JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2024
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IF 9.4
Jianwang Wu,Mei Lin,Ming Liu,Zuliang Chen
Hydrogen peroxide (H 2 O 2 ) is a crucial eco-friendly oxidizer with increasing demand due to its wide range of applications. Activating O 2 with catalysts to generate H 2 O 2 on-site offers a promising alternative to traditional production methods. Here, we design unique crystalline/amorphous heterophase Fe-Mn core–shell chains (ZVI-Mn) for efficient on-site generation of H 2 O 2 and manipulation of subsequent H 2 O 2 activation. The yield of H 2 O 2 on-site produced by ZVI-Mn in water within 5 min was 103.7 mg·L -1 , which was much greater than that of zero-valent iron (ZVI) and amorphous Mn (A-Mn) (0 and 42.5 mg·L -1 ). Raman and density functional theory (DFT) calculations confirmed that *OOH is the key species involved in the on-site generation of H 2 O 2 . Electrochemical tests confirmed the excellent electron-transferring ability, while electron paramagnetic resonance (EPR) revealed oxygen vacancy defects in the catalysts, which proved to be conducive to improving the catalytic activity of ZVI-Mn. Additionally, by regulating the pH of aqueous solution , ZVI-Mn can simultaneously achieve efficient on-site generation of H 2 O 2 and in-situ removal of enrofloxacin from aqueous solution.
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INTERNATIONAL JOURNAL OF MOLECULAR SCIENCES
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2024
·Vol. 25
·期 18
·9855
·
IF 4.9
Yiting Luo,Rongkui Su
Tetracycline’s accumulation in the environment poses threats to human health and the ecological balance, necessitating efficient and rapid removal methods. Novel porous metal–organic framework (MOF) materials have garnered significant attention in academia due to their distinctive characteristics. This paper focuses on studying the adsorption and removal performance of amino-modified MIL-101(Fe) materials towards tetracycline, along with their adsorption mechanisms. The main research objectives and conclusions are as follows: (1) NH2-MIL-101(Fe) MOF materials were successfully synthesized via the solvothermal method, confirmed through various characterization techniques including XRD, FT-IR, SEM, EDS, XPS, BET, and TGA. (2) NH2-MIL-101(Fe) exhibited a 40% enhancement in tetracycline adsorption performance compared to MIL-101(Fe), primarily through chemical adsorption following pseudo-second-order kinetics. The adsorption process conformed well to Freundlich isotherm models, indicating multilayer and heterogeneous adsorption characteristics. Thermodynamic analysis revealed the adsorption process as a spontaneous endothermic reaction. (3) An increased adsorbent dosage and temperature correspondingly improved NH2-MIL-101(Fe)’s adsorption efficiency, with optimal performance observed under neutral pH conditions. These findings provide new strategies for the effective removal of tetracycline from the environment, thus holding significant implications for environmental protection.
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CHEMPHYSCHEM
·
2025
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IF 2.2
Li Ma,Wei-Ming Yang,Lin Xue,Jie Zhang,Ke-Xin Lin,Pei-Jian Chen,Xiang Zhang,Hai-Shun Liu
Graphical The co-catalysis of iron-nickel bimetals can not only achieve the complete degradation of organic pollutants but also continue to be recycled. The introduction of Ni enhances the reducibility of the 3D Fe 50 Ni 50 catalyst surface, promotes electron transfer, enriches the surface with Fe (II) during degradation, maintains activity, and provides a self-healing effect. Advanced oxidation processes offer a potent, eco-friendly solution for degrading organic wastewater. Creating high-activity and stability catalysts is crucial to addressing water pollution concerns. Nevertheless, due to constraints in their preparation, prevalent catalysts often lack satisfactory cyclic stability and pose challenges in recovery. This research introduces an innovative catalyst, the 3D printed Fe-Ni porous framework (3D Fe 50 Ni 50 ), characterized by its high activity, robust stability, and straightforward recovery process. The catalytic performance of 3D Fe 50 Ni 50 is attributed to the synergistic effects of its bimetallic constituents and its distinct porous architecture. Under optimal conditions, the kinetic reaction constant reaches 1.56 min −1 . It represents a 26-fold increase over commercially available Fenton's reagent ZVI powder. And the Fe 50 Ni 50 catalyst can be employed cyclically up to 132 times, maintaining a degradation efficiency of over 90% relative to its initial performance. The findings of this article suggest that incorporating Ni augments the catalyst surface's reducibility, facilitating electron transfer. This bestows the catalyst with a nice self-healing ability, ensuring sustained degradation. This investigation paves the way for the design of catalysts with heightened activity and stability and presents promising applications in wastewater treatment.
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APPLIED CATALYSIS A-GENERAL
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2015
·
IF 3.942
Pei Wu,Xuegang Luo,Sizhao Zhang,Ke Li,Fangwei Qi
A novel photo/thermocatalyst was synthesized using co-precipitation. The catalyst above was used to degrade the dye methylene blue (MB), via the processes of thermocatalytic degradation (TCD) and photo/thermocatalytic degradation (PTCD). The catalysts were characterized using X-ray diffraction (XRD), field emission scanning electron microscopy (FESEM), energy dispersive X-ray spectroscopy (EDX), X-ray photoelectron spectroscopy (XPS), UV–Vis diffusion reflectance spectroscopy (DRS), diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS), the Brunauer–Emmett–Teller (BET) technique, and the terephthalic acid photo-luminescence probing technique (TA-PL). Fe-doped Sr 2 Bi 2 O 5 powder was found to exhibit a high thermocatalytic activity and a high photo/thermocatalytic activity for the degradation of MB. The TCD and PTCD MB removal efficiencies reached 92.6 and 98.8%, respectively. Furthermore, HO and O 2 − were not found to be the predominant active radicals. Holes were found to be generated in both two TCD and PTCD; however, TA-PL and radical scavenger experiments indicated that more holes were formed in PTCD. This study discussed the probable thermocatalytic and photo/thermocatalytic mechanisms, finding them to be in good agreement with results.
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TALANTA
·
2022
·
IF 6.556
Xiaofang Chen,Min Feng,Xiaoyi Xie,Yi Zhang,Jie Zhang,Xiupei Yang
Single-atom catalysts have attracted enormous research interest in the field of catalysis owing to their remarkable catalytic activity, excellent stability and outstanding atom utilization. Herein, a new single atom based on single Fe atoms on fluorine-doped (Fe–SAs@FNC) ultrathin carbon nanosheets was successfully synthesized by a polymer-assisted heating method. Experimental evidence showed that the resultant Fe–SAs@FNC with Fe–N 4 sites exhibits superior peroxidase-like activity, which oxidizes the colorless 3,3′,5,5′-tetramethylbenzidine (TMB) to produce a blue product in the presence of hydrogen peroxide (H 2 O 2 ). Based on this, an ultrasensitive and highly selective colorimetric detection method for p -phenylenediamine (PPD) in hair dyes and PPD in hair after dyeing was established, which had a wide linear range (0.2–50 μM) and low detection limit (0.07 μM). This method shows satisfactory sensitivity and selectivity.
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Journal of Materials Chemistry B
·
2021
·Vol. 9
·期 34
·6811-6817
·
IF 6.331
Xiao Liang,Yingxuan Chen,Kai Wen,Haobo Han,Quanshun Li
In the past two decades, the number of reports on the construction of uric acid (UA) sensors has increased dramatically, as it is a vital factor in the diagnosis of physiological functions and diseases. Among these sensors, cascade colorimetric detection based on peroxidase mimics has received great attention owing to the advantages of easier operation and more intuitive results. Herein, we report a simple UA detection method via the integration of urate oxidase (UOx) and PCN-222(Fe) with peroxidase-like activity, in which UOx is immobilized in PCN-222(Fe) by physical adsorption. UOx could catalyze the UA oxidation to produce H2O2, and then PCN-222(Fe) catalyzed the oxidation of 3,3′,5,5′-tetramethylbenzidine (TMB) in the presence of H2O2 to generate a blue product with a maximum absorbance at 652 nm. Under optimal conditions, the increasing absorbance at 652 nm was proportional to the UA concentration. The linear range for UA detection was 10–800 μM with a limit of detection of 3.5 μM, and the cascade system has been successfully utilised for the detection of UA in human serum samples to demonstrate the accuracy of the proposed method. In conclusion, the cascade catalytic system based on the immobilization of UOx in PCN-222(Fe) has the potential to be used as a rapid and sensitive sensor for UA detection.
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MICROCHIMICA ACTA
·
2019
·Vol. 186
·期 7
·1-8
·
IF 5.479
Yang Fencheng,Jiang Guodong,Yan Feng,Chang Qing
Iron-carbon (Fe/C) magnetic nanocubes were synthesized by direct pyrolysis of Prussian blue nanocubes under an inert gas atmosphere. They are shown to possess intrinsic peroxidase mimicking activity to catalyze the oxidation of peroxidase substrate N , N -diethyl- p -phenylenediamine sulfate salt to form a purple colored product in the presence of H 2 O 2 . The values for K m and V max are 74 μM and 46 nmol s −1 , respectively. Steady-state kinetic analysis also indicates that the catalysis reaction follows a ping-pong mechanism. Based on these findings, an ultrasensitive colorimetric H 2 O 2 assay was worked. Absorbance (best value measured at 550 nm) increases linearly in the 10 nM to 0.2 mM H 2 O 2 concentration range, and the limit of detection is 1.5 nM. The method was also applied to the quantification of glucose, which is oxidized by glucose oxidase in the coexistence of H 2 O 2 . The response covers the 0.1 to 500 μM glucose concentration range, and the limit of detection is 16 nM. The method was applied to the determination of H 2 O 2 in rainwater samples. The glucose assay was used to analyze serum samples, and satisfactory results were obtained. Other attractive features include good chemical activity, low cost, easy storage, and high catalytic efficiency.
Schematic presentation of converting Prussian blue nanoparticles into Fe/C magnetic nanocubes by a pyrolysis technique and the use of glucose oxidase and Fe/C magnetic nanocubes to establish a one-step spectrophotometric method for the determination of glucose and hydrogen peroxide.
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JOURNAL OF FOOD COMPOSITION AND ANALYSIS
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2022
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IF 4.52
Haishuai Peng,Yuanyuan Hui,Meixue Pu,Ding Yang,Aiqing Zhao,Weizhe Wang,Shan Wu,Bini Wang
Streptomycin (STR) residues in dairy products could cause serious health risks for human or affect the quality of the dairy products fermented by lactic acid bacteria , thereby resulting in economic losses. Thus, STR detection methods need to be developed quickly, simply, and sensitively. In this study, polyethyleneimine (PEI)-functionalized NH 2 -MIL-101(Fe) (PEI-Fe-MOF) was characterized and found to exhibit an enhanced electrochemical characteristics, when compared to Fe-MOFs. [email protected] core-shell NPs could further amplify its electrochemical signal. Based on the PEI-Fe-MOF/ [email protected] NPs nanocomposites, we have developed a novel electrochemical aptasensor to detect STR rapidly. When detected under optimal conditions, a wide linear range between 0.1 and 200 nM was observed for the aptasensor with a detection limit of 0.033 nM. Furthermore, the developed aptasensor has been satisfactorily applied for the rapid STR detection in dairy products with recoveries ranging from 98.2% to 110.1%. Therefore, our method can be considered a new effective method for the rapid detection of STR in dairy products.
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CHEMISTRY-A EUROPEAN JOURNAL
·
2023
·
IF 4.3
Ruosong He,Yang Wang,Meng Li,Jianxin Liu,Yongqiang Gu,Wenhang Wang,Qiang Liu,Noritatsu Tsubaki,Mingbo Wu
Graphical Core-shell structured Fe-based catalyst Na−Fe 3 O 4 @C with confinement effect delivered higher productivity of light olefins compared with the naked Na−Fe 2 O 3 counterpart. Multiple characterization and DFT calculation verified that the timely carbon chain-growth termination, as well as unique CO 2 /H 2 ratio and electronic property on the catalytic interface played vital roles in boosting light olefins synthesis. Even though Fe-based catalysts have been widely employed for CO 2 hydrogenation into hydrocarbons, oxygenates, liquid fuels, etc., the precise regulation of their physicochemical properties is needed to enhance the catalytic performance. Herein, under the guidance of the traditional concept in heterogeneous catalysis-confinement effect, a core-shell structured catalyst Na−Fe 3 O 4 @C is constructed to boost the CO 2 hydrogenation performance. Benefiting from the carbon-chain growth limitation, tailorable H 2 /CO 2 ratio on the catalytic interface, and unique electronic property that all endowed by the confinement effect, the selectivity and space-time yield of light olefins (C 2 = −C 4 = ) are as high as 47.4 % and 15.9 g mol Fe −1 h −1 , respectively, which are all notably higher than that from the shell-less counterpart. The function mechanism of the confinement effect in Fe-based catalysts are clarified in detail by multiple characterization and density functional theory (DFT). This work may offer a new prospect for the rational design of CO 2 hydrogenation catalyst.
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CERAMICS INTERNATIONAL
·
2020
·
IF 3.83
Cong Li,Yefei Li,Juan Wang,Bo Li,Dawei Yi,Jing Shi,Qiaoling Zheng,Yimin Gao,Siyong Zhao
The preparation, microstructure and mechanical properties of ZTA particles reinforced Fe matrix composites (ZTA P /Fe composites) were systematically investigated. The X-ray diffraction (XRD), scanning electron microscopy (SEM) and electron probe microanalysis (EPMA) were used to analyze the microstructure and phase constituents, the hardness ( H) , Young's modulus ( E ) and plasticity factor ( δ A ) were determined as well. The nickel-chromium double-layer coated ZTA P of core-shell structure was prepared by electroless plating and multi-arc ion plating technologies. The modified ZTA P is consisted of the α -Al 2 O 3 , t -ZrO 2 , α -Cr and γ -Ni phases. In addition, the compressive strength of ceramic preforms is high due to a compact sintering neck formed among ZTA P during high temperature sintering . The preferred sintering process for ZTA ceramic preforms is determined as 1350 °C + 1 h, in this case the preforms show the remarkable porosity and highest compressive strength which are 27.8% and 35.0 MPa, respectively. The interfacial metallurgical chemical reactions occurred during infiltration casting process, which ensure the excellent metallurgical interfacial bonding of the ZTA P /Fe composites. The interface contains double transition layers, which refer to silicate and CrFe phases, respectively. The H , E and δ A of interfacial double transition layers were measured by the nano-indentation method, the values of which are situated between the ZTA P and iron matrix.
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SCIENCE OF THE TOTAL ENVIRONMENT
·
2021
·
IF 7.963
Meng Xia,Zheng Shen,Minyan Gu,Wenbo Chen,Wenjie Dong,Yalei Zhang
Microalgae residue was efficiently converted into lactic acid with a high yield (33.9%) under mild reaction conditions (210 °C, 2 h) over a Fe-Sn-Beta catalyst. Under the action of homogeneous H 3 O + and distinct Lewis acid sites on the catalyst, the production of lactic acid from microalgae residue underwent three main reaction steps: hydrolysis, isomerization , and retro-aldol condensation. Results demonstrated that the lipid component had a strong inhibitory effect on the production of lactic acid due to the formation of aromatics, esters, and complex nitrogenous heterocyclic compounds , which covered or poisoned the Lewis acid sites of the catalyst. The protein component acted as a chemical buffer that enhanced the production of lactic acid by controlling the release of monosaccharides from the carbohydrate fraction of microalgae and maintaining the catalytic activity of the catalyst. Thus, microalgae residue demonstrated great promise for the production of value-added chemicals.
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Nano Research
·
2020
·Vol. 13
·期 8
·2079-2084
·
IF 8.183
Wang Hong-Hui,Lv Li-Bing,Zhang Shi-Nan,Su Hui,Zhai Guang-Yao,Lei Wei-Wei,Li Xin-Hao,Chen Jie-Sheng
The rational design of highly active and stable atomically dispersed M-X 4 (M = Fe, Co, Ni, etc., X = C, N) -based catalysts holds promises for wide application in almost all realms of catalysis. Despite great effort in the construction of specific M-X 4 centers, the possible effect of non-coordinated heteroatoms on the catalytic activity of metal centers has been rarely explored. Herein, we develop a new type of M-X 4 catalyst composed of Fe-N 4 centers and non-coordinated B heteroatoms (FeNC+B) and find the key role of non-coordinated B adjacent to Fe-N 4 centers in tailoring their electron density and final catalytic selectivity. The experimental and theoretical results demonstrated that non-coordinated boron atoms could decrease the electron density of Fe-N 4 centers to a suitable level and thus boost the selective production of nitriles from amine oxidation by depressing the formation of imines due to the flattened energy barrier of the reversible conversion of imines back to amines. As a reusable heterocatalyst, the state-of-the-art FeNC+B catalyst provides a turn-over frequency (TOF) value of 21.6 mol benzonitrile ·mol Fe −1 ·h −1 (100 °C), outpacing that of bench-marked nonnoble-metal-based homogeneous catalyst by a factor of 3.4.
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