RARE METALS
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2023
·Vol. 42
·期 10
·3443-3454
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IF 8.8
Zhou Ming-Jie,Zhang Wen-Tao,Li Zhun,Feng Tao,Lan Si,Peng Zhen,Chen Shuang-Qin
Metallic glasses (MGs) are promising heterogeneous catalysts in water remediation, due to their superior efficiency, selectivity, reusability and corrosion resistance. However, few works are focused on the influence of inorganic anions that are abundant in wastewater. Herein, four common inorganic anions were added in a heterogeneous Fenton-like system (Fe–MG/H 2 O 2 ) to study inorganic anions’ influence on MGs’ catalytic performance during methylene blue (MB) degradation. Evidence demonstrated that chloride ions and dihydrogen phosphate ions had an adverse effect on the catalytic performance of Fe–MG, whereas Fe–MG/H 2 O 2 system sustained high efficiency in the presence of sulfate ions and nitrate ions during the Fenton-like process. By studying the structure, surface morphology, and evolution of active species, it was found that inorganic anions had a significant effect on the surface morphology of Fe–MG and the generation of active species. This work will provide essential references for MGs as heterogeneous catalysts in practical applications. Graphical abstract
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CHEMICAL ENGINEERING JOURNAL
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2026
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IF 12.5
Xiaohan Guo,Yanfang Liu,Hongxiang Zhu,Xiaohui Yu,Feng Shi,Qinqin Liu,Qiang Liu,Ying Xu
Asp donates electrons to reprogram Fe O clusters of MIL-53(Fe). • This electronic switch redirects dominant ROS from •OH to •O 2 − . • The mechanism enables neutral-pH POD-like activity of MIL-53(Fe)@Asp. • The Asp-modified nanozyme integrates with GOX for cascade glucose sensing. MIL-53(Fe) exhibits peroxidase-like activity only under acidic conditions, limiting its biosensing applications. We overcome this by using aspartic acid (Asp) as a structure-directing agent to modify MIL-53(Fe) (MIL-53(Fe)@Asp) via hydrothermal synthesis followed by Asp coordination. Unlike conventional pH-reduction strategies, Asp modification does not alter bulk pH but induces intrinsic electronic restructuring of Fe O clusters, as confirmed by increased Fe 3+ /Fe 2+ ratio and introduction of N → Fe coordination (XPS). At pH 6.9, the TMB-based activity of MIL-53(Fe)@Asp is 27-fold higher than that of pristine MIL-53(Fe). Steady-state kinetics show favorable Km values (TMB 0.27 mM, H 2 O 2 1.38 mM) at neutral pH. Mechanistic studies (ROS identification, EPR, band structure, DFT) reveal that Asp exerts an electron-donating effect that reprograms the electron distribution of Fe O clusters, activating the otherwise inactive MIL-53(Fe) framework at neutral pH and diversifying the catalytic pathways to include a less pH-dependent •O 2 − route alongside the partially maintained •OH pathway. This pathway diversification enables efficient neutral-pH peroxidase-like catalysis, with •O 2 − as the dominant pathway. Leveraging this, we construct a cascade nanoplatform (MIL-53(Fe)@Asp@GOX) integrating glucose oxidase, which exhibits excellent cascade activity at neutral pH. The method is applied to glucose detection in blood and saliva, demonstrating good linearity, precision, selectivity, and recovery. The glucose concentrations determined by our sensor correlated well with those obtained using a commercial assay kit. Notably, the limit of detection for glucose in saliva reaches 2.08 μM, offering a promising route toward non-invasive glucose sensing. This work establishes a design principle for creating pH-adaptive catalytic microenvironments in Fe-MOFs through electronic restructuring and pathway diversification, overcoming a long-standing limitation of MIL-53(Fe) for biomedical applications. Download: Download high-res image (111KB) Download: Download full-size image
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JOURNAL OF HAZARDOUS MATERIALS
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2026
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IF 10.6
Zhaorui Li,Simeng Gan,Xiaofeng Huang,Fei Wang,Xin Sun,Kai Li,Ping Ning
Preparation of Highly Crystalline Fe₂O₃-Based Catalyst (WCS600) from Copper Slag. • Thermal Reconstruction Tunes Fe–O Coordination and Oxygen Vacancies in WCS600. • Oxygen vacancies promote nitrate adsorption and activation and construct the Fe–OH working interface. • ICCUS-derived H₂ supply can reduce the NH₃ production cost to below 1.15 $ kg -1 . The synergistic treatment of copper slag valorization and nitrate wastewater remediation represents a critical pathway toward the high–value utilization of metallurgical solid waste and nitrogen resource recovery. This study employs a strategy synergistically coupling thermal reconstruction with surface defect engineering to convert the Fe–containing phases in copper smelting slag into an Fe₂O₃–based electrocatalyst, designated as WCS600. At −0.6 V vs. RHE, WCS600 achieves an NH₃ production rate of 7.16 mg h⁻¹ cm⁻² and a FE NH3 of 91.56%. Characterization and DFT calculations reveal that cathodic polarization induces the electrochemical reconstruction of surface oxygen vacancies, dynamically generating an interface enriched with mixed–valence Fe²⁺/Fe³ ⁺ species and hydroxylated Fe–OH. This interface promotes the directional conversion of nitrogen–containing intermediates, thereby enhancing NH₃ selectivity. In a simulated acidic smelting wastewater system, WCS600 exhibits excellent stability and resistance to interference, with Fe leaching remaining below the safety threshold. Further techno–economic analysis indicates that, under specific scenarios coupling low–carbon hydrogen sources, the NH₃ production cost of WCS600 could be reduced to below 1.15 $ kg⁻¹ . This study provides a theoretical foundation and practical guidance for the synergistic resource–oriented treatment of solid waste and nitrate wastewater, as well as for the development of scalable electrochemical ammonia synthesis. Download: Download high-res image (227KB) Download: Download full-size image
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AQUACULTURE
·
2023
·
IF 4.5
Xiangjie Mao,Wangwang Chen,Xianmei Long,Xiaomei Pan,Guoqing Liu,Wenguang Hu,Dianchao Gu,Qingsong Tan
The aim of this study was to investigate the effects of dietary iron (Fe) levels on the growth performance, health status, meat quality, and intestinal flora of juvenile largemouth bass ( Micropterus salmoides ) and to determine the dietary Fe requirement of largemouth bass . Largemouth bass was fed with 6 isonitrogenous and isocaloric experimental diets containing Fe levels of 42.26, 50.79, 66.61, 80.86, 123.13, and 201.87 mg/kg for 10 weeks. The results showed that both final body weight (FBW) and specific growth rate (SGR) tended to increase and then decrease with increasing dietary Fe level, reaching their highest values of 50.34 g and 3.58%/d at a dietary Fe concentration of 80.86 mg/kg respectively. Feed efficiency (FE) and protein efficiency ratio (PER) increased linearly with increasing dietary Fe level. Total serum protein (TP) and urea nitrogen (UN) decreased linearly with increasing dietary Fe level. Serum superoxide dismutase (SOD) and catalase (CAT) enzyme activities tended to increase and then decrease with increasing dietary Fe level, while serum malondialdehyde (MDA) level tended to decline and then increase. In addition, increased dietary Fe level tended to improve muscle hardness and chewiness , thus improving meat quality. Analysis of the intestinal flora showed that the abundance of microorganisms such as Plesiomonas , Peptostreptococcaceae , and Lactococcus in the genus level increased significantly at dietary Fe concentrations of 80.86 mg/kg and 201.87 mg/kg, indicating that appropriate levels of dietary Fe can increase the diversity of intestinal microorganisms . Optimal dietary Fe levels for juvenile largemouth bass were determined to be between 73.81 and 83.22 mg/kg based on the broken-line regression analyses of SGR, FE, or hemoglobin content.
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Journal of Environmental Chemical Engineering
·
2023
·
IF 7.7
Chen Yang,Xuefeng Hu,Yao Huang,Baiyu Liu,Junhan Yang
We report a rational and scalable synthetic approach to prepare Fe-decorated carbon nitride materials assisted by carbonized polyamine (C-Fe@PDA-CN). The material exhibited extremely high activity and stability for the degradation of 2-mercaptobenzothiazole (MBT) and other organic pollutants (phenol, BPA , MB , and RhB) under visible light irradiation. Furthermore, escape from CN to C-Fe@PDA provides an electron transfer channel to facilitate carrier separation and accelerate the generation of active species, as confirmed by photoluminescence , photoelectrochemical, and electron paramagnetic resonance (EPR). Fe exists in the material coordinated with the pyrrole nitrogen of polydopamine. This coordination structure is conducive to the generation of singlet oxygen ( 1 O 2 ). It is confirmed by steady-state phosphorescence spectroscopy (PH) that 1 O 2 originates from electron transfer. Superoxide radicals are generated by electron transfer and then oxidized into 1 O 2 by holes. The main intermediates of MBT degradation were identified by the LC-MS method, and a possible photocatalytic mechanism based on quenching experiments and EPR tests was proposed.
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2023
·
IF 22.1
Yang Wang,Shiyuan Lin,Meng Li,Chuanyong Zhu,Hao Yang,Pei Dong,Mingjie Lu,Wenhang Wang,Jianlin Cao,Qiang Liu,Xiang Feng,Han Hu,Noritatsu Tsubaki,Mingbo Wu
The direct transformation of CO 2 into valuable chemicals with the aid of sustainable energy-generated H 2 has attracted enormous interest owing to the integrated functions of carbon elimination and non-fossil fuel-derived products supply. As one of the most promising catalysts for CO 2 hydrogenation, the chemical properties of Fe-based catalysts, such as electronic structure and coordination environment, have been widely studied. However, the mass/heat transfer effects in Fe-based catalysts are also crucial to the targeted product selectivity and catalytic stability, but have been rarely investigated due to the lack of facile fabrication protocols. Herein, we precisely fabricate and tailor the architecture of the Fe-based monolithic catalysts by a direct ink writing (DIW)-type three-dimensional (3D) printing technology under the guidance of the computationally controlled printing procedure. The Fe-based monolithic catalyst with spiral-type architecture delivers extremely high light olefins selectivity (52.6%) and space time yield (STY, 451.8 g CH2 kg cat −1 h −1 ) from CO 2 hydrogenation. Based on the mass-transfer simulation, the spiral-structured channels in the Fe-based monolithic catalyst lower the coverage of intermediates and products on the catalytic interface due to the optimal mass-transfer effect, thus maximizing the utilization of active sites and timely terminating the carbon-chain growth. More in-depth, the density functional theoretical (DFT) simulations verify that the relatively electron-rich catalytic interface with low intermediate coverage could facilitate the desorption of olefins and decelerate the C-C coupling step, which synergistically guarantee the enhanced light olefins synthesis performance. Furthermore, the enhanced heat-transfer effect endowed by the 3D architecture prolongs the life-time of catalyst by avoiding undesirable active site aggregation and carbon deposition. The powerful strategy for catalyst fabrication not only provides a new concept of regulating the CO 2 hydrogenation performance of Fe-based catalysts but also holds a great promise to spread into other catalytic systems for targeted synthesis.
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MICROPOROUS AND MESOPOROUS MATERIALS
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2023
·
IF 5.2
Yan Gao,Shumin Zhao,Miao Yan,Yongxia Li,Jianshe Zhao
In this work, the encapsulating peroxo-polyoxometalate in the mesoporous of metal-organic framework (MIL-101(Fe)) to synthesize composite according to the principle of host-guest matching. The structure of the host-guest composite was analyzed by a variety of methods, and the catalytic activity for desulfurization was investigated under mild conditions. The composites combine the advantages of peroxo-polyoxometalate (high efficiency) and MIL-101(Fe) (good recyclability and high porosity), showing synergistic effect between host and guest. The sulfur-containing organic compounds in simulated liquid fuel can be almost completely removed under the catalysis of PW 4 @MIL-101(Fe). The catalyst PW 4 @MIL-101(Fe) can be reused for 10 times without prominent decrease in desulfurization activity, indicating that it has good reusability due to the confinement effect between the window size of MIL-101(Fe) and molecular size of PW 4 . In addition, several control experiments and electron spin resonance experiment were researched to explore the possible mechanism, and the results show that the active component in the catalyst can promote the decomposition of H 2 O 2 into ·OH and thus accelerate the desulfurization reaction. This work discloses a facile and environmentally friendly method to prepare the "host-guest matching" catalyst with high activity and stable reusability, which provides ways for further developments in heterogeneous catalyst based on POM and MOF.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2023
·
IF 9.9
Tianwei Wang,Quan Zhang,Kang Lian,Gaocan Qi,Qian Liu,Ligang Feng,Guangzhi Hu,Jun Luo,Xijun Liu
Metal-organic frameworks (MOF) derived carbon materials are considered to be excellent conductive mass transfer substrates, and the large specific surface area provides a favorable platform for loading metal nanoparticles . Tuning the coordination of metals through polyacid doping to change the MOF structure and specific surface area is an advanced strategy for designing catalysts. Modification of Fe-doped ZIF-8 pre-curing by pyrolysis of phosphomolybdic acid hydrate (PMo), Fe nanoparticles confined by Mo and N co-doped carbon frameworks (Fe-NP/MNCF) were fabricated, and the impact of PMo doping on the shape and functionality of the catalysts was investigated. The Zn-air battery (ZAB) driven CO 2 electrolysis was realized by using Fe-NP/MNCF, which was used as bifunctional oxygen reduction reaction (ORR) and carbon dioxide reduction reaction (CO 2 RR) catalysts. The results show that the half-wave potential (E 1/2 ) of Fe-NP/MNCF is 0.89 V, and the limiting diffused current density ( j L ) is 6.4 mA cm −2 . The ZAB constructed by Fe-NP/MNCF shows a high specific capacity of 794.8 mAh g Zn −1 , a high open-circuit voltage (OCV) of 1.475 V, and a high power density of 111.6 mW cm −2 . Fe-NP/MNCF exhibited efficient CO 2 RR performance with high CO Faraday efficiency (FE CO ) of 87.5 % and current density for the generation of carbon dioxide ( j CO ) of 10 mA cm −2 at −0.9 V vs RHE. ZAB-driven CO 2 RR had strong catalytic stability. These findings provide new methods and techniques for the preparation of advanced carbon-based catalysts from MOFs.
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PubMed
高影响因子
International Journal of Coal Preparation and Utilization
·
2023
·
IF 2.1
Xuexia Wang,Wencheng Xia,Yaoli Peng,Guangyuan Xie
Iron-assisted pyrolysis (Fe-assisted pyrolysis) is a high-efficiency technique to remove sulfur from low-rank coal. However, the sulfur removal mechanism of Fe-assisted pyrolysis did not compressively address. For filling this gap, this study explored the sulfur removal mechanism of diphenyl sulfone during Fe-assisted pyrolysis based on the factor optimization of desulfurization performance. The iron powder under the optimal conditions of Fe-assisted pyrolysis was characterized with X-ray diffractometer (XRD) and X-ray photoelectron spectroscopy (XPS), showing that FeS and some FeS2 were formed on the surface of post-pyrolysis iron powder. Gas chromatography (GC) analysis manifested that the addition of iron powder in the pyrolysis process could considerably reduce the SO2 emission. GC and Fourier transform infrared spectrometer (FTIR) analyses demonstrated that there was C–S bond broken in the diphenyl sulfone structure during Fe-assisted pyrolysis. From the results of thermogravimetry-mass spectrometry (TG-MS), the addition of iron powder in the pyrolysis process could enhance the reaction rate and reduce the temperature required for the reaction. We believe that the results of the present study provided a theoretical basis for a profound understanding of the desulfurization mechanism of Fe-assisted pyrolysis.
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CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Jiahang Liu,Xiaoyang Li,Yingying Chu,Ling Yuan,Ruolin Lv,Weiming Zhang
The conventional Fe(III)/H 2 O 2 system is of low efficiency on the removal of most organic pollutants. However, we discovered that the Fe(III)/H 2 O 2 system was robust on remediating tetracycline (TC) in water (0.109 min −1 for the pseudo-first kinetic constant), and the reaction was even slightly faster than that in the conventional Fe(II)/H 2 O 2 system (0.105 min −1 ). The addition of TC could also initiate the degradation of other refractory pollutants in the Fe(III)/H 2 O 2 system. Complexation between Fe(III) and TC with the stoichiometric ratio of 1:1 was observed. Electron transfer from TC to Fe(III) gave rise to the slight production of Fe(II), which served as the initiator of the following Fenton reaction. •OH was ascertained as the main reactive species through quenching experiments, EPR tests and the probe method, while O 2 • − /HO 2 • was also a subsidiary contributor. Hydroquinone intermediates were proved to be generated through the hydroxylation of the benzene ring of the TC molecule by •OH and thus facilitate the reductive transformation of Fe(III) to Fe(II). This study analyzes the relationship between molecular structural features of TC and the catalytic efficiency of ferric Fenton-like reactions. We expect to shed light on new mechanistic insights on autocatalysis in the Fenton-like catalytic processes.
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CERAMICS INTERNATIONAL
·
2023
·
IF 5.2
Xiao Lin,Zhongyu Long,Long Jiang,Zhiyuan Liu,Changyong Liu,Zhangwei Chen
High-performance SiOC(Fe) wave-absorbing ceramics, containing a large number of carbon nanowires, were successfully prepared using a combination of photopolymerization 3D printing technology and the polymer-derived ceramic pyrolysis method. By employing an optimized segmented slow heating scheme with extended holding time, the pyrolysis of SiOC(Fe) ceramics at 1000 °C facilitated the growth of carbon nanowires, Fe 3 C and SiO 2 grains. These carbon nanowires were interlaced and interconnected within the samples, forming abundant conductive networks. This highly conducive network efficiently converted electromagnetic energy into thermal energy, effectively dissipating electromagnetic waves, and consequently enhancing the microwave absorption performance of ceramics. Moreover, this approach not only reduced ceramic cracks but also improved the dielectric loss performance of the materials, achieving a minimum reflectivity value of −35.72 dB. The SiOC(Fe) ceramics added with 5 wt% VcFe effectively enhanced the magnetic loss of the material, reduced the difference between the relative complex permeability (μ r ) and the relative complex dielectric constant (ε r ), and improved the impedance matching between the material surface and air, thereby further improving its microwave absorption performance. This resulted in an increase in the maximum effective absorption bandwidth of the material to 12.7 GHz at 5 mm. This study offers a promising solution for the preparation of ceramic matrix composite materials incorporating carbon nanowires, magnetic particles and ceramic precursors, which would be potentially valuable for radar detection and sensor applications .
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ADVANCED FUNCTIONAL MATERIALS
·
2023
·Vol. 34
·期 2
·2308849
·
IF 19
Yashuai Pang,Minsen Xie,Xinghao Lu,Zhao Wan,Zhuohang Zhong,Waqas Muhammad,Xiang Long Huan,Yinghua Niu,Zhen Zhang,Weiqiang Lv
Lithium–sulfur (Li–S) batteries have attracted wide attention as high-energy-density energy storage devices, but their practical applications are hindered by the severe shuttle effect and sluggish kinetics of lithium polysulfides (LiPSs). To address these challenges, polar mediators are employed to chemisorb and catalyze LiPSs, but most of them suffer from low electronic conductivity and poor catalytic activity. Here, a novel strategy is reported to enhance both properties by dispersing Fe(III) atoms in VO 2 nanoribbons(Fe-VO 2 ), creating electronic metal-support interactions (EMSI) that modulate the electronic structure and charge transfer of VO 2 . Theoretical calculations reveal that EMSI lowers the energy barrier for the decomposition of Li 2 S from 1.60 to 1.32 eV and increases the electronic conductivity of VO 2 . Fe doping reduces the Li-ions diffusion barrier from 1.42 eV in VO 2 to 0.99 eV in Fe-VO 2 . The Fe-VO 2 catalyst shows strong adsorption and fast converstion of LiPSs, resulting in high energy density and long cycling life of Li-S batteries. The cathode with Fe-VO 2 maintains a higher capacity retention of 67% after 500 cycles at 1 C, compared with 52.4% and 53.6% for the carbon black based cathode and VO 2 based cathode, respectively. This work demonstrates the potential of EMSI for designing efficient catalysts for Li–S batteries and provides new insights into the electronic structure engineering of polar mediators.
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