ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH
·
2024
·Vol. 31
·期 17
·25273-25286
·
IF 0
Chen Junxia,Yang Zhenzhen,Li Weigang,Yang Yuying,Zhu Feng,Huo Zongli,Zhou Qing
The poor conductivity, poor stability, and agglomeration of iron-based metal organic framework MIL-88A(Fe) limit its application as persulfate (PS) activator in water purification. Herein, MXene-supported MIL-88A(Fe) composites (M88A/MX) were synthesized to enhance its adsorption and catalytic capability for tetracycline (TC) removal. Scanning electron microscope (SEM), X-ray diffractometer (XRD), Fourier transform infrared spectrometer (FT-IR), and X-ray photoelectron spectroscopy (XPS) were used to characterize prepared materials, confirming the successful attachment of MIL-88A(Fe) to the surface of MXene. M88A/MX-0.2 composites, prepared with 0.2 g MXene addition, exhibit optimal degradation efficiency, reaching 98% under conditions of 0.2 g/L M88A/MX-0.2, 1.0 mM PS, 20 ppm TC, and pH 5. The degradation rate constants of M88A/MX-0.2 were 0.03217 min −1 , which was much higher than that of MIL-88A(Fe) (0.00159 min −1 ) and MXene (0.00626 min −1 ). The removal effects of reaction parameters, such as dosage of M88A/MX-0.2 and PS; initial solution pH; and the presence of the common co-existing constituents (humic acid and the inorganic anions) were investigated in detail. Additionally, the reuse of M88A/MX-0.2 showed that the composites had good cycling stability by recurrent experiments. The results of electron paramagnetic resonance (EPR) and quenching experiments indicated that ·OH, ·SO 4 − , and ·O 2 − were involved in the M88A/MX-0.2/PS system where persulfate oxidation process was activated with prepared M88A/MX-0.2. In addition, the intermediates of photocatalytic degradation were determined by HPLC–MS, and the possible degradation pathways of the target molecules were inferred. This study offered a new avenue for sulfate-based degradation of Fe-based metal organic framework.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2025
·
IF 9.7
Runlai Liu,Qi Chen,Jinjing Qiu,Cheng Liu,Jionghua Wu,Jimmy C. Yu,Ling Wu
The construction of metal–organic frameworks that possesses the tunable metal active sites and synergistic effect for the reactant activation is an attractive strategy for the optimization of photocatalytic performance. Herein, a series of MIL-88A(Fe 1-x Cu x ) were synthesized for photocatalytic nitrogen reduction reaction (NRR). It was characterized that the Fe 2+ and oxygen vacancies were produced in MIL-88A(Fe) due to the partly reduction of ligand fumaric acid in synthesis process. The substitution of Fe 3+ with Cu 2+ induces charge imbalance and lattice distortion, further increasing the content of Fe 2+ and oxygen vacancies. The optimal sample MIL-88A(Fe 0.95 Cu 0.05 ) (CMA-5 %) exhibits the highest nitrogen fixation performance of 68.6 μmol·g −1 ·h −1 , which is 8 times higher than that of the pristine material. It is attributable to the synergistic effect of the abundant Fe 2+ and oxygen vacancies as active sites to promote N 2 coordination and photogenerated carrier separation, resulting in the efficient conversion of activated N 2 to NH 3 . Furthermore, the in-situ Diffuse Reflectance Infrared Fourier Transform Spectroscopy provide clear evidence of the behavior of the N 2 adsorption and activation on the catalyst. Finally, we propose a potential mechanism at molecular level regarding the relationship between the synergistic effect and the nitrogen fixation activity.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2022
·
IF 9.136
Mingyu Li,Chaoqun Li,Zhao Chunrui,Tianren Li,Jingjing Jiang,Zhonghui Han,Chongjun Zhang,Haoran Sun,Shuangshi Dong
Fe-based metal organic framework with high active site exposure, wide light absorption and fast H 2 O 2 activation are pivotal for photo-Fenton degradation of contaminants. However, insufficient active site exposure, weak visible light adsorption and low charge transfer efficiency in iron-oxo clusters usually lead to the slow Fe(II)/Fe(III) cycle. In this study, we develop a novel citric acid (CA)-modified MIL-88A(Fe) strategy to boost photo-Fenton efficiency by accelerating Fe(II)/Fe(III) cycle for emerging contaminants removal. Relationship between CA coordination mode and photo-Fenton performance was studied by using methylene blue (MB) and carbamazepine (CBZ) as model contaminants. It was found that the degradation rate constants of MIL-88A(Fe)-CA-3 were 6.5 and 2.6 times higher than those in the pristine MIL-88A(Fe) for MB and CBZ degradation, respectively. The optimized MIL-88A(Fe)-CA-3 also exhibited good recyclability, enabling multiple cycles in photo-Fenton reaction. The results of experimental characterizations and density functional theory calculations demonstrated that ligand substitution was conductive to active site exposure, visible light absorption, charge carrier transfer and Fe 2+ /Fe 3+ redox cycle, which are responsible for an improved photo-Fenton performance.
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Molecular Catalysis
·
2022
·
IF 5.089
Weiwen Wang,Jianing Qu,Chaojie Li,Lexin Guo,Xianxin Fang,Guanghui Chen,Jihai Duan
Biomimetic photocatalytic nitrogen fixation is considered as a potential alternative to the Haber-Bosch method, which is an ideal pathway for nitrogen reduction. The development of efficient bionanocatalysts is a serious challenge in the current field of biomimetic nitrogen fixation. Here, we introduced a second metal in the MIL-88A/Fe mesh by metal doping to build a Mo-doped MIL-88A(Fe/Mo)/Fe mesh biomimetic system. The catalyst is a rod-like structure synthesized in situ by hydrothermal method using iron mesh as the substrate, and its rough surface is favorable for the adsorption of N 2 . The introduction of Mo provides a two-electron transfer pathway for the reaction, and the formation of the "MoFe cofactor" effectively promotes charge separation and inhibits the photoelectron-hole complexation. In addition, we kept the catalyst above the liquid surface and provided the proton source through water vapor, which solved the problem of the low solubility of N 2 in water and poor mass transfer efficiency. The results show that the biomimetic photocatalyst has good photoresponsiveness in the whole visible region, and the synergistic effect between the two metals makes the MIL-88A (Fe/Mo 0.017 )/Fe mesh exhibit better photocatalytic performance, and its nitrogen fixation efficiency reaches about 9.6 times that of the original MIL-88A/Fe mesh. This study provides a new idea for the design of photocatalytic ammonia biomimetic photocatalysts.
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JOURNAL OF SOLID STATE CHEMISTRY
·
2024
·
IF 3.2
Xuechang Ren,Ju An,Suying Ding,Zhenyu Yang,Miao Tian,Ning Fu
MoS 2 /MIL-88A (Fe) composite catalyst was prepared by in-situ formation method. The material was characterized by SEM, TEM, XRD and XPS, and the Rhodamine B(RhB) was activated and degraded by persulfate (PMS). The results showed that M-10/M 1:2 had the best degradation effect on RhB, the rate constant was 0.66420 min −1 , and the degradation rate could reach 1.89–14 times that of other doped composite catalysts. The SEM results showed that M − 10 had the least sulfur content, fewer MoS 2 flower layers and more exposed Mo 4+ atoms, which improved the electron transfer efficiency and accelerated the degradation reaction. The XPS spectra before and after M-10/M 1:2 reaction showed that the REDOX reaction of Fe 3+ /Fe 2+ and Mo 4+ /Mo 6+ on the catalyst surface played an important role in the activation of PMS. The results of free radical capture experiment and ESR test showed that the main active substances in M-10/M 1:2 /PMS reaction system were SO 4 •− , 1 O 2 , •O 2 − , and •OH, which only played a role in the degradation of RhB. Finally, based on the ESR results of M-10/M 1:2 /PMS system and the changes of Fe and Mo elements in XPS characterization before and after the reaction, the degradation mechanism of M-10/M 1:2 /PMS system was proposed.
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Molecular Catalysis
·
2022
·
IF 5.089
Nan Li,Changping Jian,Yaping Song,Li Wang,Ata Ur Rehman,Yanghe Fu,Fumin Zhang,De-Li Chen,Weidong Zhu
Herein, we reported a facile and scalable approach for the synthesis of Fe-based MOF MIL-88A(Fe) via a simple liquid-phase route at atmosphere pressure, and its application as a heterogeneous catalyst for the efficient aerobic oxidation of cyclohexene to value-added 2-cyclohexene-1-ol. Over 130 g of spindle-shaped MIL-88A(Fe) nanocrystals with high crystallinity, monodispersed particle size, and large specific surface area were easily synthesized per batch according to our method. The resultant MIL-88A(Fe) exhibited a high catalytic activity (conversion: 81%) with 70% selectivity for 2-cyclohexene-1-ol in the aerobic oxidation of cyclohexene with O 2 as the sole oxidant under mild reaction conditions (0.5 MPa of O 2 , 353 K for 8 h), outperforming the analogues reported in the literatures. The combined experimental and theoretical approach support the reaction mechanism of the oxidation of cyclohexene via both the free radical reaction pathway and Fe-mediated reaction pathway, resulting in the selective formation of 2-cyclohexene-1-ol.
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Journal of Environmental Chemical Engineering
·
2026
·Vol. 14
·期 5
·123857
·
IF 7.5
Weitian Yang,Ning Gan,Jiahao Yu,Siyi Zhao,Hao Yi,Ting Guo,Zuoping Zhao
The efficient removal of nanoplastics from aquatic environments remained a critical environmental challenge. Herein, MIL-88A(Fe) was employed as the precursor to fabricate a series of magnetic iron oxide/carbon composites (M-T, M = MIL-88A(Fe), T = 300–800 °C) via controlled pyrolysis. Among them, the optimized M-600 preserved a spindle–like morphology, with superparamagnetic Fe 3 O 4 nanoparticles uniformly embedded in the carbon matrix. M-600 exhibited exceptional adsorption performance with excellent magnetic separability, achieving 97.46% removal efficiency for polystyrene nanoplastics (PSNPs) (pH=7, 0.3 g·L −1 , 25 °C). It worked within the pH range of 2.0–7.0. The efficiency was 63.97% after five cycles, and the maximum adsorption capacity was 69.97 mg·g −1 . The adsorption kinetics followed the pseudo-first-order model, while the adsorption isotherm was well fitted by the Sips model. Its favorable wettability facilitates interfacial contact, and the efficient capture of PSNPs was dominated by electrostatic attraction and further strengthened by π–π stacking interactions. Overall, this study provides a technically reliable and promising strategy for nanoplastic removal.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2023
·
IF 9.9
Qun Ding,Xuejun Zou,Jun Ke,Yuying Dong,Yubo Cui,Hongchao Ma
Herein, a ternary TiO 2 /MIL-88A(Fe)/g-C 3 N 4 heterojunction is successfully constructed through a facile hydrothermal strategy for enhancing solar energy harvesting and efficiency of catalytic nitrogen reduction induced by enlarged light absorption range, increasing interfacial charge transfer ability and desirable stability. Under the simulated sunlight irradiation, the N 2 fixation experiment shows that the yield of NH 3 reaches 1084.31 μmol/(g·h) over the TiO 2 /MIL-88A(Fe)/g-C 3 N 4 photocatalyst, and the yield is significantly enhanced, which is 33.68 and 13.94 times that is higher than the pure TiO 2 and g-C 3 N 4 , respectively. In a mean time, the excellent performance of the photocatalytic N 2 fixation over the ternary TiO 2 /MIL-88A(Fe)/g-C 3 N 4 is verified based on density function theory calculation and the decisive step over the composite is investigated by calculating Gibbs free energies of nitrogen reduction paths. The performance enhancement mechanism of TiO 2 /MIL-88A(Fe)/g-C 3 N 4 is speculated, which indicates that the hybridized three-component system presents a desirable Z-scheme band alignment, resulting in the improvement of separation and transfer efficiency of photoinduced charge carriers. The article shows a new and high-efficiency TiO 2 /MIL-88A(Fe)/g-C 3 N 4 photocatalysis for excellent nitrogen reduction ability.
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高影响因子
APPLIED CATALYSIS A-GENERAL
·
2024
·
IF 4.7
Meng Xia,Shuai Zhang,Kaihao Xu,Chengxue Zhang,Xiaocong Wang
In arid and semi-arid areas, the remediation of saline-alkaline soils polluted by organic contaminants is challenging. In this study, the adsorption–photocatalysis synergistic removal of organic contaminants was realised using the MIL-88A(Fe) catalyst, and the saline-alkaline soils were remediated simultaneously. The adsorption isotherm of catalyst conformed to Langmuir model, and the photocatalytic degradation of PHE in an optimal visible light system achieved a PHE degradation efficiency of up to 86.2 % within 30 min. Based on the identification of active oxygen species, the PHE photocatalytic degradation was primarily driven by holes (h + ) and superoxide radicals (·O 2 - ), followed by hydroxyl radicals (·OH) and singlet oxygen ( 1 O 2 ). Furthermore, the determined physical and chemical properties of the saline-alkaline soils indicated that the soil pH value decreased to 6.82, effectively increasing the absorbable nitrogen content and improving soil fertility. This study offers a new strategy for the removal of organic contaminants under special soil medium conditions.
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OPTICAL MATERIALS
·
2021
·
IF 3.08
Qianwen Li,Limei Li,Xuanyu Long,Yu Tu,Lanqing Ling,Jiabao Gu,Liwei Hou,Yi Xu,Nan Liu,Zequan Li
Photocatalysis provides an exciting way to directly utilize solar energy to degrade environmental pollution. This process, however, suffers from rapid recombination of the photogenerated charges leading to low efficiency and instability. Herein, we report a novel MIL-88A(Fe)/Bi 2 WO 6 heterojunction as a highly efficient photocatalyst for degradation of organic compounds under visible-light irradiation. When tested in 10 mg/L Rhodamine B (RhB), such catalyst can get remarkable degradation efficiency, up to 96%, at 50 min visible-light irradiation time. Significantly, it also shows super performance for Tetracycline (TC). Moreover, MIL-88A(Fe)/Bi 2 WO 6 exhibited excellent photostability and recyclability. The superior photocatalytic activity of MIL-88A(Fe)/Bi 2 WO 6 may be the formation of a heterojunction between MIL-88A(Fe) and Bi 2 WO 6 with high surface area, which provides abundant active sites to drastically promote interactions between photocatalyst and reactants. Furthermore, the related electrochemical analysis and free radicals trapping experiments indicated that both •O 2 − and h + have significant effect in the degradation process. Our findings of the work not only provide a novel insight to the design and develop MOF-based heterojunction photocatalysts but also suggest its great potential application value for environmental remediation.
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CHEMICAL ENGINEERING JOURNAL
·
2020
·
IF 10.652
Ranran Yuan,Jinli Qiu,Cailiang Yue,Chen Shen,Dawei Li,Changqing Zhu,Fuqiang Liu,Aimin Li
Hierarchical MIL-88A(Fe)@ZnIn 2 S 4 heterostructures were synthesized via a facile low-temperature solvothermal method. The combination of MIL-88A(Fe) and ZnIn 2 S 4 produced excellent photocatalytic properties under sunlight irradiation. The enhanced separation efficiency of the photogenerated charge carriers facilitated the optimal photocatalytic performances of 12.5%-HMIL@ZIS, with 100% the of hexavalent chromium (Cr(VI)) and 99.6% of the sulfamethoxazole being converted within 9 min and 60 min at pH 5, respectively. The kinetic rate constants of Cr(VI) reduction (0.5864 min −1 ) and sulfamethoxazole (SMZ) degradation (0.0958 min −1 ) were approximately 15 and 5 times larger than those previously reported. The formation of ·O 2 − could promote the super-high conversion of Cr(VI). Meanwhile, the synergetic effect of 1 O 2 and ·O 2 − played a dominant role in the degradation of sulfamethoxazole. Furthermore, the satisfactory photocatalytic performances could be maintained after four cycles. This work provides new insights into the design of metal-organic framework based photocatalysts and indicates the great potential for efficient purification of actual wastewater.
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Journal of Environmental Chemical Engineering
·
2024
·
IF 7.4
Huayu Wang,Yanhua Cao,Changsheng Guo,Ming Ge
Heterogeneous catalyst/persulfate advanced oxidation process has been widely used in antibiotic wastewater treatment . As-designed MIL-88A(Fe)/g-C 3 N 4 composite catalyst firstly activated peroxydisulfate (PDS) to degrade tetracycline (TC) in this work. Activating PDS by MIL-88A(Fe)/g-C 3 N 4 has a higher efficiency and rate toward TC degradation compared with MIL-88A(Fe) and g-C 3 N 4 . After 60 min, the optimal MIL-88A(Fe)/g-C 3 N 4 -5 activated PDS to degrade about 80% of TC in water. The existence of g-C 3 N 4 increases the specific surface area and active Fe 2+ content of MIL-88(Fe), promotes PDS adsorption and utilization, thus showing an excellent catalytic performance for PDS activation. MIL-88A(Fe)/g-C 3 N 4 activated PDS oxidation process synergistically removed TC by free radicals (O 2 •− , •OH and SO 4 •− ) with non-free radicals ( 1 O 2 ), and the effect of some important operating factors on TC removal, the TC degradation pathways and toxicity of TC intermediates were analyzed. Moreover, the MIL-88A(Fe)/g-C 3 N 4 -5 powdered catalyst was designed into a catalytic membrane, which could remove 96% of TC in a short time (<10 min). The cycle tests confirm that powdered MIL-88A(Fe)/g-C 3 N 4 composite catalyst and its catalytic membrane have a good recyclability and stability, demonstrating that this catalyst possesses a practical application potential in the treatment of TC polluted wastewater.
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