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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高影响因子
Journal of Environmental Chemical Engineering
·
2025
·
IF 7.2
Yibing Feng,Kun Qiao,Xiaohan Jiang,Huiling Ji,Jiang Meng,Jigang Wang
A photocatalysis–self-Fenton system (PSFs) offers a viable solution to the continuous hydrogen peroxide (H 2 O 2 ) dosing and insufficient Fe 2 + regeneration challenges in conventional Fenton chemistry. An oxygen-doped g-C 3 N 4 microrod (OCNT)-based PSFs was synthesized via a facile oxalic acid-mediated supramolecular self-assembly route, enabling efficient pollutant degradation. In situ H 2 O 2 production was achieved through a two-electron oxygen reduction reaction (2e − -ORR), with photogenerated electrons accelerating Fe 2+ /Fe 3+ cycling and enhancing H 2 O 2 utilization. The system exhibited an apparent rate constant of 0.071 min −1 for tetracycline (TC) removal, 12.2- and 4.2-fold higher than pristine g-C 3 N 4 and a photo-Fenton system, respectively. Density functional theory (DFT) calculations and experimental results indicated that oxygen heteroatom doping increased the molecular dipole moment and optimized the band structure, while the one-dimensional microrod morphology exposed abundant active sites. These synergistic effects facilitated charge-carrier separation, improved interfacial mass transfer, and promoted the two-electron oxygen-reduction pathway, thereby accelerating Fe 2+ /Fe 3+ cycling and hole oxidation. The platform demonstrated broad pH adaptability, strong anti-interference capability, and long-term operational stability. This work provides an effective strategy for on-site H 2 O 2 generation and utilization in photocatalytic–Fenton systems for the degradation of organic contaminants.
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JOURNAL OF ENVIRONMENTAL MANAGEMENT
·
2025
·
IF 8.4
Yaxing Bai,Xuefeng Hu,Huixian Du,Meng Gao,Zilong Li,Yuhuan Fei
To expand the utilization of discarded walnut shells and enhance the photocatalytic activity of graphitic carbon nitride(g-C 3 N 4 ), the carbon-rich graphitic carbon nitride anchored with Fe sites (FeW-CN) was synthesized via a walnut shell-based biochar-assisted strategy. Unlike the direct thermal copolymerization of melamine for g-C 3 N 4 , the iron-loaded walnut shell-based biochar (FeW) was first synthesized, followed by thermal copolymerization of melamine with FeW to form FeW-CN. The C substitution on the triazine ring enhanced the light absorption and electron migration for FeW-CN. And the Fe sites interacting with N-(C) 3 further improved the migration and the utilization rate of photogenerated carriers. During the degradation of 2-Mercaptobenzothiazole, FeW-CN showed excellent photocatalytic performance and stability compared with g-C 3 N 4 . Moreover, FeW-CN maintained excellent photocatalytic performance in river water. Combination of electron paramagnetic resonance with active species quenching experiments, the synergistic mechanism of singlet oxygen, holes, and superoxide radicals was confirmed in the FeW-CN system. Compared to g-C 3 N 4 , the Fe sites and C substitution enhanced the production of singlet oxygen.
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Surfaces and Interfaces
·
2025
·
IF 6.3
Huixiao Duo,Yan Hao,Jiayuan Yue,Qianxing Lu,Yuetan Dong,Ke Chen,Yanyan Kong,Shushu Ding,Qing Zhu,Jiejia Li
The extensive use of non-steroidal anti-inflammatory drugs (NSAIDs), particularly diclofenac (DIC) and indomethacin (IND), poses escalating ecological and health risks due to incomplete degradation in water systems. Conventional remediation methods face challenges including low efficiency and toxic intermediate generation. Herein, we developed a novel MXene/Zr-Fe-MOF-derived carbon heterostructure (MXene/Zr-Fe@C) featuring bimetallic Zr/Fe active sites anchored on MXene nanosheets. The heterostructure design of MXene/Zr-Fe@C enables exceptional synergistic adsorption of NSAIDs from aqueous environments. Systematic adsorption experiments in single-component (DIC or IND) and binary (DIC+IND) systems revealed competitive adsorption behaviors and synergistic effects. MXene/Zr-Fe@C demonstrated satisfactory adsorption capacities (277.7 mg/g for DIC and 238.09 mg/g for IND, surpassing conventional adsorbents. These exceptional performances stem from the bimetallic site selectivity and synergistic domain interactions of MXene/Zr-Fe@C. The Zr/Fe@C provide selective coordination site, while MXene and carbon matrix promote the non-polar interaction with aromatic rings of NSAIDs. Remarkably, the composite exhibited excellent regenerability, retaining 83% of adsorption capacity after 54 regeneration cycles. Overall, the synergistic interfacial effects between MXene's conductive surfaces and ordered porosity of MOF-derived carbon enhance structural stability, efficient mass transfer and site accessibility. These findings establish MXene/Zr-Fe@C heterostructures as versatile platforms for NSAIDs remediation, providing foundational insights for sustainable water purification technologies addressing emerging pharmaceutical contamination challenges.
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APPLIED SURFACE SCIENCE
·
2020
·
IF 6.182
Chenrui Liu,Yun Liu,Zhi Dang,Shuai Zeng,Chengcheng Li
In this paper, a kind of novel core-shell structured heterogeneous photo-Fenton catalyst, boron-doped reduced graphene oxide wrapped Fe 3 O 4 (Fe 3 O 4 @B-rGO) composite, was successfully synthesized by heating the mixture of Borane-Tetrahydrofuran adduct and graphene oxide wrapped Fe 3 O 4 (Fe 3 O 4 @GO) under reflux conditions. The core-shell structure of the catalyst had been confirmed by X-ray diffraction (XRD), Raman spectroscopy, scanning electron microscopy (SEM), transmission electron microscopy (TEM), X-ray photo electron spectra (XPS), and electron energy loss spectrum (EELS). The experimental results for Bisphenol A (BPA) degradation demonstrated that the as-prepared catalyst exhibited much higher photo-Fenton catalytic activity than Fe 3 O 4 and reduced graphene oxide wrapped Fe 3 O 4 (Fe 3 O 4 @rGO). Additionally, Fe 3 O 4 @B-rGO with mass concentration of doped boron at 9.3% exhibited the optimum catalytic property, in which system the BPA degradation kinetic rate constant was almost 1.96 times and 1.82 times of that in the systems with Fe 3 O 4 and Fe 3 O 4 @rGO, respectively. Finally, the mechanism analyses verified that OH, O 2 − and h + were the main reaction species in this system, and photo-electron generated by boron doped reduce graphene oxide (B-rGO) can accelerate the redox between Fe(II) and Fe(III). The excellent photo-Fenton performance, stability and magnetic separation properties make it promising for the degradation of organic compounds in waste water under visible light.
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Carbon Neutralization
·
2022
·Vol. 1
·期 1
·49-58
·
IF 0
Xiao-Hao Liu,Wei-Hong Lai,Jian Peng,Yun Gao,Hang Zhang,Zhuo Yang,Xiang-Xi He,Zhe Hu,Li Li,Yun Qiao,Ming-Hong Wu,Hua-Kun Liu
Developing low-cost and high-voltage manganese (Mn)-based Na superionic conductor (NASICON) cathode materials have attracted extensive interest. The low capacity and cycling instability of Na 4 MnAl(PO 4 ) 3 (NMAP), however, limits its performance in sodium-ion batteries (SIBs). Herein, a binary Na 4 Mn 0.5 Fe 0.5 Al(PO 4 ) 3 (MNFAP) is fabricated to ease the structural instability and, in turn, deliver an improved reversible capacity of 102 mAh g −1 at 0.1 C and a high energy density of 287.7 Wh kg −1 . The synergistic interaction of Fe and Mn in Na 4 Mn 0.5 Fe 0.5 Al(PO 4 ) 3 /C composite leads to a one-phase solid-solution reaction mechanism with high structural reversibility. Theoretical calculations have also been performed to explain the upshifted voltage platform of both Fe 2+ /Fe 3+ and Mn 3+ /Mn 4+ redox potentials. The rational design of NASICON-type cathodes by regulating their composition with dual metal ions provides new perspectives for developing high-performance SIBs.
研究领域:
材料科学
·
电化学
·
能源存储
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JOURNAL OF ELECTRONIC MATERIALS
·
2023
·Vol. 52
·期 9
·5946-5954
·
IF 2.1
Lu Yuting,Bian Zhenglan,Chu Fenghong,Lu Jianwei,Hou Guoqiang,Hou Shili
In this paper, a hydrothermal strategy is reported for the synthesis of nitrogen-doped carbon dots (NCD) which used citric acid (CA) and urea as reactants with different pristine molar ratios of carbon/nitrogen atoms (C/N). The fluorescence emission wavelength of the aqueous solutions of NCD can be tuned from 462 to 546 nm under a single and uniform UV light excitation (365 nm). Through many characterization analysis methods, it is demonstrated that graphitic N and C=O extended the effective conjugation length which reduced the energy gap between the highest occupied molecular orbital (HUMO) and the lowest unoccupied molecular orbital (LUMO). This is considered to be responsible for the redshift and tunability of the fluorescence emission of NCDs with different C/N molar ratios. This will be useful for designing a synthetic strategy of long-wavelength fluorescence emission carbon dots (CDs) in a non-benzene ring precursor system. As a potential fluorescence sensor, the as-prepared NCDs can specifically detect Fe 3+ ions and Al 3+ ions in aqueous solutions. Additionally, the NCDs not only are nontoxic but also exhibit large and stable fluorescence intensity, indicating that they have broad potential application in the fields of sensors and optoelectronic devices.
研究领域:
材料科学
·
分析化学
·
生物传感
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JOURNAL OF HAZARDOUS MATERIALS
·
2023
·
IF 13.6
Tong Zhang,Yuan Chen,Tao Wang,Chang Liu,Dan He,Bin Liu,Yuanyuan Liu
Advanced oxidation processes are widely used to remove petroleum hydrocarbons from soil, but usually consume large quantities of ferrous and acidify the soil. This study tested an advanced oxidation approach based on percarbonate in laboratory experiments. It removed 88% petroleum hydrocarbons in soil with a pH increase from 8.2 to 10.2. ·OH and ·CO 3 - were the main reactive species, and degraded 41% and 37% PHCs from soil respectively. The o-dihydroxybenzene structure in catechin was found to reduce ferric to ferrous, and prolong the generation of ·OH from 120 s to over 1800 s. The petroleum hydrocarbons were degraded to intermediates including alkanes and olefins through hydrogen-abstraction by ·OH and ·CO 3 - , and by dimerization and β-scission of alkyl radicals. These intermediates were then oxidized to CO 2 and H 2 O by ·OH and ·CO 3 - . The main residual intermediates in the soil were low-molecular-weight n-alkanes and branched alkanes, and they were found to inhibit the growth of oats ( Avena sativa L. ) much less than the original petroleum hydrocarbons. These findings provide a fundamental basis for designing effective technologies which use percarbonate to remove organic pollutants .
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Nanoscale
·
2022
·Vol. 14
·期 18
·7055-7074
·
IF 8.307
Rutong Song,Jun Yao,Mei Yang,Zhongbin Ye,Zhuang Xie,Xiang Zeng
Water pollution control is one of the major challenges currently faced. With the development of photocatalytic technology, an increasing number of new and efficient catalysts have been developed, but most of the catalysts have limited light capture ability and catalytic degradation efficiency. Therefore, in this work, hydrogen peroxide was further introduced to establish a photo-Fenton system to improve the photocatalytic effect by constructing a Z-scheme, and the degradation ability of the catalyst was maximized. Moreover, we successfully adhered bismuth tungstate nanosheets onto the surface of a MIL-101(Fe) framework and changed the number of active sites with iron ions of different doping amounts. We found that the number of active sites in the photo-Fenton system does not increase linearly, but increases and decreases regularly, which is similar to the change in band structure after doping. In addition, the results of the radical scavenger experiment and electron paramagnetic resonance (EPR) revealed that both hydroxide radical (˙OH) and superoxide radical (˙O2−) participated in methylene blue (MB) degradation, of which ˙OH was the main active species for pollutant degradation. Based on high-performance liquid chromatography-mass spectrometry (HPLC-MS) analysis, the possible degradation pathways were proposed. We believed that this work will provide insights into the heterojunction photo-Fenton system.
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CHEMICAL ENGINEERING JOURNAL
·
2022
·
IF 16.744
Yanan Shang,Xinning Liu,Yanwei Li,Yue Gao,Baoyu Gao,Xing Xu,Qinyan Yue
The synthesis of a highly efficient and stable single atom catalyst (SAC) for peroxydisulfate (PDS) activation remains a challenge. Herein, a reconstructed iron single atom catalyst (Fe-SAC) with both abundant conjugated π-π sp 2 structured carbon and reactive Fe-N 4 sites was first reported to improve the decomposition of organics in PDS/SACs systems. Enhanced organics adsorption can be achieved by the conjugated π-π sp 2 structured carbon via π-π interaction to decrease the migration distance of reactive species to organic molecules. In addition, PDS tended to be attached onto the Fe-N 4 sites accompanied by the peroxymonosulfate (PMS) generation via S-O breakage of PDS, accelerating the generation of radicals. As a result, organics decomposition via PDS activation by reconstructed Fe-SAC was significantly higher (∼6 times) than the conventional Fe-SAC because of the synergistic effect of the resulting dual reaction sites. This work provides a new strategy to enhance the catalytic performances in PDS/SACs systems.
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Journal of Environmental Chemical Engineering
·
2023
·
IF 7.7
Yizhuang Wang,Bingbing Liu,Hu Sun,Yanfang Huang,Guihong Han
Bauxite residue (red mud) is a typical solid waste discharged from the aluminum metallurgy industry and can be considered as an alternative resource for the recovery of iron (Fe), aluminum (Al), and titanium (Ti). Acid leaching is an effective technique for the simultaneous extraction of valuable metals from red mud, whereas the leachate with various metals confronts the difficulty of metals separation. In this work, a selective separation and recovery of Fe, Al and Ti from red mud leachate by the preferential Fe-Ti iso precipitate flotation followed by a reduction-hydrolyzation process was proposed. In the iso precipitate flotation process, the cupferron was acted as an Fe-Ti synchronous chelation agent and hexadecyl trimethyl ammonium bromide (CTAB) was used as an anionic collector for the flotation separation of Fe-Ti chelate. The generated fine hydrophobic chelates are rapidly separated from solution by flotation with the assistance of CTAB, in which 99.3% Fe and 99.8% Ti were transferred into the flotation product, while 96.7% Al remained in the leachate, realizing the first separation of Al. Reduction-hydrolyzation was further conducted to separate Ti and Fe from the dissolving solution of the flotation product. Hydrolysis thermodynamic analysis indicated that the required hydrolysis pH range of Fe 2+ was much different from that of TiO 2+ and Ti 3+ . After selective reduction of Fe 3+ to Fe 2+ by KI, 99.8% Ti was concentrated in the residue while 94.8% Fe remained in the solution. Eventually, the comprehensive recoveries of Fe, Ti, and Al are 94.1%, 99.7%, and 96.7%, respectively.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2020
·
IF 16.683
Runliang Zhu,Yanping Zhu,Haiyang Xian,Lixia Yan,Haoyang Fu,Gangqiang Zhu,Yunfei Xi,Jianxi Zhu,Hongping He
The generation of Fe(II) from Fe(III) is the rate-limiting step in the heterogeneous Fenton reaction, and accelerating this step is critical for enhancing the reaction efficiency and also the subject of extensive studies. In this work, the oxidized multi-walled carbon nanotubes (CNTs) were coupled with ferrihydrite (Fh) to synthesize novel and highly efficient heterogeneous Fenton catalysts (CNTs/Fh). Interestingly, the calculated apparent rate constants by 3%CNTs/Fh could reach ∼7.1 times as high as that by Fh, well in agreement with the accelerated decomposition rate of H 2 O 2 , as well as the enhanced generation rate of Fe(II) and hydroxyl radicals in the CNTs/Fh system. The density functional theory calculations and the cyclic voltammograms curves both well indicated that the Fe(III)/Fe(II) redox cycling on CNTs/Fh could be significantly enhanced during the Fenton reaction, from both dynamic (accelerating the electron transfer from H 2 O 2 to Fh) and thermodynamic (lowering Fe(III)/Fe(II) redox potential) aspects.
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