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 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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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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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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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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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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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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