Polymers
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2016
·Vol. 8
·期 11
·389
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IF 2.944
Lihua Guo,Xinyu Jing,Shuoyan Xiong,Wenjing Liu,Yanlan Liu,Zhe Liu,Changle Chen
A series of alkyl- and aryl-substituted iminopyridine Fe(II) complexes1a–7aand Co(II) complexes2b,3b,5b, and6bwere synthesized. The activator effect, influence of temperature, and, particularly, the alkyl and aryl substituents’ effect on catalytic activity, polymer molecular weight, and regio-/stereoselectivity were investigated when these complexes were applied in isoprene polymerization. All of the Fe(II) complexes afforded polyisoprene with high molecular weight and moderatecis-1,4 selectivity. In contrast, the Co(II) complexes produced polymers with low molecular weight and relatively highcis-1,4 selectivity. In the iminopyridine Fe(II) system, the alkyl and aryl substituents’ effect exhibits significant variation on the isoprene polymerization. In the iminopyridine Co(II) system, there is little influence observed on isoprene polymerization by alkyl and aryl substituents.Keywords:iminopyridine;Iron(II);Cobalt(II);isoprene polymerization;selectivity
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APPLIED ORGANOMETALLIC CHEMISTRY
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2024
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IF 3.7
Yi Jing Jia,Jin Quan Tao,Hao Ran Liu,Wen Bin Huang,Rongpeng Yao,Miaomiao Niu,Rongrong Li,Qiang Wei,Ya Song Zhou
To enhance the CO 2 hydrogenation activity and low-carbon olefin selectivity of Fe-based catalysts, a strategy involving the use of metal promoters to modulate the structure of active metal centers in catalyst preparation was proposed. The incipient wetness impregnation method was used to introduce modifying agents K and/or Co into the Fe/Al 2 O 3 catalyst. Characterization techniques such as XRD, BET, SEM, HRTEM, H 2 -TPR, XPS, CO 2 -TPD, NH 3 -TPD, and TG were employed to investigate the effects of the modifying agents on the dispersion, reducibility, electronic properties, and acid–base properties of active metal species. Furthermore, the influence of K and Co modification on the CO 2 hydrogenation activity and low-carbon olefin selectivity of Fe/Al 2 O 3 catalysts was explored. The results revealed that the introduction of K generated more basic sites and electron-rich active metal centers in the catalyst, facilitating the adsorption and activation of CO 2 , while suppressing the hydrogenation of olefins and the formation of methane, thus improving the selectivity towards low-carbon olefins. Co promoter facilitated the dispersion of Fe species, exposing more active sites and enhancing the FTS reaction activity, leading to more CO being converted into C 2+ hydrocarbon products. Under the synergistic effect of K and Co, the CO 2 conversion activity of the Fe-based catalyst significantly increased, achieving a CO 2 conversion rate of 37%, while the selectivity towards C 2 -C 4= increased to 31.9%.
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2024
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IF 20.2
Hongwei Zhu,Xu Yin,Yi Wang,Kajia Wei,Liankai Gu,Yonghao Zhang,Zhenshan Duan,Zhen Huang,Haoming Chen,Weiqing Han
This study developed a self-supported MOF/FeOOH heterojunction cathode without binders for boosted Fe(Ⅲ) reduction in heterogeneous electro-Fenton (EF) processes. The electron transport channels from FeOOH to in-situ grown NH 2 -MIL-88B(Fe) were established through the spontaneous formation of an internal electric field (IEF), which enhanced the electrical conductivity and disrupted the chemical inertness of the Fe(Ⅲ) reduction. The MOF/FeOOH cathode increased sulfamethazine (SMT) removal up to 95.76 %, 2.5 times better than using PTFE as binders. After ten-consecutive degradation experiments, the Fe(Ⅱ) content at cathode surface increased from 39.23 % to 56.73 %. Density functional theory (DFT) calculations and advanced characterization techniques demonstrated the efficient Fe(Ⅲ) reduction and H 2 O 2 activation during the reaction. These results elucidate the promoting effect of modulating the “contact” between the catalyst and current collectors, as to provide a feasible and promising strategy for the development of efficient heterogeneous EF cathodes.
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CHEMICAL ENGINEERING JOURNAL
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2024
·
IF 13.3
Junjie Cheng,Xinman Tu,Pengxuan Wu,Rentao zhou,Shaohua Luo,Li Zhang,Jianping Zou,Yanhong Li,Hannah M. Johnson,Qiang Zhang
In the reaction systems involving peroxymonosulfate (PMS) activation, the degradation of organic pollutants is influenced by the distinct roles played by the oxidation of free radicals and non-free radicals. The synergistic effect resulting from both oxidation pathways is often more efficient compared to a single oxidation pathway, as it allows for the optimal utilization of oxidation capacity and adaptation to complex reaction environments. Nitrogen-doped carbon substrates hosting single-atom catalysts (SACs) are anticipated to serve as an optimal platform for managing the dual oxidation pathways in the PMS activation reaction. This is attributed to the availability of numerous reaction sites that meet the activation requirements. However, there's a lack of substantial reports on this subject. Herein, we synthesized a series of single-atoms Fe nitrogen-doped carbon catalysts with different coordination structures by adjusting the coordination numbers between Fe and N atoms. It is used to investigate the reaction pattern of PMS over SACs, so as to enhance the catalytic efficacy of SACs through distinct coordination structures. The experimental and theoretical results indicate that PMS functions as both an electron receiver and provider on FeN x /C catalysts. Moreover, the specific arrangement of the Fe-N-C structure influences the exchange of electrons between the catalysts and PMS. Hence, the co-oxidation pathway of free radicals ( OH, SO 4 − and O 2 − ) and non-free radicals ( 1 O 2 ) can be modulated by altering the coordination number of Fe and N atoms during PMS activation. The elimination efficiency of tetracycline hydrochloride was significantly enhanced due to the abundance of both free radical and non-free radical species generated in the FeN 3 /C/PMS reaction system, exhibiting a degradation kinetic constant of 0.564 min −1 . In addition, it showed promising potential for application in practical wastewater degradation, exhibiting high anti-interference to general environmental disturbances (such as humic acid, chloride ions, bicarbonate ions and nitrate ions).
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FUEL
·
2024
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IF 6.7
Wenxia Zhang,Hongtao Zhang,Mohamed Abbas,Juan Zhang,Zhijun Huang,Sibudjing Kawi,Jiangang Chen
The advancement of large-scale and environmentally-friendly solid-state synthesis methods is of paramount importance for the production of precipitated catalysts, notably Fe-based catalysts utilized in Fischer-Tropsch synthesis (FTS). In this study, we present an innovative solvent-independent, wastewater-free solid-state approach for the synthesis of highly efficient Fe/ZrO 2 catalysts, elucidating the mechanisms of promotion within this specific methodology. The prepared catalysts underwent rigorous evaluation under industrially-relevant FTS conditions (230–270 °C, 20 bar, and WHSV = 5400 mL/(g cat ⋅h)). A comprehensive suite of characterization techniques was employed to establish the intricate interplay between catalytic activity and structural attributes. We meticulously examined the impact of Na as an alkali promoter and the role of transition metals (Cu and Mn) in enhancing FTS catalytic performance. The catalytic outcomes obtained clearly demonstrate the pivotal role of the synergistic interaction between Mn and Na within the Na-Mn-Fe/ZrO 2 catalyst system in driving the FTS reaction. This synergism significantly enhances FTS performance, yielding an impressive CO conversion rate (89.91 %) while maintaining low selectivity to CH 4 (7.75 %). The incorporation of Mn and Na into the catalyst matrix enhances the dispersion of Fe 2 O 3 , thereby improving the reducibility of Mn/Fe oxides and elevating the electron density on the catalyst surface. These factors facilitate the formation of active Hägg iron carbide (χ-Fe 5 C 2 ), stimulating chain propagation and ultimately leading to the generation of valuable C 5+ hydrocarbon products, which underscores its potential as an optimal candidate for future industrial applications in Fe-based Fischer-Tropsch synthesis.
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MATERIALS RESEARCH BULLETIN
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2025
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IF 5.7
Hangxi Liu,Haorong Sun,Peng Zhao,Kangle Shang,Ming Fang,Xiaoli Tan,Long Yu,Bin Ma
Nitrite ions originate from various natural and anthropogenic sources and can cause health issues including methemoglobinemia and potential carcinogenic effects. As the nitrite in water has become an increasing threat to human health, the accurate evaluation of nitrite is urgently needed for environmental quality and safety management. In this paper, we designed a CTAB/SF5/GCE sensor, which exhibited an obvious enhancement compared to the pristine glassy carbon electrode (GCE). The morphology characterization confirmed the hexagonal nanosheets of SnS 2 and the even distribution of Fe element. The energy band, Tafel plots, and EIS spectroscopy were employed to investigate the enhancement mechanism, demonstrating that improving charge transfer on the sensing interface is crucial in enhanced signals. Cyclic voltammetry (CV) was adopted as the electrochemical method to measure the nitrite in water and a sensitivity of 0.129 μA·μM −1 was exhibited in the range of 30–500 μM, and the limit of detection (LOD) was calculated to be 6.51 μM. The reliability including the repeatability, reproducibility, and stability of this sensor were estimated and showed satisfactory results. The test in real samples and the assessment of interfering substances showed the CTAB/SF5/GCE possesses a large potential in the practical application of electrochemical sensing of nitrite.
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
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2024
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IF 4.9
Tao Tian,Jie Zhang,Sijie Ge,Lijiang Tian
Persulfate oxidation is a promising technology for air pollution control but still suffers from degrading refractory volatile organic compounds (VOCs) under mild conditions. Metal-doped metal-organic frameworks (MOFs) offer a novel strategy to enhance persulfate activation and VOCs degradation. Herein, a novel bimetallic MIL-101 (Fe, Cu) is prepared for more effective degradation of gaseous benzene via persulfate activation. Under optimal conditions (Fe/Cu ratio of 1:4, persulfate concentration of 7 mM/L, pH of 5, and reaction temperature of 70 °C), the MIL-101(Fe1, Cu4) activated persulfate system achieves a benzene degradation efficiency of 79.1 %, a value significantly higher than that of MIL-101(Fe) (20.1 %). The enhanced performance can be attributed to the synergistic effect of Fe²⁺/Fe³⁺ and Cu²⁺/Cu⁺ redox interactions facilitating the activation of persulfate and generation of radical species. Density functional theory (DFT) calculations indicate an increase in the adsorption energy of MIL-101(Fe) in the presence of Cu doping from −3.46 eV to −5.92 eV along with a rise in the Fermi energy level from 0.5 eV to 1.33 eV, enhancing the electron density and mobility. A reaction energy diagram is provided to illustrate the reaction pathways and transition states involved in the degradation of benzene. Overall, the incorporation of Cu in MOFs significantly enhances the efficiency of persulfate-based oxidation systems toward VOCs degradation.
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CHEMOSPHERE
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2024
·
IF 8.1
Juan Qiao,Zhenyu Zhao,Zhengwei Zhou,Deli Wu
Palladized iron (Pd/Fe) represents one of the most common modification strategies for nanoscale zero-valent iron (nZVI). Most studies prepared Pd/Fe by reducing iron salts and depositing Pd species on the surface of pre-synthesized nZVI, which can be called the two-step method. In this study, we proposed a one-step method to obtain Pd/Fe by the concurrent formation of Fe 0 and Pd 0 and investigated the effects of these two methods on 4-chlorophenol (4-CP) removal, with carboxymethylcellulose (CMC) coated as a surface modifier. Results indicated that the one-step method, not only streamlined the synthesis process, but also Pd/Fe-CMC one-step , synthesized by it, exhibited a higher 4-CP removal rate (97.9%) compared to the two-step method material Pd/Fe-CMC two-step (82.4%). Electrochemical analyses revealed that the enhanced activity of Pd/Fe-CMC one-step was attributed to its higher electron transfer efficiency and more available reactive species, active adsorbed hydrogen species (H ads *). Detection of intermediate products demonstrated that, under the influence of Pd/Fe-CMC one-step , the main route of 4-CP was through hydrodechlorination (HDC) to form phenol and H* was the main active specie, supported by EPR tests, quenching experiments and product analysis. Additionally, the effects of initial 4-CP concentration, initial pH, O 2 concentration, anions such as Cl − , SO 4 2− , HCO 3 − , and humic acid (HA) were also investigated. In conclusion, the results of this study suggest that Pd/Fe-CMC one-step , synthesized through the one-step method, is a convenient and efficient nZVI-modifying material suitable for the HDC of chlorinated organic compounds.
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Green Chemical Engineering
·
2024
·
IF 9.1
Ruichang Xue,Rongrong Deng,Yan Li,Mengqiu Gao,Jiafu Wang,Qibo Zhang
Developing electrocatalysts with excellent activity, high stability, and low cost is vital for large-scale hydrogen production through electrochemical water splitting. Herein, a bifunctional Ni–Fe–P catalyst in situ grown on Fe foam (Ni–Fe–P/FF) is developed by a simple one-step solvothermal process in the deep eutectic solvent (DES) of ethylene glycol and choline chloride (named Ethaline). The unique solvent environment of Ethaline assisted with the regulating effect of the introduced Fe(III) ions shows an essential role in governing the preparation process. The developed Ni–Fe–P/FF acts as the efficient bifunctional electrocatalyst for water splitting in 1.0 M KOH, requiring overpotentials of 82 mV (229 mV) and 263 mV (370 mV) to deliver 10 mA cm −2 (100 mA cm −2 ) for oxygen and hydrogen evolution reactions, respectively. Furthermore, the self-supported catalyst-assembled electrolyzer also exhibits good catalytic performance with a low voltage of 1.83 V to drive 100 mA cm −2 and good stability over 100 h. This work offers a facile approach to fabricating high-performance bifunctional Ni–Fe–P electrocatalysts to catalyze water splitting.
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ENVIRONMENTAL RESEARCH
·
2024
·
IF 7.7
Zhenbin Chen,Haohan Cai,Feng Huang,Zongping Wang,Yiqun Chen,Zizheng Liu,Pengchao Xie
β-lactam antibiotics, extensively used worldwide, pose significant risks to human health and ecological safety due to their accumulation in the environment. Recent studies have demonstrated the efficacy of transition metal-activated sulfite systems, like Fe(Ⅲ)/HSO 3 − , in removing PPCPs from water. However, research on their capability to degrade β-lactam antibiotics remains sparse. This paper evaluates the degradation of 14 types of β-lactam antibiotics in Fe(Ⅲ)/HSO 3 − system and establishes a QSAR model correlating molecular descriptors with degradation rates using the MLR method. Using cefazolin as a case study , this research predicts degradation pathways through NPA charge and Fukui function analysis, corroborated by UPLC-MS product analysis. The investigation further explores the influence of variables such as HSO 3 − dosage, substrate concentration , Fe(Ⅲ) dosage, initial pH and the presence of common seen water matrices including humic acid and bicarbonate on the degradation efficiency. Optimal conditions for cefazolin degradation in Fe(Ⅲ)/HSO 3 − system were determined to be 93.3 μM HSO 3 − , 8.12 μM Fe(Ⅲ) and an initial pH of 3.61, under which the interaction of Fe(Ⅲ) dosage with initial pH was found to significantly affect the degradation efficiency. This study not only provides a novel degradation approach for β-lactam antibiotics but also expands the theoretical application horizon of the Fe(Ⅲ)/HSO 3 − system.
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MOLECULES
·
2024
·Vol. 29
·期 5
·925
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IF 4.2
Xingli Ding,Li Sheng,Ge Zhang,Min Ji,Yu Li
Fluorescent film sensors are ideal for the real-time outdoor detection of heavy metal ions of Fe3+, but they are limited because of their low sensitivity and long response time due to their special structure. In this work, we constructed a fluorescent hydrogel for the specific detection of Fe3+, utilizing poly(9-fluorenecarboxylic acid) (PFCA) as the sensing moiety and sodium alginate (SA) as the cross-linking substrate, which exhibited a rapid and selective recognition of Fe3+among a panel of 16 anions and 21 cations. It can sense Fe3+at 0.1 nM immediately owing to the porous network structure of thePFCA-SAfilm that provided enhanced ion transport channels and active sites, and the “molecular line effect” of polymer PFCA. Moreover, we successfully applied this platform to detect Fe3+in four different vegetable samples. This work provides an innovative and effective strategy for fabricating green and sustainable fluorescent sensors.
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JOURNAL OF POWER SOURCES
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2025
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IF 7.9
Zhongtao Shang,Tao Zhang,Qiao Yang,Dingke Wang,Yuyi Liao,Dongjia Xie,Yiyang Dai,Yuan Wang,Shaojun Yuan
Nanocomposites consisting of metal oxide and carbon materials are usually preferred as electrode for electrochemical energy storage. Nonetheless, their unsatisfied capacitance hinders the reached energy density of aqueous supercapacitors (SCs). Herein, Fe 2 O 3 /carbon heterointerface was constructed on porous carbon fiber (PCF), which could serve as an efficient active site for stabilizing K + and Na + storage. The theoretical calculations revealed the enhanced accumulation and transfer of charges around the Fe 2 O 3 /carbon interface, thus favoring the electron transfer and boosting the faradaic reaction. The interactions of Fe 2 O 3 and PCF was found to simultaneously cause faster ion transfer and more surface charge storage, which made the as-prepared Fe 2 O 3 @PCF electrode deliver a superior SCs performance in 2 M KCl or 1 M Na 2 SO 4 electrolyte. The asymmetric aqueous supercapacitor devices consisted of Fe 2 O 3 @PCF and MnO 2 /CC electrodes with maximum operating potential of 2.0 V achieved a high areal energy density of 0.126 mWh cm −2 at a power density of 1.2 mW cm −2 along with good stability.
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