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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JOURNAL OF ALLOYS AND COMPOUNDS
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2025
·
IF 6.3
Juan Huang,Xiaomin Lang,Mochou Zhang,ZiTao Liu,Yongbin Yang,Jianrong Liu,Hua Lin
The high cost of precious metals limits their use as effective catalysts for water electrolysis, while non-precious metal catalysts are more affordable but often underperform. A promising strategy to improve electrocatalytic performance and reduec costs is to incorporate noble metals onto non-precious substrates. This study successfully synthesized a trace Ru-doped FeNi 2 Ru 0.01 metal aerogel catalyst utilizing a one-step reduction method, resulting in a distinctive core-shell structure. The aerogel exhibits an overpotential of only 228 mV at a current density of 50 mA cm −2 and a stable operation time of up to 70 hours. Analysis reveals that the high specific surface area and porous architecture of the FeNi 2 Ru 0.01 aerogel facilitate the dispersion and exposure of trace Ru. In this configuration, Ru can serve as an active site following oxidation and aid in transforming Ni into the active species NiOOH, significantly boosting OER activity. This research provides a novel approach to optimizing metal aerogel catalysts through precious metal doping and lays a strong foundation for sustainable energy conversion and storage technologies.
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RARE METALS
·
2025
·
IF 11
Ma Jingwen,Li Junbin,Tian Ying,Liu Jinhao,Wang Ruiting
Fe–N–C single-atom catalysts are considered among the most promising non-precious metal-based catalysts for oxygen reduction reaction (ORR), but issues such as low utilization of active sites and the easy aggregation of single atoms severely hinder their application in fuel cells and metal–air batteries. Herein, a single-atom Fe-embedded hierarchical porous hollow carbon fiber catalyst (Fe SAC/HCNF) is reported for ORR. The hollow channels and the porous structure of the fibers facilitate the exposure of single-atom active sites, and offer multidimensional mass transfer pathways to promote the transport of reactants, thus significantly enhancing catalytic performance. Additionally, the abundant micropores exert spatial confinement, which is beneficial for preventing the aggregation of single atoms. Leveraging its unique structural advantages, the Fe SAC/HCNF catalyst demonstrates outstanding ORR activity with low metal loading, boasting a high half-wave potential of 0.905 V, a substantial double-layer capacitance ( C dl ) of 41.1 mF cm −2 , and a notable kinetic current density of 45.2 mA cm −2 in alkaline media. Furthermore, the liquid Zn–air battery (ZAB) using Fe SAC/HCNF catalyst as the air cathode exhibits excellent battery performance and long-term cycling durability nearly 600 h. And the flexible quasi-solid-state ZAB can be stably cycled in various flat/bent states, which is promising for applications in flexible electronic devices. Graphical
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Journal of Environmental Chemical Engineering
·
2025
·
IF 7.2
Haishuo Wang,Xinke Tian,Zhichun Li,Jie Zhang,Shiyin Li,Heyong Huang
Lake eutrophication leads to the excessive proliferation of cyanobacteria in aquatic environments, resulting in microcystin-LR (MCLR) concentrations exceeding regulatory limits. The associated environmental risks and health concerns attract widespread attention. As one of the most active chemical substances in aquatic environments, dissolved organic matter (DOM) plays a critical role in the phototransformation of MCLR. In environments where Fe(II) and Mn(II) coexist, the phototransformation process of MCLR may be influenced. Among fulvic acid (FA), humic acid (HA), cyanobacteria-derived DOM (CDOM), and reed leaf-derived DOM (RDOM), FA has the highest apparent reaction rate constant for MCLR at 0.03567 h -1 . Using isopropanol, furfuryl alcohol, and sorbic acid as quenchers, the contributions of different photochemically produced reactive intermediates(PPRIs) to MCLR photodegradation follow the order: 3 DOM⁎ > ·OH > 1 O 2 . As pH increases, changes in the conformation and charge distribution of DOM and MCLR suppress MCLR photodegradation. The addition of Fe(II) or Mn(II) enhances the photodegradation of MCLR by DOM. Electron paramagnetic resonance tests and radical quenching experiments indicate that the introduction of Fe(II)/Mn(II) increases ·OH production. The enhanced ·OH promotes MCLR photodegradation more effectively than the suppression caused by Fe(II)/Mn(II) quenching of ³DOM⁎. Product analysis reveals that demethylation, hydroxylation, decarbonylation, decarboxylation, denitration, and bond cleavage are the main pathways of MCLR photodegradation. These findings provide valuable insights into the migration and transformation of MCLR in complex environments, contributing to a deeper understanding of the fate of pollutants in natural water systems, particularly in the presence of metal ions.
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CHEMISTRY-A EUROPEAN JOURNAL
·
2020
·Vol. 26
·期 45
·10314-10320
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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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CHEMICAL ENGINEERING JOURNAL
·
2022
·
IF 16.744
Yanni Jiang,Zhongjuan Wang,Jianbo Huang,Feng Yan,Ye Du,Chuanshu He,Yang Liu,Gang Yao,Bo Lai
Singlet oxygen ( 1 O 2 ) is an effective reactive oxygen species in disinfection due to its long lifetime and sensitivity to bacteria. This study tried to develop a 1 O 2 dominated process for bacterial inactivation by visible light (vis) photocatalysis assisted by PMS. A novel CuS-modified MIL-101(Fe) (CSMF) photocatalyst was synthesized for the first time. Compared with MIL-101(Fe), CuS-modified MIL-101(Fe) enhanced the photocatalytic performance by increasing absorption of visible light, narrowing down the bandgap and promoting photo carrier separation efficiency. 7.5-log Gram-negative Escherichia coli (E. coli) could be inactivated by Vis/CSMF/PMS system within 40 min, showing much better performance of 3.5-log E. coli inactivated by Vis/PMS system. The Vis/CSMF/PMS system is applicable in a broad pH range from 3.0 to 9.0, remaining quite steady disinfection efficiency after regenerations of the catalyst. Quenching experiments and electron paramagnetic resonance (EPR) analysis demonstrated 1 O 2 was the dominated ROS rather than OH • and SO 4 •− . Three pathways, including photo-generated electrons (e − ) and O 2 dependent pathway, photo-generated holes (h + ) dependent pathway and CSMF enhanced PMS dissociation pathway, were evidenced to responsible for 1 O 2 formation by aeration experiments and specific 1 O 2 fluorescence probe. 1 O 2 in water attacked the bacterial cell membranes first, got inside the cell and up-regulated the level of intracellular ROS, which further led to cell membrane damage and DNA degradation so as to irreversible cell death. In addition, the developed Vis/CSMF/PMS system could also efficiently inactivate gram-positive bacteria Staphylococcus aureus and fecal coliform bacteria in practical wastewater, suggesting its wide applicability as a promising alternative to conventional disinfection process.
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IONICS
·
2025
·
IF 2.6
Zhou Yongkang,Su Zihao,Miao Jie,Peng Gongchang,Wang Hao
O3-type NaNi 1/3 Fe 1/3 Mn 1/3 O 2 (NFM) is recognized as a highly promising cathode material for sodium-ion batteries owing to its cost-effectiveness, substantial theoretical capacity, and facile synthesis. Nevertheless, this material suffers from rapid capacity decay caused by structural degradation and irreversible phase transitions at high voltages (> 4.0 V vs. Na + /Na). Herein, partial substitution of Fe 3+ sites with Ti 4+ in the transition metal layer was implemented. Systematic investigations via X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), scanning electron microscopy (SEM), and transmission electron microscopy (TEM) reveal that Ti substitution effectively stabilizes the layered framework by suppressing detrimental phase transitions through enhanced structural pillar effects. The optimized NaNi 1/3 Fe 0.23 Mn 1/3 Ti 0.1 O 2 delivers a specific capacity of 144.1 mAh g −1 within 2.0–4.2 V at 0.1 C, demonstrating 71.3% capacity retention after 100 cycles at 1 C (130 mA g −1 ). This work establishes a viable strategy for enhancing structural stability in O3-type cathodes through selective cation substitution. Graphical
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ACS Applied Nano Materials
·
2025
·
IF 5.5
Xudong Zhao,Shuibo Wang,Hua Li,Yushi Wei,Yiming Li,Haocheng Li,Hongbo Yu,Kaijie Li,Haotian Li,Hongfeng Yin
Preventing nanoparticle migration and agglomeration on the surface of supported heterogeneous catalysts, especially at tailored bimetallic sites, poses a significant challenge. The reverse water–gas shift (RWGS) reaction is considered a promising route for converting CO2 into CO, an essential feedstock for industrial chemical production. Herein, a core–shell nanostructure anchoring on the surface was developed, which consists of a PtFe bicomponent core (∼2.6 nm) and a nitrogen-doped carbon nanoshell (∼1.3 nm). This structural design enhances the CO2 adsorption saturation, weakens the CO adsorption strength, and promotes hydrogen spillover. This PtFe core–shell material (Pt/Fe = 1:1) demonstrates an elevated reaction rate of 12.58 molCO2 gPt–1 h–1, with nearly 100% CO selectivity at 450 °C and atmosphere pressure. The activity is 5.1-fold higher than that of the Pt nanoparticle, attributed to the tuned geometric and electronic properties. The nitrogen-doped carbon nanoshell preserves the core–shell morphology at a high temperature. Moreover, the in situ experiments reveal the H-assisted dissociation/activation of the CO2 pathway for RWGS. The integration of the bimetallic synergy and core–shell structure is a potent strategy for thermal catalytic processes.
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npj Clean Water
·
2025
·Vol. 8
·期 1
·1-17
·
IF 11.4
Xu Dan,Cao Xiaolin,Zhou Jie,Lin Zhihao,Wang Jing,Han Jiatong,Chen Ge,Liu Guangyang,Xu Xiaomin,Zhang Yanguo,Xu Donghui
To address the environmental threats posed by dye pollution, it is crucial to develop adsorbents with high selectivity and adsorption capacity for the removal of chemical dye pollutants. In this study, five types of Ni/Fe-MOFs were synthesized via a one-pot solvothermal method by varying the Ni/Fe molar ratio. Their physicochemical structures, surface morphologies, and compositions were characterized through a series of techniques, and their adsorption performances for different dyes were preliminarily investigated. The results demonstrated that the Ni/Fe ratio significantly affects the microstructure and adsorption performance of the MOFs. As the molar ratio of Ni/Fe increased, the structures of the five materials transformed from nanoflowers (Fe-MOFs) to nanospheres (Ni/Fe(3:1)MOFs) , and eventually to rhombic blocks (Ni-MOFs) . The specific surface area decreased from 281.3 m²/g (Fe-MOFs) to 67.11 m²/g (Ni/Fe(1:1)MOFs) and further to 0.5369 m²/g (Ni-MOFs) . XPS analysis confirmed the synergistic coordination between Ni and Fe, and FT-IR spectra revealed characteristic peaks for hydroxyl groups on the MOF surface and carboxylate ligands. XRD analysis indicated that materials with higher Ni content were more prone to ligand decomposition, which is consistent with the weight loss observed in the TG-DSC between 230 and 350 °C. The materials exhibited selective adsorption for different dyes. Under optimal conditions, the maximum adsorption capacities for Eosin Y (EY), Neutral Red (NR), and Acid Fuchsin (AF) were 54.92 mg/g (Fe-MOFs) , 636.31 mg/g (Ni-MOFs) , and 79.30 mg/g (Ni/Fe(1:1)MOFs) , respectively. The adsorption kinetics followed a pseudo-second-order model, and the adsorption isotherms conformed to the Langmuir model, while Fe-MOFs and Ni/Fe(1:1) MOFs also exhibited compatibility with the Freundlich model. The adsorption mechanism primarily involved monolayer adsorption as the dominant process, with localized multilayer adsorption, as well as chemisorption, hydrogen bonding, hydroxyl interactions, and electrostatic interactions. These MOFs demonstrated high dye removal efficiency in actual water samples and fruit and vegetable juices, exhibiting excellent reusability and anti-interference capabilities. Importantly, compared with the single system, Fe-MOFs and Ni/Fe(1:1)MOFs exhibit competitive adsorption, and Ni-MOFs exhibit synergistic adsorption in the binary system. This study confirms that by adjusting the Ni/Fe molar ratio, MOFs with high selectivity and adsorption performance for different dyes can be designed, providing new theoretical insights and technical support for environmental remediation and food safety applications.
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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
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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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