantitation limits of 0.11–0.27 μg/L. The linear ranges were from 0.2–40 or 0.5–100 μg/L ( r 2 >0.996) for the analytes, and the relative recoveries were in the range from 83.5% to 107.3% with the relative standard deviations (RSD) between 0.2% and 8.0% ( n =6). In addition, computational simulation was primarily used to predict the adsorption of MIL-101(Cr) toward sulphonamides (SAs), and also demonstrated the molecular interactions and free binding energies with the molecular modeling method. The results revealed that the combination of experimental and computational study not only accurately recognized the adsorption of MIL-101(Cr) on SAs, but also provided a new strategy on the trace contaminant analysis.
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
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2023
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IF 5.2
Binxia Zhao,Nan Shao,Xingliang Chen,Jixian Ma,Yijia Gao,Xiaoqian Chen
As a novel photocatalyst with visible light responsiveness, Bi 2 WO 6 has excellent activity in treating wastewater containing organic pollutants and noble metals. However, its photocatalytic action is limited due to the rapid recombination of photogenerated electrons and holes. Based on the study of Bi 2 WO 6 , a type Ⅱ heterojunction photocatalyst (WO 3 /Bi 2 WO 6 ) and a Z-scheme heterojunction photocatalyst (CdS/Bi 2 WO 6 ) were constructed. Composites exhibited higher catalytic activity than pure Bi 2 WO 6 . The degradation efficiency of RhB(50 mg/L) and reduction efficiency of Cr(VI) (50 mg/L) by 5%WO 3 /Bi 2 WO 6 catalyst within 60 min of photocatalytic reaction was 98.82% and 53.82%, respectively. The degradation efficiency of RhB and reduction efficiency of Cr(VI) by 15%CdS/Bi 2 WO 6 catalyst was 99.52% and 69.52%, respectively. By studying the structural composition , microscopic morphology, photoelectrochemical performance, and light absorption performance of the catalysts of the two different systems. These mechanisms may help to explain the reasons for the enhanced activity of the composite photocatalysts. In addition, mixed wastewater containing organic pollutants (RhB) and heavy metal ions (Cr(VI)) was used to simulate real and complex wastewater, which provided more ideas for wastewater treatment problems.
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高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2019
·
IF 8.355
Feihu Mu,Qiong Cai,Hao Hu,Jian Wang,Yun Wang,Shijian Zhou,Yan Kong
To solve the problem of energy shortage and environmental pollution, the construction of properly designed photocatalysts is a promising method. Here, UiO-66-(COOH) 2 /ZnIn 2 S 4 Z-scheme photocatalyst decorated with MoS 2 nanosheets was designed and constructed as a novel 3D hierarchical structure via hydrothermal methods. In this particular 3D hierarchical structure, the UiO-66-(COOH) 2 nanoparticles are decorated in the interweaving petal nanosheets of ZnIn 2 S 4 microspheres, while the co-catalyst of MoS 2 is folded at the edge of these interweaving petals. The excellent heterojunctions with highly exposed catalytic active sites are correspondingly built, and the close interfacial interaction between UiO-66-(COOH) 2 , MoS 2 and ZnIn 2 S 4 create a stage for fast transfer of photogenerated electrons, which are both effective for the photocatalytic reaction process. Also, the Z-scheme charge-transfer process improves the oxidizability and reducibility between UiO-66-(COOH) 2 and ZnIn 2 S 4 . As a result, the optimized UiO-66-(COOH) 2 /MoS 2 /ZnIn 2 S 4 photocatalyst exhibits excellent photocatalytic hydrogen production (18.794 mmol h −1 g −1 ) and reduction of Cr(VI) (0.06850 min −1 ) under simulated solar light irradiation, which are 15.3 and 6.7 times higher than that of bare ZnIn 2 S 4 , respectively, and also the prominent stability and excellent recyclability are obtained. This study provides new insights into the research on the Z-scheme system containing MOF components for growing energy and environmental demands.
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