Small
·
2025
·
IF 12.1
Haiyang Shi,Lei Zhang,Xinhua Huang,Qingquan Kong,Abdukader Abdukayum,Yingtang Zhou,Guoyou Cheng,Sanshuang Gao,Guangzhi Hu
The design and fabrication of nanocatalysts with high accessibility and sintering resistance remain significant challenges in heterogeneous electrocatalysis. Herein, a novel catalyst is introduced that combines electronic pumping with alloy crystal facet engineering. At the nanoscale, the electronic pump leverages the chemical potential difference to drive electron migration from one region to another, separating and transferring electron-hole pairs. This mechanism accelerates the reaction kinetics and improves the reaction rate. The interface electronic structure optimization enables the CoFe/carbon nanotube (CNT) catalyst to exhibit outstanding oxygen reduction reaction (ORR) and oxygen evolution reaction (OER) performance. Specifically, this catalyst achieves an ORR half-wave potential (E₁/₂) of 0.895 V, outperforming standard Pt/C and RuO₂ electrocatalysts in terms of both specific activity and stability. It also demonstrates excellent electrochemical performance for OER, with an overpotential of only 287 mV at a current density of 10 mA cm⁻ 2 . Theoretical calculations reveal that the carefully designed crystal facets reduce the energy barrier of the rate-determining steps for both ORR and OER, optimizing O₂ adsorption and promoting the oxygen capture process. This study highlights the potential of developing cost-effective bifunctional ORR–OER electrocatalysts, offering a promising strategy for advancing Zn–air battery technology.
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JOURNAL OF INDUSTRIAL AND ENGINEERING CHEMISTRY
·
2024
·
IF 5.9
Fuhao Gan,Chunmei Gao,Shifeng Ji,Yunqing Xing,Tianming Gong,Lihui Tian,Yiming Bai,Zhuolong Wu
In this study, the iron-based metal–organic framework MIL-53(Fe) was successfully prepared by a solvent method and used as a photocatalyst for the efficient degradation of DDBAC under visible light. The morphology, structure and photocatalytic properties of MIL-53(Fe) were investigated by SEM, XRD, XPS and UV–vis DRS characterization methods. The optimum conditions for the degradation of DD pathways of DDBAC were analyzed in combination with DFT calculations. Based on molecular orbital theory and free radical quenching experiments, it was demonstrated that hydroxyl radicals were the main contributors in the oxidative degradation of DDBAC. The toxicity of DDBAC and its intermediates was evaluated by culturing Chlorella vulgaris, and the results showed that the Vis/MIL-53(Fe)/H 2 O 2 system was capable of solution detoxification.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2025
·
IF 21.1
Ruting Huang,Peidong Ma,Yeyin Zhang,Kaiming Chen,Liping Wang,Ranran Wang,Xianyang Shi,Ying Yu
The enrichment efficiency during the high-value conversion of carbon dioxide still presents certain limitations in practical applications. Iron-cobalt-based metal-organic framework (MOF) nanoparticles, which exhibit lower toxicity to Microcystis aeruginosa , have been successfully introduced into microalgae solutions to address the issue of low CO 2 concentration in interfacial reactions. When 1,4-naphthalenedicarboxylic acid was employed as an organic ligand under synthesis conditions of 130°C, pH 3.5, and a reaction time of 15 h, the resulting MOF exhibited a CH₄ yield of 92.6 μmol g⁻¹ h⁻¹ in the photocatalytic system at room temperature (25°C). The combination of Microcystis aeruginosa with the optimal Fe-Co-MOFs system achieved a selectivity of up to 96.1 % in converting CO 2 into CH 4 . When Microcystis aeruginosa was cultured in a modified medium with a pH of 6.78 and 5 mg of NDC-T130 at 25°C for 12 h, an OD 600 of 0.192 ± 0.01 was observed. The CH₄ yield from the Microcystis aeruginosa -NDC-T130 co-culture composite system was 1.46 times that of the Fe-Co-MOFs. Density-functional theory calculations indicate that carbon dioxide molecules preferentially adsorb on the crystal surfaces of (CoFe 2 )O 4 (113) and (Co 0.457 Fe 0.543 )(Co 1.543 Fe 0.457 )O 4 (311), with the Co site being more likely to serve as the reactive site for CO 2 photoreduction to CH 4 within the Fe-Co-MOFs. Transcriptome analysis demonstrates that MOFs enhance the dark reactions of microalgae and facilitate further CO 2 fixation for photosynthesis and electron transfer, which are crucial for improving the high-value CO 2 conversion efficiency of this system. This strategy provides both experimental and theoretical support for iron-based MOFs as photocatalytic materials, regardless of CO 2 concentration.
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JOURNAL OF MEMBRANE SCIENCE
·
2024
·
IF 8.4
Lina Zhang,Ziren Wan,Jia Deng,Fangzhou Li,Jingqi Dong,Wulin Yang,Shaodong Xie,Guanghe Li,Fang Zhang
The catalytic membrane, combining confinement effect with advanced oxidation processes , exhibits great potential as an efficient technology for removing contaminants and mitigating membrane fouling . Herein, the Prussian blue analogues (PBAs) functionalized graphene oxide (GO) membranes, referred as PGMs, was successfully fabricated. It exhibited a package-like confined structure where Co–Fe PBAs were encapsulated within interconnected GO nanosheets . The surface properties, internal structure as well as the catalytic performance of PGMs were controlled by adjusting the amount of Co–Fe PBAs anchored on GO nanosheets . The designed PGM as efficient peroxymonosulfate activator exhibited exceptional catalytic performance, achieving complete removal of bisphenol A (BPA) with a retention time of 31 ms. The corresponding first-order rate constant was 6000 min −1 , which surpassed conventional batch system by four orders of magnitude (0.2194 min −1 ). Moreover, the redox cycle involving Fe 2+ and Co 3+ , coupled with the effective suppression of ion leaching from Co–Fe PBAs nanoparticles (<10 μg/L) through GO protective layers, ensured the stable catalytic performance of PGM over 144 h. This study employs a novel approach to confine catalytic nanoparticles within two-dimensional nanosheets, demonstrating the potential applications of the resulting confined membrane in water treatment.
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INORGANIC CHEMISTRY
·
2024
·
IF 4.3
Shuo Chen,Kaiqin Yue,Jiawei Shi,Zhicheng Zheng,Yuanqing He,Hao Wan,Gen Chen,Ning Zhang,Xiaohe Liu,Renzhi Ma
Most nonoxide catalysts based on transition metal elements will inevitably change their primitive phases under anodic oxidation conditions in alkaline media. Establishing a relationship between the bulk phase and surface evolution is imperative to reveal the intrinsic catalytic active sites. In this work, it is demonstrated that the introduction of Fe facilitates the phase transition of orthorhombic CoSe2 into its cubic counterpart and then accelerates the Co–Fe hydroxide layer generation on the surface during electrocatalytic oxygen evolution reaction (OER). As a result, the Fe-doped cubic CoSe2 catalyst exhibits a significantly enhanced activity with a considerable overpotential decrease of 79.9 and 66.9 mV to deliver 10 mA·cm–2 accompanied by a Tafel slope of 48.0 mV·dec–1 toward OER when compared to orthorhombic CoSe2 and Fe-doped orthorhombic CoSe2, respectively. Density functional theory (DFT) calculations reveal that the introduction of Fe on the surface hydroxide layers will tune electron density around Co atoms and raise the d-band center. These findings will provide deep insights into the surface reconstitution of the OER electrocatalysts based on transition metal elements.
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CATALYSIS LETTERS
·
2025
·Vol. 155
·期 2
·1-15
·
IF 2.4
Li Ziyuan,Luo Mingsheng,Yang Zhi,Cui Xiaoteng,Yang Wenshuai,Xia Lingman,Shao Changke,Rahman Roshni
To effectively mitigate the global warming issue, it is crucial to develop advanced technologies that can significantly reduce carbon dioxide emissions. CO 2 hydrogenation for methanol synthesis is increasingly recognized as a promising chemical approach for the green-house gas utilization. In this study, we present a highly active, selective and stable Mo modified ZnCu-MOF and ZnCuAl-LDH composite catalysts, which achieves 18% CO 2 conversion and 70% methanol selectivity at 230 °C, 3.0 MPa at a space velocity of 3600 mL·g cat −1 ·h −1 . Furthermore, after 140 h of operation, the catalyst demonstrates superior durability. In-situ DRIFT results reveal that this CO 2 hydrogenation reaction over the ZnCu-MOF and ZnCuAl-LDH composite catalysts proceeds through key intermediate formate species, ultimately leading to the methanol formation. In contrast, the Mo-modified catalysts facilitate the CO insertion reaction (CO 2 → CO*, CO* + *CH x → CH 3 OH), thereby enhancing the methanol yield. Graphical
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SCIENCE OF THE TOTAL ENVIRONMENT
·
2024
·
IF 8.2
Guohui Wang,Qixin Zhang,Lailai Qin,Kaixuan Tan,Chunguang Li,Lianshun Li,Tinggui Yang,Xiaojuan Liu
A novel metal-organic framework (MOF) material, MIL-100(Fe)-DMA, was synthesized using the solvothermal method. The structure of the MOF was characterized using scanning electron microscopy-energy dispersive X-ray spectroscopy, N 2 adsorption–desorption isotherms, X-ray diffraction analysis, Fourier-transform infrared spectroscopy, X-ray photoelectron spectroscopy, and Mössbauer spectroscopy. Batch adsorption experiments were performed to investigate the effects of initial Sr 2+ and Cs + concentrations, adsorption time, pH, and coexisting cations on the adsorption performance of the material. The adsorption mechanism was further elucidated using adsorption kinetics and isotherm models. The results indicated that the adsorption of Sr 2+ and Cs + does not significantly affect the MOF material structure. As reaction time and initial ion concentration increased, the adsorption capacity of MIL-100(Fe)-DMA for Sr 2+ and Cs + increased rapidly and then gradually reached equilibrium. Optimal adsorption occurred under alkaline conditions, with maximum adsorption capacity observed at pH = 8. The adsorption process for Sr 2+ and Cs + was well described by the pseudo-second-order kinetic model, the Weber–Morris model, and the Langmuir adsorption isothermal model. The adsorption process was mainly identified as monolayer chemical adsorption, influenced by multiple factors. Characterization combined with density functional theory calculations revealed that the unsaturated carboxylic acid groups on the surface of the MOFs play a crucial role in the interaction with Sr 2+ and Cs + .
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MOLECULES
·
2024
·Vol. 29
·期 2
·307
·
IF 4.2
Zixuan Li,Qinghong Shi,Xiaoyan Dong,Yan Sun
Co-immobilization of laccase and mediator 2,2′-azino-bis(3-ethylbenzothiazoline-6-sulphonic acid) (ABTS) for wastewater treatment could simultaneously achieve the reusability of laccase and avoid secondary pollution caused by the toxic ABTS. Herein, Fe-induced mineralization was proposed to co-immobilize laccase and ABTS into a metal–organic framework (ZIF-8) within 30 min. Immobilized laccase (Lac@ZIF-8-Fe) prepared at a 1:1 mass ratio of Fe2+to Zn2+exhibited enhanced catalytic efficiency (2.6 times), thermal stability, acid tolerance, and reusability compared to free laccase. ABTS was then co-immobilized to form Lac+ABTS@ZIF-8-Fe (ABTS = 261.7 mg/g). Lac@ZIF-8-Fe exhibited significantly enhanced bisphenol A (BPA) removal performance over free laccase due to the local substrate enrichment effect and improved enzyme stability. Moreover, the Lac+ABTS@ZIF-8-Fe exhibited higher BPA removal efficiency than the free laccase+ABTS system, implying the presence of a proximity effect in Lac+ABTS@ZIF-8-Fe. In the successive malachite green (MG) removal, the MG degradation efficiency by Lac@ZIF-8-Fe was maintained at 96.6% at the fifth reuse with only an extra addition of 0.09 mM ABTS in each cycle. As for Lac+ABTS@ZIF-8-Fe, 58.5% of MG was degraded at the fifth cycle without an extra addition of ABTS. Taken together, this research has provided a novel strategy for the design of a co-immobilized laccase and ABTS system for the degradation of organic pollutants.Keywords:laccase;mediator;co-immobilization;MOFs;organic pollutants;biodegradation
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JOURNAL OF MAGNETISM AND MAGNETIC MATERIALS
·
2024
·
IF 2.5
Zhangqiao Zhou,Qi Li,Meiqi Wen,Ruilin Zhou,Xian Wang
The coatings play a crucial role in enhancing the performance of soft magnetic composites (SMCs). This study aims to create coatings for Fe-Ni-Mo SMCs using polysilazane (PSZ) as the precursor. The transformation mechanism of the PSZ/resin mixture is studied by analyzing functional groups and chemical bonds at various temperatures. During the self-polymerization process of PSZ at 350 °C, N–H, C = C–H, Si-H bonds, –CH 3 , and Si-CH 3 groups undergo crosslinking reactions to form C–C and Si-N bonds. When the temperature reaches 600 °C, PSZ polymer cleavage, O-Si-C and Si-N-Si bond dominate in the coating. Additionally, PSZ can effectively enhance the heat resistance of silicone resin through its reaction with Si-OH groups, which has a significant effect on increasing the resistivity of SMCs and reducing high frequency core loss. Optimizing the PSZ content to 0.5 wt% enhances the magnetic properties of Fe-Ni-Mo SMCs, resulting in a μ e of 74.0 at 100 kHz and a corresponding core loss ( P cv ) of 547.7 mW/cm 3 at 100 kHz/100 mT. The findings provide valuable insights for optimizing PSZ content to improve magnetic performance in SMCs.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2024
·
IF 9.4
Qiyu Li,Lei Zhao,Zhaozhao Zhu,Pei Xiong,Jiayu Zuo,Jun Song Chen,Rong Li,Rui Wu
Zinc-air batteries (ZABs) have garnered significant interest due to their environmental friendliness, low cost, and high energy density. However, their practical application is significantly hindered by high overpotential and sluggish reaction kinetics. Here, we propose a hollow nitrogen-doped carbon supported atomically dispersed Fe and Mn sites (FeMn-HNC) through a facile NaCl-assisted pyrolysis strategy. The synthesized FeMn-HNC catalyst possesses a hollow porous structure, resulting in exceptional oxygen reduction reaction (ORR) catalytic activity, remarkable durable stability, and good tolerance to methanol. Furthermore, integrating this catalyst into ZABs demonstrates significant performance advantages, achieving a maximum power density of 223.1 mW cm −2 and a high specific capacity of 804.3 mAh g −1 . This study offers a promising approach for boosting the power density and specific capacity of nitrogen-doped carbon catalysts in ZABs.
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INDUSTRIAL CROPS AND PRODUCTS
·
2025
·
IF 6.2
Zhanjun Li,Yunwei Liu,Mingru Kong,Yibin Xu,Kunlun Wang,Ke Ma,Qi Shen,Qingfen Zhang
To increase the extraction efficiency of quercetin from Pinus koraiensis seed scales (PKSS), an innovative chitosan-Cu-Fe (CS-Cu-Fe) ionic liquid system for efficient ultrasonic-assisted extraction (UAE) of PKSS quercetin (PKSSQ) was designed. A first-order kinetic model was applied to analyse the extraction performance, and key factors influencing the process were systematically optimized. The optimal conditions were as follows: 2.00 g sample, 0.016 mol [BMIM]Br, 0.6 %, 100 W, 53°C, 12:1 mL/g, and 14 min. Under these conditions, the actual PKSSQ yield was 2.92 mg/g ± 0.02 mg/g, which closely aligned with the theoretical yield of 2.96 mg/g. The extraction kinetics were compared across different methods, and the stability of the CS-Cu-Fe system was evaluated through recovery experiments. The CS-Cu-Fe was characterized using Fourier transforms infrared (FT-IR) spectroscopy, thermogravimetric analysis (TGA), X-ray diffraction (XRD), hysteresis loop (HL) measurement, electrical conductance (EC) measurement and scanning electron microscopy (SEM) of the extracted residues. CS-Cu-Fe demonstrated exceptional thermal stability, magnetic properties, and catalytic activity, significantly enhancing the PKSSQ extraction efficiency. FT-IR analysis revealed minimal spectral changes in CS-Cu-Fe, with notable EC differences. Owing to its stable core functional groups, CS-Cu-Fe maintained excellent thermal stability, crystal structure, soft magnetism, and catalytic efficiency. This study highlights the efficiency of the CS-Cu-Fe ionic liquid system in UAE of PKSSQ and the role of its stable core functional groups in improving the extraction and catalytic performance. This innovative approach provides a robust theoretical foundation for extracting and developing natural products from PKSS, with promising future applications.
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Molecular Catalysis
·
2024
·
IF 3.9
Nan Zhou,Xiaoqing Jia,Siyuan Chen,Huafan Li,Feifei Li,Botao Qiao,Hailian Tang,Guoyi Bai
CO 2 methanation is an effective way for CO 2 recycling, and nickel-based catalysts have attracted much attention in this field due to their excellent CH 4 selectivity and cost-effectiveness; however, their applications are limited by their suboptimal catalytic activity. In this work, the catalytic activity of Ni-rutile-based catalysts was increased by almost an order of magnitude simply by doping the rutile with Fe. Series characterizations show that three factors that mainly contributed to the improved catalytic performance of the Ni/Fe-Rutile, which are the reduction of the Ni size, the increase of the basic sites, and the inhibition of the encapsulation of the Ni particles by the support. With Fe doping, the OH and oxygen vacancies on the rutile surface were reduced, which made the support difficult to reduce and thus suppressed the encapsulation of Ni by the support. As a result, the number of exposed active sites on the Ni/Fe-Rutile which with a smaller Ni size was further successfully increased, and the catalytic activity was significantly improved. This study provides new ideas for the design of activity-enhanced supported catalysts from the perspective of tuning the metal-support interaction and may be applicable to other reducible oxide-supported metal catalysts.
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