Journal of Inorganic and Organometallic Polymers and Materials
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2025
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IF 4.9
Yu Qinyuan,Li Jiahui,Wang Yufen,Wei Xuedong
Transition metal sulfides (TMS) have drawn increasing research interest owing to their unique electronic structure. They hold broad prospects in accelerating the sluggish oxygen evolution reaction (OER) during water electrolysis. Metal-organic frameworks (MOFs) feature controllable electronic structures and specific surface areas, which facilitate the adsorption of reactants and expedite interfacial electron transfer. Leveraging the above-mentioned advantages of the two materials, a kind of composite electrocatalyst, CuCo 2 S 4 @MIL-53(Fe)/NF, was synthesized by growing MIL-53(Fe) in-situ onto CuCo 2 S 4 nanowires supported on nickel foam. This composite electrocatalyst can accelerate charge transfer, significantly increase the number of active sites, and enhance both electrocatalytic activity and stability. The electrocatalyst CuCo 2 S 4 @MIL-53(Fe)/NF can drive the OER with an overpotential of 390 mV at a current density of 100 mA·cm −2 . Moreover, it still demonstrates excellent catalytic activity after 75 h of testing. This study not only broadens the avenues for sulfide composites but also provides an experimental basis and support for the direct combination of metal chalcogenides and Fe-based MOFs as electrocatalysts.
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CHEMICAL ENGINEERING JOURNAL
·
2025
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IF 13.2
Yiting Zhao,Yahui Wei,Shaonan Gu,Pengfei Yan,Hongbo Zhang,Jingyun Jiang,Qun Xu,Buxing Han
Utilizing renewable electricity to obtain “green” hydrogen is challenging due to the deterioration of active site activity and mass transfer capabilities at high current densities. Herein, a unique Fe-rich Ni x Fe 3−x O 4 @CP (Fe-NFC) self-supported electrode, directed by a special deep eutectic solvent (DES)-philic interface on the carbon paper (CP) collector, is developed. The Fe-NFC electrode exhibits high intrinsic catalytic activity and a stable catalyst-collector interface, enhancing oxygen evolution reaction (OER) activity and stability at elevated current densities. The regulated electronic structure of Fe-NFC is ascribed to the unique DES-philic carbon directing effect, which optimizes the adsorption energy of intermediates to further accelerate the O 2 formation during the OER process. The catalyst-collector interface also improves the mass transfer, which is favorable for the OER process at high current densities. Fe-NFC achieves a low OER overpotential of 360 mV at 1.5 A cm −2 and maintains stability for over 100 h. This work demonstrates the effectiveness of DES-interfaced engineering in optimizing active site structures and highlights the critical role of mass transport in OER at high current densities, offering a new direction for designing advanced functional materials for other gas evolution reactions.
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LANGMUIR
·
2024
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IF 3.7
Zhuangzhi Sun,Jiawei Lin,Suwei Lu,Yuhang Li,Tingting Qi,Xiaobo Peng,Shijing Liang,Lilong Jiang
The electrochemical nitrogen reduction reaction (eNRR) has emerged as a promising strategy for green ammonia synthesis. However, it suffers unsatisfactory reaction performance owing to the low aqueous solubility of N2 in aqueous solution, the high dissociation energy of N≡N, and the unavoidable competing hydrogen evolution reaction (HER). Herein, a MIL-53(Fe)@TiO2 catalyst is designed and synthesized for highly efficient eNRR. Relative to simple MIL-53(Fe), MIL-53(Fe)@TiO2 achieves a 2-fold enhancement in the Faradaic efficiency (FE) with an improved ammonia yield rate by 76.5% at −0.1 V versus reversible hydrogen electrode (RHE). After four cycles of electrocatalysis, MIL-53(Fe)@TiO2 can maintain a good catalytic activity, while MIL-53(Fe) exhibits a significant decrease in the NH3 yield rate and FE by 79.8 and 82.3%, respectively. Benefiting from the synergetic effect between TiO2 and MIL-53(Fe) in the composites, Fe3+ ions can be greatly stabilized in MIL-53(Fe) during the eNRR process, which greatly hinders the catalyst deactivation caused by the electrochemical reduction of Fe3+ ions. Further, the charge transfer ability in the interface of composites can be improved, and thus, the eNRR activity is significantly boosted. These findings provide a promising insight into the preparation of efficient composite electrocatalysts.
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Journal of Environmental Chemical Engineering
·
2024
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IF 7.4
Hao Wang,Renting Huang,Wei Mao,Hao Xu,Chutong Ling,Junru Zhao,Fan Yi,Yongxin Zhou,Jinghong Zhou
Iron-based metal-organic frameworks (MOFs) represent a potentially important tool for controlling organic pollutants . However, the structural stability of most iron-based MOFs in the aqueous environment is limited. Therefore, this study sought to improve the aqueous stability and photocatalytic activity of MIL-101(Fe) using an in-situ modification strategy. A novel and highly water-stable MIL-101(Fe)@IPA 4 was prepared using ligand regulation. Owing to the in-situ modification effect, MIL-101(Fe)@IPA 4 exhibited remarkable hydrophobicity with a water contact angle at 102.4° while maintaining minimal leaching of iron ions (0.46 mg/L), even after five cycles of photocatalysis . Under MIL-101(Fe)@IPA 4 /UV/H 2 O 2 conditions, the removal rates of ciprofloxacin and total organic carbon reached 100% and 49.16%, respectively, within 60 min. These researches suggest that introducing IPA improves the light absorption properties of MIL-101(Fe)@IPA 4 and facilitates electron-hole separation, thereby promoting the generation of active species. The ecotoxicity assessment of major degradation intermediates of ciprofloxacin was conducted using the ECOSAR system. Our findings provide novel insights for enhancing the water stability of iron-based MOFs through an in-situ modification strategy, which is crucial for pollution control efforts.
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Nano Today
·
2024
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IF 13.2
Ke Zhu,Wenlei Qin,Yuwen Chen,Xiaoyin Liang,Haoran Xin,Zhihan Huang,Hector F. Garces,Yaping Gan,Mika Sillanpää,Rongliang Qiu,Guoqing Guan,Kai Yan
Constructing the coordination environment of single-atom catalysts (SACs) can be an attractive technical strategy to regulate the generation of reactive oxygen species for Fenton-like reactions. Herein, we have constructed an asymmetric coordination of Fe single-atom catalyst (Fe SA -NS-PCNS) with abundant N-Fe-S bridge (Fe SA -N 3 S 1 ) for robust Fenton-like reactions. 82.5 % of singlet oxygen ( 1 O 2 ) selectivity and high turnover frequency of bisphenol A degradation (0.568 min −1 ) were achieved at mild conditions. Experimental works and theoretical analyses illustrated that S doping breaks the inert environment of the original N-Fe-N symmetric coordination equilibrium and modulates the electron density of the atomic Fe center, which is beneficial for boosting PMS adsorption and reducing the energy barriers of vital *OH and *O intermediates. The coupling between the Fe SA -N 3 S 1 interface and peroxymonosulfate molecule boosts in-situ electron transfer through the N-Fe-S bridge, which induces more electron flow from the low valence Fe to OH* on the surface of Fe-*O-H, forming a high yield of 1 O 2 . Moreover, we designed the Fenton-like reactions by Fe SA -NS-PCNS membrane reactor for an efficient contaminant removal rate of over 90 % even after 11 cycles. This work provides a novel perspective on developing SACs with asymmetric coordination to regulate reactive oxygen species for the treatment of organic contaminants in water bodies.
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INTERNATIONAL JOURNAL OF MOLECULAR SCIENCES
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2025
·Vol. 26
·期 3
·953
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IF 4.9
Jianan Chen,Longjiong Chen,Leliang Wu,Chengyu Yan,Ningxin Sun,Guilong Peng,Shaogui Yang,Huan He,Chengdu Qi
Currently, iron-catalyzed low-valent sulfur species processes are regarded as potentially valuable advanced oxidation processes (AOPs) in wastewater treatment. As a commonly used low-valent sulfur species in the food industry, metabisulfite (MBS) can undergo decomposition to bisulfite when dissolved in water. Therefore, the combination of MBS with dissolved Fe(III) at environmentally relevant concentrations is proposed in this study to accelerate organic contaminants degradation while simultaneously minimizing the production of iron sludge. The results show that the Fe(III)/MBS process could degrade various organic contaminants, including acid orange 7 (AO7), and the removal efficiency of AO7 obeyed the pseudo-first-order kinetic. The rate constant values exhibited variations depending on the initial concentrations of Fe(III) and MBS, pH values, as well as the reaction temperature. Moreover, the contribution of HO•and SO4•−to AO7 degradation was estimated as 51.59% and 46.45%, respectively. Furthermore, Cl−showed a minimal effect while HCO3−and humic acid resulted in a significant inhibitory effect on AO7 degradation. The satisfactory degradation of AO7 was achieved in three real water bodies. Ultimately, the results of gas chromatography–mass spectrometry and the theoretical calculations greatly facilitate the proposal of AO7 degradation pathways, including N=N cleavage, hydroxylation, and hydrogen abstraction. The findings of this study indicate that the Fe(III)/MBS process may be a promising AOP for further application in organic contaminants degradation during wastewater treatment.
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JOURNAL OF HAZARDOUS MATERIALS
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2010
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IF 4.144
Zhanqiang Fang,Xinhong Qiu,Jinhong Chen,Xiuqi Qiu
Polybrominated diphenyl ethers have been identified as a new class of organic pollutants with ecological risk due to their toxicity, bioaccumulation, and global distribution. Proper remediation technologies are needed to remove them from the environment. In this paper, Ni/Fe bimetallic nanoparticles were synthesized by chemical deposition and used to degrade decabromodiphenyl ether (BDE209). The characteristics of Ni/Fe nanoparticles were analyzed by transmission electron microscopy, X-ray diffractometry, X-ray photoelectron spectroscopy, and Brunnaer–Emmett–Teller surface area analysis. Ni/Fe bimetallic nanoparticles with diameters in the order of 20–50 nm could effectively degrade BDE209 in the solvent (tetrahydrofuran/water). Influence factors, such as Ni/Fe nanoparticle dosage, initial BDE209 concentration, and Ni loading, on the removal of BDE209 were studied. The results indicated that the degradation of BDE209 followed pseudo-first-order kinetics, and the degradation rate of BDE209 increased with increasing the amount of nano Ni/Fe particles, Ni/Fe ratio, and decreasing the initial concentration of BDE209. Through analyzed the mass balance of the BDE209 removal, degradation was the main process of BDE209 removal. The mechanism of debromination was deduced by analyzing the reaction products using gas chromatography–mass spectrometry, the bromide ion in the solution and varying the solvent conditions. Stepwise hydrogen reduction is the main process of debromination, and the hydrion play an important role in the reaction. Moreover, the experiment of long term performance and leaching of Ni were also carried out to test the stability and durability of Ni/Fe nanoparticles in BDE209 degradation.
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BIOMACROMOLECULES
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2024
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IF 5.5
Yidan Chen,Tiantian Feng,Xiaohong Zhu,Yuting Tang,Yao Xiao,Xiuhua Zhang,Sheng-Fu Wang,Dong Wang,Wei Wen,Jichao Liang,Huayu Xiong
Reactive oxygen species (ROS) have emerged as a promising treatment option for antibacterial and biofilm eradication. However, their therapeutic efficacy is significantly hampered by the unique microenvironments of diabetic wounds. In this study, we designed and synthesized porphyrin-based Fe covalent organic frameworks (Fe-COF) through a Schiff base condensation reaction. Subsequently, Fe-COF were encapsulated with hyaluronic acid (HA) through electrostatic adsorption, resulting in a novel formulation named HA-Fe-COF for diabetic wound healing. HA-Fe-COF were engineered to respond to hyaluronidase in the infected wound, leading to the controlled release of Fe-COF. Those released Fe-COF served a dual role as photosensitizers, generating singlet oxygen and localized heating when exposed to dual light sources. Additionally, they acted as peroxidase-like nanozymes, facilitating the production of ROS through enzymatic reactions. This innovative approach enabled a synergistic therapeutic effect combining photodynamic, photothermal, and chemodynamic modalities. Furthermore, the sustained release of HA from HA-Fe-COF promoted angiogenesis, collagen deposition, and re-epithelialization during the diabetic wound healing process. This “all-in-one” strategy offers a novel approach for the development of antimicrobial and biofilm eradication strategies that minimize damage to healthy tissues in vivo.
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JOURNAL OF NANOPARTICLE RESEARCH
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2024
·Vol. 26
·期 9
·1-15
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IF 2.1
Yin Yanbing,Zhang Xueli,Jiang Bei,Wang Zhou,Feng Yongming,Li Xueying
Developing efficient catalysts for visible light reactions is vital in the field of photocatalysis. This study focuses on the synthesis of novel ternary composites (α-DMACoPc/TiO 2 /MIL-101 (Fe)) by leveraging the excellent adsorption properties of MIL-101 (Fe), the photosensitizing capabilities of phthalocyanine, and the photocatalytic potential of TiO 2 . The nanocomposites’ structural and optical attributes were thoroughly analyzed. X-ray powder diffraction (XRD) was utilized to showcase the crystalline nature of the composites. Furthermore, Fourier transform infrared (FT-IR) studies confirmed the formation of ternary nanocomposites. Optical absorption investigations demonstrated the tuning of the optical band gap from the UV to the visible range. The results indicated that nearly 94% of the organic material was decomposed after 150 min of exposure to simulated sunlight from a xenon lamp. This high efficiency can be attributed to the synergistic interaction among the composites, enhancing light absorption. The composite’s robust stability was evidenced through cyclic tests. Valuable information was provided to advance the design and synthesis of photocatalysts consisting of metal–organic frameworks synergized with semiconductors. Exploring the possibility of mesoporous materials was based on MOFs for photodegradation of organic pollutants. The photocatalytic degradation of organic pollutants by MOFs mesoporous materials was also investigated. The potential of composite materials in the field of dye degradation of industrial waste is confirmed. The good recycling photocatalytic reusability indicates the promising application of this photocatalyst. Graphical Abstract
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Journal of Environmental Sciences
·
2024
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IF 5.9
Qianyu Xu,Haoyang Fu,Jiyuan Gu,Liyu Lei,Lan Ling
The overuse of antibiotics and antitumor drugs has resulted in more and more extensive pollution of water bodies with organic drugs, causing detrimental ecological effects, which have attracted attention towards effective and sustainable methods for antibiotics and antitumor drug degradation . Here, the hybrid nanomaterial (g-C 3 N 4 @Fe/Pd) was synthesized and used to remove a kind of both an antibiotic and antitumor drug named mitoxantrone (MTX) with 92.0% removal efficiency, and the MTX removal capacity is 450 mg/g. After exposing to the hybrid material the MTX aqueous solution changed color from dark blue to lighter progressively, and LC-UV results of residual solutions show that a new peak at 3.0 min (MTX: 13.2 min) after removal by g-C 3 N 4 @Fe/Pd appears, with the simultaneous detection of intermediate products indicating that g-C 3 N 4 @Fe/Pd indeed degrades MTX. Detailed mass spectrometric analysis suggests that the nuclear mass ratio decreased from 445.2 (M + 1H) to 126.0 (M + 1H), 169.1 (M + 1H), 239.2 (M + 1H), 267.3 (M + 1H), 285.2 (M + 1H), 371.4 (M + 1H) and 415.2 (M + 1H), and the maximum proportion (5.63%) substance of all degradation products (126.0 (M + 1H)) is 40-100 times less toxic than MTX. A mechanism for the removal and degradation of mitoxantrone was proposed. Besides, actual water experiments confirmed that the maximum removal capacity of MTX by g-C 3 N 4 @Fe/Pd is up to 492.4 mg/g (0.02 g/L, 10 ppm).
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Journal of Environmental Chemical Engineering
·
2024
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IF 7.4
Ping Zhang,Dan Zou,Chunhua Dong,Feiping Zhao,Weichun Yang,Mengying Si,Zhihui Yang
Heavy metal polluted soil remediation is a global concern. Therefore, it is urgently needed to develop new ways for soil remediation . Although the electrochemical method is a simple, efficient, and promising process, the reaction mechanism of arsenic (As) in contaminated soil treated by the electrochemical method is rarely noticed. Herein, electrochemical techniques were developed for As removal from contaminated soil, which can be effectively achieved by using a Fe sacrificial anode to form Fe 3+ species and by combining manganese oxide in soils for remediation. The results showed that the As was changed from an unstable to a stable state, and As pollutions were effectively removed by this electrochemical method. Further, the dissolution kinetics of Fe and Mn oxides , arsenic reaction kinetics and the phase transformation process during the remediation process were investigated by cyclic voltammetry (CV) methods. From the simulation experiments, it was found that As(III) should be oxidized by Mn 4+ and Fe 3+ to form As(V), and As(V) was the main reactant with Fe and Mn oxides for As removal. Consequently, the current work may provide a new insight into solve As contamination in soil, and provide some new insights into the interaction mechanism between multiple components.
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JOURNAL OF HAZARDOUS MATERIALS
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2024
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IF 12.2
Yongzhen Dong,Jiawei Liu,Liqin Kong,Dongyang Deng,Long Wu,Yiping Chen
This study presents the development of a magnetic relaxation switching (MRS) immunosensor for the sensitive detection of chlorpyrifos (CPF) with a signal amplification strategy using Pd/Cu-TCPP(Fe) hybrid nanosheets and polydopamine (PDA). Pd/Cu-TCPP(Fe) nanosheets, which exhibit high peroxidase-like activity and excellent storage stability, making them suitable replacements for natural enzymes in biosensors, are further functionalized with goat anti-mouse IgG (Ab 2 ) to construct an immunosensor. The mechanism relies on the competition between free CPF and the immobilized bovine serum albumin-CPF conjugates for antibody binding, which modulates the aggregation of magnetic nanoparticles (MNPs) that are related to the transverse relaxation time. The optimized immunosensor shows a linear detection range from 0.5 ng/mL to 100 ng/mL and a limit of detection (LOD) of 0.24 ng/mL, outperforming traditional enzyme-linked immunosorbent assay (ELISA) methods by achieving an LOD that is about 9 times lower. Real sample analysis demonstrates the applicability of the Pd/Cu-TCPP(Fe)-PDA-MRS immunosensor for detecting CPF residues in tomato and water samples, with results well consistent with those obtained using gas chromatography. This work highlights the potential of nanomaterials in enhancing the performance of MRS immunosensors for pesticide residue analysis in environmental and food safety monitoring.
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