ChemCatChem
·
2024
·
IF 3.8
Chengzhuo Yu,Jin Xu,Yarui Wang,Silong Wang,Li Xiong,Fanglan Geng,Zesen Shang,Huasheng Wu,Jitao Lv,Lixia Zhao,Yawei Wang
Graphical Untill now, reactive oxygen species (ROS) are difficult to generate in the natural light conditions, since most photocatalysts require external strong stimuli. We surprisingly found the ROS generation on MIL-100(Fe)/TiO 2 driven by mild natural light. The ROS generation patterns and mechanism of MIL-100(Fe)/TiO 2 was revealed by chemiluminescence (CL) and density functional theory (DFT). Reactive oxygen species (ROS), as one kind of the most highly oxidizing oxidants, are difficult to generate and utilize in the natural light conditions, since many materials require external strong stimuli for ROS release to be effective as pollutant degradation or biocide. In this work, we surprisingly found the ROS generation on MIL-100(Fe)/TiO 2 driven by mild natural light. Then ROS generation patterns and mechanism was revealed by chemiluminescence (CL) and density functional theory (DFT). Meanwhile, rhodamine B (RhB) can also be removed by MIL-100(Fe)/TiO 2 under natural light, which further evidence the ROS generation under the natural light. This work provides a new direction for spontaneously generating ROS releasing without external strong stimuli and has the broad potential applications in the field of pollutant degradation or antimicrobials under natural conditions.
研究领域:
环境科学
·
材料科学
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产品关联
DOI
高影响因子
RENEWABLE ENERGY
·
2021
·
IF 8.001
Hui Li,Junchi Wang,Xiaoling Ma,Yangyang Wang,Guoning Li,Min Guo,Ping Cui,Wanpeng Lu,Shoujun Zhou,Mingzhi Yu
Solid catalyst loss is inevitable by using the traditional separation methods of centrifugation or filtration. To this end, the carbonized MIL−100(Fe) is used to support ammonium sulfate ((NH 4 ) 2 SO 4 ) for synthesizing magnetic solid acid on the purpose of biodiesel production . Influence of preparation factors of loading amount, activation temperature, and activation time on catalytic activity are initially evaluated. With that, the prepared catalyst (CIS) is comprehensively investigated to obtain the optimal esterification parameters for biodiesel production . Moreover, characterizations of TG, XRD, BET, SEM, EDS, FTIR, py−FTIR, VSM, XPS, and Hammett indicator are conducted to elucidate the structure−function relationship between physicochemical property and catalytic activity . Results indicated the CIS is a superparamagnetism material with the saturated magnetism of 22 emu/g, which could be easily recovered from mixture with external magnet. Furthermore, the maximum conversion of 95.68% is obtained with mild conditions: molar ratio of methanol/oleic acid of 8:1 and catalyst amount of 8 wt% at 70 °C for 2 h. Negligible impact is detected for CIS with presence of 5 wt% water content, even with 20 wt% water content, the conversion of 85.88% is still achieved.
研究领域:
化学工程
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催化材料
·
可再生能源
✓ 已验证
产品关联
DOI
高影响因子
PROCESS BIOCHEMISTRY
·
2021
·
IF 3.757
Kun Xiao,Rennv Wang,Congyang Liu,Meini Wang,Wei Dong,Tao Pan
PAH biodegradation aided by surfactants and cyclodextrins has been widely studied because the former's micelles and the latter's hydrophobic cavities can increase the apparent solubility of PAHs. In this work, the effects of Triton X-100 (TX-100) and β-cyclodextrin (β-CD) on the bioavailability and biodegradation of phenanthrene (PHE) were investigated. The degrading microorganism used was Moraxella osloensis CFP312, a new strain screened from polluted soil and could form biofilms on crystalline PHE. At the same concentrations, β-CD solubilized less PHE than TX-100 but promoted PHE biodegradation. The two solubilizers had almost no different effects on CFP312 hydrophobicity; however, β-CD significantly eluted fewer cells from biofilms on crystalline PHE than TX-100. Microscopy observation revealed that the residual structure of the biofilm treated with β-CD was more complete than that of the biofilm treated with TX-100. This effect is beneficial to the function of biofilms and conducive to mass transfer from the exposed area in the crystalline PHE to the aqueous phase. Although TX-100 and β-CD could enhance the mass transfer of PHE to the aqueous phase, the latter significantly improved the bioavailability and biodegradation of PHE mainly because its solubilization was accompanied by easy desorption and retention of the biofilm functional integrity.
研究领域:
环境科学
·
微生物学
✓ 已验证
DOI
高影响因子
Journal of Materials Chemistry A
·
2024
·Vol. 12
·期 26
·16043-16051
·
IF 10.7
Keying Su,Shan Yang,Yulu Zhu,Yujia Liang,Yawen Tang,Xiaoyu Qiu
High-entropy alloy (HEA) nanoparticles have been recognized as one kind of efficient electro-catalyst for water splitting. However, their higher catalytic activity is restrained by the difficulty in precisely shaping the HEAs into ordered facets and fully exposed surface structures. Herein, we report a seed-mediated conformal growth and partial etching method for the controlled synthesis of PtIrRuRhPd HEA cubic nanocages (CNCs), which feature the ordered {100} facets and ultrathin shells of five atomic layers. The slow injection of a PtIrRuRh layer on Pd nanocubes and the subsequent capture of dissociative Pd atoms in the etching step are responsible for the formation of nearly equimolar PtIrRuRhPd HEAs. Due to the synergistic effects derived from the multicomponent high-entropy effects, the ordered (100) facets, and the ultrathin feature, the PtIrRuRhPd HEA CNCs exhibit significantly high electro-catalytic activities for hydrogen and oxygen evolution reactions in an acidic medium, with overpotentials of 20 mV and 272 mV at 10 mA cm−2 (η10), respectively. As electrodes for a water electrolyzer, the PtIrRuRhPd HEA CNCs afford an η10 as low as 196 mV, together with superior long-term durability for 200 000 s.
研究领域:
材料科学
·
电催化
·
能源化学
✓ 已验证
产品关联
DOI
高影响因子
DALTON TRANSACTIONS
·
2015
·Vol. 44
·期 41
·18227-18236
·
IF 4.197
Ruowen Liang,Rui Chen,Fenfen Jing,Na Qin,Ling Wu
H3PMo12O40 molecules have been successfully encapsulated in the cavities of MIL-100(Fe) via a facile hydrothermal method (denoted as HPMo@MIL-100(Fe)). A series of characterization has corroborated the insertion of H3PMo12O40 within the cavities of MIL-100(Fe). The resulting HPMo@MIL-100(Fe) nanocomposites have exhibited much higher photoactivity than the original-MIL-100(Fe) toward the photocatalytic selective oxidation of benzylic alcohols and the reduction of Cr(VI) under visible light irradiation (λ ≥ 420 nm). The higher photoactivity of HPMo@MIL-100(Fe) can be attributed to the integrative effect of enhanced light absorption intensity and more efficient separation of photogenerated electron–hole pairs. The host porous structure of MIL-100(Fe) can achieve a uniform composition with H3PMo12O40, which is significantly important for producing highly reactive dispersed H3PMo12O40 molecules and enhancing the photocatalytic activity of HPMo@MIL-100(Fe) nanocomposites. And the immobilized H3PMo12O40 molecules are more convenient for recycling. Importantly, almost no Fe and Mo ions leach from the MIL-100(Fe) during the reaction, which verifies the photostability of the HPMo@MIL-100(Fe). In addition, possible photocatalytic redox reaction mechanisms have been investigated.
研究领域:
材料科学
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环境科学
·
化学工程
✓ 已验证
产品关联
DOI
PubMed
高影响因子
CHROMATOGRAPHIA
·
2024
·
IF 1.2
Shao Xiaozhen,Xu Guangfu,Chen Jiaquan,Miao Pandeng,Yang Ke,Du Yingxiang,Yu Tao
Metal–organic frameworks (MOFs) have a wide range of applications in separation and analytical sciences due to their unique structures. MIL-100(Fe) was immobilized on the inner wall of the capillary column based on the immobilized cysteine (Cys)-triggered in situ growth (ICISG) strategy. By applying this column to capillary electrophoresis, a novel enantioselective separation system based on MIL-100(Fe) nanomaterial was established. By utilizing lactobionic acid (LA) as the chiral selector and optimizing the experimental conditions such as buffer pH, LA concentration and the methanol addition ratio, the CEC system demonstrated a significantly enhanced enantioseparation ability for six basic drugs. The modified capillary column was characterized by scanning electron microscope (SEM), energy-dispersive X-ray spectroscope (EDS) and X-ray diffractometer. The experimental results showed that MIL-100(Fe) was successfully grown on the inner wall of the capillary column. In the present study, the repeatability of the coated column was investigated and the relative standard deviations (RSDs) of the resolution and the migration time for intra-day, inter-day and inter-column were within 8%, proving the good repeatability of the coated column.
研究领域:
分析化学
·
药物科学
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产品关联
DOI
高影响因子
Biomedical Physics & Engineering Express
·
2024
·Vol. 10
·期 4
·045004
·
IF 1.3
Mingjia Feng,Yan Li,Yanfang Sun,Tianqi Liu,Khaydar E Yunusov,Guohua Jiang
The transdermal drug delivery based on microneedles (MNs) provides a suitable and painless self-administration for diabetic patients. In this work, the hydrogel-forming MNs were firstly fabricated using poly(vinyl alcohol) (PVA) and chitosan (CS) as matrix. A hypoglycemic drug, metformin (Met), had been loaded into MIL-100(Fe). Then, both of free Met and Met-loaded MIL-100(Fe) were integrated into hydrogel-forming MNs for regulation of blood glucose levels (BGLs) on diabetic rats. After penetrated into the skin, the free Met could be firstly released from MNs. Due to the absorption of interstitial fluid and subsequent release of loaded Met from MIL-100(Fe), leading to a sustainable and long-term drug release behaviors. A notable hypoglycemic effect and low risk of hypoglycemia could be obtained on diabetic rat models in vivo. The as-fabricated hydrogel-forming MNs expected to become a new type of transdermal drug delivery platform for transdermal delivery of high-dose drugs to form a long-term hypoglycemic effect.
研究领域:
药物递送
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糖尿病治疗
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材料科学
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生物医学工程
✓ 已验证
产品关联
DOI
PubMed
高影响因子
SCIENCE OF THE TOTAL ENVIRONMENT
·
2024
·
IF 8.2
Guohui Wang,Qixin Zhang,Lailai Qin,Kaixuan Tan,Chunguang Li,Lianshun Li,Tinggui Yang,Xiaojuan Liu
A novel metal-organic framework (MOF) material, MIL-100(Fe)-DMA, was synthesized using the solvothermal method. The structure of the MOF was characterized using scanning electron microscopy-energy dispersive X-ray spectroscopy, N 2 adsorption–desorption isotherms, X-ray diffraction analysis, Fourier-transform infrared spectroscopy, X-ray photoelectron spectroscopy, and Mössbauer spectroscopy. Batch adsorption experiments were performed to investigate the effects of initial Sr 2+ and Cs + concentrations, adsorption time, pH, and coexisting cations on the adsorption performance of the material. The adsorption mechanism was further elucidated using adsorption kinetics and isotherm models. The results indicated that the adsorption of Sr 2+ and Cs + does not significantly affect the MOF material structure. As reaction time and initial ion concentration increased, the adsorption capacity of MIL-100(Fe)-DMA for Sr 2+ and Cs + increased rapidly and then gradually reached equilibrium. Optimal adsorption occurred under alkaline conditions, with maximum adsorption capacity observed at pH = 8. The adsorption process for Sr 2+ and Cs + was well described by the pseudo-second-order kinetic model, the Weber–Morris model, and the Langmuir adsorption isothermal model. The adsorption process was mainly identified as monolayer chemical adsorption, influenced by multiple factors. Characterization combined with density functional theory calculations revealed that the unsaturated carboxylic acid groups on the surface of the MOFs play a crucial role in the interaction with Sr 2+ and Cs + .
研究领域:
材料科学
·
环境科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Environmental Technology & Innovation
·
2022
·
IF 7.758
Zhen Jiao,Zhijia Miao,Heluan An,Qing Li,Xiangyuan Meng
Water eutrophication caused by phosphate emissions has become a serious environmental issue. In this study, we used the solvothermal method to prepare a novel Ce-doped MIL-100(Fe). Scanning electron microscope observations suggest that Ce-doped MIL-100(Fe) consisted of irregular polyhedrons in the size range of tens of micrometers. Spectroscopy results show that cerium atoms (Ce) were successfully doped into the MIL-100(Fe) frameworks. The specific surface area and pore size of the Ce-doped MIL-100(Fe) were 2.6 m 2 /g and 3.4 nm, respectively. Adsorptive kinetics indicated that the pseudo-second-order model with a high correlation coefficient of ( R 2 : 0.9950) fitted better than the pseudo first-order model with R 2 of 0.9436. The adsorptive isotherms showed that for these adsorption reactions, the Langmuir model matched much better than the Freundlich model for this adsorption. These facts suggest that adsorption is chemical sorption, which occurred on a homogeneous surface. The adsorption capacity of the Ce-doped MIL-100(Fe) was as high as 12.03 mg/g. The adsorption capacity of the Ce-doped MIL-100(Fe) depended strongly on the solution pH, ionic strength, and the coexisted ions. The study also found that the precipitation reaction and complexation interaction might be dominated in the adsorption. This study may contribute to the design of bimetal organic frameworks, and might add new insights into the removal of phosphate.
研究领域:
环境科学
·
材料科学
✓ 已验证
DOI
高影响因子
SPECTROCHIMICA ACTA PART A-MOLECULAR AND BIOMOLECULAR SPECTROSCOPY
·
2017
·
IF 2.536
Nan Gao,Pengcheng Huang,Fangying Wu
In this study, we have developed a method for rapid, highly efficient and selective detection of melamine . The negatively charged citrate ions form an electrostatic layer on gold nanoparticles (AuNPs) and keep the NPs dispersed and stable. When citrate-capped AuNPs were further modified with Triton X-100, it stabilized the AuNPs against the conditions of high ionic strength and a broad pH range. However, the addition of melamine caused the destabilization and aggregation of NPs. This may be attributed to the interaction between melamine and the AuNPs through the ligand exchange with citrate ions on the surface of AuNPs leading Triton X-100 to be removed. As a result, the AuNPs were unstable, resulting in the aggregation. The aggregation induced a wine red-to-blue color change, and a new absorption peak around 630 nm appeared. Triton X-100-AuNPs could selectively detect melamine at the concentration as low as 5.1 nM. This probe was successfully applied to detect melamine in milk. Furthermore, paper-based quantitative detection system using this colorimetric probe was also demonstrated by integrating with a smartphone.
研究领域:
食品科学
·
纳米技术
·
分析化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Chemical Engineering Journal Advances
·
2023
·
IF 0
Mengsi Cheng,Ying Fang,Zhaoguang Yang,Xinghao Liu,Bo Qiu,Tong Zhang,Haipu Li,Wenbo Zhao
MIL-100(Fe) was modified by amino groups (MIL - 100(Fe) - NH 2 ) to enhance the removal of antimonate (Sb(V)) with low concentration (50−200 μg/L) from natural water through batch adsorption experiments. With the initial Sb(V) concentration up to 200 μg/L, the residual Sb(V) concentration after treated by MIL - 100(Fe) - NH 2 was only 3.52 ± 0.131 μg/L, lower than the drinking water standards (5 μg/L) in China, while that was much higher (94.2 ± 3.52 μg/L) after pristine MIL-100(Fe) treatment. Based on results of XPS analysis, and adsorption kinetics and isotherms, we concluded that Sb(V) substituted the terminal −OH groups of MIL-100(Fe) to form inner-sphere complexes by coordination reactions with Fe nodes and be adsorbed by hydrogen bonding as well. The grafted amino groups (−NH 2 ) adsorbed Sb(V) by hydrogen bonding and facilitated the coordination reactions between Sb(V) and Fe nodes. The higher K L value (0.0116 ± 0.00,118 L/μg) obtained by fitting with the Langmuir isotherm model, while that of unmodified MIL-100(Fe) was 4.74 × 10 −4 ± 5.85 × 10 −5 L/μg, also confirmed that the −NH 2 groups greatly enhanced the affinity between MIL-100(Fe) and Sb(V). Furthermore, MIL - 100(Fe) - NH 2 still worked nicely in a wide pH range (2 − 12), with varied ionic strength (0.05 µmol/ L −1.5 mol/L), coexisting ions (CO 3 2− , NO 3 − , SO 4 2− , Cl − , H 2 PO 4 − ), and even in the real water bodies. Additionally, MIL - 100(Fe) - NH 2 exhibited good reusability and low Fe leaching (99.92 μg/L). We hope MIL - 100(Fe) - NH 2 become a candidate for effective removal of Sb(V), even other heavy metals from natural waterbodies.
研究领域:
环境科学
·
材料科学
✓ 已验证
DOI
SEPARATION AND PURIFICATION TECHNOLOGY
·
2025
·
IF 9
Yeshuang Wang,Mingxian Duan,Zhelin Su,Chao Yang,Bingning Wang,Jiawei Kou,Huiling Fan
The abundant Fe 3+ Lewis acidic sites and well-developed pore structure endow the Fe-MOFs with great potential for H 2 S catalytic oxidation at room temperature, but their performance is inferior owing to the insufficient redox ability of the Fe 3+ species inherent in frameworks. Herein, an effective protocol was proposed for the first time to remarkably improve the catalytic oxidation performance of MIL-100(Fe) under ambient conditions through the introduction of Fe 2+ coordinatively unsaturated site (CUS) species into the framework. As expected, the sample after modification had a superior H 2 S breakthrough capacity of 267.3 mg S/g, an 18.4-fold increase compared with that without Fe 2+ CUS (14.5 mg S/g). The introduced Fe 2+ species triggered the Fe 3+ /Fe 2+ redox cycle for H 2 S catalytic oxidation by enhancing the oxidative ability of the Fe 3+ CUS intrinsic to the framework. Moreover, the Fe 2+ CUS was also found act as an active site for O 2 activation into O 2 ∙– , which not only provides an additional pathway for H 2 S catalytic oxidation but also accelerates the redox cycling of Fe 3+ /Fe 2+ during the catalytic oxidation process. On the basis of the experimental findings, a plausible catalytic mechanism involving mixed-valence iron sites in MIL-100(Fe) was proposed.
研究领域:
材料科学
·
催化化学
✓ 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）