APPLIED SURFACE SCIENCE
·
2021
·
IF 6.707
Limeng Yang,Wendou Chen,Cuihong Sheng,Hailiang Wu,Ningtao Mao,Hui Zhang
Peroxymonosulfate (PMS)-based advanced oxidation processes (AOPs) are encouraging methods for wastewater treatments, but the recycling of used PMS activators in powder form from the wastewater treatment system is still problematic. In this paper, we designed a novel and highly effective carbocatalyst for PMS activation, which was achieved by pyrolyzing the hybrids of metal–organic framework MIL-101(Fe) and dicyandiamide immobilized on the surface of carbon cloth (CC), and a facile route for the preparation of fibrous catalysts was developed. The resultant CC loaded with Fe/N-codoped carbocatalyst exhibited desirable reusability and good stability for the degradation of organic dyes. The mechanism of the novel Fe/N-codoped carbocatalyst for PMS activation including the specific roles of N species and Fe-N binding was investigated. It was demonstrated in electrochemical impedance spectroscopy (EIS) results that the CC facilitated the electron transport of the carbocatalyst in AOPs. It was shown in the radical quenching and electron paramagnetic resonance (EPR) experiments that both the radical and non-radical pathways were accountable for the degradation of contaminants, and the non-radical path was principal. It was also evident in the X-ray photoelectron spectroscopy (XPS) and density functional theory (DFT) results that pyridinic N and graphitic N were the main active species for PMS activation.
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CHEMICAL ENGINEERING JOURNAL
·
2021
·
IF 13.273
Dan Yu,Jiahong He,Taiping Xie,Qiang Xu,Quanxi Zhu,Jun Yang,Jibin An,Feng Ye,Jiankang Wang,Bin Xiang
It is of significant to explore activation mechanism of peroxymonosulfate (PMS) for development of more active and robust metal oxide catalyst. Here, we discover a key role of Sr-O bond in boosting the catalytic activity of SrCo 0.81 Fe 0.19 O 2.78 perovskite. In this catalytic system, oxygen vacancy, Fe 4+ /Fe 3+ , and Co 3+ /Co 2+ redox cycles synergistically enhanced catalytic activity of SrCo 0.81 Fe 0.19 O 2.78 for antibiotic degradation with 100 % Florfenicol (FF) removal in 27 min. Moreover, this catalyst presented excellent stability although oxygen vacancy had a decrease after reuse. The influential factors including coexisting anions on FF degradation were systematically studied. Comparative experiments and theoretical calculation indicate Sr-O ionic bond provides electrons for Co-O and Fe-O covalent bonds to accelerate Fe 4+ /Fe 3+ , and Co 3+ /Co 2+ redox cycles for PMS activation . Finally, the FF degradation pathway over SrCoFe perovskite/PMS system was identified by LC-MS/MS.
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SENSORS AND ACTUATORS B-CHEMICAL
·
2024
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IF 8
Dehao Kong,Yong Wang,Jiayin Han,Yuan Gao,Fengrong Liu,Weirong Zhou,Yubing Gao,Geyu Lu
Triethylamine monitoring plays a vital role in industrial safety and marine environmental protection. Co 3 O 4 has been proved to be a promising sensitive material for triethylamine detection. Promoting gas reactions on the surface of sensitive materials is the key to realizing high-performance gas sensors. In this work, MgO microrods were used as sacrificial templates to prepare nanosheet-assembled hollow microtubular Co-Fe bimetallic oxides. The large specific surface area, small crystallite size, and stretched lattice of Co-Fe bimetallic oxides boosted surface gas reactions and improved the response to triethylamine vapor. The modulation in the energy band structure caused by doping-occupied sites of iron on the gas-sensing properties was also considered. The preferential occupation of tetrahedral sites by multivalent iron reduced the work function and band gap of the material, thus enhancing the formation of ion-adsorbed oxygen. In these cases, the sample with about 20 % iron content (CF2) showed the optimum triethylamine sensing performance at 195 °C, with a detection limit as low as 1 ppm, a gas response of 10.9 for 100 ppm triethylamine, and a 58 % shorter recovery time. In addition, it also exhibited excellent selectivity and repeatability. The gas adsorption model was additionally used to analyze the response and recovery process from an energy perspective. This work contributes insights into the sensitivity enhancement and response-recovery process modulation of spinel oxide gas sensors, mainly in terms of crystal structure and doping sites.
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Catalysts
·
2025
·Vol. 15
·期 11
·1032
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IF 4
Jingmo Zhou,Chaoyue Liu,Wenke Zhao,Faizan Ahmad,Yaning Zhang
This study pioneers the application of metal-doped Fe-Al as multifunctional redox catalysts for tunable syngas production from plastics via a microwave-assisted process (CLG). We rationally designed a series of redox catalysts (Ni, Ca, Ce, Sr, Co) to unlock efficient H2-rich syngas production from (high-density polyethylene) HDPE. A class of metal-doping (Ni, Ca, Ce, Sr, and Co) Fe-Al redox catalysts was engineered, with Ni-doped Fe-Al (Ni-Fe-Al) exhibiting the excellent H2-rich syngas production (75.32 mmol/gHDPE syngas, 47.09 mmol/gHDPE H2). This is attributed to the improved redox activity, which facilitates efficient lattice oxygen transfer and catalytic reforming reactions, alongside improved microwave absorption and a porous structure that promotes reactant access. This strategic material design, coupled with process parameter optimization (800 W, redox catalyst/plastic = 2.0), developed a highly efficient HDPE-to-syngas conversion system. The process produced a high-quality syngas (90.03% H2+ CO, H2/CO ratio = 2.27) with a rapid heating rate (233.0 °C/min) and minimal energy input (3.52 kWh/molgas). This work provides not just an effective upcycling route for plastics, but a fundamental blueprint for designing advanced redox catalysts to unlock the full potential of microwave-CLG.
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Journal of Environmental Chemical Engineering
·
2025
·Vol. 14
·期 1
·120546
·
IF 7.2
JinCheng Dai,Shuyue He,Xiyu Song,Hongjuan Zhang,Ruyi Xie
The construction of heterojunction photo-Fenton catalysts to activate hydrogen peroxide for the efficient degradation of organic pollutants in water has attracted considerable attention. Herein, a CuBi 2 O 4 @MIL-53(Fe) Z-scheme heterojunction catalyst was successfully prepared by solvothermal method for tetracycline (TC) degradation. In this catalytic system, the heterogeneous photocatalytic reaction and the Fenton reaction form a strong synergistic effect in the degradation of organic pollutants through the transfer of photogenerated electrons. The results indicate that in the presence of trace concentrations of H 2 O 2 (2.60 mM), 0.20 g/L of MC-15 (with CuBi 2 O 4 accounting for 15 % of the mass of MIL-53(Fe)) exhibited the highest catalytic activity, with a TC (150 mg/L) removal rate of 94.0 % after 50 min of visible light irradiation. Interestingly, the MC-15 catalyst can still achieve a removal rate of 62.1 % of TC even under dark conditions. Furthermore, in degradation experiments, MC-15 exhibited high environmental stability and applicability in different natural water system. The excellent catalytic performance of the light/MC-15/H 2 O 2 system is attributed to the quick separation of photogenerated electron-hole pairs from Z-scheme heterojunction CuBi 2 O 4 @MIL-53(Fe) and the accelerated bimetallic ions cycle. A possible photo-Fenton catalytic mechanism of MC-15 catalyst is proposed based photoelectrochemical tests, free radical capture experiment and electron paramagnetic resonance (EPR) analysis. This study provides a reference for the development of iron-based metal-organic framework composite photo-Fenton catalysts.
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
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2025
·
IF 5.4
Mingli Yue,Bixian Wang,Jianbo Zhao,Liangzhong Lv,Ying Fu,Fei Ye
Cancer, the world’s second leading killer, has increasing crude incidence rates and faces multiple prevention/control challenges. Curcumin (Cur) has anticancer activity but low bioavailability, restricting its use in cancer therapy. A nanomaterial (Fe₃O₄/PDA@Cur) for targeted curcumin delivery is developed in this work, which has a magnetic Fe 3 O 4 core made by solvothermal synthesis and a polydopamine (PDA) shell made by one-pot synthesis. Results show that drug loading rate reached 40.3 % when the mass ratio of Fe₃O₄/PDA: Cur was 1:3. The hemolysis rate was measured to be 1.24 % in the hemocompatibility test. The complex exhibited good antibacterial efficacy against both Staphylococcus aureus ( S. aureus , MIC 250.0 μg/mL and MBC 500.0 μg/mL), Escherichia coli ( E. coli , MIC 625.0 μg/mL and MBC 1250.0 μg/mL), which was attributed to the properties of the incorporated PDA. The material has good blood compatibility and antibacterial effects, and it effectively prevents secondary infection at the tumor site and red-blood-cell lysis. Notably, at pH 5.0, drug release reached 75.5 % via pH-responsive mechanisms which tumor microenvironment (pH 5.0–6.5), drug release is accelerated in these regions, enabling targeted therapy that minimizes toxicity to normal cells and systemic side effects, thereby enhancing treatment safety. This complex, which possesses both drug delivery and antibacterial properties, holds significant clinical importance for preventing opportunistic infections during tumor treatment.
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Nature Communications
·
2025
·Vol. 16
·期 1
·10455
·
IF 15.7
Jin Sijia,Tan Wenxian,Huang Yilin,Wang Yi,He Zhiqiao,Zhang Haiyan,Song Shuang,Cai Yaqi,Zeng Tao
Fe-N 5 single-atom catalysts (SACs) hold great promise for water decontamination, however, the fundamental relationship between their high coordination shell environment and catalytic performance in Fenton-like reactions remains poorly understood. Here, we precisely regulate the high coordination shell defects of a model SAC with well-defined axial Fe-N 5 configurations to elucidate the impact of remote interactions on peroxymonosulfate (PMS) activation. Experimental and theoretical studies confirm that remote modulation of Fe-N 5 sites through high coordination shell defects profoundly enhance Fenton-like catalytic activity, enabling FeN 5 -SD 2 to achieve a turnover frequency (TOF) value of 0.338 min⁻ 1 , surpassing state-of-the-art SACs. Our findings reveal a critical volcano-type correlation between defect content and catalytic efficiency, where coordinated modulation of Fe d -band center positioning and PMS adsorption energetics governs reaction dynamics. Only the FeN 5 -SD 2 configuration with an optimal level of defects density and moderate adsorption energy enables sufficient O-O bond elongation in PMS to lower the energy barrier for selective singlet oxygen ( 1 O 2 ) evolution. This study unveils the mechanistic role of higher coordination shell defects in regulating Fe-N 5 active sites and introduces a well-defined model to investigate the structure–property correlations of higher coordination shells in SACs for Fenton-like reactions.
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PubMed
高影响因子
JOURNAL OF THE EUROPEAN CERAMIC SOCIETY
·
2025
·
IF 6.2
Xiang Wang,Haoran Wang,Min Li,Qingtao Guo,Ben Ge,Xingyu Xiong,Zhibin Yang
This work focuses on the development of high-performance La 0.1 Sr 1.9 TiFeO 6-δ (LSTF)-based fuel electrode materials through targeted Co substitution at the Ti site and Fe site. By selectively substituting Ti or Fe with Co element, lattice contraction and change of the Fe 3 ⁺/Fe 4 ⁺ ratio in LSTF double perovskite are achieved. La 0.1 Sr 1.9 Ti 0.8 Co 0.2 FeO 6-δ (LSTCF) material obtains higher oxygen vacancy concentration and better CO 2 adsorption capacity. Electrochemical impedance spectroscopy (EIS) test demonstrates that the La 0.1 Sr 1.9 TiFe 0.8 Co 0.2 O 6-δ (LSTFC) electrode exhibits superior performance in gas transport process, while the LSTCF electrode demonstrates significant advantages in oxygen ion conductivity and dissociative adsorption of CO 2 species. The single cell with the LSTCF electrode exhibits superior electrolysis performance, achieving a current density of 1.07 A·cm −2 at 800 °C and 1.8 V for CO 2 electrolysis. This work provides a novel pathway for the development of catalysts for solid oxide electrolysis cell (SOEC) fuel electrodes.
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JOURNAL OF THE ELECTROCHEMICAL SOCIETY
·
2022
·Vol. 169
·期 3
·034506
·
IF 4.386
Shuiyun Shen,Lin Li,Cehuang Fu,Guanghua Wei,Xiaojing Cheng,Jiewei Yin,Xiaohui Yan,Gang Wu,Junliang Zhang
A highly active Fe/N doped porous carbon electrocatalyst is constructed benefiting from the elaborate employment of benzimidazole (BIm) as nitrogen precursor. Compared with 2-methylimidazole (2-MIm), BIm can strongly capture Fe ions and strengthen the Fe–N bond, thus more Fe–N4 active sites form in the electrocatalyst with an enhanced catalytic activity towards oxygen reduction. The optimal sample exhibits a half-wave potential of 0.80 V vs RHE in acidic media.
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SOLID STATE SCIENCES
·
2023
·
IF 3.5
Ningxia Li,Qi Luo,Meiyan Cui,Zhiying Zhao,Zhangzhen He
New fluorophosphate compounds H A 5 M 6 (OH) 4 F 4 (HPO 4 ) 8 ( A = K, Rb; M = Fe, Ga) were synthesized by a fluorine-rich hydrothermal method . These compounds crystallize in the monoclinic system with a P2 1 /n space group, exhibiting an open framework structure built by [PO 3 (OH)] groups, [MO 4 (OH)F], and [MO 4 F 2 ] octahedra, where ten-membered-ring channels, eight-membered-ring channels, six-membered-ring channels, and the linear M 3+ trimers are seen. The characterizations were carried out by powder XRD , EDS , FT-IR spectra, and magnetic measurements. The results confirmed that H A 5 Fe 6 (OH) 4 F 4 (HPO 4 ) 8 ( A = K, Rb) show a quite similar magnetic behavior, possessing an antiferromagnetic ordering at 14.7 K and 15.6 K, respectively. The changes of the magnetic entropy for such antiferromagnetic orderings can be estimated as ∼10.7 J mol −1 K −1 and ∼13.4 J mol −1 K −1 .
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WATER RESEARCH
·
2022
·
IF 13.4
Zhengyuan Zhou,Jingyao Huang,Guilu Zeng,Rumin Yang,Zhiqiang Xu,Zhikang Zhou,Shuguang Lyu
S(IV)-based advanced oxidation process has been applied for contaminants remediation. However, as a traditional source of sulfite (SO 3 2− ), Na 2 SO 3 is extremely soluble in water, resulting in a high concentration of SO 3 2− to quench the generated reactive oxygen species (ROS). In this work, CaSO 3 was introduced instead of Na 2 SO 3 for its slow-released SO 3 2− ability and Fe(III)/CaSO 3 system was established for the removal of trichloroethylene (TCE) and other organic contaminants. The degradation efficiency of TCE reached 94.0% and TCE could be completely dechlorinated and mineralized, while the removal of other contaminants was all over 85.0% at the optimal tested conditions. Through EPR detection, ROS scavenging and probe tests, and quantification of ROS amounts, it was concluded that the dominant ROS in Fe(III)/CaSO 3 system were SO 4 − · and 1 O 2 , of which the transformation mechanism of SO 4 − · to 1 O 2 was revealed and demonstrated comprehensively. The synergistic contaminants degradation performance in different sulfur-iron-containing systems and in the presence of oxidants was evaluated. The effects of various solution conditions were assessed and Fe(III)/CaSO 3 system was of higher resistance on complex solution matrixes, suggesting the broad-spectrum and application perspective for the remediation of complex contaminants in actual water.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2022
·
IF 4.326
Jinshuo Qiao,Xiangjun Chen,Chengyi Ai,Zhenhua Wang,Wang Sun,Kening Sun,Chunming Xu
Direct carbon solid oxide fuel cells (DC-SOFCs), which can efficiently convert chemical energy of carbonaceous fuels into electricity, have recently gained much research attention as they offer an effective way to address future economic and environmental challenges. Herein, B-site Ti-substituted (PrBa)0.95Fe2–xTixO6−δ (PBFTx, x = 0–0.3) materials are synthesized via a sol–gel combustion method and evaluated as anode materials for DC-SOFCs. Ti doping enhances the phase structure stability of the material under a reducing atmosphere. X-ray diffraction, scanning electron microscopy, and transmission electron microscopy analyses demonstrate the exsolution of metallic Fe nanoparticles on the surface of the PBFTx perovskite lattice after the materials are treated under a reducing atmosphere, which can improve the catalytic performance of DC-SOFC anode. Among the Ti-doped samples (x = 0.1–0.3), PBFT0.2 shows the largest adsorption capacity for CO and the highest electrical conductivity in air. Using pure nano-activated carbon as a fuel, the single cell supported by La0.9Sr0.1Ga0.8Mg0.2O3 electrolyte with PBFT0.2 as an anode achieves the maximum power densities of 527, 281, and 146 mW·cm–2 at 800, 750, and 700 °C, respectively. The above excellent performance of PBFT0.2 indicates that it has great potential for application in DC-SOFC anode.
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