INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
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2024
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IF 3.8
Douhao Yang,Ruiting Jian,Jianjun Yan,Ao Zhang,Bowen Liu,Zhongwei Liu
Defect engineering has a great effect on the properties of metal–organic frameworks (MOFs). In this study, the defective UiO-66-NH2 MOFs are successfully prepared by a rapid Ar plasma modification method. At certain experimental conditions (15 W radio frequency input power, 20 Pa working pressure, and 120 s Ar plasma modification time), the afforded UiO-66-NH2 shows significant enhancement in photocatalytic reduction of Cr(VI), and a maximum reduction efficiency of 68.5% is obtained. Advanced characterizations show that the plasma treatment generates missing-linker defects within the UiO-66-NH2 structure, which can enhance the separation of photogenerated electrons and holes and improve the photoreduction capability. The findings not only contribute to a better understanding of the relationship between the structure and performance of MOFs but also provide a simple approach for defect engineering of MOFs.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2024
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IF 9.4
Bing Hou,Xinyu Yang,Ling Wang,Tao Shi,Muhammad Akram,Lei Wang,Jun Wan,Baoyu Gao,Jingwen Pan
Cerium-based adsorbents possessed unique advantages of valence variability and abundant oxygen vacancies in hexavalent chromium (Cr(VI)) adsorption, but high cost and unstable properties restricted their application in Cr(VI) contained wastewater treatment. Herein, a series of bimetallic adsorbents with different cerium/iron ratios (CeFe@C) were prepared by adding inexpensive Fe into Ce-based adsorbents (Ce@C), and the effect of Fe doping on adsorption properties of Ce@C for Cr(VI) was investigated thoroughly. Compared with pristine Ce@C, CeFe@C exhibited excellent removal performance for Cr(VI), and the improved maximum adsorption capacity reached 75.11 mg/g at 25℃. Benefiting from Fe doping, CeFe@C had good regeneration property, with only 25 % decrease after five adsorption–desorption cycles. Contents of trivalent cerium (Ce(III)) and oxygen vacancies (O v ) in bimetallic adsorbents were positively correlated with divalent iron (Fe(II)) doping, indicating that the formation of Ce(III) and surface defects on Ce@C could be effectively regulated by Fe doping. Density functional theory (DFT) calculation results further proved that the doped Fe enhanced the electron transfer effectively and lowered the energy barriers of Cr(VI) adsorption onto Ce@C surface, strengthening the reduction and complexation to Cr(VI). This study provides new insights for improving the Cr(VI) removal performance by modified Ce-based adsorbents, and further promotes the utilization potentiality of low-cost and low-toxicity Ce-based adsorbents in Cr(VI)-containing wastewater treatment.
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INORGANIC CHEMISTRY
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2025
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IF 4.7
Longying Duan,Ting Cheng,Yanyue Zhu,Yuping Wang,Yanxin Gao,Jinhong Bi
Environmental concerns are driving the development of eco-friendly and effective methods for contaminant monitoring and remediation. In this study, a lanthanide porphyrin-based MOF with dual fluorescence sensing and photocatalytic properties was synthesized and applied for the detection and combined removal of Cr(VI) and ciprofloxacin (CIP). Using different excitation wavelengths, the material exhibited selective detection of Cr(VI) via fluorescence quenching and CIP through fluorescence enhancement. The variation in color intensity of Tb-MOF on 3D EEM spectra enabled simultaneous detection of both contaminants. Additionally, Tb-MOF demonstrated a synergistic removal effect, achieving over 95% removal rates of Cr(VI) and CIP within 90 min, with consistent sensing and catalytic performance across four cycles. Mechanistic investigations revealed that (i) strong coordination between Tb3+ and CIP altered the surface potential of Tb-MOF, enhancing Cr(VI) adsorption; (ii) as an efficient electron acceptor, Cr(VI) promoted electron transfer and its reduction to Cr(III); and (iii) superoxide radicals generated via a type I mechanism played a key role in CIP degradation. This research underscores the potential of Tb-MOF as a multifunctional platform for simultaneous detection and synergistic remediation of mixed pollutants.
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高影响因子
ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH
·
2024
·Vol. 31
·期 19
·28695-28705
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IF 0
Liu Hongyu,Ye Wei,Zhang Huan,Wang Huicai,Wei Junfu
Here, polyaniline/polyvinylidene fluoride (PANI/PVDF) nanofiber composite membrane was fabricated using electrostatic spinning technology to remove hexavalent chromium Cr(VI). The employment of PANI not only extremely enhanced the hydrophilic property of the nanofiber membrane, but also facilitated the transfer of Cr 2 O 7 2− from water to the membrane. The PANI/PVDF membrane had an extremely excellent performance in getting rid of Cr(VI) and a quite large flux (250 L/m 2 h). The maximum adsorption quantity of the membrane could reach 334.5 mg/g in which adsorption played 52.12% part and reduction played 47.87% part. The removal rate could reach nearly 100% immediately in the permeate solution under filtration while it needed 240 min to reach 100% only by static adsorption. Therefore, the interception of the membrane and the adsorption reduction of PANI had synergistic effect on removal of Cr(VI). Furthermore, the removal rate of Cr(VI) could still reach 95.97% after reused 8 times. The membrane showed a very good reusability and application prospect. Graphical Abstract
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Journal of Environmental Chemical Engineering
·
2024
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IF 7.4
Min Zhang,Mingxuan Du,Yuhang Ren,Yun Zhu,Yunyuan Dong,Jianming Liao,Xiaobin Chen,Qifu Zheng,Hongfei Yin
Element doping is generally employed to modify photocatalysts by optimizing their electronic structure, and light absorption , as well as improving charge separation and transfer, which are key factors in photocatalysis . In this study, a simple one-step solvothermal route was employed to synthesize N, O co-doped ZnIn 2 S 4 . Systematical analyses demonstrate that the introduction of N and O co-doping leads to enhanced light absorption, increased specific surface areas , and improved charge separation and transfer in comparison to the unmodified ZnIn 2 S 4 . As expected, compared with bare ZnIn 2 S 4 , the as-prepared N, O co-doped ZnIn 2 S 4 exhibits superior photocatalytic H 2 evolution and Cr(VI) photoreduction performance. The H 2 evolution rate of the N, O co-doped ZnIn 2 S 4 reaches 2254.0 μmol g −1 h −1 , which is 2.8 times of pristine ZnIn 2 S 4 . Moreover, the Cr(VI) photoreduction efficiency reaches 99.5 % within 50 minutes, and the apparent kinetic constant is nearly 4 times the bare ZnIn 2 S 4 . This work contributes to the modification of ZnIn 2 S 4 for photocatalytic H 2 generation and Cr(VI) reduction.
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Journal of Environmental Chemical Engineering
·
2024
·
IF 7.4
Mengyuan Huang,Yuanyuan Yang,Hui Cao,Min Yuan,Tai Ye,Liling Hao,Jinsong Yu,Fengqin Yin,Fei Xu,Xiuxiu Wu
Cr(VI) is a representative heavy metal which has significant toxicity to biological organisms. Ion-imprinted polymers (IIPs) have been recognized as effective adsorbents to remove Cr(VI) from environment. Among them, imidazole derivatives are expected to serve as potential monomers for Cr(VI)-IIPs, but the binding mechanisms of monomers with Cr(VI) remain unclear, which makes Cr(VI)-IIPs design having rare sound theory to be guideline. In this work, the suitable functional monomer of Cr 2 O 7 2- -IIPs was screened among five imidazole derivatives (adenine, cytosine, uric acid, l-histidine, 1-methacryloyl imidazole) with a target-monomer binding affinity guide strategy, and the optimal self-assembling conditions were investigated using theoretical calculations and experimental methods. Adenine exhibited the highest potential among the five candidate monomers, followed by cytosine. The optimal ratio of target and monomer was determined to be 2:3. Furthermore, a 5:5 mixture of ethanol and cyclohexane was identified as the most suitable solvent for the pre-polymerization environment, while epichlorohydrin acted as the most appropriate crosslinker. Additionally, the binding nature of non-covalent interaction between target and monomer was identified to be electrostatic-dominated hydrogen bonding. These mechanistic insights provide valuable theoretical support for the rational design of Cr 2 O 7 2- -IIPs, which are significant for IIPs development as adsorbents for contaminants detection and removal from environment.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2024
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IF 8.1
Chen Wang,Xiaohui Wu,Mingjie Huang,Tao Zhou,Juan Mao,Xiangling Zhang
Treatment of Cr(VI)-contaminated wastewaters by conventional reduction methods has been intensively challenged by alkaline environments. In this study, a novel copper-iron oxide composite (Cit@CuFeO) enriched with oxygen vacancies (OVs) was developed by ball milling with citric acid ligand (Cit). The material demonstrated efficient Cr(VI) removal within a broad pH range (6.0–12.0). Intriguingly, simultaneous and nearly complete in-situ immobilization of Cr(III) occurred, instead of precipitated in strong alkaline circumstances. Characterizations of the Cit@CuFeO revealed that ball milling of Cit could introduce abundant OVs into the oxide structure, serving as pivotal active sites linearly correlated with Cr(VI) capture and removal. These generated OVs could also boost electron conduction in Cit@CuFeO and cause a positive shift in the zeta potential , thereby enabling the adsorption of negative CrO 4 2- at high pH. Furthermore, DFT calculation verified that the surface-attached Cit would significantly decrease the adsorption energy of Cr(VI) at OVs sites, competitively excluding the occupancy of common inorganic anions especially CO 3 2– and thus favoring the Cr(III) immobilization under alkaline conditions. This study has provided a green functional material for the one-step remediation of alkaline Cr(VI) wastewaters without the need for acidification.
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SPECTROCHIMICA ACTA PART A-MOLECULAR AND BIOMOLECULAR SPECTROSCOPY
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2024
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IF 4.3
Yi Gu,Yang Jiao,Ya Ruan,Jing Yang,Yaling Yang
Herein, a nanocomposite of Cu,Ce-containing phosphotungstates (Cu,Ce-PTs) with outstanding laccase-like activity was fabricated via a one-pot microwave-assisted hydrothermal method. Notably, it was discovered that both Fe 3+ and Cr 6+ could significantly enhance the electron transfer rates of Ce 3+ and Ce 4+ , along with generous Cu 2+ with high catalytic activity, thereby promoting the laccase-like activity of Cu,Ce-PTs. The proposed system can be used for the detection of Fe 3+ and Cr 6+ in a range of 0.667–333.33 μg/mL and 0.033–33.33 μg/mL with a low detection limit of 0.135 μg/mL and 0.0288 μg/mL, respectively. The proposed assay exhibits excellent reusability and selectivity and can be used in traditional Chinese medicine samples analysis.
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
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2024
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IF 4.9
Mengjie Huang,Mengjia Zhang,Xinyu Huan,Yuanyi Li,Wei Wei,Yong Zhang
Microplastics (MPs) commonly undergo aging in various environmental media, affecting both their environmental behavior and Trojan-horse effect for contaminants. However, the mechanisms underlying the different impact of various aging processes on the Trojan-horse effect of polyamide (PA) MPs towards metal oxyanions remain unclear. This study explored how chemical aging and UV irradiation impact the structural characteristics and Cr(VI) adsorption of PA MPs under various influencing factors. Results showed that both aging processes enhanced the negative surface charge, surface oxygen content, and roughness of PA MPs, with FTIR correlation spectroscopy confirming an increase in O-containing functional groups. Cr(VI) adsorption onto aged PA sharply increased by 17.4 % (14 days of UV irradiation), 39.4 % (42 days of UV irradiation), and 21.7 % (chemical aging) compared to original PA. Salinity and natural organic matter had adverse effects on Cr(VI) adsorption. Spectroscopic analyses highlighted the crucial role of hydrophilic amide groups in controlling Cr(VI) adsorption onto aged PA, involving hydrogen bonding, electrostatic interactions, and reduction. Aged PA exhibited higher adsorption capacities but also greater desorption under simulated seawater and intestinal fluid, suggesting increased migration potential for Cr(VI). This study provides helpful insights into assessing the environmental risk of co-existing PA MPs and metal oxyanions, particularly considering the effect of aging processes.
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CRYSTENGCOMM
·
2025
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IF 2.6
Han Fang,Jia-Peng Han,Bo Zhang,Deng-Bo Liu,Xing-Wang Li,Jing-Yu Li,Yutong He,Mei-Hui Yu
The heavy metal ion pollution has become one of the most serious environmental problems, which promotes the continuous exploration of new materials and methods to achieve efficient detection of heavy metal ions. Luminescent metal-organic frameworks (LMOFs) featuring the designable and functional structures and tunable luminescence properties exhibit excellent potential for the recognition and detection of heavy metal ions. Herein, a Cd(II)-based luminescence MOF {[Cd2(2F-bpdc)2(tib)]}n (NKM-103) (tib=1,3,5-tris(1-imidazolyl)benzene, 2F-H2bpdc= 3,3'-difluorobiphenyl-4,4'-dicarboxylic acid) has been designed and synthesized successfully. Derived from the characteristic of ligand with conjugated units, NKM-103 shows well fluorescence emission performance and potential as a sensor for detecting both Fe(III) cations and Cr(VI) anions (Cr2O72- and CrO42-) through turn-off effect. Moreover, NKM-103 for all three kinds of ions shows low detection limit and high selectivity.
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Journal of Environmental Chemical Engineering
·
2024
·
IF 7.4
Zewan Qin,Qing Guan,Yating Lu,Yu Tian,Xia Yang
The naphthalene tetracarboxdiimide (NDI) modified NH 2 -UiO-66(Zr) and NH 2 -MIL-101(Cr) (NDI/UZr and NDI/MCr for short) metal organic frameworks (MOFs) materials with strong covalent bond O C–N–C O were designed and prepared by solvothermal method. The comprehensive physical and chemical properties of the materials were characterized, and the adsorption and photocatalytic properties of the materials were evaluated by using methylene blue (MB) and Cr(VI) in single and mixture system. When the initial concentration of MB was 50 mg·L −1 , the photocatalytic degradation rate constant of NDI/MCr(2:1) was 10.3 and 13.8 times higher than that of NH 2 -MIL-101(Cr) and NDI/UZr(2:1), respectively. Additionally, NDI/MCr(2:1) exhibited 1.6 times higher reaction rate constant than that of NDI/UZr(2:1) for the removal of 10 mg∙L −1 Cr(VI). The enhanced adsorption and photocatalytic ability over NDI/MOFs were attributed to the MOFs larger specific surface area and wider spectral response, and NDI showed high electron affinity, superior charge carrier transport properties. Free radical and electron capture experiments indicated that h + , •O 2 − , and e − were the main active species in the NDI/MOFs system. Among them h + and •O 2 − played an essential role in the removal of MB, while e − and •O 2 − contributed to the photocatalytic reduction of Cr(VI). The mechanism of the photocatalytic process was discussed in detail.
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CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Zishen Lin,Chunli Zheng,Zhenxing Wang,Yuanzhe Peng,Guoqing Geng,Aibin Zhu,Chi He
As one category of promising and efficacious purification material toward environmentally harmful heavy metals, sulfidated amorphous zero-valent Iron (S@AZVI) exhibits unparalleled removal performance. Due to the disruptive crystal growth however, the irreversible loss of Fe 0 component during conventional synthesis route poses a substantial hindrance to its industrial application. To address this, we propose a post-sulfidation strategy to hinder the transformation of Fe 0 by altering the shell composition of AZVI from Fe 2 O 3 to FeS, which maintains a remarkable Fe 0 content up to 75.7 % over finally obtained S@AZVI, far higher than the material obtained through the one-step sulfidation . Attributing to the synergy of FeS shell and substantial Fe 0 , S@AZVI demonstrates impressive performance as the lowest free corrosion potential (−1.050 V) and work function (4.058 eV), and subsequently exhibits a notable enhancement in the removal efficiency of Cr(VI) and Ni(II), surpassing AZVI by 1.8 and 2.0 times, respectively. Results reveal that the adsorption, reduction, and coprecipitation constitute the mechanisms governing the removal of Cr(VI) and Ni(II). In practical electroplating wastewater experiments, S@AZVI effectively removes Cr(VI) and Ni(II) within a 60-min timeframe, meeting established emission standards. These findings provide valuable insights for future AZVI material synthesis for heavy metal elimination.
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