CHEMICAL ENGINEERING JOURNAL
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2022
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IF 16.744
Ji Shu,Kanming Wang,Virender K. Sharma,Xiping Xu,Nasri Nesnas,Hongyu Wang
This paper presents Fe(VI) combined with Ti/Zn layered double hydroxide (Fe(VI)-Ti/Zn LDH) as a composite to degrade organic pollutants (pesticides and pharmaceuticals) under visible light (VL). The Fe(VI)-LDH/VL system was shown to effectively activate Fe(VI) and simultaneously enhance separation and migration of electrons-holes on the Ti/Zn LDH surface. Furthermore, the Fe(III) particles resulting from the Fe(VI) reduction were adsorbed and coordinated onto the LDH surface to form an in-situ heterojunction photocatalyst which narrowed the wide bandgap from 3.08 eV to 1.44 eV of the LDH and achieved further oxidation of pollutants. Detailed kinetic and mechanistic investigations using the pesticide, imidacloprid (IMI), revealed multi-oxidant intermediate species (Fe V /Fe IV , OH, h VB + and O 2 − ) involved in degrading the parent micropollutant and yielding oxidized products. This study also assessed the application of Fe(VI)-Ti/Zn LDH composite to other pesticides and pharmaceuticals (carbaryl (CAB) and metribuzin (MBZ), trimethoprim (TMP) and carbamazepine (CBZ)), and exhibited satisfactory micropollutants removal. The newly reported VL-induced Fe(VI) activation system, based on Fe(VI)-Ti/Zn LDH composite, may be an effective multi-oxidant strategy to oxidize pollutants in water.
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CHEMOSPHERE
·
2022
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IF 8.943
Guang Yang,Zhiyang Cheng,Huanzhong Bao,Lianbao Zhang,Hongwei Zhang,Hui Jia,Jie Wang
It was important to regulate the formation of Fe-hydroxyl during ferrate (Fe(VI)) oxidation and hydrolysis which was beneficial for interfacial adsorption of natural organic matter (NOM). Based on the influence of weak magnetic field (WMF) on the physical and chemical characteristics of particles in chemistry. This study investigated the effect of WMF on Fe(VI) oxidation and Fe(III) flocculation performance by regulating iron species during hydrolysis, for NOM removal. Results indicated WMF efficiently accelerate the removal of NOM that the reactions rate constants in magnetization system was twice as much as the control group. With the structure and electrochemical analysis, WMF enhanced Hydrogen-bond and caused much polar hydroxyl groups combined with iron ions, further triggered Fe(III) transformed to amorphous Fe-hydroxide and ferrihydrite with large specific surface area and high surface activity which removed the pollutants by adsorption and co-precipitation, instead of crystalloid Fe 2 O 3 and Fe 3 O 4 . In addition, the nucleation aggregation behavior and interaction energy of Fe-(oxy)hydroxide revealed that the lower free energy obtained in magnetization system, could lead to higher nucleation rate, and promoted the aggregation. WMF increased hydrophobicity of Fe-(oxy)hydroxides, further more easily adsorbed with humic acid (HA) and bovine serum albumin (BSA) with lower interaction energies than in control group. The selective removal mechanism of Fe-(oxy)hydroxide hardly to aggregate with pollutants which caused by the difference of electrostatic interaction, was illustrated that electronegativity HA and SA were liable to electrostatically attract with Fe-(oxy)hydroxide and removed while the low electronegativity BSA was difficult to remove which its attraction was weakened.
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高影响因子
JOURNAL OF ENVIRONMENTAL MANAGEMENT
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2022
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IF 8.91
Zhixing Xiao,Lizhuang Yang,Chuang Chen,Dan Chen,Xue Zhou
Redox reactions between humic substances and Fe(III) compounds play a critical role in the biogeochemical cycle of pollutants. Most humic substances in soils and sediments are in a solid form (i.e. humin (HM)). In order to assess the contribution of electron shuttling via HM within the electron transfer network in natural environments and to predict environmental fate of pollutants associated with iron oxides , it is necessary to understand the electron transfer processes from HM to the environmentally relevant Fe(III) minerals, and to examine the redox reversibility of HM. The results of this study demonstrated that non-reduced HMs could only donate electrons to dissolved ferric citrate and poorly crystalline ferrihydrite , but reduced HMs could also reduce hematite and magnetite that had high crystallinity . The degree of reduction depended on the difference in redox potential and the crystallinity of the Fe(III) compounds. The electron-accepting capacities of different HMs correlated well with their organic carbon content, and quinones and Fe-bound organic component were important electron-accepting groups in HMs. Furthermore, the redox reversibility experiments demonstrated that HMs could maintain stable electron transfer capacities over three reduction-oxidation cycles, indicating that the HM could be an environmentally sustainable electron shuttle. Our results suggest that (1) HM may play an unrecognized and important role in biogeochemical cycles of pollutants in Fe(III) mineral-rich environments; (2) electron shuttling through HM to ferric citrate and ferrihydrite can occur even in the presence of O 2 ; and (3) HM would be a promising material for environmental remediation.
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高影响因子
MICROCHEMICAL JOURNAL
·
2023
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IF 4.8
Zhi Luo,Yusheng Wu,Dongmiao Qin,Shuo Meng,Chujie Zeng,Biyang Deng
A luminescent reagent, 3,4,9,10-perylenetetracarboxylic acid (PTCA), was linked to a metal–organic framework (MOF) Fe(III)-MIL-88B-NH 2 through an amide reaction to form a [email protected] (III)-MIL-88B-NH 2 complex, and then gold nanoparticles (AuNPs) were grown in situ. Thus, the [email protected] (III)-MIL-88B-NH 2 @Au electrochemiluminescence (ECL) probe was obtained. The MOF of 2-aminoterephthalic acid with large specific surface area, pore sizes, and structures, which served both as the carrier and a co-reaction promoter, promoted the conversion of more S 2 O 8 2- into SO 4 •- , further enhancing the ECL signal of PTCA. An electrochemiluminescence resonance energy transfer (ECL-RET) platform was designed for the ultrasensitive and highly selective detection of cystatin C (CysC). The developed ECL-RET biosensor presented a linear range from 0.01 pg/mL to 100 ng/mL and a detection limit of 2.2 fg/mL (S/N = 3). Moreover, all the results showed that the developed ECL-RET biosensor broadened the application in the fields of biosensing and medical diagnosis.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2020
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IF 5.774
Fangke Yu,Yi Wang,Hongrui Ma,Minghua Zhou
In this study, we demonstrated that hydrothermal synthesized FeS 2 was highly efficient to catalyze the H 2 O 2 decomposition for diclofenac sodium (DCF) degradation in a wide range of initial pH (3–9) by heterogeneous electro-Fenton (EF) process, and this “Pyrite-EF” showed a better performance for the mineralization of DCF in comparison with the classic EF process. Effect of pyrite content on the hydroxyl radicals generation and iron dissolution produced by the decomposition of hydrogen peroxide (H 2 O 2 ), and applied current density on the degradation kinetics and mineralization efficiency were studied. Moreover, toxicity assessment by means of microtox method showed the solution toxicity was removed after treatment. Experimental results revealed that the enhancement of DCF degradation rate in the Pyrite-EF process was attributed to the molecular oxygen activation induced by more surface bound ferrous ions on FeS 2 , generating superoxide anions to accelerate the Fe(II)/Fe(III) cycle on the FeS 2 surface, which favored the H 2 O 2 decomposition to generate more hydroxyl radicals for the DCF degradation via a heterogeneous EF-like process. These findings could provide some new insights into the molecular oxygen activation induced by FeS 2 and the subsequent heterogeneous Pyrite-EF degradation of organic pollutants from wastewater.
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RSC Advances
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2016
·Vol. 6
·期 73
·69370-69380
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IF 3.289
Juncai Zhang,Youning Chen
With chloromethylated polystyrene resin being the base material, a new type of salicylic acid-type chelating resin with high capacity was prepared by grafting glycidyl methacrylate (GMA) on the surface of the resin via surface-initiated atom transfer radical polymerization and followed by the derivatization with 5-aminosalicylic acid. Fourier-transform infrared spectrometry and X-ray photoelectron spectroscopy were used to characterize the surface composition of the resin. It was found that the grafting degree of GMA increased linearly with the extension of ATRP time and GMA concentration. The maximum adsorption capacities of the resin were up to 4.23 mmol g−1 for Fe(III), 4.02 mmol g−1 for Ag(I), 2.36 mmol g−1 for Ni(II) and 1.75 mmol g−1 for Cu(II) at pH 4.0, respectively. The adsorption kinetics of the four metal ions conform to the model of pseudo second-order kinetics, and adsorption equilibria were better characterized by the Langmuir equation. Thermodynamic parameters were calculated to understand the nature of the adsorption process. The resin possesses excellent desorption rate and reusability. All these results indicate that the resin could be potentially applied to the efficient removal of heavy metal ions from waste water.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2025
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IF 9
Huiping Zeng,Jiahao Wu,Yong Chen,Jiongru Liang,Simin Li,Su Han,Dong Li,Jie Zhang
Developing sustainable, low‐carbon technologies to remove antibiotics from wastewater is vital to reduce ecological and health risks and meet dual carbon targets of peaking and neutrality. In this work, a surface-modified Platanus leaf powder (PLP) adsorbent was fabricated via metal-phenolic network (MPN) assembly. At pH 8, Fe(III)-tannic acid (TA) coordinated MPNs self-assembled to generate a supramolecular nanocoating on PLP, yielding the Fe(III)-Tannic networks on PLP (FTN@PLP) composite. Batch adsorption studies demonstrated an impressive maximum tetracycline (TC) uptake of 118.9 mg/g. The removal performance was systematically investigated by varying the Fe/TA ratio, pH, adsorbent dosage, initial concentration, coexisting ions, and humic acid. Adsorption kinetics, isotherm modeling and characterization study revealed that TC uptake was driven by a cooperative mechanism involving electrostatic attraction, Fe 3+ complexation, and hydrogen bonding. Additionally, FTN@PLP effectively removed representative dye pollutants. When evaluated for tetracycline (TC) removal over five successive adsorption–desorption cycles, the adsorbent maintained regeneration efficiencies exceeding 80 %. Life cycle assessment (LCA) indicated that the preparation route has a low environmental impact; leveraging plant polyphenols and biomass waste provides a promising pathway for carbon-reduction and biomass valorization. This novel strategy integrates material innovation with stewardship, providing a solution for wastewater treatment under low-carbon guidelines.
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ACS Applied Materials & Interfaces
·
2025
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IF 8.2
Jiangnan Xu,Xiu Luo,Weiwei Su,Guorong Jia,Huawei Cai,Danni Li,Rou Li,Xiangdong Wang,Yefa Yang,Tao Wang,Changjing Zuo
Transarterial radioembolization (TARE) is a primary palliative treatment for advanced liver cancer. Nonetheless, its therapeutic efficacy is frequently hindered by resistance to tumor cell apoptosis induced by inter-radiotherapy. Induction of multiple cell death modalities provides a potential solution to this challenge. Ferroptosis, a distinct form of cell death from apoptosis, is dependent on the intracellular Fe2+-mediated Fenton reaction for the production of hydroxyl radicals (·OH) and is gaining recognition as a promising approach for cancer treatment. In this study, we synthesized a therapeutic radionuclide iodine-131 (131I)-based TARE agent by combining 131I-labeled iron-based MIL-88B(Fe) nanoparticles (NPs) (abbreviated as 131I-MIL-88B(Fe)) with Lipiodol to achieve a combined apoptosis–ferroptosis tumor therapy. Specifically, a mixture of Lipiodol and 131I-MIL-88B(Fe) NPs was injected into the liver tumors through the hepatic artery. Lipiodol blocks the arterial blood supply of the tumor, causing tumor tissue necrosis, whereas 131I inter-radiotherapy damages deoxyribonucleic acid (DNA) through direct action or indirectly via the production of ·OH through H2O radiolysis, leading to tumor cell apoptosis. Importantly, hydrated electrons (eaq–), a byproduct of H2O radiolysis, promoted the conversion of Fe3+ to Fe2+ in MIL-88B(Fe) NPs, enhancing the efficacy of the Fenton reaction and triggering ferroptosis. In vitro experiments demonstrated that compared to 131I alone, 131I-MIL-88B(Fe) NPs significantly enhanced ferroptosis-mediated tumor cell death due to 131I-induced Fe2+ production, which increased catalytic activity in the Fenton reaction. In a rat model bearing orthotopic N1S1 liver tumors, TARE with Lipiodol and 131I-MIL-88B(Fe) NPs induced tumor cell necrosis, apoptosis, and ferroptosis, resulting in improved therapeutic outcomes. This study leverages eaq– to facilitate Fe3+/Fe2+ conversion for efficient ferroptosis, turning waste into a valuable resource. This demonstrated the innovative integration of multiple treatment strategies to augment the efficacy of TARE in liver cancer therapy.
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ENVIRONMENTAL SCIENCE & TECHNOLOGY
·
2025
·
IF 11.3
Yiming Sun,Chenying Zhou,Shuang Meng,Shuang Zhong,Yang Liu,Chuanshu He,Peng Zhou,Bo Lai
Heteroatom doping has been applied as an excellent method for mediating the catalytic reactivity of carbon materials. To overcome the inherent defect of slow Fe(III) reduction in Fenton chemistry, this work finds that boron-doped carbon materials demonstrate high cocatalytic activity in boosting Fenton oxidation. During Fenton chain reactions catalyzed by boron-doped reduced graphene oxide (B-rGO, the typical boron-doped carbon material), highly reactive near-free Fe(III) formed on the B-rGO surface can dramatically promote H2O2 mediated Fe(III) reduction, which strongly accelerates the rate-determining reaction in Fenton chain reactions to generate hydroxyl radicals. The results of DFT calculations, electrochemical analysis, characterizations (XAFS, in situ Raman, and HAADF-STEM), and pH-dependent performance reveal that doped boron atoms can modulate the electron-deficient iron atom of FeOH2+ by stretching the Fe–O bond (from 163.6 to 179.2 pm), which forms near-free Fe(III) on the B-rGO surface with higher oxidation capability than free Fe(III), and the Fe(III) oxidation potential is positively and linearly related to the boron content of B-rGO (R2 = 0.96). Moreover, near-free Fe(III) can dramatically oxidize H2O2 (a green electron donor) to accelerate Fe(II) regeneration, thereby promoting Fenton chain reactions for long-lasting Fenton oxidation. These discoveries afford a strategy for designing green and sustainable cocatalysts to overcome the intrinsic weaknesses of classical Fenton chemistry.
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CHEMOSPHERE
·
2021
·
IF 7.086
Hang Liu,Hua Yin,Minghan Zhu,Zhi Dang
Organophosphorus flame retardants (OPFRs) have been regarded as one of the most rebarbative classes of emerging contaminants due to their persistence and toxicity. In the current study, Fe-based metal organic framework (MIL-88A) was synthesized and employed as photo-Fenton catalyst for the degradation of tris-(2-chloroisopropyl) phosphate (TCPP), a typical representative of OPFRs. The observations indicated that visible light could boost the reduction of ≡Fe III to ≡Fe II in Fe–O clusters of MIL-88A during the photo-Fenton system and consequently induce the transformation of H 2 O 2 to OH, which realized efficient degradation of TCPP. Due to the excellent function of MIL-88A, the effective pH application range of photo-Fenton system was extended in comparison with traditional Fenton system. The degradation efficiency of TCPP was visibly influenced in presence of humic acid (HA). MIL-88A exhibited a commendable reusability and stability after 3 times cycle. As the photo-Fenton reaction proceeded, TCPP was disintegrated to several kinds of carboxylated, dechlorinated and hydroxylated products. The observations of metabolomics endorsed that the interference of intermediate products mixture on E. coli weakened to a certain extent. In conclusion, carboxylation , dechlorination , hydroxylation and oxidation of TCPP were likewise effective for its detoxification, revealing that heterogeneous photo-Fenton system driven by Fe-based metal organic framework will be an attractive and safe treatment technique for OPFRs control.
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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 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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