TRANSACTIONS OF TIANJIN UNIVERSITY
·
2023
·Vol. 29
·期 6
·453-461
·
IF 7.1
Qiu Wenhao,Han Qing,Yu Xiaogang,Xiang Zhonghua
Developing nonprecious metal-nitrogen-doped carbon (M–N–C) catalysts with high activity and stability is critical to their widespread use in fuel cells; however, these catalysts still face considerable challenges. Herein, a novel iron atom-cluster strategy for the synthesis of iron-based N–C catalyst comprising Fe nanoparticles (Fe NPs) surrounded by Fe-N x sites is developed for oxygen reduction reactions in an acidic fuel cell. Iron oxide NPs were incorporated into zeolitic imidazolate framework-8 (ZIF-8)-derived carbon materials and pyrolyzed at high temperatures using NaCl as a modifier to produce Fe NPs and Fe-N x composite active sites. The half-wave potential of the optimized Fe NP /FeNC-NaCl material was substantially improved to 0.81 V. Furthermore, even after 15,000 cycles, the half-wave potential of the catalyst remained essentially unchanged. As a cathode catalyst for fuel cells, it realized a high peak power density of 436 mW/cm 2 under a practical H 2 -air atmosphere. Therefore, this study presents a new approach for designing and synthesizing electrocatalytic materials with high catalytic activity and stability.
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ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH
·
2023
·Vol. 30
·期 33
·80817-80827
·
IF 5.8
Huang Guofu,Wang Mianmian,Sun Xinying,Liu Haijian,Liu Fangfang
In this work, pomegranate peel extracts were used as the green reducing agent to synthesize Cu/Fe nanoparticles (P-Cu/Fe nanoparticles) and removed tetrabromobisphenol A (TBBPA) in aqueous solution. P-Cu/Fe nanoparticles were amorphous and irregularly spherical. The surfaces of nanoparticles contained Fe 0 , Fe 3+ oxides (hydroxides), and Cu 0 . The bioactive molecules from pomegranate peel were extremely important for the synthesis of nanoparticles. P-Cu/Fe nanoparticles had excellent removal performance for TBBPA, and 98.6% of TBBPA (5 mg L −1 ) was removed within 60 min. The removal reaction of TBBPA by P-Cu/Fe nanoparticles was well-fitted with the pseudo-first-order kinetic model. The Cu loading was critical for TBBPA removal with an optimum value of 1.0 wt%. A weakly acidic condition (pH 5) was more favorable for the removal of TBBPA. The removal efficiency of TBBPA increased with the rise of temperature and decreased with increasing initial TBBPA concentration. The activation energy ( E a ) was 54.09 kJ mol −1 , indicating that the removal of TBBPA by P-Cu/Fe nanoparticles was mainly surface-controlled. Reductive degradation was the main mechanism of TBBPA removal by P-Cu/Fe nanoparticles. In conclusion, green synthesized P-Cu/Fe nanoparticles using pomegranate peel waste show great potential for the remediation of TBBPA in aqueous solution.
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CELLULOSE
·
2023
·Vol. 30
·期 15
·9607-9623
·
IF 5.7
Wang Zhile,Yu Dehai
The photocatalytic degradation of organic pollutants represents an efficacious, energy-conserving, and eco-friendly methodology. MIL-101 is a porous crystalline material composed of metal ions (or metal clusters) and organic linkers. As a prominent metal-organic framework material, MIL-101 exhibits remarkable thermal and chemical resilience, rendering it ideal for diverse applications encompassing gas storage, separation, and catalytic processes. However, its potency in the degradation of dye molecules is impeded by its innate hydrophobicity and predisposition to precipitate in aqueous solutions. In this study, MIL-101(Fe)/cellulose nanocrystal (CNC) hybrid nanoparticles (MCs) with high photocatalytic activity were prepared by in situ growth. Owing to their unique amphiphilicity and interfacial adsorption, the Pickering emulsions stabilised by MCs showed uniform particle size and stability. The MCs were uniformly adsorbed at the oil–water interface of the emulsion and dispersed in the water phase through a three-dimensional network with clusters. This facilitated complete contact of the MCs with pollutants, thereby significantly increasing the photocatalytic efficiency. The tuneable wettability of MIL-101(Fe) induced by CNCs considerably affected the stabilization and photocatalytic degradation performance. In the presence of 0.5 wt% CNCs, the MCs had a three-phase contact angle of 92°, resulting in the highest photocatalytic degradation rate and emulsion stability of the samples studied herein. An emulsion was produced with a constant emulsification index of 100% by using 0.4 wt% MCs and an oil-phase volume fraction of approximately 0.2. The MC-stabilised emulsion system exhibited high photocatalytic degradation efficiency for Rhodamine B. Moreover, the MCs could be recycled several times while ensuring a degradation efficiency within an acceptable range. Herein we introduce a new approach for improving and fabricating green, sustainable photocatalysts for the degradation of organic pollutants in aqueous systems.
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Nano Research
·
2024
·Vol. 17
·期 6
·4924-4933
·
IF 9.5
Fan Yu,Yi Yu,Rong Hongpan,Zhang Jiatao
Carbon-based single-atom catalysts (SACs) have been widely studied in the field of biomedicine due to their excellent catalytic performance. However, carbon-based SACs usually aggregate during pyrolysis, which leads to the reduction of catalytic activity. Here, we describe a method to improve the monodispersion of SACs using silicon dioxide as a protective layer. The decoration of silicon dioxide serves as a buffer layer for individual nanoparticles, which is not destroyed during the pyrolysis process, ensuring the single-particle dispersion of the nanoparticles after etching. This approach increased the hydroxyl groups on the surface of Fe-SAC (Fe-SAC-SE) and improved its water solubility, resulting in a four times enhancement of the peroxidase (POD)-like activity of Fe-SAC-SE (58.4 U/mg) than that of non-protected SACs (13.9 U/mg). The SiO 2 -protection approach could also improve the catalytic activities of SACs with other metals such as Mn, Co, Ni, and Cu, indicating its generality for SACs preparation. Taking advantage of the high POD-like activity, photothermal properties, and large specific surface area of Fe-SAC-SE, we constructed a synergistic therapeutic system (Fe-SAC-SE@DOX@PEG) for combining the photothermal therapy, catalytic therapy, and chemotherapy. It was verified that the photothermal properties of Fe-SAC-SE@DOX@PEG could effectively improve its POD-like activity, exhibiting excellent tumor-killing performance at the cellular level. This work may provide a general approach to improve the performances of SACs for disease therapy and diagnosis.
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Frontiers of Chemical Science and Engineering
·
2023
·Vol. 17
·期 7
·930-941
·
IF 4.5
Tian Guodong,Duan Chao,Zhou Bingxu,Tian Chaochao,Wang Qiang,Chen Jiachuan
Membrane technology for wastewater remediation has aroused wide interest owing to its unique properties and potential applications. However, it remains challenging to explore green, efficient and robust membrane material and technique for complex wastewater treatment. Herein, we proposed using a simple electrospinning and in situ seeding method to fabricate a lignin-based electrospun nanofiber membrane (LENM) decorated with photo-Fenton Ag@MIL-100(Fe) heterojunctions for efficient separation of oil/water emulsions and degradation of organic dye. Thanks to the embedded lignin in LENM, an ultrahigh MIL-100(Fe) loading (53 wt %) with good wettability and high porosity was obtained. As a result, the hybrid Ag@MIL-100(Fe)/LENM exhibited excellent oil/water emulsions separation efficiency (more than 97%) without a compromise of water flux. Moreover, the hybrid membrane showed an excellent dye removal with degradation of 99% methylene blue within 30 min under illumination, which is attributed to a synergy of dye adsorption/enrichment and photo-Fenton catalytic degradation from Ag@MIL-100(Fe). Therefore, the lignin-based photo-Fenton hybrid membrane can lay the foundation for the preparation and application of green, sustainable and versatile membrane materials and technologies for efficient complex wastewater remediation.
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CHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 13.2
Ping Li,Chengbin Wang,Guitao Zhang,Kaicai Fan,Yifei Liu,Bin Li,Porun Liu,Lingbo Zong,Lei Wang
Chlor-alkali electrolysis with oxygen depolarized cathode (ODC), which can save up to 30 % in energy, primarily involves two electrochemical reactions: the chlorine evolution reaction (CER), and the oxygen reduction reaction (ORR). However, electrocatalysts used in this field is the platinum-group metals (PGMs), which significantly increase the preparation cost. Herein, we synthesize Fe single-atom anchored on carbon nanotubes (Fe-N@CNTs) via a pre-coordination strategy as an active and durable ORR catalyst. The resulting Fe-N@CNTs displays excellent ORR performance with a large half-wave potential (E 1/2 ) of 0.905 V and excellent durability over 30,000 CV test in 0.1 M KOH electrolyte. Projected density of states (PDOS) analysis demonstrates that geometric strain lowers the d-band center of Fe, weakening the adsorption strength of ORR intermediates at Fe N 4 active sites. Density functional theory (DFT) calculations show that geometric strain effects reduce the potential determining step (PDS) energy barrier and optimize the binding strength of *OH of ORR. Both Fe-N@CNTs-based aqueous Zn-air battery (A-ZAB) and quasi-solid-state Zn-air battery (QSS-ZAB) display excellent charge/discharge cycling stability with small charge/discharge voltage gaps over 1700 h and 100 h, respectively. Importantly, Fe-N@CNTs||RuO 2 chlor-alkali flow cell requires low cell potential of 1.58 V to reach 300 mA cm −2 at 80 °C, and delivers excellent stability over 230 and 110 h at 100 and 300 mA cm −2 , respectively. Fe-N@CNTs||RuO 2 maintains approximately 100 % caustic current efficiency at the current density of 300 mA cm −2 . This work contributes to the development of stable, uniformly dispersed atomic-scale metal ORR catalysts and expands their applications in chlor-alkali electrolyzer.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2025
·
IF 9
Xianyun Ma,Bowen Zhu,Zuopeng Li,Min Wang,Chang-qing Miao,Yajia Liu,Sanbing Zhang
Defect engineering is a promising approach for constructing highly efficient catalytic activity based on metal–organic frameworks (MOFs). In this study, a defective MOFs, referred to as quasi-MIL-100(Fe), was synthesized by moderate synthesis method and then careful thermal treatment at an atmosphere ranging from 150 to 450 °C, linking crystalline materials and the associated metal oxides. MIL-100(Fe) heat-treated at 250 °C (referred to as M-250) partially breaks coordination bonds, resulting in a crystalline-to-amorphous transformation, increased porosity, and elimination of ligands. Compared to pristine MIL-100(Fe), M-250 possessed more reactive sites and exhibited the highest photo-Fenton degradation of ciprofloxacin with 95.6 % removal efficiency in 90 min, despite the unfavorable photo properties for photo-Fenton performance due to the destruction of the crystal structure. Additionally, density functional theory (DFT) calculations, combined with free radical quenching and mass spectrometry analysis, elucidated the catalytic mechanism. These findings highlight the significant potential of quasi-MOFs for applications in the photo-Fenton reaction.
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Magnetochemistry
·
2025
·Vol. 11
·期 6
·49
·
IF 2.5
Yujie Zhou,Yuzhe Fu,Xiaoxue Niu,Bohan Wu,Xinghan Liu,Fu Hao,Zichuan Ma,Hao Cai,Yuheng Liu
Antibiotic resistance has been recognized as a global threat to human health. Therefore, it is urgent to develop effective strategies to address the contamination of water environments caused by antibiotics. In this study, Fe/Mn bimetallic-modified biochar (FMBC) was synthesized through a one-pot oxidation/reduction-hydrothermal co-precipitation method, demonstrating an exceptional photocatalytic-Fenton degradation performance for oxytetracycline (OTC). Characterization techniques including FTIR, SEM, XRD, VSM, and N2adsorption–desorption analysis confirmed that the Fe/Mn bimetals were successfully loaded onto the surface of biochar in the form of Fe3O4and MnFe2O4mixed crystals and exhibited favorable paramagnetic properties that facilitate magnetic recovery. A key innovation is the utilization of biochar’s inherent phenol/quinone structures as reactive sites and electron transfer mediators, which synergistically interact with the loaded bimetallic oxides to significantly enhance the generation of highly reactive ·OH radicals, thereby boosting catalytic activity. Even after five recycling cycles, the material exhibited minimal changes in degradation efficiency and bimetallic crystal structure, indicating its notable stability and reusability. The photocatalytic degradation experiment conducted in a Fenton-like reaction system demonstrates that, under the conditions of pH 4.0, a H2O2concentration of 5.16 mmol/L, a catalyst dosage of 0.20 g/L, and an OTC concentration of 100 mg/L, the optimal degradation efficiency of 98.3% can be achieved. Additionally, the pseudo-first-order kinetic rate constant was determined to be 4.88 min−1. Furthermore, this study elucidated the detailed degradation mechanisms, pathways, and the influence of various ions, providing valuable theoretical insights and technical support for the degradation of antibiotics in real wastewater.
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JOURNAL OF POWER SOURCES
·
2025
·
IF 7.9
Junlong Feng,Le Hu,Xiaowei Wu,Ziqin Liu,Kaiquan He,Pu Hu,Chaoqun Shang
The uncontrollable Li dendrite accumulation accompanied by low Coulombic efficiency severely hampers the sustainable and practical application of lithium metal batteries (LMBs). To tune the uneven Li + flux caused by irregular pores on commercial separator and realize modulated Li + plating/stripping behaviors, in this work, we report the modification of commercial polypropylene separator with etched Co/Fe-based Prussian blue analogue (PP@PBA-X, X represents the HCl etching time). The optimal PBA-4 with acid etching for 4 h possesses regulated micro-/meso-/macro-porous structure, which ensures homogeneous Li + flow of PP@PBA-4 with high Li + transference number of 0.76 and further hinders the growth of Li dendrites. With the assistance of PP@PBA-4, the Li||Li cell shows stable cycling performance for 500 h at 1 mA cm −2 with fixed specific capacity of 1 mAh cm −2 , while the full Li-S battery with limited Li supply delivers favorable cycling stability for almost 430 cycles with 60 % capacity retention and high Coulombic efficiency of 99.95 % at current density of 500 mAg −1 .
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CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Li Yin,Baixue Xing,Ziyuan Liu,Lihua Lu
Herein, a novel ternary-atomic Fe/Zn/Ir nanozyme (Fe/Zn/Ir TAzyme) with peroxidase (POD)-like and luminescence properties is fabricated through coordinating Ir(III) complex into the as-prepared Fe/ZIF-8. The preparation procedures avoid high-temperature and pyrolysis which endue Fe/Zn/Ir nanocomposite with high stability and can be scaled up. Once Fe/Zn/Ir TAzyme catalyzes the substrate TMB to produce blue oxidized TMB (oxTMB), its luminescence is quenched by the generated oxTMB. Ascribed to its high POD-like activity and interesting luminescence property, a dual-mode sensing platform for the detection of melatonin (MT) is fabricated. In the presence of increasing concentrations of MT, the absorbance of the detection system declines, while the emission of the detection system grows. The detection platform exhibits the limits of detection (LODs) in colorimetric and luminescence detections are 8.9 nM and 8.8 nM, respectively, which can mutually validate the assay results. More importantly, Fe/Zn/Ir TAzyme has been fabricated into test swabs to monitor MT in the way of portable and naked-eye detection. This double-role TAzyme provides new conceptions for researchers to explore novel and highly efficient nanozymes in future.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2025
·
IF 9
Yulan Zheng,Peng Cheng,Zikuo Li,Chuhao Fan,Jinchao Wen,Yue Yu,Li Jia
To achieve the efficient removal of gaseous elemental mercury in coal-fired flue gas, the study successfully prepared the isostructural bimetallic MOFs-based biochar composite by introducing the transition metal Fe into the UiO-66 by solvothermal method and using in-situ growth method for structural design. In addition, the effect of doping the secondary metal Fe and biochar on the Hg 0 removal performance and the corresponding quantitative correlation mechanism was established. The results showed that the overall mercury removal performance of the samples after Fe modification was improved. The optimal Fe loading ratio was 10 %, which corresponded to the adsorption capacity of 127.65 μg·g −1 . The biochar promoted the electron transmission and transfer of the overall reaction system by exerting the carrier effect. The 10 %Fe-UiO-66@20 %BC composite showed the best Hg 0 removal performance, with the corresponding adsorption capacity of 150.74 μg·g −1 . Fe 3+ , lattice oxygen, and chemisorbed oxygen jointly participated in the oxidation process of Hg 0 and finally oxidized Hg 0 to HgO.
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Materials
·
2024
·
IF 3.1
Xiaofei Hao,Ran Wang,Xiumin Tan,Xiufeng Zhang,Xupo Liu,Zhaoyang Wu,Dongli Yuan
Fabricating efficient oxygen evolution reaction (OER) electrocatalysts is crucial for water electrocatalysis. Herein, the spinel-type high-entropy oxides of (Co, Fe, Mn, Ni, Cr) 3 O 4 were synthesized through the high-temperature calcination approach. The influences of calcination temperatures on structures and electrochemical properties were investigated. The optimized catalyst of HEO-900 contains the hybrid structure of regular polyhedrons and irregular nanoparticles, which is beneficial for the exposure of electrochemically active sites. It was identified that the abundant high-valence metal species of Ni 3+ , Co 3+ , Fe 3+ , Mn 4+ , and Cr 3+ are formed during the OER process, which is generally regarded as the electrochemically active sites for OER. Because of the synergistic effect of multi-metal active sites, the optimized HEO-900 catalyst indicates excellent OER activity, which needs the overpotential of 366 mV to reach the current density of 10 mA cm −2 . Moreover, HEO-900 reveals the prominent durability of running for 24 h at the current density of 10 mA cm −2 without clear delay. Therefore, this work supplies a promising route for preparing high-performance multi-metal OER electrocatalysts for water electrocatalysis application.
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