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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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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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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PubMed
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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
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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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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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SPECTROCHIMICA ACTA PART A-MOLECULAR AND BIOMOLECULAR SPECTROSCOPY
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2024
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IF 4.3
Jiaying Zeng,Ting Zhang,Geyu Liang,Jingwen Mo,Jianxiong Zhu,Longhui Qin,Xiaojun Liu,Zhonghua Ni
Hexavalent chromium (Cr(Ⅵ)) is a significant environmental pollutant because of its toxic and carcinogenic properties and wide use in various industries. Hence, there is an urgent need to develop accurate and selective approaches to detect the concentration of Cr(Ⅵ) in agricultural and aquaculture products to help humans avoid potential hazards of indirectly taking in Cr(Ⅵ). In this work, we report a “turn off–on” fluorescent sensor based on citric acid coated, 808 nm-excited core–shell upconversion nanoparticles (CA-UCNPs) and self-assembled copper porphyrin nanoparticles (nano CuTPyP) for sensitive and specific detection of Cr(Ⅵ). Nano copper 5, 10, 15, 20-tetra(4-pyridyl)-21H–23H- porphine obtained by acid-base neutralization micelle-confined self-assembly method function as an effective quencher due to its excellent optical property and water solubility. Through electrostatic interactions, positively charged nano CuTPyP are attracted to the surface of negatively charged CA-UCNPs, which can almost completely quench the fluorescence emission. In the presence of Cr(Ⅵ), nano CuTPyP can discriminatively interact with Cr(Ⅵ) and form nano CuTPyP/Cr(Ⅵ) complex, which separates nano CuTPyP from CA-UCNPs and restores the fluorescence. The sensing system exhibits a good linear response to Cr(Ⅵ) concentration in the range from 0.5 to 400 µM with a detection limit of 0.36 µM. The sensing method also displays high selectivity against other common ions including trivalent chromium and is applied to the analysis of Cr(Ⅵ) in actual rice and fish samples with satisfactory results.
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DIAMOND AND RELATED MATERIALS
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2024
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IF 4.3
Tao Chen,Luzhao Xing,Shaojun Niu
Here, a novel magnetic nitrogen-rich biochar (MNRB), synthesized by attaching Fe 3 O 4 @SiO 2 -NH 2 particles with core-shell structure on crab shell derived/nitrogen-rich biochar (NRB), was used as absorbent and reductant to remove hexavalent chromium in aqueous systems. Characteristics of the material demonstrated that the MNRB was rich in nitrogen-containing functional groups and that the Fe 3 O 4 @SiO 2 -NH 2 magnetic particles with a diameter of approximately 150 nm were successfully added on the MNRB surface by strong ether linking (C-O-C). The maximum removal capacity of MNRB was 152.9 mg·g −1 , which was considerably higher than most reported magnetic biochar. Study of the removal mechanisms revealed that the Cr(VI) removal by MNRB involved three steps: (1) adsorption of Cr(VI) anions by protonated functional groups; (2) reduction of Cr(VI) anions to Cr(III) cations by electron-donor groups; and (3) chelation of Cr(III) cations by amine groups. The easy regeneration, satisfactory reusability, and remarkable performance in batch tests reflected the high potential of MNRB for treating Cr(VI)-contaminated water.
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ACS Applied Electronic Materials
·
2025
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IF 4.7
Ting Zhang,Xiaoqian Zhang,Qinan Mao,Fangyi Zhao,Heyi Yang,Xinyue Li,Jiasong Zhong
Lanthanide doping has been instrumental in tuning the emissions of double perovskite halides (DPHs) into the near-infrared (NIR) region. However, the limited penetration depth of UV excitation and typically low photoluminescence quantum yield (PLQY) of these materials restrict their utility in biomedical applications. In this paper, Cr3+-doped lead-free DPHs (Cs2NaScCl6:Cr3+) have been explored, featuring a broadband NIR emission spanning 800–1300 nm and an impressive PLQY of 76.9%. Oriented toward biological applications, we employ Yb3+ as a codopant to be introduced into Cs2NaScCl6:Cr3+. The novel Cs2NaScCl6:Cr3+,Yb3+ crystal powder displays a red-shifted emission (peaking at 995 nm) with a remarkably narrower full width at half-maximum (fwhm) of 51 nm. Importantly, the efficient energy transfer between Cr3+ and Yb3+ enables Cs2NaScCl6:Cr3+,Yb3+ to maintain a PLQY of 46.1% upon 780 nm excitation. Leveraging its NIR-I excitable and NIR-II emissive properties, Cs2NaScCl6:Cr3+,Yb3+ presents great potential in biodetection and bioimaging applications. Its superior energy transfer efficiency, high PLQY, and favorable spectral characteristics position this material as a promising candidate for advanced biomedical techniques requiring deep tissue penetration and high imaging contrast.
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
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2024
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IF 4.9
Tien Tran Nguyen,Minh Kim Nguyen,Vipin Kumar,Ha Huu Do,Anh Thi Kim Le,Anh Van Nguyen,Jin Seog Gwag,Pham Cam Nam,Le Gia Trung
The widespread use and subsequent release of antibiotics by humans and animals pose health and environmental risks, compelling their removal from aquatic ecosystems. MIL-101(Cr), a metal-organic framework (MOF), exhibits versatile applications in antibiotic adsorption owing to its exceptional structural characteristics. In this context, MIL-101(Cr) nanoparticles are successfully prepared via the hydrothermal method to remove pefloxacin (PEF) from aqueous solutions. The resulting MIL-101(Cr) adsorbents showcase high crystallinity (97.6%), a large surface area (3166 m 2 /g), broad nanopore sizes, good thermal stability, and efficient reusability. Factors including initial PEF concentration, pH, dosage of adsorbent, and temperature are thoroughly investigated. The findings reveal a good adsorption capacity (254.3 mg/g) with an optimal removal efficiency (99.7%) at 308 K in a neutral pH of 7.0 when the adsorbent dosage is 250 mg/L and the initial PEF concentration is 200 mg/L within 80 min of contact. Among the three adsorption isotherms (Langmuir, Freundlich, Temkin models), the Langmuir equation best fits the studies, indicating a maximum adsorption capacity of 253.8 mg/g at 25°C, while the experimental equilibrium adsorption capacity is 229.2 mg/g at the same temperature. Adsorption kinetics aligns with the pseudo-second-order model. Thermodynamic parameters and activation energy affirm the endothermic and spontaneous behavior of the adsorption process, attributed to both physisorption and chemisorption. This study highlights the promising potential of synthesized MOF nanocrystals as an effective adsorbent for antibiotics in wastewater treatment and environmental remediation.
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Journal of Environmental Chemical Engineering
·
2024
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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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Journal of Environmental Chemical Engineering
·
2024
·
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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