CHEMICAL ENGINEERING JOURNAL
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2024
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IF 13.3
Jianyue Yan,Peng Liu,Jiawen Li,Hao Huang,Shengfu Tong,Wenbo Song
The electrocatalytic nitrate reduction reaction to ammonia (NRA) offers a promising alternative to traditional ammonia synthesis methods. In nature, enzymes containing molybdenum and iron sites catalyze the reduction of nitrate and nitrite ions. Drawing inspiration from these enzymes, we synthesized a carbon-coated nano-octahedra of FeMo-based nitride (FeMoN@C NO) by pyrolyzing phosphomolybdic acid hydrate (POM) doped Fe-NH 2 -MIL-101 to catalyze NRA. Experimental results demonstrate that in an alkaline environment, FeMoN@C NO exhibits a suitable hydrogen evolution reaction (HER) capacity, and the protons or hydroxyls produced effectively facilitate the hydrogenation reaction in the ammonia synthesis process. Additionally, the introduction of Mo increases the number of active sites and effectively reduces the thermodynamic barrier in NRA, thereby enhancing the rate of ammonia synthesis. As a result, FeMoN@C NO displays outstanding NH 3 Faradaic efficiency (FE) of 98.2 % and an NH 3 yield of 434.16 µmol/h cm −2 . Building upon the excellent electrocatalytic properties of FeMoN@C NO, a new Zn-nitrate battery system is assembled in this work, which exhibits an outstanding peak power density of 3.23 mW cm −2 and an FE of 91.58 % for NH 3 production. This work provides a new perspective for designing enzyme-mimicking nitrate reduction catalysts and broadens the application of Zn-based batteries.
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JOURNAL OF MOLECULAR STRUCTURE
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2025
·
IF 4.7
Zhaobo Wang,Tao Yu,Xiaomao Liu,Jinsheng Li,Xuanwen Liu,Rui Guo
To improve the performance of MIL-100(Fe) in the photo-peroxydisulfate (photo -PDS) degradation system, this study introduced the amino-containing bidentate ligand 5-aminoisophthalic acid (AIA) to simultaneously engineer structural defects and photosensitive sites, thereby synergistically enhancing both photocatalytic activity and metal-mediated catalytic capability. This study synthesized MIL-100(Fe) materials with varying AIA incorporation levels (denoted as M-x %NH₂) and systematically investigated the effects of AIA integration on the catalyst. Degradation experiments were performed in the photo-PDS system using rhodamine B (RhB) as a model pollutant. The results demonstrate that the introduction of AIA induced multiple advantageous effects in the photo-PDS process:1.It enhanced the visible-light absorption capacity;2.Improved the separation efficiency of photogenerated charge carriers;3.Generated defects to increase metal active sites, thereby accelerating PDS activation. Among the samples, M-30 % NH₂ exhibited the optimal performance, achieving nearly complete degradation of RhB within 50 min. The pseudo-first-order rate constant (k) was three times higher than that of unmodified MIL-100(Fe). The catalyst retained approximately 90 % degradation efficiency after five consecutive cycles and demonstrated robust performance across pH 3–9, along with the capability to degrade diverse organic pollutants. Quenching experiments confirmed sulfate radicals (·SO 4 ⁻) and hydroxyl radicals (·OH) as the main active species, and the degradation pathways were elucidated. This study provides foundational insights for modifying MIL-100(Fe) and developing high-efficiency PDS catalysts.
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COMPOSITES PART B-ENGINEERING
·
2025
·
IF 14.2
Weibin Bai,Jialin Chen,Xinghang Chen,Shijing Zheng,Shuhao Yuan,Rongkun Jian,Yucai Lin
Due to fast response and precise controllability, photothermal responsive shape memory materials have developed into a promising platform for intelligent sensing systems. In this paper, we have developed a multifunctional composite material by combining molecularly-engineered polyurethane matrix with biomass photothermal nanoparticles. The shape memory polyurethane was synthesized using polytetramethylene 2000 as the soft segment, hexamethylene diisocyanate as the hard segment, and 1,4-butanediol/4,4′-dithiodianiline as chain extenders, achieving an optimized structure with coordinated balance between soft and hard segments. The urushiol-iron polymer encapsulated Fe 3 O 4 composite particles (urushiol-Fe particles) prepared through a one-step chelation/oxidation of natural urushiol and green-vitriol, provided outstanding photothermal conversion while maintaining excellent interfacial compatibility. By controlling the nanoparticle content (less than 1 wt%) to optimize interfacial interactions, the composite exhibits enhanced mechanical tensile strength (17.21 MPa), excellent shape memory performance (95.56 % fixation, 97.78 % recovery), and wide-temperature-range shape memory (37–80 °C), along with multifunctionalities including on-demand sterilization (100 % inhibition), rapid photothermal ethanol-assisted self-healing (95.58 % recovery in 30 min), durable light-triggered actuation (1000+ cycles) and precise light triggered shape deformation performance. Furthermore, the designed combination logic device driven by photothermal-environment synergy significantly improved temperature detection accuracy. This study establishes an innovative system for photothermal-responsive intelligent materials while opening new pathways for advanced sensing systems with excellent functionality and reliability. Future research should focus on overcoming thermal inertia-induced response delays and optimizing manufacturing processes to enable real-world applications across diverse fields including smart remote sensing, environmental surveillance, soft robotic systems, and biomedical instrumentation.
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MINERALS ENGINEERING
·
2025
·
IF 5
Qinbo Cao,Yan Yan,Heng Zou,Haiyu Zhang,Dianwen Liu,Shuming Wen
The S 2 O 8 2− /Fe 2+ system can be used to depress PbS, where the activation of S 2 O 8 2− leads to the generation of SO 4 • − radicals that oxidize PbS. However, a high S 2 O 8 2− /Fe 2+ dosage is needed for PbS depression (0.15 mol/L). In this study, ultrasonication was employed to improve the depression ability of S 2 O 8 2− /Fe 2+ . The flotation and contact angle results implied that 120-kHz ultrasonication enhanced the depression ability of S 2 O 8 2− /Fe 2+ for PbS, resulting in a decrease in the S 2 O 8 2− /Fe 2+ dosage. Ultrasonication induced hot spots (5000 K) in the PbS slurry and on the PbS surface. These hot spots may cause the thermal activation of S 2 O 8 2− to generate SO 4 • − radicals, facilitating the oxidation of PbS. Thus, the ultrasound-assisted treatment increased the oxidation level of PbS. The XPS study revealed that ultrasonication favored the oxidation of S 2− on the PbS surface to SO 4 2− , such that the surface was covered with PbSO 4 and the hydrophobicity of PbS was lowered. However, ultrasonication did not considerably increase the oxidation state of the CuFeS 2 surface; thus, CuFeS 2 could still be floated and separated from PbS. This study provides a novel strategy for separating PbS–CuFeS 2 mixtures.
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LANGMUIR
·
2025
·
IF 3.9
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.
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Materials Today Bio
·
2025
·
IF 10.2
Hongjin Xue,Yunqian Li,Xinyu Ma,Qi Zhang,Junkai Zhu,Xiaoli Ni,Jianfeng Qiu,Zhengjun Li,Zhen Mu
Psoriasis is a chronic skin condition with significant unmet medical needs, characterized by high levels of reactive oxygen species (ROS) and accompanying oxidative stress. In this study, we developed a novel single-atom iron nanozyme (Fe-N 3 ), designed to mimic natural antioxidant enzymes, for the effective treatment of psoriasis. By optimizing the local coordination environment of Fe atoms, Fe-N 3 demonstrated superior superoxide dismutase (SOD), catalase (CAT), ascorbate peroxidase (APx), and glutathione peroxidase (GPx)-like activities compared to Fe-N 4 . These properties enable efficient ROS scavenging and oxidative stress alleviation. Theoretical analyses revealed that Fe-N 3 possesses lower energy barriers for ROS decomposition, explaining its superior catalytic performance. Furthermore, in vitro and in vivo experiments have demonstrated that Fe-N 3 nanozyme exhibited remarkable therapeutic effects with extremely low cytotoxicity, effectively inhibiting pathological epidermal proliferation, downregulating key inflammatory factors, and reducing the expression levels of psoriasis-associated pathway proteins. This work highlights the promise of single-atom nanozymes in the curing of inflammatory skin diseases, advancing the transformative role of nanotechnology in biomedicine.
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Journal of Environmental Sciences
·
2025
·
IF 6.3
Mengqi Bu,Li Yi,Yingjie Wen,Minli Wang,Hao Yang,Chaohao Chen,Dengsong Zhang,Xu Chen,Zhiyi Lu
Electro-activating peroxydisulfate (PDS) based on the cathode represents a highly promising advanced oxidation process; however, its longevity is constrained by cathode leaching. In this work, we demonstrate that the γ-FeOOH/Fe Foam and α-Fe 2 O 3 /Fe Foam obtained by engineering a protective layer containing iron and oxygen on Fe Foam exhibit significantly extended service life of 53 h and 47 h, 2.94-fold and 2.61-fold longer than that of the original Fe Foam (18 h), while showing similar pseudo-first-order kinetics. Structural evolution analysis and density functional theory simulations reveal that surface oxygen plays a crucial role in reducing the leaching of Fe from the cathode by immobilizing Fe ions and converting them in-situ into stable Fe 3 O 4 . The electro-activation mechanism of PDS on the cathode, the degradation pathways of atrazine (ATZ), and the effects of operating conditions are systematically investigated and elucidated. This work underscores the pivotal role of surface oxygen in prolonging the longevity of Fe-based cathodes, thereby contributing to the development of protective layers.
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WATER RESEARCH
·
2025
·
IF 12.4
Rundong Chen,Wenxiao Zheng,Shishu Zhu,Fangshu Qu,Hengyi Fu,Li Tian,Huarong Yu,Jianyi Zhou,Lele Tu,Chunhua Feng
Coagulation with Fe(III) salts is a prevalent phase separation method for organic wastewater treatment. Nevertheless, our industrial applications have shown that using Fe(III) coagulants in landfill leachate treatment leads to an unexpected increase in the bio-toxicity of the effluent. This observation prompts us to identify the toxic compounds and explore their formation mechanisms. Laboratory experiments demonstrate that while Fe(III) coagulation removed approximately 92% of the total organic matter from landfill leachate, it increased the acute bio-toxicity by about 14.5 times relative to the untreated effluent. Molecular analysis of the dissolved organic matter (DOM) in the leachate using Fourier transform ion cyclotron resonance mass spectrometry revealed a significant generation of chlorinated organic compounds during coagulation process. Compared to the Fenton system, the chlorinated compounds formed after coagulation showed a lower oxidation level and predominantly saturated and reduced state. The mechanistic studies suggest that reactive oxygen and chlorine species have a minimal role in the coagulation-induced chlorination. Instead, it is proposed that the redox reaction between Fe(III) and DOM leads to the formation of phenolic radicals, which facilitate nucleophilic reactions with Cl − (as an electron donor), thereby generating chlorinated compounds.
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Journal of Environmental Chemical Engineering
·
2025
·Vol. 13
·期 2
·116098
·
IF 7.2
Ruiling Luo,Zhongcheng Yang,Yucheng Wang,Yue Yang,Lanyue Qi,Junwen Qi,Zhigao Zhu,Yujun Zhou,Jiansheng Li
Bisphenol (BPA) poses significant risks to the environment. Application of advanced oxidation processes with membrane filtration systems is an effective approach to pollutants removal and membrane fouling control. Herein, we successfully fabricated a Fe-loaded ZIF-8 hollow fiber carbon microfiltration membrane and applied it to the in-situ electro-Fenton process for BPA removal. The graphitic-N promotes the efficiency of electron transfer and the adsorption capacity of O 2 , while the introduction of pyridinic-N on the membrane enhances the selectivity of 2e - oxygen reduction reaction, facilitating the production of hydroxyl radicals. According to the results, the contact angle and resistance of the membrane were 65° and 33.2 Ω, respectively. The hydrophilicity facilitates a water film formation on the surface of membrane, thus preventing deep membrane pore blockage by pollutants. The good conductivity could accelerate electrochemical reactions and enhance electrostatic repulsion. Therefore, the BPA removal rate was 38.29 % with 0.72 L/(m 2 ·h·bar) flux loss for continuous 4-hour filtration under microfiltration conditions. For the control group without bias, the removal rate at the 4th hour was only 16.8 % with 3.59 L/(m 2 ·h·bar) flux loss, indicating a significant weakening of adsorption effect and severe membrane fouling. This study lays the foundation for the application of electro-Fenton technology in wastewater treatment with membrane as cathode.
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JOURNAL OF THE ENERGY INSTITUTE
·
2025
·
IF 6.2
Ruobing Wang,Hongli Zheng,Changfu You,Haiming Wang
Chemical looping reforming of methane (CLRM) is a promising technology for syngas production, offering efficient utilization of CH 4 to generate syngas with a desirable H 2 /CO ratio for downstream applications. This study investigated the influence of Ni incorporation in Y-Fe-Al garnet-type oxygen carriers (OCs) in CLRM. The Ni 0.2 -Y-Fe-Al OC demonstrated a pronounced enhancement in performance compared to its undoped counterpart, elevating the methane conversion from 66.6 % to 98.4 % and increasing the syngas yield from 5.79 to 8.38 mmol g −1 at 850 °C. The incorporated Ni species introduced additional active sites for methane activation, enhanced surface basicity, and improved lattice oxygen mobility, which collectively facilitated the selective oxidation of methane to syngas, especially at low temperatures (<850 °C). Cyclic tests confirmed that Ni incorporation enhanced the redox stability and mitigated phase segregation, leading to sustained high reactivity over multiple cycles. In situ DRIFTS analysis verified that the fundamental reaction pathway, proceeding via the -CH 3 →-CH 2 →-CHO intermediates, remained unaltered after Ni addition. This work established that incorporating Ni in garnet-type OCs is an effective strategy for enhancing both redox activity and cyclic stability in CLRM systems.
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Catalysts
·
2025
·Vol. 15
·期 12
·1108
·
IF 4
Heng Yang,Chuang Zhu,Yongwei Zhang,Manting Gu
Single-atom catalysts are highly efficient electrocatalysts for water splitting with exceptional atomic utilization, but atomic aggregation can impair their catalytic performance. To address this challenge, a Fe-Co-Ni single-atom bifunctional catalyst supported on nitrogen-doped graphene oxide was designed and employed for overall water splitting in alkaline electrolyte. The catalyst’s composition, structure, and morphology were systematically characterized using XRD, XPS, SEM, and high-angle annular dark-field scanning transmission electron microscopy (HAADF-STEM). Electrochemical evaluations were performed to assess its activity and stability toward both the hydrogen evolution reaction (HER) and oxygen evolution reaction (OER). The results demonstrate that strong metal-nonmetal interactions between the Fe, Co and Ni single atoms and the nitrogen-doped graphene oxide support facilitate stable and uniform anchoring of the metal centers on the wrinkled carbon framework. The total metal loading reaches approximately 6.78 wt%, ensuring a high density of accessible active sites. Furthermore, synergistic electronic coupling among the Fe, Co, and Ni centers enhances charge transfer kinetics and modulates the D-band electronic states of the metal atoms. This effect weakens the adsorption strength of hydrogen and oxygen-containing intermediates, thus promoting faster reaction kinetics for both HER and OER. Consequently, the FeCoNi/CNG catalyst delivers low overpotentials of 77 mV for HER and 355 mV for OER at a current density of 10 mA cm−2in alkaline conditions. When integrated into an alkaline water electrolyzer, the system achieves a cell voltage of only 1.68 V to attain a current density of 10 mA cm−2, underscoring its outstanding bifunctional catalytic performance.
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ANALYST
·
2020
·Vol. 146
·期 3
·896-903
·
IF 3.978
Xiaolei Xie,Yufei Wang,Xiaobin Zhou,Junyang Chen,Mengke Wang,Xingguang Su
Single-atom nanozymes have drawn wide attention in bio-sensing for their remarkable merits such as low cost, high stability, and maximum atom utilization. Herein, a colorimetric strategy based on Fe–N–C single-atom nanozymes (Fe/NC-SAs) was established for the detection of alkaline phosphatase (ALP) activity. The Fe/NC-SAs prepared by pyrolysis have excellent peroxidase-like activity and can oxidize 3,3′,5,5′-tetramethylbenzidine (TMB) to a blue color product in the presence of hydrogen peroxide (H2O2). When ascorbic acid (AA) is added to the system, the blue color fades, and the absorbance has a linear relationship with the concentration of AA. Alkaline phosphatase (ALP) can catalyze the hydrolysis of ascorbic acid 2-phosphate (AAP) to produce AA. Thus, a strategy based on Fe/NC-SAs for the detection of ALP activity was established, which provided a linear range of 0.1–1.5 U L−1 and a limit of detection as low as 0.05 U L−1. Besides, Fe/NC-SAs showed high stability under harsh conditions. Moreover, an Fe/NC-SA-based assay was successfully validated using human serum samples for ALP determination with satisfactory results, and has broad prospects in the field of biosensing.
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