Journal of Environmental Chemical Engineering
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2024
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IF 7.4
Guohua Du,Yu Yang,Long Tian,Xinyu Chen,Yuchen Zhang,Jingjing Zhao,Feiyang Luo,Shaoyun Shan,Tianding Hu,Yunfei He
The adsorption of tetracycline wastewater has garnered significant attention owing to its potential threats to human health and the ecological environment during excessive flooding. In this study, a novel Fe-based biomass aerogel (FGA) was synthesized using a microwave-assisted method for efficient tetracycline (TC) adsorption. FGA exhibited exceptional stability, wide adaptability, and excellent recyclability while demonstrated extremely high adsorption (up to 1366 mg·g −1 ) for TC at room temperature. The synthesized FGA was experimentally characterized through morphological observation and determination of chemical composition. The effects of different pH levels, initial concentration of TC, adsorption dosage, and coexisting inorganic ions on the adsorption performance of TC adsorption in experimental studies. The adsorption process of TC onto the FGA was heat-absorbing and spontaneous, aligning with the proposed pseudo-second-order kinetic model and Freundlich isothermal model. Electrostatic interaction, hydrogen bonding interaction, complexation and pore filling were identified as involved mechanisms during the adsorption process based on both characterization results and adsorption experiments.
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CHEMICAL ENGINEERING JOURNAL
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2021
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IF 13.273
Chen Qiao,Zahid Usman,Tai Cao,Souleymen Rafai,Zhitao Wang,Youqi Zhu,Chuanbao Cao,Jiatao Zhang
High-valence Ni and Fe metal sites have demonstrated a crucial role in enhancing the catalytic performances of NiFe-LDH electrocatalysts in oxygen evolution reaction (OER). Although considerable OER catalytic performances achieved under high overpotential, the catalytic talent of NiFe-LDH electrocatalysts at low overpotential is rarely realized due to the absence of high-valence Ni and Fe sites. We herein report a surface engineering route to fabricate sulfated NiFe-LDH nanosheets via ion exchange strategy in sulfate-rich media. XPS results reveal a modified surface electronic structure with high-valence Ni and Fe after ion exchange reaction. Computational PDOS results suggest that computed d-band centers (ε d ) of Fe and Ni for sulfated NiFe-LDH show a significant downward shift resulting an increased valence of metal cation with orbital volume shrinkage. The high-valence Fe can facilitate a optimized multi-electron process of Ni center from [Ni II -OH] − /[Ni III -OH] − to Ni IV -OOH rather than Ni II /Ni III to Ni IV at low overpotential. The high-valence Ni can serve as the highly active center for O-O coupling during OER process. Combined with the synergetic action of high-valence Fe and Ni, the sulfated NiFe-LDH nanosheets exhibit much larger reaction kinetics and outstanding electrocatalytic activity on glassy carbon electrode (η 10 = 219 mV, η 50 = 288 mV) with a remarkable long-term stability.
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NANOTECHNOLOGY
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2022
·Vol. 33
·期 13
·135503
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IF 3.953
Shuyang Hu,Qiuyan Shuai,Yulong Lin,Yan Fu,Meng Li
L-3,4-dihydroxy-phenylalanine (L-dopa) is the most widely used drug in Parkinson's disease treatment. However, development of cost-effective and high-throughput sensors to accurate enantioselective discrimination of L-dopa and D-dopa remains challenging to date. Herein, on the basis of the peroxidase-mimic activity of chiral FexCuySe nanoparticles, we demonstrated a novel colorimetric sensor for determination of chiral dopa. The surface chiral ligand, L/D-histidine (L/D-His), endowed the nanozymes with enantioselectivity in catalyzing the oxidation of dopa enantiomers. According to the values of kcat/Km, the efficiency of L-His modified nanoparticles (L-FexCuySe NPs) towards L-dopa was 1.56 times higher than that of D-dopa. While, D-His can facilely reverse the preference of the nanozyme to D-dopa. On the basis of high catalytic activity and enantioselectivity of L-FexCuySe NPs in oxidation of L-dopa, the L-FexCuySe NPs-based system can be utilized for detection of L-dopa. The linear ranges for L-dopa determination were 5 μM–0.125 mM and 0.125 mM–1 mM with a detection limit of 1.02 μM. Critically, the developed sensor has been successfully applied in the quality control of clinical used L-dopa tablets. Our work sheds light on developing simple and sensitive chiral nanomaterials-based sensors for drug analysis.
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ACS Sustainable Chemistry & Engineering
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2025
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IF 7.3
Mingzhi Zhang,Shujuan Wang,Hongwei Guo,Fan Lv,Tianjiao Ling,Yi Cao,Hongwei Li,Huihua Wang,Jinxin Chen,Ruiqi Guo
Self-supported electrodes featuring transition metals encapsulated within carbon nanotubes (CNTs) are promising bifunctional catalytic electrodes for overall water splitting due to their binder-free fabrication (eliminating costly Nafion), high electrical conductivity, mechanical strength, and low cost. However, challenges remain, including insufficient catalytic activity and stability, as well as underutilization of the CNTs’ functionality. Herein, we strategically modified a Fe-based self-supported electrode with ultrafine IrOx nanoclusters (IrOx NCs), creating Fe@CNTs/IrOx NCs/CC, which exhibits enhanced bifunctional performance for the hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) in 1.0 M KOH. The optimized Fe10@CNTs/IrOx NCs/CC requires low HER and OER overpotentials of 36.7 mV and 203.5 mV at the current density of ± 10 mA cm–2. It also shows a high mass activity of 214.8 A gIr–1 at 100 mV. Moreover, water splitting cells employing Fe10@CNTs/IrOx NCs/CC as both the anode and cathode require only 1.50 V to reach 10 mA cm–2 and demonstrate stable operation exceeding 100 h. Detailed theoretical calculations prove that the IrOx NCs synergistically enhance HER kinetics by promoting both the H2O adsorption-dissociation efficiency and optimized *H desorption. For the OER process, they significantly lower the energy barrier of the rate-determining step (*O → *OOH), thereby accelerating the overall water splitting process of Fe10@CNTs/IrOx NCs/CC. This work highlights an innovative research route for boosting the water splitting performance through targeted modification of the self-supported electrode.
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Materials Today Chemistry
·
2025
·
IF 6.7
Shasha He,Huirou Zhou,Hongjian Chen,Xinglin Qin,Rahim Rahimi,Hongjie Jiang
Nitrite is a common harmful ion found in water and food, and its excessive intake poses significant risks to human health. Accordingly, devising a detection strategy for nitrite that is fast, highly responsive, durable, and ecologically sustainable holds significant importance. In this study, a surface-modified Fe/Cu bimetal-doped Co 3 O 4 catalyst was successfully synthesized, and its 1 wt% aqueous dispersion was drop-cast onto carbon cloth (CC) to fabricate a binder-free flexible electrode (KH792@(C)Fe/Cu–Co 3 O 4 CC) for electrochemical sensing of nitrite. This electrode demonstrated remarkable electrocatalytic activity toward NO 2 − in phosphate buffer solution (0.1 M PBS, pH 7.4), offering a broad linear detection range (6.65 μM–5.0 mM), an exceptionally rapid response time (0.1 s), as well as a low detection limit of 6.65 μM, demonstrating both its high sensitivity and practical applicability. This enhanced performance is largely credited to the cooperative effect between KH792 functional organic units and the Fe/Cu–Co 3 O 4 composite oxide framework. On one hand, the introduction of organic molecules enhances the electrode's electron transfer capability and surface hydrophilicity. On the other hand, the dual-metal doping induces a high density of surface defects and oxygen vacancies, enhancing the density of active sites and facilitating both the adsorption and electron transport processes of nitrite. Moreover, the catalyst was successfully applied to commercial disposable screen-printed electrodes, which were compatible with portable electrochemical workstations, underscoring its potential for low-cost and on-site nitrite detection.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2025
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IF 9
Xiaodong Chen,Wanting Dai,Chengli Luo,Runqing Guo,Guilong Peng,Shiqiang Wei,Zhenmao Jiang
s Single-atom Fe catalysts are attractive for antibiotic removal via peroxymonosulfate (PMS) activation, with support design being crucial. The metal triazolate framework (hereafter MET) serves as an ideal template due to extremely high theoretical nitrogen content; however, the changes in physicochemical properties and reaction mechanisms during its thermal activation remain unclear. In this work, Fe@C-X catalysts were synthesized by pyrolyzing Fe@MET-6. Characterization revealed that the material features Fe N 4 coordination structure and “bubble-like” hierarchical pores formed during pyrolysis play a key role in enhancing catalytic performance. These structures not only increase specific surface area and pore volume, but also anchor dense Fe N 4 sites and facilitate efficient electron transfer. Consequently, Fe@C-700/800 exhibited rate constants of 0.1152 and 0.2766 min −1 for LEV degradation, respectively, an order of magnitude higher than Fe@C-600 (0.0105 min −1 ). Mechanistic studies indicated that the “bubble”, induced structural optimization governs the PMS activation pathway: the Fe@C-600/PMS system relies on a singlet oxygen ( 1 O 2 ) mechanism, while Fe@C-700/800 with developed conductive networks follow an electron-transfer-dominated route. Additionally, the Fe@C-700 with high LEV degradation and energy-efficiency demonstrated excellent recyclability, strong potential for practical applications and reduced toxicity of degradation intermediates. This study provides new insights into designing efficient single-atom catalysts by regulating MOF-derived architectures.
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JOURNAL OF ELECTROANALYTICAL CHEMISTRY
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2025
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IF 4.1
Yaoxia Yang,Fuxing Zhou,Ruirui Zhang,Bolin Xiong,Zhen Yao,Dongfei Sun,Qingtao Wang,Zhiwang Yang
Hydrogen is the most suitable green energy for the current era, and electrolyzing water to produce hydrogen is the most efficient preparation method. The development of efficient oxygen evolution reaction (OER) electrocatalysts is crucial for sustainable energy conversion. In our work, we construct a hierarchical CNFS@NiFe-LDH/NF heterostructure by integrating ZIF-67-derived cobalt sulfide with nickel‑iron layered double hydroxide (LDH) and bimetallic sulfides on nickel foam (NF). This composite synergistically combines the high surface area and active sites from the MOF-derived sulfide, the tunable layered structure and abundant -OH groups from the LDH-which facilitate OH − adsorption and O O formation-as well as electronic modulation effects from the bimetallic sulfides. The catalyst exhibits excellent OER performance with an overpotential of 236 mV at 10 mA cm −2 and a Tafel slope of 42.23 mV dec −1 under alkaline conditions, and maintains high conductivity and low charge transfer resistance throughout operation. Meanwhile, the catalyst showed excellent stability for at least 66 h during the OER process at 50 mA cm −2 , which demonstrates outstanding durability. Moreover, this catalyst have satisfactory hydrophilicity/aerophobicity. This work provides an effective strategy for designing high-performance and stable electrocatalysts via heterogeneous interface engineering.
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APPLIED SURFACE SCIENCE
·
2025
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IF 6.9
Xiao-ru Meng,Pei-dong Wu,Shuai Gao,Zhen Fang
Oxygen reduction catalyst (Fe/Fe 3 N/C) with Fe/Fe 3 N encapsulated carbon active sites were synthesized by coated Fe , N layer onto cellulose-derived carbon through the coordination of iron (Fe 3+ ) and formamide solution with cellulose and subsequent carbonization to enhance electrical conductivity of biochar surfaces as cathode in fuel cells. Fe/Fe 3 N/C catalyst exhibited a half-wave potential of 0.74 V vs . reversible hydrogen electrode in 0.5 M H 2 SO 4 with excellent stability over 100 h. Electrochemical impedance spectroscopy tests showed that the charge transfer resistance was only 1.671 Ω using this novel method, indicating that the cellulose-derived carbon in the core significantly enhanced the electron transport efficiency. Quantum mechanical calculations confirmed strong coordination interaction between the carbonyl groups in formamide and the hydroxyl groups in cellulose with Fe to form Fe/Fe 3 N structure by carbonization. This study provides an effective renewable material solution for Proton exchange membrane fuel cells.
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ENVIRONMENTAL RESEARCH
·
2025
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IF 7.7
Han Zheng,Haotian Guo,Peng Dai,Jiaquan Zhang,Dongliang Wang,Muhammad Faheem,Ziguo Liu,Min Tao,Ping Song,Ying Huang
Valorizing waste vinasse into Fe-doped multifunctional biochar offers an efficient route to boost peroxymonosulfate (PMS) activation and improve wastewater purification. In this study, a magnetic porous Fe-doped vinasse biochar (FVB 700 ) was synthesized via co-pyrolysis of vinasse and ferrous oxalate. The obtained material exhibited a synergistic effect between adsorption and PMS catalytic activation for efficient bisphenol A (BPA) removal. Specifically, FVB 700 , with primary iron species (Fe 0 , Fe 3 C, and Fe 3 O 4 ), rapidly adsorbed BPA through monolayer chemisorption, and the adsorbed BPA was subsequently degraded via PMS activation. Quenching experiments and EPR analysis identified singlet oxygen ( 1 O 2 ) as the dominant nonradical species responsible for BPA degradation in the FVB 700 /PMS system. Density functional theory analysis revealed Fe 3 C as the main catalytic center, anchoring PMS via its terminal -SO 4 oxygen and reacting with another adsorbed HSO 5 − to generate 1 O 2 . The FVB 700 /PMS system retained high performance across a wide pH range (4-11), resisted common water matrix interferents (Cl − , NO 3 − , HCO 3 − , H 2 PO 4 − , and humic acid), and achieved 78.9 %-90.2 % BPA removal in actual water bodies (tap water, groundwater, and pharmaceutical wastewater). Moreover, in a continuous-flow fixed-bed reactor, it maintained over 90 % BPA removal for 8 days, underscoring its long-term stability and practical applicability. Degradation pathway analysis and ECOSAR prediction showed detoxification of BPA into low-hazard intermediates. This study presents an eco-friendly, “waste-to-resource” strategy that integrates Fe-doping with an adsorption-oxidation synergy for the sustainable and efficient remediation of organic contaminants in water.
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PubMed
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Results in Chemistry
·
2025
·
IF 4.2
Weiyan Shi,Xinning Zhang,Xin Yang,Long Bai,Jinsong Yu,Fei Xu,Tai Ye
Recently, enthusiasm for catalysts-based nanozymes in various catalytic systems has been growing significantly. However, the low catalytic capacity of reported enzyme-mimic catalysts has not met the requirements for practical applications. In this work, Co-Fe Prussian blue analogs yolk-shelled nanocubes (Co-Fe PBAs YSHCs) successfully prepared by a template-assisted ion exchange method are demonstrated for efficient AA sensing. The as-prepared Co-Fe PBAs YSHCs display superior and desirable peroxidase-like activity. The unique YSHCs structures can expose large active sites and enhance the stability during the colorimetric sensing process. As a result, the Co-Fe PBAs YSHCs sensing platform can sensitively and accurately determine AA in both colorimetric and smartphone sensing modes, the wide linear ranges for AA were 1–95 μM with a low limit of detection of 0.9 μM. In addition, the Co-Fe PBAs YSHCs sensing platform can be explored for AA detection in human serum samples, yielding satisfactory recoveries. This work provides an ideal method for preparing catalysts and pioneers the investigation of nanozymes with peroxidase-like activity in biosensing platform.
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JOURNAL OF FOOD COMPOSITION AND ANALYSIS
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2025
·
IF 4.6
Huakuo Zhou,Peng Li,Yifei Li,Yi Ke,Xia Zhang,Jun Meng
In recent years, most of the studies on nanozymes have focused on improving their catalytic activity and direct synthesis, but this task is still very complex. Bimetallic oxides are particularly popular due to their mixed valence and synergistic effects between different metal ions. In this study, Fe-Mn bimetallic oxide nano-cubes were prepared by fast and effective solvothermal synthesis, and nano-flower-like structures were grown on the surface of Fe-Mn oxide nanocubes via controlled etching. The synthesized Fe-Mn bimetallic oxide nano-flowers (FMBO NFs) have great oxidase-like activity. On this basis, a simple, economical and accurate colorimetric sensor was established by combining 3,3',5,5'-tetramethylbenzidine (TMB). Exposure to L-cysteine (L-Cys) inhibited the catalytic activity of FMBO NFs. As the concentration of L-Cys increased, the absorbance at 652 nm decreased, with a good linear relationship in the range of 0.01-1000 μM, with a limit of detection (LOD) of 3.99 × 10 -11 M, and the detection of L-Cys in the actual sample egg yolk was successfully achieved. This study provides theoretical support for the effective design of bimetallic oxide nanozyme activity, and can guide the development of an accurate detection system for the analysis of L-Cys in food.
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ChemSusChem
·
2024
·
IF 7.5
Tao Xu,Meihui Jiang,Siyu Mo,Xianhui Wang,Tianlin Ren,Zhichen Liu,Zhicheng Wang,Yicheng Qiu,Lingying Gu,Xu Wang,Xuhui Mao
Graphical We designed a carbon-coated aluminum oxide carrier and reinforced it with Mn−Fe bimetal assemblages to prepare a high-performance catalyst Mn−Fe/C-Al 2 O 3 . Mn−Fe/C-Al 2 O 3 catalyst exhibited satisfactory catalytic ozonation activity and stability in the degradation of p -nitrophenol. Experiments and theoretical calculations revealed the internal degradation mechanism of the Mn−Fe/C-Al 2 O 3 catalyst, underscoring the role of the carbon-coated and bimetallic active unit in O 3 activation. Catalysts with high catalytic activity and low production cost are important for industrial application of heterogeneous catalytic ozonation (HCO). In this study, we designed a carbon-coated aluminum oxide carrier (C-Al 2 O 3 ) and reinforced it with Mn−Fe bimetal assemblages to prepare a high-performance catalyst Mn−Fe/C-Al 2 O 3 . The results showed that the carbon embedding significantly improved the abundance of surface oxygen functional groups, conductivity, and adsorption capacity of γ-Al 2 O 3 , while preserving its exceptional mechanical strength as a carrier. The prepared Mn−Fe/C-Al 2 O 3 catalyst exhibited satisfactory catalytic ozonation activity and stability in the degradation of p -nitrophenol (PNP). Electron paramagnetic resonance (EPR) and quenching experiments reveal that radical ( ⋅ OH and ⋅ O 2 ⋅ ) and nonradical oxidation ( 1 O 2 ) dominated the PNP degradation process. Theoretical calculations corroborated that the anchored atomic Fe and Mn sites regulated the local electronic structure of the catalyst. This modulation effectively promoted the activation of O 3 molecules, resulting in the generation of atomic oxygen species (AOS) and reactive oxygen species (ROS). The economic analysis on Mn−Fe/C-Al 2 O 3 revealed that it was a cost-competitive catalyst for HCO. This study not only deepens the understanding on the reaction mechanism of HCO with transition metal/carbon composite catalysts, also provides a high-performance and cost-competitive ozone catalyst for prospective application.
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