JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2025
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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.
研究领域:
材料科学
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光催化
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化学工程
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产品关联
DOI
PubMed
高影响因子
ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH
·
2024
·Vol. 31
·期 17
·25273-25286
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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.
研究领域:
环境科学
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材料科学
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DOI
PubMed
NEW JOURNAL OF CHEMISTRY
·
2024
·
IF 2.7
Yanhua Gao,Hongya Liu,Dongfeng Zhang,Ying Chen,Yuning Liang,Juan Ren
In this paper, M88/BCB Z-scheme heterojunction photocatalysts were synthesized by a one-step hydrothermal method. A series of characterization analyses showed that the introduction of iron-based MOF material M88 with mixed valence (Fe2+/Fe3+) increased not only the specific surface area of BCB, which was 2.2 times higher than that of BiOCl0.1Br0.9 solid solution, but also the existence of Fe2+/Fe3+ redox centers promoting the in situ photoFenton-like reaction, which could generate more ˙O2− and ˙OH. In addition, the introduction of M88 further enhances the visible light response capability of BCB and the separation efficiency of photogenerated carriers. Under visible light for 120 min, 10% M88/BCB can degrade 89.74% of TC, which is 2.1 times and 1.6 times higher than that of M88 and BCB, respectively. A possible photocatalytic degradation mechanism of Z-scheme heterojunctions was proposed based on the study of the band structure and the capture experiment of active species.
研究领域:
材料科学
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环境科学
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产品关联
DOI
高影响因子
ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH
·
2024
·
IF 0
Hammad Eman N.,Eltaweil Abdelazeem S.,Abouelenein Saeyda A.,El-Subruiti Gehan
Water contamination by heavy metals, especially chromium (VI), poses a critical environmental issue due to its carcinogenic nature and persistence in the environment. Addressing this, the current study develops an efficient adsorbent, CPBr-MIL-88A@AmGO, which utilizes the synergistic capabilities of Cetylpyridinium bromide–modified MIL-88A and amine-functionalized graphene oxide to enhance Cr(VI) removal from aqueous solutions. The obtained results indicate that CPBr-MIL-88A@AmGO achieves its highest removal efficacy at pH 2, where the interaction of CPBr and AmGO’s positively charged centers significantly contributes to the adsorption processes. According to the Langmuir isotherm model, the composite’s adsorption capacity reached a maximum of 306.75 mg/g. The adsorption kinetics adhered to a pseudo-second-order model along with the endothermic nature of the process. Although the presence of SO 4 2- ions significantly reduces adsorption capacity, other interfering ions including Na + , K + , Ca 2+ , Cl - , and NO 3 - only slightly affect it. Remarkably, the composite maintains high removal efficiency, over 82%, even after 7 recycling tests, underscoring its potential for practical applications in water treatment systems. The proposed mechanism involves the contribution of electrostatic attractions, ion exchange, complexation, and the reduction of Cr(VI) to Cr(III) in the removal process. This study not only offers a potent solution for Cr(VI) remediation but also contributes to sustainable water resource management.
研究领域:
环境科学
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材料科学
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产品关联
DOI
PubMed
Journal of Water Process Engineering
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2024
·
IF 6.3
Tianmin Gong,Chunmei Gao,Shifeng Ji,Yunqing Xing
2-Methyl-4-chlorophenoxyacetic acid (MCPA) is a herbicide that poses a threat to the environment. In this study, MIL-88A was utilized as a photocatalyst to degrade MCPA. Results demonstrated that the Light/MIL-88A/H 2 O 2 system exhibited remarkable photo-Fenton catalytic activity . Under optimal conditions of pH = 3.8, H 2 O 2 concentration of 1.2 mL/L, MIL-88A dosage of 0.2 g/L and an initial MCPA solution concentration of 50 mg/L, the degradation efficiency reached its peak, achieving a 99.9 % degradation rate of MCPA within 60 min. The morphology, structure, and photocatalytic performance of MIL-88A were investigated using characterization techniques such as SEM, XRD , XPS , and UV–vis DRS . Free radical quenching experiments and ESR characterization demonstrated that the main active material in the degradation of MCPA was •OH. The possible degradation pathways of MCPA were hypothesized by combining the results of Gaussian software and LC-MS analysis. Furthermore, the toxicity of MCPA was evaluated using T.E.S.T. software and mung bean germination experiments. The results revealed that the degradation of MCPA by Light/MIL-88A/H 2 O 2 system could achieve solution detoxification .
研究领域:
环境科学
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化学工程
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产品关联
DOI
高影响因子
APPLIED CATALYSIS A-GENERAL
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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.
研究领域:
环境科学
·
土壤修复
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产品关联
DOI
高影响因子
JOURNAL OF SOLID STATE CHEMISTRY
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2024
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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.
研究领域:
环境科学
·
催化化学
✓ 已验证
DOI
高影响因子
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.
研究领域:
材料科学
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环境科学
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生物化学
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DOI
高影响因子
INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES
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2024
·
IF 7.7
Xinxin Wang,Ruixue Meng,Shiyong Zhao,Zhenyu Jing,Yonghui Jin,Jie Zhang,Qiujiu Du,Xinxin Pi,Long Chen,Yanhui Li
To ensure the sustainable development of the nuclear industry, the effective capture of radioiodine from nuclear wastewater has attracted much attention. Herein, a novel MIL-88A(Al)/chitosan/graphene oxide (MCG) composite aerogel was prepared by using crosslinked chitosan and graphene oxide as the 3D network skeleton, and MIL-88A(Al) nanocrystalline particles were introduced into the skeleton by freeze-drying method. MIL-88A(Al) adsorption capacities for volatile and soluble iodine were 2.02 g g −1 and 850.00 mg g −1 , respectively. Owing to the synergistic effect of MIL-88A(Al), GO, CS, and the hierarchically porous structures of the MCG aerogel, the adsorption capacities for volatile and soluble iodine by the MCG aerogel were increased to 2.62 g g −1 and 1072.60 mg g −1 , respectively. Furthermore, the adsorption performance of the MCG aerogel for volatile and soluble iodine could be maintained at 83 % and 82 % after 5 cycles, suggesting excellent recoverability. Meanwhile, the adsorption mechanism studies showed the interactions between iodine and N H, Al O, and C O in MCG aerogel. Furthermore, the adsorption process is consistent with the Elovich kinetic and Sips isotherm models. MCG aerogels are potential candidates for enhanced radioiodine adsorption due to their high radioiodine capture performance and excellent recyclability.
研究领域:
材料科学
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环境科学
·
核工业
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产品关联
DOI
PubMed
高影响因子
JOURNAL OF MEMBRANE SCIENCE
·
2023
·
IF 9.5
Hongai Zheng,Mengyao Li,Shuangyan Jiang,Cunzheng Xiao,Meilin Zhu,Yao Zhou,Derui Wang,Xin Sun,Daquan Zhang,Lizhi Zhang
Herein, the MIL-88A/Carbon quantum dots (CQDs) was synthesized by a hydrothermal method , and the polyvinylidene fluoride (PVDF) membrane modified by the MIL-88A/CQDs was fabricated by vacuum-assisted suction filtration. Compared with the pristine membrane, MIL-88A/CQDs modified membrane based on collaborative photo-Fenton/filtration process shows better removal efficiency for methylene blue (MB), rifampicin (RIF), methyl orange (MO), and Rhodamine B (RhB). In addition, the anti-fouling properties of the modified membrane are significantly improved, and the flux recovery of the MIL-88A/CQDs modified membrane increased from 56% to 89%, and the irreversible fouling ratio (R ir ) decreased from 44% to 11%. Significantly, the modified membrane contaminated by MB within 20 min can achieve self-cleaning through the photo-Fenton process. Finally, a possible membrane antifouling mechanism is proposed: superoxide radicals (•O 2 - ) and hydroxy radicals (•OH) are the main active substances. CQDs accelerates the e − and h + separation of MIL-88A and promotes the circulation of Fe substances. The fundamental research will present a promising strategy for improving antifouling properties of membrane.
研究领域:
材料科学
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环境工程
·
化学工程
✓ 已验证
产品关联
DOI
高影响因子
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.
研究领域:
环境科学
·
材料科学
✓ 已验证
DOI
高影响因子
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.
研究领域:
材料科学
·
催化化学
·
有机合成
✓ 已验证
产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）