COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
·
2024
·
IF 4.9
Peng Wang,Chenyu Gao,Qianpeng Dong,Lianlian Wang,Dianming Chu,Yan He,Wenjuan Bai
s The application of carbon nanotubes in materials science is rapidly expanding, leading to an increasingly urgent demand for large-scale synthesis. Central to the growth of carbon nanotubes is the development of effective catalysts; thus, the large-scale production of these catalysts becomes crucial for successful carbon nanotube synthesis. Extensive research has been conducted on the mechanisms and regulation of interfacial interactions between metals and supports during catalyst synthesis. This paper is based on the interface interactions between common metal catalysts such as Fe, Co, Ni, and Al 2 O 3 , and Fe-Co, Fe-Ni, and Fe-Co-Ni metal catalysts were prepared by a one-step method. The catalysts were synthesized through a "one-step process," and the formation mechanisms of bimetallic and trimetallic catalysts, as well as the influence of interfacial interactions on catalyst formation and catalytic activity, were thoroughly investigated. The results indicate that with the involvement of Fe, Co and Ni on the surface of Al 2 O 3 maintain a small size morphology due to interfacial interaction. Meanwhile, the nanoparticles form a doped structure with Al 2 O 3 , effectively avoiding the deactivation of nanoparticles caused by agglomeration. In addition, the three catalysts for growing CNTs were analyzed in order to investigate the effects of different concentrations of metal ratios and time of carbon source on the catalytic activity, which provides new ideas for improving the catalyst design system.
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Water Supply
·
2020
·Vol. 21
·期 3
·1016-1024
·
IF 0.9
Dong Zijun,Li Mu,Chen Meifen,Gu Yurong,Jiang Chengchun,Sun Feiyun
The transformation of iodide (I − ) and hypoiodous acid (IO − ) by Fe (II)-activated peroxydisulfate (PDS) in the presence of natural organic matter (NOM) was investigated. In the water of a reservoir in Shenzhen, four kinds of organic matter were detected: iodoform > diiodo-bromomethane > dibromo-iodomethane > dichloromethane. As pH increased from 3 to 10, I − conversion rate decreased from 31.0% to 11.0%. There is basically no iodic acid ( ) generated under alkaline conditions, probably due to these organic matters. When PDS concentration is low, PDS can oxidize part of I − to IO − , and the oxidation of I − into reaction and continued oxidation reaction exist at the same time, so some is generated in the system. As the proportion of Fe (II) increases, the generation rate of gradually increases. When Fe 2+ /PDS is 1:5, 2:5, and 3:5, the conversion rates of are 4.7%, 6.5%, and 8.4%, respectively. There are two main reasons for this: (i) the reaction of IO − produced in the system with humic acid (HA) inhibits the further conversion of IO − to ; (ii) both HA and I- in the system can react with PDS, resulting in a reduction in the oxidation rate of I − . Formation of I-DBPs by Fe (II)/PDS process in real water was evaluated. I-DBPs generation in various reaction conditions was examined. Existence of HA showed apparent inhibition on IO 3 − generation.
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MOLECULES
·
2025
·Vol. 30
·期 11
·2331
·
IF 4.6
Ajeesh Kumar Somakumar,Ivo Romet,Agnieszka Grabias,Marcin Kruk,Shusaku Hayama,Damian Wlodarczyk,Justyna Barzowska,Yadhu Krishnan Edathumkandy,Eduard Feldbach,Puxian Xiong,Yaroslav Zhydachevskyy,Monika Trzaskowska,Hanka Przybylinska,Andrzej Suchocki
An extensive experimental study of trivalent iron (Fe3+) ions in orthorhombic lithium gallate nanocrystals was undertaken. Various spectroscopic methods, such as Raman spectroscopy, extended X-ray absorption fine structure, the Mössbauer effect, electron paramagnetic resonance, photoluminescence, thermoluminescence, and cathodoluminescence were used to investigate the synthesized phosphor. This study revealed the existence of multiple Fe3+sites, out of which the tetrahedral sites are preferentially occupied. Extensive optical studies showed that the Fe3+doped lithium gallate phosphor is a promising candidate for various luminescence and thermoluminescence-related applications in the near-infrared regime.
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JOURNAL OF MATERIALS SCIENCE-MATERIALS IN ELECTRONICS
·
2013
·Vol. 24
·期 8
·3095-3100
·
IF 1.486
Gao Feng,Zhang Jing,Song Hongzhang,Qin Zhen,Yang Delin,Hu Xing
The influence of Fe doping on the lattice structure and thermoelectric properties of GdBaCo 2− x
Fe
x
O 5+ δ
( x = 0.0, 0.2, 0.4, 0.6, 0.8, 1.0) ceramics was studied from room temperature to 525 K. The results show that presence of Fe will increase both electrical resistivity and Seebeck coefficients of the samples. Due to the lattice misfit and carrier concentration reduction caused by Fe, the thermal conductivity of the sample decreases. The activation energy of conductivity is larger than that of thermopower calculated in the semiconductive region, which means that the conduction mechanism may be determined as a small polaron hopping model. The optimum Fe doping amount is x = 0.6, which results in a ZT value 0.02 at 373 K.
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CHEMICAL ENGINEERING JOURNAL
·
2021
·
IF 13.273
Ting Yang,Shisuo Fan,Yang Li,Qi Zhou
A high-efficient iron-based heterogeneous catalyst is desired to active peroxymonosulfate (PMS). Due to a large catalytic contribution of atomically dispersed Fe-N x sites, single-atom iron–nitrogen-carbon catalysts exhibit superior performance in the catalytic activation of PMS. Herein, a sequence of Fe-N-C SACs with atomically dispersed Fe-N x sites, Fe SA -N-C and Fe SA -N/C, were prepared from Fe-doped ZIF-8 and FePc@ZIF-8, respectively. Single-atom Fe-N x sites were confirmed to be the main active sites for PMS activation. Fe SA -N/C-20 with a higher density of Fe-N x sites exhibited superior catalytic performance to N/C, Fe SA -N-C, Fe SA -N/C-15, and Fe SA -N/C-25 for BPA degradation. Integrated with chemical quenching experiments, electron spin resonance (ESR), in-situ Raman spectra, and electrochemical analysis, a nonradical pathway was demonstrated to dominate the degradation of BPA in the PMS + Fe SA -N/C-20 system. More importantly, the nature of this nonradical pathway was found to be an electron-transfer regime instead of a high-valent iron or singlet oxygenation process. The BPA was adsorbed onto the Fe-N x site by a “donor–acceptor complex” mechanism to form a nonradical PMS* intermediate during the process. Benefiting from this mechanism, the PMS + Fe SA -N/C-20 system showed wide pH adaptation and high resistance to inorganic anions.
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CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Lei Su,Yifan Li,Zhenkai Wang,Yao-Yin Lou,Qi-Zheng Zheng,Zhangxiong Wu,Sheng-Peng Sun
Iron-based catalysts are widely used in peroxysulfate-based AOPs but suffering from low catalytic performance at neutral pH conditions, which limits the application in groundwater remediation. Herein, this study investigated the efficacy, mechanism and long-term durability of Fe-doped nitrogen carbon (Fe@NC) armor catalysts toward peroxysulfate activation for the degradation of anthropogenic phenolics (APs) in groundwater matrices. The results showed that nonradical activation of Oxone (i.e., HSO 5 – ) was obtained over the as-prepared Fe-3 % @NC-700 catalyst, high-valent Fe species ( Fe(IV) O) and 1 O 2 were identified as the dominant reactive species for the efficient degradation of APs by experiments and density functional theory (DFT) calculations. Notably, the DFT results indicated that HSO 5 – was favorably adsorbed on the Fe atoms owing to the electrostatic interaction, which transformed exothermically into SO 4 2– and 1 O 2 over Fe 3 C, accompanied by the generation of Fe(IV) O. Additionally, the Fe-3 % @NC-700 catalyst displayed long-term activity for in situ activation of Oxone in groundwater matrices without pH adjustment, resulting in ΔAPs: ΔOxone stoichiometry efficiencies at 4.2–5.0 % . Wheat seeds germination tests revealed that the biotoxicity of the treated water was reduced notably by the present catalytic system, which holds large potential application in treatment of APs-contaminated groundwater.
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Journal of Materials Chemistry A
·
2025
·
IF 9.5
Hui Wang,Xuefeng Zhang,Xiangfeng Wu,Yewei Kang,Yirui Huang,Zhaoye Zhao,Ziyan Li,Tingting Zhou,Junchuan Wang,Wei Zhu,Chengsi Pan
Bimetallic iron-based metal organic frameworks (MFe-MOFs) exhibit promising photocatalytic properties but face challenges typical of pristine MOFs, including low photoresponsive activity, inadequate band gap regulation, and weak photoconductivity. Here, we designed porphyrin-based COFs (TpPAM-COFs) to serve as a shell grown on NH2-Fe-MIL-101 nanoparticles (NPs) using an in situ solvothermal approach. Subsequently, a ligand-anchoring full-range metallization process was applied to introduce hetero metal ions throughout the core–shell composites, establishing a type-II scheme heterojunction (Fe/Cu-M@PC-Cu) via covalent bonding between NH2-Fe/Cu-MIL-101 and Cu-TpPAM-COFs. The Cu-TpPAM-COF shell, with broad light absorption range, enhanced the generation of photogenerated electrons, facilitating the reduction of Cu2+ and Fe3+ within the Fe/Cu-M@PC-Cu heterojunction and promoting the regeneration of Cu+ and Fe2+ Fenton active sites. Moreover, rapid electron transfer between Fe3+ and Cu+ centers amplified the Fe3+/Fe2+ redox cycle, accelerating the catalytic decomposition of H2O2 and increasing ·OH radical production. Additionally, the optimized bandgap structure of Cu-TpPAM-COFs enhanced the oxidation capacity, as evidenced by the Fe/Cu-M@PC-Cu composite achieving exceptional photo-Fenton catalytic efficiency with 92.7% tetracycline hydrochloride (TCH) degradation in 35 minutes, surpassing that of most reported similar catalysts. Furthermore, the composite showed excellent stability, with only an 11.9% loss in photo-Fenton degradation efficiency after 8 cycles, highlighting its great potential for addressing challenging environmental pollutants.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2024
·
IF 20.2
Beizhao Chen,Meng Zhang,Li Wang,Li Li,Qi Han,Xun Liu,Mengxia Wang,Bei Liu,Yi Jiang,Zhongying Wang
The singlet oxygen ( 1 O 2 )-based nonradical AOP process, realized in carbon materials after nitrogen and metal doping, has drawn much attention in recent years. However, the exclusive generation of 1 O 2 in the specialized two-dimensional (2D) catalytic membranes and the associated contaminant degradation mechanisms remain unclear. Herein, a Fe-doped crystalline carbon nitride (Fe-CCN) material without additional nitrogen doping was developed to preferentially initiate 1 O 2 -based nanoconfined oxidation of organic pollutants in the 2D Fe-CCN membrane/PMS system. Density functional theory calculation revealed that the Fe-O-N configuration formed after Fe doping altered the electronic structure of Fe centers, enhancing PMS adsorption and promoting the thermodynamically favorable generation of the –O* intermediate, leading to fast and highly selective 1 O 2 generation. EPR characterization and ROS quenching experiment also confirmed that the Fe-CCN activated PMS, generating nearly 100 % 1 O 2 . The Fe-CCN membrane/PMS system exhibited excellent resistance to natural organic matter (NOM) interference and dramatically increased Bisphenol A (BPA) degradation kinetics, approximately 590 times faster than in conventional batch systems. Enhanced 1 O 2 exposure concentration within the Fe-CCN membrane nanochannels was supported by EPR data and 1 O 2 exposure simulations. Furthermore, The Fe-CCN membrane/PMS system showed wide pH tolerance, excellent pollutant degradation performance, and high stability. This work underscores the practical significance of 1 O 2 -based oxidation reactions in membrane-confined AOPs for the rapid and efficient removal of organic contaminants from water.
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ENVIRONMENTAL RESEARCH
·
2024
·
IF 7.7
Bin Nie,Haojun Dong,Jincan Yan,Shengyu Zhang,Shuang Zhong
The activation of peroxymonosulfate (PMS) by heterogeneous catalysts presents an exciting but challenging strategy for degrading persistent organic pollutants in water. Iron oxychloride (FeOCl) is considered a promising heterogeneous catalyst due to its unique oxygen bridge structure, which could render it more active by facilitating the iron valence transitions between Fe(II) and Fe(III). However, the limited Fe(II)/Fe(III) conversion cycle rate hinders its catalytic activity, leading to unsatisfactory PMS activations in practical applications. Herein, we demonstrated the performance and the mechanistic pathway of enhanced FeOCl (CNFeOCl) catalytic activation using a graphitic carbon nitride (g-C 3 N 4 ) with a unique electronic structure as a carrier employing 2,4-dichlorophenol (2,4-DCP) as a representative pollutant. The CNFeOCl/PMS system achieved complete degradation of 2,4-DCP (30 mg/L) in a short time (<5 min), whereas the FeOCl/PMS system degraded only 35.98% under the same conditions. The high 2,4-DCP degradation rate of CNFeOCl was due to its improved Fe(II)/Fe(III) ratio (34.34%/40.03%), increased specific surface area (30.32 m 2 /g), and reduced charge-transfer resistance. Combining a series of characterizations, electron spin resonance (ESR) detection, and quenching experiments, the investigations elucidated the enhanced catalytic activation mechanism of CNFeOCl which includes dominant reactive oxygen species (ROS) generation and some key factors that generally affected the efficiency of oxidative degradation. We believe this study offers new insights into the intrinsic role of g-C 3 N 4 supported FeOCl for PMS activation and provides theoretical support to guide the rational design for developing efficient iron-based catalysts toward heterogeneous catalysis.
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JOURNAL OF HAZARDOUS MATERIALS
·
2025
·
IF 11.3
Renjie Pan,Zongchen Li,Tian-Yang Zhang,Qi Fu,Zheng-Xiong Zheng,Jun Shi,Jian Lu,Chen-Yan Hu,Yu-Lin Tang,Mohamed Gamal El-Din,Bin Xu
Peracetic acid-based advanced oxidation processes (PAA–AOPs), which generate various reactive radicals, have garnered substantial attention for degradation emerging contaminants (ECs). However, nonselective radical-based PAA–AOPs often suffer from interference by water matrix components, causing low contaminants removal efficiency. This study explores the use of amino-(NH 2 )-functionalized metal–organic frameworks (MIL-101(Fe)-NH 2 ) as heterogeneous catalysts for PAA activation, enabling the generation of high-valent iron- (Fe)–oxo species (Fe(IV)) capable of efficiently degrading ECs (80 −100 %, within 30 min). The Fe(II) clusters in MIL-101(Fe)-NH 2 , modulated by electron-donating −NH 2 groups, play a pivotal role in Fe(IV) generation. Scavenger and probe experiments confirmed Fe(IV) as the primary reactive species responsible for ECs degradation. Density functional theory calculations demonstrated that the four-electron transfer to generate Fe(IV) has lower free energy than the two-electron transfer to generate organic radicals (e.g., CH 3 COO • and CH 3 C(O)OO • ). Furthermore, thermodynamically unfavorable CH 3 COO • desorption further promotes Fe(IV) generation. The PAA/MIL-101(Fe)-NH 2 system efficiently degraded SMX ( k app = 121.2 −287.2 M −1 s −1 ) and other ECs ( k app = 40 −432 M −1 s −1 ) with minimal interference from water matrix components and excellent reusability. This study demonstrates that MIL-101(Fe)-NH 2 is a robust catalyst for PAA activation and provides a novel approach for selectively generating Fe(IV) for ECs degradation.
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WATER RESEARCH
·
2024
·
IF 11.4
Xuecong Qian,Shilong Wang,Haijun Cheng,Luwei Li,Yun Liu,Jinhao Duan,Da Wang,Jun Ma
Fe(II) and Mn(II) are abundant in groundwater and require operationally simple and efficient method to remove in drinking water treatment. The rapid oxidation of Mn(II) is essential in water treatment. This study investigates the efficiency of Mn(II) oxidation by free chlorine in the presence of Fe(II). The results demonstrate that the presence of Fe(II) significantly accelerates the oxidation rate of Mn(II) by free chlorine under neutral and alkaline conditions. The rapid oxidation of Fe(II) by free chlorine and the presence of Mn(II) promote the formation of in situ Mn(II)-doped ferrihydrite. Kinetic modeling and characterization of Fe(III) oxides confirm that the heterogeneous catalytic effect of the Mn(II)-doped ferrihydrite, rather than manganese oxides or their coupled catalytic effect, is responsible for the enhanced oxidation rates. The doped Mn(II) substitutes the tetrahedral Fe(III) ions in the ferrihydrite, introducing additional negative charges at the doped sites. The increased charge enhances Mn(II) adsorption and lowers its redox potential, thereby accelerating Mn(II) oxidation rate through direct electron transfer with adjacent free chlorine. Additionally, the lepidocrocite formed by the reaction between Fe(II) and dissolved oxygen significantly impedes the catalytic performance. These findings provide new insights into the catalytic co-oxidation mechanism of Fe(II) and Mn(II), and help the optimization of water treatment engineering practices.
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Small
·
2024
·
IF 13
Feng Li,Shiyuan Xu,Xueru Zhao,Guorui Ma,Zhulin Niu,Xing Zhong,Jing Li
Fe-doped NiOOH electrocatalysts have attracted wide interest for the exceptional oxygen evolution reaction (OER) performance, but the precise role of Fe doping on the improved intrinsic activity remains unclear. Herein, the molecular probe technique combined with density functional theory calculation is used to reveal the influence of the Fe atom on the rate-determining step of the OER reaction, where the pre-catalyst of hierarchical self-supporting NiFe layered double hydroxide [LDH] nanosheets equipped on nickel foam (NiFe LDH/NF) is generated via a facile and industrially well-matched one-pot corrosion method. The physical characterization results reveal the reconstruction of NiFe LDH into Fe-doped NiOOH for promoted OER, which has a lower OH* adsorption energy with fast subsequent steps that help in obtaining an improved charge injection efficiency compared to NiOOH. In addition, more exposed electroactive species and facile delivery of mass/electron inside the catalytic procedure actually have a high-quality contribution to the outstanding catalytic activity. Therefore, the NiFe LDH 36 /NF electrocatalyst provides high catalytic activities of 241 and 320 mV at 10 mA cm −2 toward the OER and overall water-splitting in 1 m KOH. This work provides a promising avenue for the rational design of durable self-supporting electrodes toward large-scale water splitting.
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