WATER AIR AND SOIL POLLUTION
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2024
·Vol. 235
·期 5
·1-17
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IF 3.8
Zhou Zhuyou,Ji Yufeng,Wang Yong,Liu Menghe,Xu Ying,Liu Ruijie,Yang Mingjie,Zou Congyang
In this study, the carbon-doped bimetallic organic framework C 60 /MIL-101(Fe,Cu) catalyst was prepared for the first time via solvothermal synthesis method. The catalysts were characterized using X-ray diffraction (XRD), Fourier transform infrared spectroscopy (FT-IR), and a series of other instruments. At the same time, methylene blue (MB) was used as the target degradation material to investigate the catalytic performance of H 2 O 2 for MB degradation under visible light. The degradation experiment showed that the removal rate of C 60 /MIL-101(Fe,Cu) to MB reached 99.2% within 80 min. Furthermore, cyclic experiments demonstrated good stability and reusability of the catalyst. Finally, the degradation mechanism of the reaction was deduced by quenching experiment, UV–vis diffuse reflection and mott-Schottky plots. The results show that hydroxyl radical (·OH) and superoxide radical (·O 2 − ) play a major role in the degradation of MB during photo-Fenton process.
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CHEMOSPHERE
·
2024
·
IF 8.1
Lei Wu,Yuan Gao,Siwen Qiu,Zixuan Hu,Changbo Liu,Changsheng Yue,Jun Zhou
The porous and defective structure of biochar (BC) can accelerate surface electron transfer, promote the generation of more reactive oxygen species (ROS) by persulfate (PS), and effectively degrade organic pollutants in the soil. Electron transfer is a crucial link in this process, directly determining its oxidative degradation efficiency. In this study, using a novel strategy of enhancing electron transfer on the surface of BC by loading iron, three Fe-loaded BC activators (Fe-FeO x @BC, Fe 2 O 3 @BC and Fe 3 O 4 @BC) were synthesized to support the oxidative remediation of benzo( a )pyrene (BaP, Model compound of PAHs)-contaminated soil by PS. The results showed that Fe 3 O 4 @BC supported PS oxidation and remediation of BaP-contaminated soil had the best effect among the three BC-based activators, and the reuse effect was stable. Under the conditions of Fe 3 O 4 @BC addition of 1.00 wt%, PS addition of 0.75 wt%, reaction temperature of 35 °C, and solid-liquid ratio of 1:2.5, the removal rate of BaP in the soil reached the maximum of 93.84% at 120 min, and the soil toxicity was significantly reduced after remediation. The defect structure, conductive magnetic particles, and active functional groups on the surface of Fe 3 O 4 @BC were the key factors for activating PS to degrade BaP. With the combined action of the free radical pathway caused by ROS and the non-free radical pathway caused by 1 O 2 , electron transfer, and active functional groups, BaP was degraded to small molecules such as CO 2 and H 2 O, achieving rapid and efficient remediation of organic contaminated soil.
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高影响因子
JOURNAL OF ENVIRONMENTAL MANAGEMENT
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2025
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IF 8.4
Renhua Zheng,YingHong Huang,Beiqing Wang,DiWen Jia,Jingle Chen,Haichang Guo,Ting Wang
To enhance the removal efficiency of refractory organic pollutants in high-salinity wastewater, three types of advanced oxidation processes (AOPs), i.e., photocatalysis, Fenton catalysis, and photocatalysis coupled with Fenton catalysis, were used to degrade tetracycline (TC) and rhodamine B (RhB) in sodium sulfate solution (15 %). Different Fe-doped TiO 2 -loaded reduced graphene oxide materials prepared by adsorption-layer nanoreactor synthesis were employed as catalysts in AOPs. The differences in the mechanism of the three types of AOPs for TC and RhB degradation were explored. The results showed that Fe doping can improve the degradation performance of catalysts in these AOPs, both in freshwater and saline water. Salt ions strongly inhibited pollutant degradation in both the photocatalytic degradation and Fenton catalysis process. The synergistic photocatalytic Fenton system can resist the interference of salt ions, thus effectively degrading both TC and RhB. The removal rates of TC and RhB reached 75.21 % and 84.11 % in 3 h, respectively. In the combined photocatalytic Fenton system, the active species were mainly photogenerated holes (h + ), but some ·OH and ·O 2 − radicals also participated in the decomposition of pollutants. For the two molecules, density functional theory calculations revealed the different atomic sites that were attacked by h + and ·OH. Salt ions surrounded electrophilic atoms with large f − values in the molecule, thus hindering the h + attack on these atoms. In contrast, salt ions did not affect the atom with the largest f 0 . More h + and ·OH were generated in the photocatalytic Fenton system, effectively reducing the interference of salt ions with pollutant degradation.
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CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Lianzhong Shen,Lin Wang,Yu Ye,Zhouwei Li,Qizhou Dai
The fabrication of various defects on the surface of metal single-atom catalysts can improve their electrochemical CO 2 reduction reaction (CO 2 RR) ability, and the current mainstream research focuses on the defect modification of heteroatom doping, while there are fewer studies on intrinsic defects on carbon substrates. Herein, a series of catalysts with both Fe-N 4 sites and intrinsic defects were synthesized on the ZIF-8 surface by pyrolytic etching at a suitable temperature under ammonia atmosphere. Electrochemical tests in an H-cell showed that the catalyst achieved CO Faradaic efficiency (FE CO ) of 96.9 % and CO partial current density (J CO ) of 9.088 mA cm −2 at −0.6 V. Through further studies, we introduced a “585” ring structure to describe these intrinsic defects and found that these intrinsic defects on the carbon-based surface can act as active sites to promote CO 2 RR along with the Fe-N 4 sites. This work provides a reference for the study of intrinsic defect-modified single atomic materials.
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JOURNAL OF POLYMERS AND THE ENVIRONMENT
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2024
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IF 4.7
Zhang Xutao,Chen Weiliang,Li Xiangqi
Excellent photocatalytic performance and recyclability are crucial for the long-term use of the photocatalyst. In this study, 5 mol% Fe doped zinc oxide (ZF5), was freeze-dried with bacterial cellulose (BC)/sodium alginate (SA) solution to fabricate a novel composite aerogel capable of degrading methylene blue (MB) under visible light. Ca 2+ crosslinking and hydrophobic modifications were adopted to strengthen the aerogel skeleton and enhance the cycling photocatalytic activity, meanwhile, making the aerogel floatable persistently. The influences of pH, ZF5 dosage, and initial solution concentration on MB degradation were investigated. Benefiting from the synergy between the components and the combined modification, the optimum composite aerogel exhibits photocatalytic efficiency of up to 97.4% at an initial MB concentration of 20 mg/L within an irradiation time of 80 min. In addition, it exhibits a degradation efficiency of 79.7% even after 8 cycles, showing great potential in visible-light-driven degradation of MB.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2024
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IF 8.1
Bo Qin,Bin Wang,Jiang Li,Tao Wang,Xiaoyi Xu,Li'an Hou
Non-radical catalytic oxidation processes can eliminate refractory pollutants from wastewater containing complex substrates such as dissolved organic matter, but the production of selective non-radicals is challenging during the activation of peroxymonosulfate (PMS). Herein, a novel magnetic carbon-based catalyst (Fe 3 O 4 @CD-8, where 8 represents an annealing temperature of 800 ℃) with N and Fe species as catalytic active sites was fabricated to remediate sulfamethoxazole (SMX)-containing water. It showed excellent SMX removal efficiency and facilitated singlet oxygen ( 1 O 2 ) production. The characterization results revealed that Fe 3 O 4 @CD-8 had a microscopically hierarchical pore structure and an overall core–shell-like structure. Due to its large specific surface area, N-containing species, and Fe nanoparticles, 0.1 g/L Fe 3 O 4 @CD-8 removed almost 100% SMX (24 min) and achieved a 44.1% mineralization (40 min) efficiency in the presence of 0.5 mM PMS. This catalytic system also maintained its removal performance in the presence of inorganic anions and humic acids and over a wide pH range of 3–11, showing good tolerance to various environmental factors. 1 O 2 was confirmed to be the predominant active species for SMX degradation using the Fe 3 O 4 @CD-8/PMS system. Density functional theory (DFT) calculations, intermediate monitoring, and toxicity evaluation demonstrated that SMX was transformed into low-toxicity molecules and completely mineralized into CO 2 and H 2 O. The addition of Fe nanoparticles enhanced PMS adsorption and facilitated the Fe(III)/Fe(II) redox cycle to accelerate the activation of PMS. This study provides new insights and strategies for the controlled production of non-radicals for remediating antibiotic-containing wastewater.
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2024
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IF 20.2
Hui Li,Li Du,Ying Zhang,Xu Liu,Shuang Li,Chun Cheng Yang,Qing Jiang
The rational construction of high-efficiency transition metal phosphides catalysts for hydrogen evolution reaction (HER) is crucial since their sluggish kinetics of water dissociation remain severe barriers for HER performance. The theoretical calculations indicate a unique adsorption-diffusion-decomposition mechanism for H 2 O molecules on CoP (111) surface. Herein, Fe could decrease H 2 O decomposition barrier energies and increase the amount of active sites, along with Cr could accelerate H 2 O adsorption, diffusion and increase the conductivity of the reaction surface. Aided by this mechanism, a self-supported electrode of Cr and Fe dual-doped CoP nanorod arrays grown on nickel foam was prepared. The electrode only requires an overpotential of 27 mV at 10 mA cm −2 for alkaline HER with excellent durability for 400 h. Moreover, the catalyst presents only 1.505 V at 10 mA cm −2 for alkaline water electrolysis. This work provides an in-depth understanding on catalytic mechanism of CoP-based materials.
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CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Xinqi Wang,Lili Zhang,Ning Wang,Shaohui Sun,Hao Wan,Renzhi Ma,Wei Ma
Conjugated metal polyphthalocyanine (MPPc) organic skeletons, a kind of novel porous materials containing inherent M−N 4 highly active sites, are of great significance for oxygen reduction reaction (ORR). Herein, bimetallic Fe-Co phthalocyanine covalent polymers (denoted as FeCoPPc) were prepared as ORR electrocatalysts through a solvothermal process and subsequent oxidation treatment. Meanwhile, the effect of axial oxygen-containing ligands of metal centers on the catalytic kinetic processes was also investigated. Benefiting from the highly exposed bimetal active sites and the finely designed ligand structure, FeCoPPc with optimized Fe/Co ratio and ClO 3 − coordination (Fe 0.9 Co 0.1 PPc-ClO 3 ) displayed an outstanding ORR electrocatalytic activity and superior durability compared to 20 % Pt/C, manifested by an onset potential of 0.986 V vs. reversible hydrogen electrode (RHE) and a half-wave potential of 0.923 V vs. RHE in a 0.1 M KOH solution. This work may guide the rational design of high-performance electrocatalysts to regulate the catalytic activity.
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CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Shuya Zhang,Qiming Chen,Qianqiao Wang,Xinyu Luo,Mingjun Cen,Wenchao Peng,Yang Li,Qicheng Zhang,Xiaobin Fan
The electrochemical oxygen reduction reaction (ORR) plays a crucial role in air-breathing energy conversion systems. However, its kinetics are constrained by a multistep proton-coupled electron transfer process, wherein the adsorption of the OOH* introduces high energy barriers. Herein, we present N-doped carbon-supported ultrafine V-incorporated Fe 3 C nanoparticles (V-Fe 3 C@NC) featuring abundant Fe coupling with V, serving as reaction sites for efficient ORR. Experimental characterizations confirm the incorporation of V species leads to a significant enhancement in ORR kinetics. The prepared V-Fe 3 C@NC electrocatalyst demonstrates exceptional ORR activity with a half-wave potential of 0.91 V. Density functional theory calculations elucidate that the synergy between Fe and V sites facilitates direct O–O bond breakage, circumventing the formation of the OOH* and resulting in lower ORR energy barriers. Moreover, the aluminum-air (Al-air) batteries derived from ultrafine V-Fe 3 C@NC nanoparticles display outstanding performance with a high open-circuit voltage of 1.92 V and a large specific capacity of 2309 mAh g −1 under the air environment. The elucidation and understanding of synergy in dual reaction sites present a novel approach for the rational design of supported metal nanoparticle electrocatalysts for energy-related applications.
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CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Yan Sun,Zhicheng Wang,Xiaohui Wu,Wen-Da Oh,Mingjie Huang,Tao Zhou
Molecular oxygen (O 2 ), a reactive oxygen species precursor, has great potential for water purification, but its spin-forbidden resistance hinders its direct involvement in the redox reactions of organic compounds under mild ambient conditions. In this study, a facile strategy was employed to synthesize sulfide-modified Fe-Cu bimetallic catalysts (FeCu-S) to enhance the activation efficiency of O 2 . The results showed that the FeCu-S material exhibited a tenfold increase in O 2 activation compared to that of the control group, primarily attributed to the increased specific surface area of the catalysts with an optimized Fe/Cu site distribution and promoted generation of Cu-containing crystalline phases (e. g., CuFeS 2 and CuO) to significantly enhanced the oxygen storage capacity. Moreover, such Cu-containing crystalline phases strengthened surface electron transfer, thus remarkably promoting the selective generation of singlet oxygen ( 1 O 2 ) for sulfamethoxazole (SMX) degradation. The FeCu-S/O 2 system maintained high activity after the fifth recycle with stable reaction pH and negligible leaching of Cu and Fe ions, also exhibited great performance in the advanced treatment of the real biological effluent and ultrafiltration effluent from landfill leachate, confirming its great potential for practical water purification applications.
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JOURNAL OF FOOD COMPOSITION AND ANALYSIS
·
2024
·
IF 4
Kai Zhang,Dan Hou,Dongping Wu,Yanxia Li,Xuemei He,Tingting Sun,Jianhua Xiong,Xiaoning Liao
Accurate detection of benzimidazole pesticide thiophanate-methyl (TM) is of vital importance due to its harm to environmental safety and human health. Herein, for the first time, we developed a sensitive nonenzymatic electrochemical sensor for TM detection based on multiwall carbon nanotubes (MWCNTs) functionalized bimetallic iron−copper organic frameworks (Fe/Cu MOF). The synthesized nanocomposites showed excellent electro-oxidation ability to TM owing to the synergistic effect between MWCNTs and Fe/Cu MOF. Fe/Cu MOF enhanced the specific surface area for MWCNTs and MWCNTs improved the conductivity for Fe/Cu MOF, which resulted in a nanocomposite with abundant catalytical active sites and superior conductivity, greatly amplifying the detection signal for TM. Under optimized conditions, the proposed sensor based on the composite presented a wide linearity from 0.3 nM to 200 nM which is wider than that of currently reported methods and a very low detection limit (LOD) of 0.1 nM far lower than the maximum residue levels (MRLs) enacted worldwide. Furthermore, the sensor showed good reproducibility, long-term stability and high anti-interference. Moreover, the sensor can be successfully employed for the determination of TM in apple and cucumber with good recoveries (80.96 %–105. 5 %), highlighting its excellent potential as an alternative to traditional techniques.
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CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Yutong Wang,Longhui Wang,Xinyan Yu,Xianbao Shen,Lijie Xu,Ying Zhang,Jiangtao Shi,Lu Gan
In this study, magnetic biochar bead ((AB + MIL-88)-C) was prepared by pyrolyzing MIL-88B(Fe) loaded alginate beads. The Fenton-like activity of (AB + MIL-88)-C was then investigated through activating peroxymonosulfate (PMS) for bisphenol A (BPA) degradation in water. The results demonstrated that (AB + MIL-88)-C exhibited superior BPA degradation capability (k = 0.160 min −1 ) than pristine MIL-88B(Fe) and alginate bead derived catalysts (k = 0.089 & 0.008 min −1 ), in which non-radical mechanisms including singlet oxygen ( 1 O 2 ) and electron transfer process contributed over 98 % of BPA degradation. Moreover, PMS consumption rate by (AB + MIL-88)-C during whole BPA degradation process was very low. Consequently, the non-radical pathway dominated oxidation system with low PMS consumption rate could maintain its activity regardless of the fluctuation of environmental parameters and water matrices. Besides, it was further demonstrated that the reaction system exhibited high degradation selectivity in which those pollutants with electron donating groups were more inclined to be degraded. Meanwhile, the degradation rate (ln k ) of respective pollutant in the reaction system correlated well (R 2 = 0.97) with their highest occupied molecular orbital position. This study provides a strategy for the development of non-radical oxidation systems with high pollutant degradation efficiency, stability and selectivity.
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