JOURNAL OF ENVIRONMENTAL MANAGEMENT
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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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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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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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APPLIED SURFACE SCIENCE
·
2022
·
IF 7.392
Jiamin Wei,Qing Wang,Mian He,Shuai Li,Yunan Zhang,Yang Yang,Shipeng Luo,Lianshe Fu,Xin Wang,Tinghai Yang
The development of highly efficient strategy to facilitate comprehensive charge transmission and effective spatial charge separation is expected as a promising approach to improve photocatalytic performance. Herein, the Fe(III) doping modified AgI/NH 2 -MIL-68(In/Fe) Z-scheme heterojunction (ANM-x composite) with unique internal and interfacial charge transmission performance was fabricated by a facile ion exchange precipitation method. The optimized ANM-50 composite exhibits the maximum photocatalytic activity for the degradation of tetracycline, which is about 9.54, 2.61 and 1.86 times higher than that of pure NH 2 -MIL-68In, NH 2 -MIL-68(In/Fe) and AgI, respectively. The characterization results displayed that Ag nanoparticles (NPs) were generated during the photocatalytic procedure, which not only served as a charge transfer-highway, but also reduced the charge flow energy barrier, thereby accelerating charge transfer efficiency and consolidating the stability of the Z-scheme heterojunction. Mechanism exploration reflected that the superior photocatalytic performance was associated with synergetic effect among the introduced Fe(III), constructed ANM Z-scheme heterojunction and the generated Ag NPs, which significantly expands visible light response range and promotes more effective internal and interfacial charge separation. This research not only designs an efficient photocatalyst for decomposing tetracycline, but also opens a new perspective for rational developing Z-scheme heterojunction with unique internal and interfacial charge flow steering.
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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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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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高影响因子
Nanoscale
·
2022
·Vol. 14
·期 18
·7055-7074
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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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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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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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FUEL
·
2024
·
IF 6.7
Guosheng Li,Yu Ding,Xiaohan Li,Kunhong Li,Xinrui Yin,Liang Zhao,Shenyong Ren,Chunming Xu,Baojian Shen
Regulation of electronic structure of metal active phase for catalysts has been known as efficient in promoting its catalytic activity; however, manipulating the activity of catalysts via controllable metal active phase electronic structure is still challenging. A non-equilibrium electronic structure Fe-based bulk catalyst has been developed via controllably adding P species, where the non-equilibrium electronic structure of Fe species is formed through the electron transfer from the Zn species through the P electronic channel. As a result, the catalytic activity of the modified Fe-based bulk catalysts has increased by 24.4–50.4%. Meanwhile, the sulfurization degree (SD) of the modified Fe-based bulk catalysts has increased by 5.6–25.9%. In addition, the HDS reaction rate constant ( k HDS ) has increased by about 2.0 times, and the DDS reaction rate constant ( k DDS ) has increased by about 2.4 times. The P modifying can regulate the directional transfer of unpaired free electrons between Fe and Zn species to form a more non-equilibrium electronic structure of Fe species, which can reduce the energy barrier of the C–S bond adsorbed on the P-modified Fe-based bulk catalysts. Importantly, the P species can be used as an active site to adsorb S-containing compounds in the modified Fe-based bulk catalysts, which is conducive to generating more coordinatively unsaturated sites (CUSs). The former can promote the formation of the more non-equilibrium electronic structure of Fe species, and the latter can adjust the adsorption active site of S-containing on the catalyst surface. Therefore, an electron transfer channel is formed among Fe, Zn, and P species, and another one is formed among Fe, P, and S-containing compounds, which form a dual-channel electron transfer behavior. Furthermore, the specific surface area, total pore volume, and reducibility of the modified Fe-based bulk catalysts have also shown varying degrees of improvement via the controllable addition of P species.
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MICROPOROUS AND MESOPOROUS MATERIALS
·
2024
·
IF 4.8
Mengkun Luan,Xiangjie Lei,Yu Fan
To increase the yield of light olefins during the catalytic pyrolysis of alkanes, a novel hierarchical Fe-incorporated ZSM-5 molecular sieve (FeM-Z5) was synthesized using an Fe-based metal-organic framework (Fe-MOF) as a mesoporogen and iron source through the dry gel conversion (DGC) method. In contrast to the conventional method of incorporating Fe species into ZSM-5 via impregnation, the DGC method incorporates Fe species into the framework of ZSM-5, decreasing the amount of Brønsted (B) acid sites and thereby inhibiting the side reactions of hydrogen transfer during the catalytic pyrolysis of alkanes. Compared with the FeN-Z5 catalyst prepared by the DGC method with Fe(NO 3 ) 3 as an iron source, FeM-Z5 had a larger amount of strong B acid sites and more mesopores with a size range of 10–40 nm originating from the decomposition of Fe-MOF; these aspects improved n-pentane pyrolysis and ethylene and propylene diffusion. As a result, the optimal FeM-Z5 catalyst exhibited the highest yield of ethylene and propylene (33.4 wt%) and the lowest deactivation rate (0.07 %/h) among the prepared catalysts during the catalytic pyrolysis of n-pentane.
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