NEW JOURNAL OF CHEMISTRY
·
2023
·Vol. 47
·期 45
·20762-20769
·
IF 3.3
Yunxiao Zhang,Wenhua Xiao,Jingqiang Zhang,Tiantian Hu,Shanxia Hu,Minjie Zhou,Zhaohui Hou,Yu Liu,Binhong He
The currently leading oxygen reduction reaction (ORR) catalysts are non-precious metal electrocatalysts. However, porous structure engineering and accessibility of Fe–N–C sites still remain a huge challenge. Here, we developed hierarchically porous Fe–N–C catalysts for cathodes of Zn–air batteries using a gas diffusion strategy, which has dense active Fe–Nx moieties. The Fe-NCNF-120 catalyst provided high kinetic current density and mass activity towards the ORR, as well as a more positive initial potential and half-wave potential (Eonset = 1.00 V, E1/2 = 0.90 V). According to experiments, the outstanding ORR activity can be attributed to the organized micro- and mesoporous structure, enhanced intrinsic activity of dense and accessible active sites Fe–Nx, and the facilitated mass and electron transport by 3D interconnected pores. As the cathode for Zn–air batteries, Fe-NCNF-120 demonstrated high power density, a high open-circuit voltage, and excellent stability. The combination of inherent activity with dense and accessible spots in this work opens up new possibilities for the design and synthesis of effective electrocatalysts for energy storage and conversion.
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CHEMISTRY-A EUROPEAN JOURNAL
·
2020
·Vol. 26
·期 45
·10314-10320
·
IF 4.857
Guiqiang Cao,Zhikang Wang,Da Bi,Jing Zheng,Qingxue Lai,Yanyu Liang
Graphical Atomic cat : A single-atom Fe@NG electrocatalyst serves as the coating of separators for high-performance Li-S batteries. Atomically dispersed Fe sites on the graphene framework promote the conversion efficiency of LiPS. The Fe@NG electrocatalyst delivers an initial capacity of 1616 mA h g −1 at 0.1 C, and a reversible capacity of 546 mA h g −1 after 200 cycles at 2 C (70 % capacity retention). Lithium-sulfur batteries have been considered as potential electrochemical energy-storage devices owing to their satisfactory theoretical energy density. Nonetheless, the inferior conversion efficiency of polysulfides in essence leads to fast capacity decay during the discharge/charge cycle. In this work, it is successfully demonstrated that the conversion efficiency of lithium polysulfides is remarkably enhanced by employing a well-distributed atomic-scale Fe-based catalyst immobilized on nitrogen-doped graphene (Fe@NG) as a coating of separator in lithium-sulfur batteries. The quantitative electrocatalytic efficiency of the conversion of lithium polysulfides is determined through cyclic voltammetry. It is also proven that the Fe-N X configuration with highly catalytic activity is quite beneficial for the conversion of lithium polysulfides. In addition, the adsorption and permeation experiments distinctly indicate that the strong anchoring effect, originated from the charge redistribution of N doping into the graphene matrix, inhibits the movement of lithium polysulfides. Thanks to these advantages, if the as-prepared Fe@NG catalyst is combined with polypropylene and applied as a separator (Fe@NG/PP) in Li-S batteries, a high initial capacity (1616 mA h g −1 at 0.1 C), excellent capacity retention (93 % at 0.2 C, 70 % at 2 C), and superb rate performance (820 mA h g −1 at 2 C) are achieved.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2025
·
IF 9
Jingru Zhang,Guangxin Yang,Junyu Zhang,Cong Kong,Jun Wang
The misuse of sulfonamide and fluoroquinolone antibiotics leads to pollution of the water environment, necessitating the development of cost-effective and efficient degradation methods. This article presents a one-step hydrothermal method (200℃, 8 h) for the preparation of Fe-N-co-doped biochar/carbon quantum dots (Fe/N/BC/CQDs) as a photocatalytic material. The Fe/N/BC/CQDs was employed for the activation of H 2 O and O 2 , facilitating the degradation of sulfonamide and fluoroquinolone antibiotics, with superoxide radicals, photo-generated holes, hydroxyl radicals, and singlet oxygen dominated the photodegradation process. Under 1 h dark and 8 h natural light conditions, the degradation efficiency of norfloxacin, sulfathiazole, sulfamethoxazole, sulfamonomethoxine, sulfadoxin, sulfamethazine (10 mg/L) by Fe/N/BC/CQDs ranged from 74.21 % to 89.23 %. The potential degradation pathways of sulfonamide and fluoroquinolone antibiotics were proposed based on ultrahigh-performance liquid chromatography tandem high-resolution mass spectrometry analysis of the intermediates. The Fe-N-doped biochar’s hierarchical pore structure enhances synergistic adsorption-catalysis effects, while the incorporated carbon quantum dots (CQDs) broaden solar spectrum utilization, effectively overcoming the high-intensity light dependency common to conventional photocatalysts. Efficient charge separation was achieved through the formation of a p-n heterojunction between Fe-N-co-doped biochar and CQDs. Additionally, the applicability of Fe/N/BC/CQDs in real water systems was confirmed, providing valuable insights for the construction of p-n heterojunction structures to degrade organic pollutants in water.
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Water
·
2025
·Vol. 17
·期 9
·1309
·
IF 3
Xiaoyan Ma,Rongbin Quan,Wenqing Cao,Weijie Zhang,Su Jiang,Jiao Feng,Jiulong Wang,Stefanos Giannakis
Electrochemical reduction is a promising strategy for the dechlorination of halogenated organic compounds, offering advantages such as enhanced electron transfer efficiency and increased hydrogen atom concentration. It has garnered significant attention for application in mitigating halogenated disinfection by-products (DBPs) in drinking water, owing to its high efficiency and simple operation. In this study, trichloroacetic acid (TCAA), a representative DBP, was selected as the target contaminant. A novel composite cathode comprising a metal–organic framework MIL-53(Fe)@C supported on an Nd magnet (MIL-53(Fe)@C-MAG) and its dechlorination performance for TCAA were systematically investigated. The innovative aspect of this study is the magnetic attachment of the MOF catalyst to the carbonized cathode surface treated through carbonization, which fundamentally differs from conventional solvent-based adhesion methods. Compared to the bare electrode, the MIL-53(Fe)@C-MAG achieved a TCAA removal efficiency exceeding 96.03% within 8 h of contact time. The structural characterization revealed that the α-Fe0crystalline phase serves as the primary active center within the MIL-53(Fe)@C catalyst, facilitating efficient electron transfer and TCAA degradation. The scavenger experiments revealed that TCAA reduction involves a dual pathway: direct electron transfer and atomic hydrogen generation. The modified MIL-53(Fe)@C-MAG electrode exhibited robust electrolytic performance over a broad pH range of 3–7, with TCAA removal efficiency showing a positive correlation with current density within the range of 10–50 mA/cm2. Furthermore, the electrode maintained exceptional stability, retaining more than 90% removal efficiency after five consecutive operational cycles. The versatility of the system was further validated by the rapid and efficient dechlorination of various chlorinated DBPs, demonstrating the broad applicability of the electrode. The innovative magnetic composite electrode demonstrates a significant advancement in electrochemical dechlorination technology, offering a reliable and efficient solution for the purification of drinking water contaminated with diverse halogenated DBPs. These results provide valuable insights into the development of electrolysis for dechlorination in water treatment applications.
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SPECTROCHIMICA ACTA PART A-MOLECULAR AND BIOMOLECULAR SPECTROSCOPY
·
2025
·
IF 4.6
Feijin Zhou,Wenying Cui,Chenggang Liu,Cheng Yao,Chan Song
The excessive presence of S 2− poses siganificant risks to human health and the environment. Therefore, the development of novel S 2− sensing methods remains crucial in daily life. Herein, Fe–N hollow mesoporous carbon nanospheres (Fe–N HMCNSs), characterized by a high specific surface area and excellent stability, were successfully prepared. Further investigation revealed that the colorimetric substrates such as 2,2′-azino-bis(3-ethylbenzthiazoline-6-sulphonate) (ABTS), o-phenylenediamine (OPD), and 3,3′,5,5′-tetramethylbenzidine (TMB), can be effectively oxidized by Fe–N HMCNSs into colored products. Based on the oxidase-like activity of Fe–N HMCNSs, a facile colorimetric method for S 2− assay was constructed for the first time. The recognition of S 2− could be fulfilled by recording the absorbance intensity and observing color changes in nanozymes-based catalytic systems. This method is simple, cost-effective, and environment-friendly, offering a wide linear range (0.25–25 µM) and a low detection limit (42.2 nM) for S 2− assay. Furthermore, integration of smartphone-based RGB analysis enabled the portable and convenient S 2− sensing using the developed colorimetric sensor. The remarkable stability of Fe–N HMCNSs under harsh conditions endows their potential applications in the fields of food safety and environmental protection.
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SENSORS AND ACTUATORS B-CHEMICAL
·
2021
·
IF 7.46
Jun Yao,Zhuang Xie,Xiang Zeng,Li Wang,Tingting Yue
Cholesterol is one of the most significant indicators to assess health status. Lanthanide metal-organic frameworks (Ln-MOFs) have a unique luminescence mechanism, which makes it possess tremendous potential in biomonitoring. Thus, on the basic of intramolecular charge transfer theory and quenching effect, the metal-organic frameworks (MOFs) doped by europium was constructed to respond to the cholesterol in serum. The charge transfer direction and the sensing mechanism of fluorescent probe were explained in detail by cross-corroboration of experiment and calculation. The possible sensing mechanism was explained at the molecular level with density functional theory (DFT). With the excitation of 350 nm, the emission peaks at 458 nm and 615 nm which corrsponded to MIL-53(Fe) and Eu centers, appeared enhancement and quenching respectively. To investigate the emission law, the density of states and partial density of states were used to explain the internal electron migration of the probe and the possible sensing mechanism. The results showed the electron transfer efficiency of MIL-53(Fe) was enhanced after Eu 3+ doping, which brought a remarkable improvement in response sensitivity. Meanwhile, the higher energy possessed by the excited state of Eu will lead to the capture of its own electrons by hydrogen peroxide, thus reducing the number of electrons returned to the ground states of Eu and eventually leading to the fluorescence quenching of 615 nm. We anticipate the proposed research is to be an emerging method in cholesterol determination and have further development in all walks of life.
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CARBON
·
2025
·
IF 11.6
Hao Lu,Xianchu Wang,Chenyu Wang,Qihang Wang,Jingjing Xie,Weiming Wang,Zhengyi Fu,Zhaoyong Zou
Zeolitic Imidazolate Frameworks (ZIF-8) has emerged as promising candidate for alleviating the aggregation of Fe 3 N-catalysts, exhibiting significantly improved oxygen reduction reaction (ORR) and oxygen evolution reaction (OER) for rechargeable zinc-air batteries. To further improve the catalytic performance, it is crucial to fabricate ZIF-8 with hierarchically porous structures, which remains challenging due to the rapid crystallization kinetics and the weak interactions. Inspired by biological porous materials, we developed a novel method using 1,3,5-trimethylbenzene TMB as a mediating molecule to dynamically regulate the organic-inorganic interface between templates and ZIF-8 precursors, achieving the micro-meso-macropores of ZIF-8, which synergistically enhances mass transport and active site accessibility. Additionally, TMB preserves the weakly alkaline environment required for ZIFs’ structural integrity by leveraging its hydrophobic co-solvent effect. The as-synthesized Fe 3 N-HPZIF-8 catalyst integrates Fe 3 N active sites, hierarchically porous structures, and pyrrolic-N dopants, resulting in the exceptional bifunctional activity in alkaline media (ΔE = 0.619 V), exceeding most benchmark catalysts. When integrated into zinc-air batteries, a peak power density of 205.2 mW cm -2 is achieved. This work presents a generalizable synthetic approach for high-performance metal-air battery catalysts.
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Journal of Environmental Chemical Engineering
·
2025
·Vol. 14
·期 1
·120955
·
IF 7.2
Yingchao Li,Juntan Wang,Zhanyu Guo,Xiaofang Ouyang,Peng Ju,Hua Yin
This study presents a novel FeMg-layered double hydroxide (LDH) modified biochar composite (LB) designed to synergistically address phosphate recovery from wastewater and heavy metal immobilization in contaminated soil. The composite exhibits an exceptional phosphate adsorption capacity of 25.02 mg/g, representing a 169.00 % increase compared to pristine biochar. The improved performance results from precipitation and anion exchange within the LDH layers. And the competitive adsorption tests further confirm that LB better retains phosphate in simulated wastewater. When repurposed as a soil amendment, phosphate-laden LB (P-LB) demonstrates remarkable heavy metal immobilization efficiencies, achieving 41.23 % Pb, 30.52 % Cu and 25.63 % As immobilization at a 1.0 % dosage, representing an 18.70–26.42 % improvement over LB. Beyond its metal stabilization capabilities, P-LB effectively enhances soil phosphorus cycling, increasing total phosphorus by 14.41 % and bioavailable phosphorus by 9.02 %. Furthermore, the remediated soil exhibits significantly enhanced enzymatic activity, with urease and sucrase activities increasing by 21.38 % and 380.10 %, respectively. Pot experiments confirm the agronomic benefits of P-LB, demonstrating a 68.16 % increase in plant height and a 39.27 % increase in biomass accumulation in the remediated soil. This integrated approach, leveraging LDH-phosphate synergy, not only achieves phosphate recovery in sewage but also realizes metal immobilization and soil fertility remediation in contaminated soil.
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PHYSICAL CHEMISTRY CHEMICAL PHYSICS
·
2015
·Vol. 17
·期 40
·26690-26702
·
IF 4.493
Shengjie Xia,Mengmeng Shao,Xiaobo Zhou,Guoxiang Pan,Zheming Ni
A series of novel organic–inorganic nanoscale layered materials were synthesized by intercalating the Ti-containing Schiff base complex into the interlayer of the ZnM layered double hydroxides (LDHs, M = Al, Cr, Fe, Ce). The hybrid material was further calcined to make metal oxide composites with highly dispersed Ti elements (Ti/ZnO–MxOy). The structural characterization and photocatalytic results showed that, after intercalation and calcination, the metal oxide composites with a unique flower-like crystal morphology not only had high specific surface area, uniform pore size distribution and narrow band gap, but also showed extremely high photocatalytic performance for hexachlorobenzene (HCB) degradation. The Ti/ZnO–Cr2O3 composite with the narrowest band gap (2.40 eV) and the highest surface area (227 m2) showed the highest photocatalytic performance for HCB (95.5% within 240 min) among the four metal oxide composites. Particularly, it was found that composites derived from layered materials with different supramolecular structure of the host and guest showed different photocatalytic properties. In addition, based on the results from ESR, GC-MS and HPLC-MS, the type and amount of hydroxyl radicals, the decomposition intermediates and the pathway of HCB degradation photocatalyzed by Ti/ZnO–MxOy composites are also discussed in detail.
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ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH
·
2022
·Vol. 30
·期 2
·4123-4136
·
IF 5.19
Li Jiacheng,Tian Tian,Jia Yannan,Xu Nannan,Yang Shujun,Zhang Chenyue,Gao Shiwei,Shen Wei,Wang Zheng
Herein, an iron-doped ZIF-8-loaded multi-walled carbon nanotube (FZM) was synthesized and its adsorption performance on tetracycline (TC) was investigated. The experimental conditions (solution pH, temperature, adsorbent dose) were optimized by Box–Behnken design (BBD) in response surface methodology (RSM). The results show that the adsorption effect of TC by FZM is optimal under the conditions of temperature = 298 K, pH = 6, and contact time = 360 min. The adsorption processes of TC by FZM follow the pseudo-second-order (PSO) kinetic and Freundlich isotherm models, indicating that chemisorption is the dominant factor and the adsorption reaction is multi-layer, with a theoretical maximum saturation capacity of 1111.11 mg/g at 298 K. The adsorption thermodynamic results indicate that the adsorption of TC by FZM is a spontaneous and endothermic process. The mechanism of TC adsorption by FZM possibly occurs through hydrogen bonding, surface complexation, π–π interaction, and electrostatic interaction. From the statistical results, the optimal adsorption capacity of TC by FZM is 599.78 mg/g at a pH of 7.1, a temperature of 312.5 K, and an adsorbent dose of 64.43 mg/L, with a deviation of 1.73% from the actual value. Furthermore, regeneration experiments demonstrate that FZM has excellent reusability with a 15% loss of adsorption capacity after four cycles. This study provides some insights to study the adsorption behavior of TC by MOFs and the optimization of the adsorption experimental conditions, and also shows the potential of FZM for TC removal.
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ANALYTICA CHIMICA ACTA
·
2021
·
IF 6.558
Jiabi Xu,Yanyan Xing,Yutong Liu,Mingzhe Liu,Xiaohong Hou
In recent decades, artificial nanozymes with excellent stability, low cost and availability have been gradually explored to avoid the limits of natural enzymes such as poor stability, high cost and difficult preparation. Herein, for the first time, we investigated the capability of nanoscale Fe 3 O 4 @MIL-100(Fe) as a nanozyme, which was quickly synthesized in situ by a microwave-assisted method within 20 min using Fe 3 O 4 as the metal precursor. The obtained Fe 3 O 4 @MIL-100(Fe) showed satisfactory intrinsic dual enzyme mimetic activities, including peroxidase (POD)- and catalase (CAT)-like activities. Moreover, a simple and effective colorimetric biosensor was fabricated to detect glutathione (GSH) based on its POD-like activity. The proposed measurement had a linear range of 1–45 μM and a limit of detection (LOD) of 0.26 μM (3.3 δ/S). It was proved that the established colorimetric sensing system could be successfully applied to detect GSH in actual biological samples. Importantly, the outstanding reusability and stability made it extremely valuable as a catalyst. The present work implied that Fe 3 O 4 @MIL-100(Fe) synthesized in situ by the microwave-assisted method was a very promising candidate for biocatalyst and biosensing.
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Journal of Physical Chemistry C
·
2017
·
IF 4.536
Wanfeng Li,Fang Zhang,Xingde Xiang,Xiucheng Zhang
Nickel-based ferrocyanides have attracted wide interest as cathode for aqueous sodium-ion batteries in fields of sustainable energies such as wind and solar, owing to excellent cycling stability and high-rate capability. However, they suffer from low specific capacities (∼60 mAh g–1). Herein, Na2Ni0.4Co0.6[Fe(CN)6] nanocrystallites are reported for the first time as high-capacity cathode for aqueous sodium-ion batteries. Its electrochemical properties and redox mechanism have been understood by combining the X-ray diffraction technique, Fourier-transform infrared spectroscopy, cyclic voltammetry, electrochemical impedance microscopy, and charge/discharge measurements. It is revealed that the material undergoes a reversible three-step single-phase reaction mechanism during Na extraction through sequential electrochemical oxidation of nitrogen-coordinated Co2+ ions and carbon-coordinated Fe2+ ions and achieves superior electrochemical performance with a high reversible capacity of 85 mAh g–1 at 0.5 C, an average operating potential of 0.62 V (vs Ag/AgCl), and a high capacity retention of 90% after 100 cycles. The combination of high specific energy and good cycling performance enables the Na2Ni0.4Co0.6[Fe(CN)6] material exhibiting promising application for high-performance aqueous sodium-ion batteries.
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