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LANGMUIR · 2024 · IF 3.7

Interfacial Engineering Boosting the Activity and Stability of MIL-53(Fe) toward Electrocatalytic Nitrogen Reduction

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.

CAS / MDL: 14402-89-2
研究领域: 材料科学 · 电化学 · 催化化学
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CHEMICAL ENGINEERING JOURNAL · 2025 · IF 13.2

Interface-induced Fe-rich NixFe3-xO4 electrode for efficient oxygen evolution at high current densities

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.

研究领域: 材料科学 · 电化学
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ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH · 2024 ·Vol. 31 ·期 6 ·9421-9432 · IF 0

Efficient composite chlorinated ethenes removal using gallic acid to enhance Fe/Ni nanoparticles activated persulfate

Che Mingda,Su Hongjian,Si Huimin,Guo Bin,Huang Renliang,Zhao Jing,Su Rongxin

As the representative volatile chlorinated hydrocarbons detected in wastewater, the removal of composite chlorinated ethenes is a major challenge in wastewater treatment. In the present study, an efficient removal system for composite chlorinated ethenes was reported, in which gallic acid was used to enhance the activation of persulfate by Fe/Ni nanoparticles. The influences of gallic acid-Fe/Ni and persulfate concentrations, initial pH value, reaction temperature, inorganic anions, and natural organic matters were evaluated in the composite chlorinated ethenes removal. Our results showed that the gallic acid-Fe/Ni-persulfate system with 9.0 mM of gallic acid-Fe/Ni and 30.0 mM of persulfate yielded about 100% trichloroethylene removal and 97.3%-98.6% perchloroethylene removal in the pH range of 3.0–12.0. Electron paramagnetic resonance analysis and radical quenching experiments indicated that SO 4 •− and • OH were the predominant radical species under acidic and alkaline conditions. Ultraviolet visible spectroscopy and inductively coupled plasma optical emission spectrometer tests revealed the Fe-gallic acid chelation could regulate the concentration of iron ions and improve the reactivity of gallic acid-Fe/Ni. These results demonstrated that the gallic acid-Fe/Ni-persulfate system was a promising strategy for treating composite chlorinated ethenes-containing wastewater.

研究领域: 环境科学 · 化学工程
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JOURNAL OF HAZARDOUS MATERIALS · 2010 · IF 4.144

Debromination of polybrominated diphenyl ethers by Ni/Fe bimetallic nanoparticles: Influencing factors, kinetics, and mechanism

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.

研究领域: 环境科学 · 化学工程
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Catalysis Science & Technology · 2024 · IF 4.4

Co–Fe catalyst supported on acidified bentonite for selective hydrogenation of cinnamaldehyde

Haixiang Shi,Yiyuan Xu,Tongming Su,Xuan Luo,Xinling Xie,Zuzeng Qin,Hongbing Ji

The surface acidity and structure of catalysts play crucial roles in cinnamaldehyde (CAL) selective hydrogenation to manufacture cinnamyl alcohol (COL). Herein, a Co–Fe-supported acidified bentonite catalyst (Co–Fe/ACBT) was prepared via sulfuric acid treatment of bentonite (BT) and the traditional impregnation method. The combination study, including FT-IR spectra of adsorbed pyridine and ammonia temperature-programmed desorption (NH3-TPD), showed that Co–Fe/ACBT has vast acidic sites mainly originating from surface unsaturated metal sites of ACBT, which prefer to adsorb polar >CO but not nonpolar >CC<. X-ray photoelectron spectroscopy (XPS) verified that the effect of electron transfer was significantly enhanced when the active metal was loaded on ACBT, leading to an increase in the electron cloud density of the Co species, which promoted the activation of >CO. Due to the modified electronic properties of Co species and abundant acidic sites, Co–Fe/ACBT exhibited a 90.5% conversion and 86.8% hydrogenation selectivity from CAL to COL, which are notably greater than those of the Co–Fe-supported bentonite catalyst (32.0% CAL conversion and 66.4% COL selectivity).

CAS / MDL: 104-55-2
研究领域: 催化化学 · 材料科学
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APPLIED CATALYSIS B-ENVIRONMENTAL · 2024 · IF 20.2

Promotion of Cu/ZnO/Al2O3 by Fe towards methanol steam reforming reaction

Haitao Yan,Didi Li,Zhaocong Jiang,Haoyuan Gu,Mengyuan Zhu,Yi-Fan Han,Minghui Zhu

Cu-based catalysts have been extensively used in the methanol steam reforming (MSR) reaction owing to low cost and high efficiency. In this work, we investigated the promotional effect of Fe on the Cu/ZnO/Al 2 O 3 catalysts prepared by an incipient-wetness impregnation method using a series of (quasi) in situ characterization techniques. The form of the Fe species was found to strongly depend on the Fe content. Fe species are present as highly dispersed FeO x in small amount of Fe with improved the dispersion of Cu. As Fe content increases, Fe species gradually transition to CuFe alloy and eventually to Fe 3 O 4 particles, leading to a decrease in Cu dispersion. With the gradual increase in Fe content, the apparent activity shows a volcanic trend, with CuAl-0.1Fe showing highest activity, whereas the intrinsic activity gradually decreases. Compared with CuAl- x Fe, adding moderate Fe to Cu/ZnO/Al 2 O 3 promotes the dispersion of Cu and Zn, forming abundant Cu-ZnO x interfacial sites, which improves both apparent and intrinsic activities. The best catalytic performance was obtained with the CuZnAl-0.1Fe catalyst, achieving the highest H 2 production rate of 134.7 mmol g cat −1 h −1 at 200 °C. This study reveals the role of Fe in Cu-based catalysts for MSR and inspires the design of improved Cu-based catalysts.

CAS / MDL: 7782-61-8 497-19-8
研究领域: 催化化学 · 材料科学
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APPLIED THERMAL ENGINEERING · 2016 · IF 3.043

Influence of Fe powders replacing Cu powders on the thermal and mechanical properties of aluminate cementitious thermal energy storage materials at high temperature

Aihong Du,Huiwen Yuan,Wei Liao,Haobo Zhou,Chunhua Lu,Zhongzi Xu

Cost-effective thermal energy storage materials are vital to the application of solar thermal power plants . One focus of this paper is improving thermal and mechanical properties of the thermal energy storage materials; the second focus lies in reducing the investment cost. On the basis of aluminate cementitious composites with 1   wt% nano-SiO 2 , 1   wt% nano-Cu and 15   wt% Cu powders, we introduced different wt% (0, 5, 10, and 15) of Fe powders to gradually replace 15   wt% Cu powders. The samples were heated at 105, 350, and 900   °C, respectively. As a result, when the content of Fe powders substitution was 10   wt%, volume heat capacity, thermal conductivity and compressive strength of the composites after heat-treatment at 900   °C were up to 2.38   MJ   m −3   K −1 , 1.45   W   m −1   K −1 , and 73.8   MPa respectively, which were 26.6%, 26.1%, and 24.0% higher than those of the composites with 15   wt% Cu powders. At the same time, the investment of the composites with 10   wt% Fe powders substitution was reduced almost 62.0%, compared with that of the composites with 15   wt% Cu powders. In addition, XRD and MIP were employed to characteristic the mineral phases and the pore structures of the aluminate cementitious composites, respectively.

研究领域: 材料科学 · 能源工程
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JOURNAL OF ALLOYS AND COMPOUNDS · 2019 · IF 4.175

Enhanced electromagnetic wave absorption of olive-like Fe3O4/Fe@C core-shell nanocomposite in Ku band

Xiang Li,Lunzhou Yu,Zhen Xiang,Erbiao Cui,Juan Xiong,Xiao Wang,Wei Lu

Core-shell structure is an effective approach to modulate the impedance matching behaviour and induce polarization relaxation at the interface for the high-performance electromagnetic wave absorption (EMWA) materials. Herein, core-shell structures of Fe 3 O 4 –Fe@C (FFC) were successfully developed by hydrothermal and thermal decomposition methods. The results showed that the phase composition, microstructure and EMWA performance were tailored by the heat treatment process. The optimized FFC hybrid exhibited a minimum reflection loss ( RL ) value of −56.3 dB with a matching thickness of 1.99 mm, and the effective bandwidth ( RL   < −10 dB, 5 GHz) covers almost the whole Ku band. The enhanced EMWA properties of the reinforced olive-like composites were mainly ascribed to the magnetic loss derived from the enhanced magnetic anisotropy, and the dielectric loss originated from the multilevel interface and polarization characteristics between the core and the shell. Therefore, this work provides an approach to design core-shell nanocomposites with enhanced EMWA performance.

研究领域: 材料科学 · 电磁学
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CHEMOSPHERE · 2020 · IF 5.778

Study on the efficacy and mechanism of Fe-TiO2 visible heterogeneous Fenton catalytic degradation of atrazine

Nan Yang,Yanping Liu,Jia Zhu,Zhongqiang Wang,Jinwei Li

In order to improve the catalytic activity and recycling performance of heterogeneous Fenton catalyst, a heterogeneous Fenton catalyst Fe/TiO 2 based on TiO 2 supported visible light response was prepared by a simple method using TiO 2 synthesized by sol-gel method as carrier and ferric nitrate as Fe source. It was characterized by SEM , EDX , XRD, UV–vis instruments. The influencing factors of catalytic degradation of atrazine by visible light heterogeneous Fenton of Fe/TiO 2 were studied and the reaction kinetics were fitted. The mineralization degree of atrazine was reflected by the removal rate of TOC. The intermediate products by the degradation of the catalytic system was analyzed and the reaction mechanism of Fe/TiO 2 –H 2 O 2 visible light system was discussed. The XRD results showed that Fe was highly dispersed on the surface of TiO 2 in the form of α-Fe 2 O 3 . The Fe/TiO 2 catalyst with heterogeneous Fenton and visible light photocatalytic activity was successfully optimized, forbidden bandwidth of Fe/TiO 2 after Fe supported was narrower, the scope of light absorption red-shifted, the electron-hole pairs were more generated, and there was a significant synergistic effect between the carrier TiO 2 and the supported Fe, which exhibited good oxidation capacity for degradation of 10 mg L −1 atrazine in pH of 3, the concentration of H 2 O 2 was 1.6 mM, and the catalyst was added at 1 g L −1 , achieving over 95% removal efficiency within 30 min, and, in the range of pH 3–7, the degradation rate of the reaction for 30 min can be maintained above 75%, which greatly broadened the range of pH application and had good recycling performance. The degradation process conformed to the quasi-first-order kinetic model . Through LC-MS analyzed, 12 intermediate products were formed during the degradation of atrazine, the final products were all cyanuric acid, and then the triazine ring was mineralized into inorganic substances such as CO 2 , H 2 O and NO 3 − by oxidation of ·OH, and the possible degradation pathways were inferred.

研究领域: 环境科学 · 催化化学
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LANGMUIR · 2025 · IF 3.9

Renewable Magnetic NH2-MIL-101(Fe) for the Efficient Removal of Bisphenol A from Aqueous Solutions

Mingyang Xiong,Yao Zeng,Ruisi Qiu,Hongxing He,Yi Zhang,Zhifeng Nie,Bing Wang

Bisphenol A (BPA) is extensively utilized as an industrial chemical in the production of certain plastics and epoxy resins. They are frequently found in environmental water and have the potential to cause risks to both the environment and human health. To efficiently remove the endocrine disruptor BPA from aqueous solutions, sea urchin-like magnetic material Fe3O4@PDA@NH2-MIL-101 (Fe) was synthesized via hydrothermal methods. Fe3O4@PDA@NH2-MIL-101 (Fe) has excellent adsorption performance, with a theoretical maximum adsorption capacity of 300.47 mg/g for BPA. The adsorption kinetics of BPA by Fe3O4@PDA@NH2-MIL-101 (Fe) followed the pseudo-second-order kinetic model and Liu’s isotherm model. Magnetic separation experiments reveal a high recovery efficiency, maintaining 94.82% of its initial adsorption capacity after five cycles. The primary adsorption mechanisms of Fe3O4@PDA@NH2-MIL-101 (Fe) on BPA included pore filling, hydrogen bonding, π–π interaction, and Lewis acid–base interaction. Additionally, the material showed excellent removal performance of BPA, with a maximum adsorbed amount of 135.27 mg/g for total organic carbon (TOC) in the shale gas fracturing flowback fluid. These findings suggest that Fe3O4@PDA@NH2-MIL-101 (Fe) holds significant potential as an adsorbent for BPA removal from actual wastewater, offering promising prospects for practical applications.

CAS / MDL: 51-61-6 7705-08-0
研究领域: 环境科学 · 材料科学
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PROCESS SAFETY AND ENVIRONMENTAL PROTECTION · 2025 · IF 7.8

Performance and mechanism of ciprofloxacin removal in water via catalytic ozonation using Fe-Mg/PDA@Al2O3

Shanshan Huang,Bolin Li,Gezi Li,Siyuan Zheng,Kanglin Tian,Weimin Xie,Simiao Wu,Jun Wang,Ying Yu,Xiaoman He

There is currently an urgent need to develop technologies for ciprofloxacin (CIP) removal in wastewater owing to its widespread usage in human and animal populations and subsequent transmission into surface water. Aluminum (Al 2 O 3 ) is an excellent carrier, and polydopamine (PDA) is a surface modifier with a high nitrogen content and strong adhesion, and may represent a potential tool for CIP removal in wastewater. However, minimal research has been conducted on using PDA to improve the interactions between carrier and active components and thus improve the ozone utilization efficiency as well as catalytic activity and stability in CIP removal schemes. To address this research gap, study successfully prepared Fe-Mg/PDA@Al 2 O 3 composite materials for the catalytic ozone removal of CIP from water. The influencing factors and degradation mechanisms of the catalytic ozone treatment of ciprofloxacin wastewater and possible antibiotic degradation pathways were proposed. The removal of CIP was mainly carried out through indirect oxidation dominated by hydroxyl radicals (•OH), in addition to catalyst adsorption and direct ozone oxidation, and the oxidative degradation of CIP conformed to a pseudo-first-order reaction kinetic model. Under ideal operating conditions, the CIP degradation efficiency of Fe-Mg/PDA@Al 2 O 3 /O 3 system reached 91.35% after 15   min. The mineralization efficiency of Fe-Mg/PDA@Al 2 O 3 /O 3 system was significantly higher than that of the single-ozone system. After four repeated uses of Fe-Mg/PDA@Al 2 O 3 , the CIP degradation efficiency remained stable, and the metal ion leaching concentration was within the limit, indicating that Fe-Mg/PDA@Al 2 O 3 demonstrated a high catalytic performance and stability.

研究领域: 环境科学 · 水处理工程
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CHEMICAL ENGINEERING JOURNAL · 2022 · IF 16.744

Simultaneous removal of algae, microcystins and disinfection byproduct precursors by peroxymonosulfate (PMS)-enhanced Fe(III) coagulation

Xin Yang,Lu Yao,Yu Wang,Xinran Zhang,Pengfei Ren

Algae blooms can clog filtration tank, release toxic cyanotoxin and produce undesirable disinfection byproducts (DBPs) in post-chlorination, which brings challenges to conventional water treatment processes. In this study, peroxymonosulfate (PMS) was tested for its ability to improve Fe(III) coagulation of Microcystis aeruginosa in water treatment. Compared with conventional Fe(III) coagulation, the presence of PMS resulted in the formation of larger floc and thus better algae and turbidity removal. The removal of algae by PMS-enhanced Fe(III) coagulation (PMS-Fe(III)) process reached 97.5% at 1 mM PMS, which was 1.5 times higher than that by Fe(III) coagulation alone. The oxidization of surface-adsorbed extracellular organic matter destabilized the algal cells and enhanced their coagulation without greatly damaging the cells’ integrity. Simultaneously, about 80% of Microcystin-LR, a cyanotoxin, was degraded in the enhanced process. Moreover, the formation of DBPs and their associated toxicity during the subsequent chlorination were decreased by 49.2% and 13.6%, respectively. The production of trihalomethanes, haloacetic acids and haloacetronitriles was particularly abated. SO 4 •- and HO • , which were formed from PMS activation through redox cycling of Fe mediated by the existing natural organic matter, were mainly responsible for algae removal. The results indicate that supplementing Fe(III) coagulation with PMS is a promising option for treating water during algal blooms.

研究领域: 环境科学 · 水处理工程
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