Small
·
2024
·
IF 13
Ziyi Xu,Shihao Wang,Wenmao Tu,Ling Shen,Lu Wu,Shilong Xu,Haining Zhang,Hongfei Pan,Xiao-Yu Yang
Stable, efficient, and economical bifunctional electrocatalysts for oxygen evolution reaction (OER) and oxygen reduction reaction (ORR) are needed for rechargeable Zn–air batteries. In this study, a directional electron transfer pathway is exploited in a spatial heterojunction of Co y Ni x @Fe─N─C heterogeneous catalyst for effective bifunctional electrolysis (OER/ORR). Thereinto, the Co/Ni alloy is strongly coupled to the Fe─N─C support through Co/Ni─N bonds. DFT calculations and experimental findings confirm that Co/Ni─N bonds play a bridging role in the directional electron transfer from Co/Ni alloy to the Fe─N─C support, increasing the content of pyridinic nitrogen in the ORR-active support. In addition, the discovered directional electron transfer mechanism enhances both the ORR/OER activity and the durability of the catalyst. The Co 0.66 Ni 0.34 @Fe─N─C with the optimal Ni/Co ratio exhibits satisfying bifunctional electrocatalytic performance, requiring an ORR half-wave potential of 0.90 V and an OER overpotential of 317 mV at 10 mA cm −2 in alkaline electrolytes. The assembled rechargeable zinc–air batteries (ZABs) incorporating Co 0.66 Ni 0.34 @Fe─N─C cathode exhibits a charge–discharge voltage gap comparable to the Pt/C||IrO 2 assembly and high robustness for over 60 h at 20 mA cm −2 .
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高影响因子
Journal of Environmental Chemical Engineering
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2024
·
IF 7.4
Haishuo Wang,Jie Zhang,Zhichun Li,Bin Shi,Shiyin Li,Heyong Huang
Microcystin-LR (MCLR) is a highly toxic pollutant widely distributed in eutrophic waters. The interplay between dissolved organic matter (DOM) and metal ions has been extensively reported; however, the impact of DOM-metal complexes on MCLR remains to be thoroughly studied. In this research, equilibrium dialysis was employed to study the kinetics and isotherms of MCLR adsorption by DOM, meanwhile the Density functional theory (DFT) calculations provided insights into the theoretical mechanisms of Fe(II)/Mn(II) involvement in the adsorption process. The adsorption kinetics revealed that the process is physicochemical, with chemisorption being the critical factor controlling the adsorption rate. The adsorption isotherms confirmed that Fe(II) alters the spatial arrangement of adsorption sites on the superficies of DOM, with the complexes of Fe(II) and DOM from the macrophyte-dominated regions of Lake Taihu (MDR-Fe(II)) showing the uppermost adsorption capacity of 6193.965 µg/g among all combinations. The influence of different cations (K + , Ca 2+ , Na + , Mg 2+ ) on the adsorption of MCLR to DOM is divergent, with metals either reducing MCLR adsorption through competition for adsorption sites or increasing it by forming ternary complexes. The pH decrease reduced the affinity of DOM to metal ions while simultaneously enhancing MCLR adsorption through changes in its ionization state. DFT calculations demonstrated that Fe(II)/Mn(II) reduces the resistance to interaction between functional groups on DOM and MCLR, with carboxyl-Fe(II)-carboxyl interactions showing the highest binding energy (ΔG = −7.253 eV). Overall, Fe(II)/Mn(II) enhances the adsorption of MCLR via altering the structure and surface electrostatic potential distribution of DOM. This research indicates that the ultimate fate of MCLR in aquatic ecosystems is affected by DOM and metal ions.
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Journal of Environmental Chemical Engineering
·
2024
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IF 7.4
Hongbin He,Bolong Liang,Shumin Lin,Yan Chen,Xin Zhang,Shu-Xuan Liang
The residues of oxytetracycline hydrochloride (OTC) in water have potential adverse effects on human health and ecological environment. Photocatalytic degradation has been widely studied in the treatment of antibiotic pollution due to its environmentally friendly and efficient characteristics. However, the band gap of traditional photocatalysts is too wide, and the recombination of photogenerated electrons and holes is serious, which has negative effects on photocatalysis . Therefore, the Z-scheme heterojunction g-C 3 N 4 @MIL-101(Fe) composite photocatalyst was synthesized by high temperature calcination combined with solvothermal method. g-C 3 N 4 @MIL-101(Fe) was characterized by XRD, FTIR , SEM, TEM and other tests. All the results showed that the compound was successful A series of photoelectric tests showed that g-C 3 N 4 @MIL-101(Fe) has a narrower band gap, stronger light absorption ability, and improved the separation rate of photogenerated electrons and holes. Under visible light irradiation, g-C 3 N 4 @MIL-101(Fe) could remove 87.68% of OTC in 300 min. g-C 3 N 4 @MIL-101(Fe) showed good potential for practical application in five real water samples and stability after six cycles. Finally, superoxide radicals and hole radicals were identified as the main reactive species in the photodegradation process. The mechanism and pathway of the photocatalytic degradation of OTC by g-C 3 N 4 @MIL-101(Fe) are proposed. This work expands the construction and application of Fe-MOF based Z-scheme heterostructure and provides a new idea for water pollution remediation.
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Water
·
2024
·Vol. 16
·期 16
·2218
·
IF 3
Zhichao Chen,Yulin Min,Xin Zhao,Penghui Shi,Hongxiu Lu
Ceramsites are extensively employed as substrates for adsorbents in studies focused on phosphorus adsorption, leaving ceramsites crafted from diatomite less explored. Diatomite-based ceramsite, with its distinct porous architecture and surface silanol functionalities, is adept at supporting a variety of metal oxides, presenting a distinct advantage over other ceramsite variants. In light of this, the present study embarked on producing diatomite-based ceramsite using diatomite as the foundational material, subsequently enhancing it through the incorporation of Fe, thus yielding an Fe-modified diatomite-based ceramsite. Through adsorption testing, the modified ceramsite demonstrated a significantly improved adsorption capacity of 4.06 mg P/g, marking a substantial enhancement from the initial capacity of 0.9 mg P/g. The process of phosphorus adsorption exhibited a strong alignment with the Langmuir isotherm model and the pseudo-second-order kinetic model. In-depth analyses employing XRD, FTIR, zeta potential, and XPS techniques have revealed that the principal mechanisms driving the adsorption process are centered on interactions involving electrostatic forces, the formation of chemical precipitates, and the exchange of ligands. This investigation not only opens new avenues for the application of diatomite-based ceramsite but also lays down a theoretical foundation for its modification, thereby enriching the spectrum of its utility.
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CHEMICAL ENGINEERING JOURNAL
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2024
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IF 13.3
Gang Li,Ruiyang Tan,Bohong Gao,Xinli Liu,Mingyuan Zhang,Ping Chen,Xinyi Wang
Developing advanced electromagnetic wave absorption (EMWA) materials is crucial for curbing electromagnetic pollution. This study presents the synthesis of core–shell Fe/Fe 3 O 4 /C composites, FFC-700 and FFC-800, derived from Prussian blue@covalent organic framework (PB@COF) via pyrolysis at 700 and 800 °C, and the hollow FFC-900 at 900 °C. Their chemical compositions, microstructures, and EMWA performances were thoroughly examined. FFC-700 and FFC-800, featuring core–shell structures and abundant interfaces, facilitate electron transfer and enhance polarization effects. Notably, FFC-700 achieved a minimum reflection loss (RL min ) of − 75.82 dB at an ultrathin thickness of 1.45 mm, with an effective absorption bandwidth (EAB) of 6.22 GHz at 1.66 mm, spanning the entire Ku-band. FFC-800 also provides substantial EMWA performance, with an RL min of − 30.14 dB at 1.61 mm and an EAB of 6.08 GHz at 1.67 mm, also covering the Ku-band. Radar cross-section (RCS) simulations reveal the absorbers’ exceptional radar stealth, with their coatings significantly reducing RCS values. The composites’ adjustable structure, balanced composition, and dielectric-magnetic synergy optimize impedance matching for full-Ku-band coverage. This work offers a promising approach to fabricating efficient EMWA materials from PBA@COF and MOF@COF precursors.
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Journal of Water Process Engineering
·
2025
·
IF 6.7
Jincheng Dai,Shuyue He,Xiyu Song,Chuliang Shen,Hongjuan Zhang,Ruyi Xie
The application of Fe-based metal-organic frameworks in photo-Fenton antibiotic degradation is limited by the low charge separation efficiency and slow Fe 3+ /Fe 2+ transition. In this study, a novel Z -scheme porous carbon nitride/mixed-valent MIL-53(Fe) (KCM-20) heterojunction photocatalyst was successfully constructed for degradation of high concentration tetracycline. On the one hand, the Z -scheme heterojunctions system is conducive to the rapid separation of photogenerated electron-hole pairs. On the other hand, the cyclic conversion of Fe 3+ /Fe 2+ in the MIL-53(Fe) photo-Fenton system can be accelerated. The KCM-20 showed the highest degradation efficiency for tetracycline. The KCM-20/light/H 2 O 2 system degraded more than 93 % of tetracycline (150 mg·L −1 ) within 75 min and exhibited the highest degradation kinetic constant, which is 8.0 and 2.4 times higher than those of carbon nitride and MIL-53(Fe), respectively. Its excellent catalytic performance can be attributed to the efficient synergy between photocatalytic reaction and Fenton reaction, producing more active species for tetracycline degradation. EPR and activity capture experiments indicate that ·O− 2, ·OH and h + are the main active species for tetracycline degradation. By analyzing the intermediate products, three degradation pathways for tetracycline were proposed. This work provides a new pathway for the preparation of efficient and cost-effective photocatalysts for the degradation of organic pollutants.
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Sustainability
·
2024
·Vol. 16
·期 20
·9051
·
IF 3.3
Huali Zhang,Kanghui Zhang,Qin Liu,Tongshan Shi,Jiaheng Cui,Jinxiu Li
This study presents a novel Fe-CNs-P/S carbon composite material, synthesized by doping elements P and S into NH2-MIL-101 (Fe) using the carbonization method. The material’s application in sustainable water treatment was evaluated, focusing on its effectiveness in activating persulfate for pollutant degradation. The research thoroughly investigates the synthesis process, structural characteristics, and performance in degrading pollutants. The results indicate that Fe-CNs-P/S-5 with 50% P and S co-doping is higher than that of other samples, where the degradation rate of TC in 30 min is as high as 98.11% under the optimum conditions, that is temperature at 25 °C, 0.05 g/L of catalyst concentration, and 0.2 g/L of PMS concentration. The composite material demonstrates robust versatility and stability, maintaining high degradation efficiency across multiple organic pollutants, with no significant reduction in catalytic performance after four cycles. Furthermore, the free radical quenching experiments display that the singlet oxygen1O2is the main active species. It is demonstrated that the doping of P and S play a role in the enhancement of PMS activation over the Fe-CNs-P/S catalyst. This material demonstrates remarkable efficacy in treating a range of organic contaminants and exhibits excellent reusability, presenting a promising approach for enhancing sustainability in water treatment applications.
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CARBOHYDRATE POLYMERS
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2024
·
IF 10.7
Shi-Kang Chen,Jin-Jin Liu,Xin Wang,Hui Luo,Wei-Wei He,Xiao-Xiao Song,Jun-Yi Yin,Shao-Ping Nie
Bacterial infection severely hinders skin wound healing, highlighting the critical application value of developing antibacterial and anti-inflammatory hydrogel dressings. In this work, we focused on β-glucan from Hericium erinaceus (HEBG) as the research object, and proposed a solvent-induced combined temperature manipulation technique to trigger multilevel self-assembly of β-glucan. Furthermore, we incorporated green synthesized near-infrared photosensitizer tannic acid (TA)/iron (III) complex into the system. A hydrogel with exceptional antibacterial properties, capable of responding to near-infrared photothermal stimuli while exhibiting remarkable stiffness and structural consistency, was successfully synthesized. Under near-infrared radiation, HEBG/TA/Fe hydrogels produced local hyperthermia and exhibited excellent antibacterial activity against bacteria-infected wounds. Moreover, the HEBG/TA/Fe hydrogel demonstrates its ability to regulate cytokines by effectively inhibiting the production of inflammatory mediators TNF-α and IL-6, while simultaneously enhancing the expression of cell proliferation factor KI-67 and markers associated with angiogenesis such as CD31 and α-SMA. Notably, the results of tissue staining revealed that the NIR + HEBG/TA/Fe 5 hydrogel could effectively promoting granulation and vascularization, improving collagen deposition in infected wounds thereby accelerating the healing process. These findings indicate that mixed hydrogels exhibit potential as viable options for the treatment of bacterial infections.
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JOURNAL OF ALLOYS AND COMPOUNDS
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2024
·
IF 5.8
Shushu Li,Maozheng Li,Ruocheng Shen,Jianfang Lu,Xiaoyan Lv,Jing Su,Yanxuan Wen
K 3 V 3 (PO 4)4 (KVP), a novel cathode material for potassium-ion batteries (KIBs), is recognized for its stable crystal structure and robust cycling performance. Despite these attributes, it is hampered by poor electronic conductivity and limited rate capability. In this research, Fe 3+ has been substituted for a portion of V 3+ to modulate the electronic structure of K 3 V 3-x Fe x (PO 4 ) 4 /C, aimed at enhancing its electrochemical performance. Theoretical calculations expectedly show that Fe doping at the V site reduces the band gap energy from 2.674 eV to 1.92 eV, thereby improving electron transfer. Both physical and chemical analyses confirm the successful integration of Fe 3+ into the crystal structure and the adjustment of relevant lattice parameters. Additionally, Fe serves as an effective catalyst, enhancing the graphitization of the carbon coating. SEM demonstrates that Fe 3+ doping encourages the development of a porous structure, which not only promotes electrolyte penetration but also provides a buffer to the crystal framework during K + deintercalation. K 3 V 3-x Fe x (PO 4 ) 4 /C, when doped with Fe 3+ , shows superior discharge capacity and long-term cycling stability compared to KVP/C. Specifically, K 3 V 2.8 Fe 0.2 (PO 4 ) 4 /C, with an Fe 3+ doping level of x=0.2, exhibits minimal electrode polarization and outstanding rate performance. After 380 cycles at 400 mA·g −1 , it maintains a discharge capacity of 46 mAh·g −1 , significantly surpassing KVP/C. These findings offer valuable insights into the commercial synthesis of scalable, high-performance rechargeable KIBs cathode materials.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2024
·
IF 9.4
Yi Jia,Fan Gao,Peizhi Wang,Shiwei Bai,Hong Li,Junbai Li
Chemodynamic therapy (CDT) via Fenton-like reaction is greatly attractive owing to its capability to generate highly cytotoxic •OH radicals from tumoral hydrogen peroxide (H 2 O 2 ). However, the antitumor efficacy of CDT is often challenged by the relatively low radical generation efficiency and the high levels of antioxidative glutathione (GSH) in tumor microenvironment. Herein, an innovative photothermal Fenton-like catalyst, Fe-chelated polydopamine (PDA@Fe) nanoparticle, with excellent GSH-depleting capability is constructed via one-step molecular assembly strategy for dual-modal imaging-guided synergetic photothermal-enhanced chemodynamic therapy. Fe(III) ions in PDA@Fe nanoparticles can consume the GSH overexpressed in tumor microenvironment to avoid the potential •OH consumption, while the as-produced Fe(II) ions subsequently convert tumoral H 2 O 2 into cytotoxic •OH radicals through the Fenton reaction. Notably, PDA@Fe nanoparticles demonstrate excellent near-infrared light absorption that results in superior photothermal conversion ability, which further boosts above-mentioned cascade catalysis to yield more •OH radicals for enhanced CDT. Taken together with T 1 -weighted magnetic resonance imaging (MRI) contrast enhancement ( r 1 = 8.13 mM −1 s −1 ) and strong photoacoustic (PA) imaging signal of PDA@Fe nanoparticles, this design finally realizes the synergistic photothermal-chemodynamic therapy. Overall, this work offers a new promising paradigm to effectively accommodate both imaging and therapy functions in one well-defined framework for personalized precision disease treatment.
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JOURNAL OF THE INDIAN CHEMICAL SOCIETY
·
2025
·
IF 3.4
Honghui Teng,Meng Zhang,Hongxue Du,Yuanqi Fang,Mingyue Piao
Three-dimensional (3D) electrochemical oxidation has emerged as a promising advanced oxidation process for wastewater treatment, owing to its high efficiency, environmental compatibility, and operational advantages. In this study, we developed a novel Fe/Mn co-loaded activated carbon (Fe/Mn-AC) particle electrode for the electrochemical oxidation of ammonium nitrogen NH 4 + -N) in wastewater. The as-prepared catalyst was systematically characterized through multiple analytical techniques including SEM-EDS, XRD, FTIR, XPS, and BET surface area analysis. Post-impregnation, SEM revealed maintained surface smoothness but reduced pore sizes, while BET measurements confirmed decreased surface area (from 732.38 to 650.83 m 2 /g), pore diameter (from 2.6 to 2.18 nm), and pore volume (from 0.43 to 0.37 cm 3 /g). XRD and XPS analyses identified iron and manganese oxides (Fe 2 O 3 , Fe 3 O 4 , Mn 2 O 3 , Mn 3 O 4 ) as the active phases. FTIR spectra exhibited characteristic bands of O–H (3462 cm −1 ), C–O (1571 cm −1 ), and C–C (1384 cm −1 ) in both AC and Fe/Mn-AC, with observable intensity variations after metal loading. Under optimized conditions (pH = 7, applied voltage = 14 V, Fe/Mn loading = 1 %, initial NH 4 + -N concentration = 100 mg/L), the 3D electrochemical system achieved an NH 4 + -N removal efficiency of 87.64 % with an energy consumption of 6.2 kW h/kg NH4+-N after 8 h of treatment. Radical quenching experiments confirmed the in-situ generation of hydroxyl radicals and electrons during the electrochemical process. The degradation mechanism study revealed that NH 4 + -N was primarily removed through indirect electro-oxidation pathways, with N 2 identified as the dominant end product.
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CHEMICAL GEOLOGY
·
2025
·
IF 3.6
Changjin Liang,Honghai Wu,Yaowei Li,Yufeng Guan
Ferrihydrite (Fh) can usually transform into phases with higher crystallinities. This may greatly alter Fh adsorption capacity for chromium ions, thereby affecting their immobilizations and fates. Foreign elements [e.g., lanthanum (La)] as impurities can become incorporated into Fh. Herein, the effect of La-substitution into Fh and the influence of the presence of Cr(VI) on Fh phase transformation and fate of Cr(VI) were investigated. X-ray diffraction (XRD), Fourier transform infrared spectroscopy (FTIR), Electro-chemical impedance spectroscopy (EIS), and X-ray photoelectron spectroscopy (XPS) and other test methods were employed to probe phase changes after the Fe(II)-induced La-substituted Fh (La-Fh) transformations. At pH 5.5, no neoformed phase was observed until 7 d for La-Fh or pure Fh at 1 mM Fe(II) aq, but all La-Fh systems underwent transformations at 5 mM Fe(II)aq. A low pH and Fe(II)aq level favored lepidocrocite (Lp) to form, whereas goethite (Gt) was the predominant phase rather than Lp as pH increased to 7.2 with higher level Fe(II)aq. However, the La-substitution inhibits the La-Fh transformation rate and path. This made 5 % La-Fh transformed to Lp after 30 d at pH 7.2 and 1 mM Fe(II)aq. The La-release was present to some extent during the transformation process. Either the inhibition to La-Fh transformation or the La-slow release favors the retention of early-adsorbed Cr(VI) on iron-mineral surface. The added Cr(VI) might promote the La-Fh transformation even under a lower-level Fe(II), primarily attributed to the rapid reduction of Cr(VI) to Cr(III) by Fe(II), which produced more liable Fe(III) in addition to the Cr(III) that can improve the mineral conductivity, thereby enhancing the La-Fh transformation. Mechanisms responsible for the Fe(II)-induced La-Fh transformation companying the La slow-release are proposed to provide insights into the reduction and immobilization of Cr(VI) under anaerobic conditions, thus demonstrating that La-Fh is a promising material for application in Cr-contaminated site remediation.
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