International Journal of Environmental Science and Technology
·
2023
·Vol. 20
·期 11
·11865-11876
·
IF 3.1
Xin X.,Liu H.,Sun J.,Gao K.,Jia R.
The composite material based on N- , S- , and Fe-doped TiO 2 (NSFe-TiO 2 ) synthesized by wet impregnation was used as a photocatalyst to rapidly degrade sulfadiazine. The photocatalytic degradation behavior and mechanism of sulfadiazine on NSFe-TiO 2 were investigated for revealing the role of degradation under ultraviolet light. The results showed that compared with TiO 2 , NSFe-TiO 2 markedly improved the efficiency in photocatalytic degradation of sulfadiazine: more than 90% of sulfadiazine could be removed within 120 min by NSFe-TiO 2 dosage of 20 mg L −1 . The process conformed to first-order reaction kinetics model. The parameters such as loaded amount of NSFe-TiO 2 , solution pH value, humic acid concentration and recycle numbers on removal efficiency were also studied. Compared to neutral and alkaline conditions, acidic condition was not conducive to the photocatalysis. HA, Ca 2+ , Cu 2+ and Zn 2+ in the actual water body had mild inhibition on sulfadiazine degradation in UV/NSFe-TiO 2 system. Fragments screened by high-resolution mass spectrometry were conducted to explore the oxidation mechanism and pathways of sulfadiazine degradation. On the whole, UV/NSFe-TiO 2 photocatalysis has a good effect on sulfadiazine removal.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2022
·
IF 24.319
Junxian Qin,Yun Pei,Yue Zheng,Daiqi Ye,Yun Hu
Fe-MOF derivative (M-300) is successfully prepared by thermal treatment using MIL-100(Fe) as a precursor. The resulting M-300 catalyst displays excellent performance in the degradation of volatile organic compounds (VOCs) and the bacteriostasis to Escherichia coli under the visible light. In addition, the catalyst also exhibits the capacity of acetaldehyde degradation under actual sunlight. The high activity is attributed to the abundant exposure of the unsaturated Fe 2+ active site, which can significantly promote the transfer of photogenerated electron and the oxygen reduction process, thus improving the efficiency of the entire photocatalytic oxidation reaction. This work shows the application prospect of MOFs derivatives in the field of indoor photocatalytic purification, and also provides a new insight into the study of catalyst modification in photocatalytic degradation of pollutants.
✓ 已验证
产品关联
DOI
高影响因子
Journal of Environmental Chemical Engineering
·
2022
·
IF 7.968
Xiaolin Han,Nannan Wang,Wei Zhang,Xiaodong Liu,Qi Yu,Juying Lei,Lei Zhou,Guangli Xiu
In this work, the presence of ascorbic acid (AsA) in MIL-88B(Fe) / H 2 O 2 system was demonstrated to significantly increase the sulfamethoxazole (SMX) degradation efficiency. The SMX degradation rate in AsA/MIL-88B(Fe) / H 2 O 2 system was 0.177 L/(mg∙min), which was 60 times that of the MIL-88B(Fe) / H 2 O 2 system. Moreover, the study shows that AsA not only promotes SMX degradation in Fenton-like systems but also expands its pH application range. The effect of coexisting anions on the catalytic performance of the AsA/MIL-88B(Fe) / H 2 O 2 system was also investigated. Then, reactive species were detected via quenching experiments, which indicated •OH as the dominant free radical contributing to SMX degradation. Meanwhile, ESR determinations confirmed the existence of •OH and O2 − • in AsA/MIL-88B(Fe) / H 2 O 2 system. The high activity of the AsA/MIL-88B(Fe) / H 2 O 2 system was attributed to the effective surface Fe(III)/Fe(II) cycle promoted by AsA, and a possible mechanism of the AsA/MIL-88B(Fe) / H 2 O 2 system is proposed. The possible pathways for SMX and AsA degradation in the AsA/MIL-88B(Fe) / H 2 O 2 system are proposed based on the identified intermediates and the ecotoxicity analysis was conducted by ECOSAR . Finally, experimental results using the actual surface water and groundwater revealed the excellent availability of AsA/MIL-88B(Fe)/H 2 O 2 system in remediating SMX contaminated water . This study presents a novel, efficient Fenton-like system using AsA and iron-based metal-organic frameworks for sulfonamide removal from water.
✓ 已验证
产品关联
DOI
高影响因子
ACS Applied Materials & Interfaces
·
2022
·
IF 10.383
Bofang Shi,Hang Li,Xiaojie Fu,Chengcheng Zhao,Mingtao Li,Maochang Liu,Wei Yan,Honghui Yang
High energy consumption in pyrolyzing precursors for catalyst preparation would limit the application of nitrogen-doped carbon-based single-atom catalysts in actual pollutant remediation. Herein, we report an Fe single atom (7.67 wt %) loaded polyaniline catalyst (Fe-PANI) prepared via a simple impregnation process without pyrolysis. Both experimental characterizations and density functional theory calculations demonstrated that isolated −N═ group sites can fasten Fe atoms through Fe–N coordination in PANI, leading to a high stability of Fe atoms in a heterogeneous Fenton reaction. Highly dispersive yet dense −N═ groups in PANI can be protonated to be adsorption sites, which largely reduce the migration distance between reactive radicals and organics. More significantly, frontier molecular orbitals and spin-density distributions reveal that electrons can transfer from reduction groups of PANI to an Fe(III) site to accelerate its reduction. As a result, a remarkably boosted degradation behavior of organics under near-neutral conditions (pH 6), with low H2O2 concentration, was achieved. This cost-effective Fe-PANI catalyst with high catalytic activity, stability, and adsorption performance has great potential for industrial-level wastewater treatment.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
JOURNAL OF HAZARDOUS MATERIALS
·
2023
·
IF 13.6
Xukai Li,Weirui Chen,Dongpo Liu,Gaozu Liao,Jing Wang,Yiming Tang,Laisheng Li
Due to its low interfacial electron migration ability and highly hydrophilic, Fe-MCM-41 (FeM) had poor activity and stability during catalytic ozonation . To this end, the secondary metal Zn and Si-F group were introduced into the framework of FeM to create surface potential difference and hydrophobic sites. Comparative characterizations showed that there existed rich acid sites with great potential difference on F-Fe-Zn-MCM-41 (FFeZnM). Additionally, because of the existence of hydrophobic and electron-withdrawing Si-F unit, the electron migration ability, hydrophobicity and acidity of FFeZnM were enhanced. The greater O 3 mass transfer was induced by Si-F group and O 3 was directly activated at Fe and Zn Lewis acid sites into •OH, •O 2 - and 1 O 2 . With •OH acting as main species, FFeZnM/O 3 achieved the superior IBP removal (93.4%, 30 min) and TOC removal (46.6%, 120 min) over those of sole O 3 and F-FeM/O 3 processes, respectively. HCO 3 - , Cl - , NO 3 - and SO 4 2- hindered IBP degradation by FFeZnM/O 3 , but high concentration humic acid (HA) exhibited promotion by forming HA-IBP complex. IBP degradation by FFeZnM/O 3 was enhanced with tap water , river water, and effluent from the secondary sedimentation tank of the sewage plant acting as medium. This study proposed an innovative approach to catalyst design for catalytic ozonation.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2023
·
IF 9.9
Ying Wang,Gareth R. Williams,Yilu Zheng,Honghua Guo,Shiyan Chen,Rong Ren,Tong Wang,Jindong Xia,Li-Min Zhu
One of the major challenges in effective cancer therapy arises because of the hypoxic microenvironment in the tumor. This compromises the efficacy of both chemo- and radiotherapy , and thus hinders patient outcomes. To solve this problem, we constructed polydopamine (PDA)-cloaked Fe-based metal organic frameworks (MOFs) loaded with d -arginine ( d -Arg), glucose oxidase (GOX), and the chemotherapeutic drug tirapazamine (TPZ). These offer simultaneous multifaceted therapy combining chemodynamic therapy (CDT)/radiotherapy (RT)/starvation therapy (ST)/gas therapy (GT) and chemotherapy. The particles further can act as contrast agents in magnetic resonance imaging. GOX catalyses the conversion of endogenous glucose and O 2 to hydrogen peroxide and gluconic acid , blocking the cells’ energy supply and providing ST. With the resultant acidification of the local environment, the breakdown of the MOF releases TPZ (for chemotherapy) and Fe 3+ , which reacts with H 2 O 2 to produce reactive oxygen species and thus stimulates the conversion of d -Arg to NO for GT and RT sensitization. The PDA coating not only seals the pores and chelates Fe 3+ to enhance the T 1 -weighted magnetic resonance imaging (MRI) properties, but also is used to graft folate bovine serum albumin (FA-BSA) and thereby target the tumor site. The combined administration of low doses of X-ray irradiation and nanoparticles reduces the side effects on healthy tissue and can prevent lung metastases in mice. This work highlights the synergistic treatment of osteosarcoma via ST/GT/CDT/RT/MRI/ chemotherapy using a PDA-cloaked MOF system.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH
·
2023
·Vol. 30
·期 37
·87830-87850
·
IF 5.8
Liu Gen,Lin Yingzi,Li Siwen,Shi Chunyan,Zhang Dongyan,Chen Lei
Fe-BOC-X
photocatalyst was successfully prepared by solvothermal method. The photocatalytic activity of Fe-BOC-X was determined by ciprofloxacin (CIP), a typical fluoroquinolone antibiotic. Under sunlight irradiation, all Fe-BOC-X showed better CIP removal performance than original BiOCl. In comparison, the photocatalyst with iron content of 50 wt% (Fe-BOC-3) has excellent structural stability and the best adsorption photodegradation efficiency. The removal rate of CIP (10 mg/L) by Fe-BOC-3 (0.6 g/L) reached 81.4% within 90 min. At the same time, the effects of photocatalyst dosage, pH, persulfate, persulfate concentration, and combinations of different systems (PS, Fe-BOC-3, Vis/PS, Vis/Fe-BOC-3, Fe-BOC-3/PS, and Vis/Fe-BOC-3/PS) on the reaction were systematically discussed. In reactive species trapping experiments, electron spin resonance (ESR) signals revealed that the photogenerated holes (h + ), hydroxyl radical (•OH), sulfate radical (•SO 4 − ), and superoxide radical (•O 2 − ) played an important role in CIP degradation; hydroxyl radicals (•OH) and sulfate radicals (•SO 4 − ) play a major role. Various characterization methods have demonstrated that Fe-BOC-X has larger specific surface area and pore volume than original BiOCl. UV–vis DRS indicate that Fe-BOC-X has wider visible light absorption and faster photocarrier transfer and provides abundant surface oxygen absorption sites for effective molecular oxygen activation. Accordingly, a large number of active species were produced and participated in the photocatalytic process, thus effectively promoting the degradation of ciprofloxacin. Based on HPLC–MS analysis, two possible decomposition pathways of CIP were finally proposed. The main degradation pathways of CIP are mainly due to the high electron density of piperazine ring in CIP molecule, which is mainly attacked by various free radicals. The main reactions include piperazine ring opening, decarbonylation, decarboxylation, and fluorine substitution. This study can better open up a new way for the design of visible light driven photocatalyst and provide more ideas for the removal of CIP in water environment.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Journal of Materials Chemistry A
·
2023
·Vol. 11
·期 27
·14900-14910
·
IF 11.9
Mengdi Liu,Sai Zhang,Min Chen,Shuxue Zhou,Limin Wu
Electrochemical nitrogen reduction reaction (NRR) is considered a promising alternative for green and sustainable ammonia (NH3) synthesis, which has, however, long suffered from low efficiency and poor selectivity. In this study, an isolated bimetallic Fe–Ru single atom catalyst was synthesized via anchoring the metal single atoms on nitrogen-doped carbon nanorod spheres. The catalyst exhibits an optimized faradaic efficiency of 29.3% along with an NH3 yield rate of 43.9 μg h−1 mg−1 for the NRR under −0.2 V vs. RHE. Control experiments and isotopic labelling test confirm that the generated NH3 originates from the nitrogen (N2) feeding gas. Computational analysis indicates that Fe acts as the active sites for nitrogen reduction. Impressively, an obvious synergistic effect exists between spatially isolated single atoms, which could be overlooked previously. The electronic structure of Fe sites is effectively influenced by Ru atoms, which results in the d-band center shift and stronger N2 adsorption, further improving NRR performance.
✓ 已验证
产品关联
DOI
高影响因子
Journal of Materials Chemistry B
·
2022
·Vol. 10
·期 42
·8760-8770
·
IF 7.571
Zhimin Mo,Xinyuan Pan,Xiaoli Pan,Lin Ye,Han Hu,Qi Xu,Xiaoxi Hu,Zushun Xu,Jie Xiong,Guangfu Liao,Shengli Yang
Fe-based metal–organic frameworks (MOFs) can be used for chemodynamic therapy (CDT) for tumors due to their unique Fenton-like effects and porous and biodegradable nature. The adsorption and transport of small molecule drugs by their structure has attracted much attention. Herein, MnO2@NH2-MIL101(Fe)@Ce6-F127 nanoparticles (MNMCF NPs) were synthesized using a facile solvothermal strategy. The small molecule photosensitizer Ce6 was adsorbed by MOFs to improve the biocompatibility of Ce6 and give it high bioavailability when injected intravenously. When the MNMCF NPs reached the tumor site, Fe-based MOFs exhibited Fenton-like properties, producing ˙OH and showing CDT effects. MnO2 could specifically respond to produce O2 in a tumor microenvironment, thereby improving the tumor hypoxia state and enhancing the efficacy of photodynamic therapy (PDT) by Ce6. Both the in vitro and in vivo experiments showed that the MNMCF-guided CDT/PDT combination therapy could effectively ablate tumors without the drawbacks of poor tolerability and potential long-term side effects. Therefore, the prepared MNMCF NPs can be used as promising candidates for synergistic CDT/PDT tumor therapy.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ENVIRONMENTAL RESEARCH
·
2022
·
IF 8.431
Xuelian Xia,Yanguo Teng,Yuanzheng Zhai
Riverbank filtration (RBF) constitutes an important part of the water cycle , which involves active natural filtration leading to pollution of river water being intercepted and retained. The RBF has the function of water purification , but retention of exogenous pollutants in the RBF system complicates biogeochemical processes due to the presence of primary active components. In this study, we verified the essential role of microbial mediation during the interactions between primary Fe minerals in the RBF system and dissolved organic matter (DOM) in river water based on lab-scale experiments. The results demonstrated that DOM from infiltration of river water increased the amount of iron (Fe) released from the sediment in RBF, leading to an increase in Fe concentration in groundwater by higher than one order of magnitude. In particular, the existence of Fe bacteria even made this effect more thorough and more complex. Abiotic reduction was shown to play a more significant role in increasing Fe release than microbe-mediated reduction. Increasing the amount of Fe released could change the distribution of Fe minerals at the sediment surface, thereby affecting the structure of the microbial community in the RBF system and decreasing the DOM concentration in the groundwater. Moreover, As and Mn were found to behave in a similar manner as Fe due to their close biochemical properties when interacting with primary minerals in sediment. This study not only provides mechanistic insight into the higher Fe concentrations encountered in the groundwater of nearby rivers but also has important practical implications for developing nature-based technologies for water pollution control and environmental remediation.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2022
·
IF 9.965
Zhihui Liu,Siyuan Sun,Fan Yang,Hongchen Liu,Yang Sun,Na Ta,Ge Zhang,Sai Che,Yongfeng Li
Transition metal-based (Fe, Co, Cu, etc.) single-atom catalysts (SAC) have been widely used in the direct oxidation of ethylbenzene and benzene. However, their catalytic performance is limited by the low metal loading. Compared with traditional SAC, dual site single-atom catalysts (DSAC) show the advantages of abundant active sites, high metal loading, and excellent catalytic performance. Herein, a novel Fe/Cu N C DSAC was prepared by facile one-pot pyrolysis of formaldehyde, dicyandiamide, and metal salts. Dicyandiamide acted as the carbon source with advantage of high nitrogen content, which promoted the formation of metal centers and increased the metal loading. Meanwhile, the synergistic effect between Fe and Cu active centers was revealed to adjust the coordination environment, thus improving the catalytic activity of oxygen activation. The synthesized Fe/Cu N C DSAC demonstrated superior catalytic performance in ethylbenzene oxidation reaction with O 2 as a green oxidant under mild reaction conditions, with a 99 % conversion of acetophenone and no significant degradation of activity after 10 circles. In addition, NaCl was added into the synthesis as a template to adjust the pore structure, and the modified Fe/Cu N C DSAC showed excellent performance in benzene oxidation reaction with high product conversion. In conclusion, this work paves the way for the construction of efficient, green, and cost-effective catalysts for the direct oxidation of ethylbenzene and benzene.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
JOURNAL OF MOLECULAR STRUCTURE
·
2022
·
IF 3.841
Feihan Yu,Wenxuan Wang,Yudong Li,Minshu Du,Feng Liu,Daxin Liang
TiO 2 is one of the most ideal photocatalytic materials, but its application is limited by many problems (e.g., wide band gap, easy carrier recombination). Co-catalyst with changes in valence could efficiently overcome the disadvantages above. Herein, a Fe species (Fe, Fe 2 O 3 )/TiO 2 was designed to fully utilize photogenerated charges and holes. The degradation rate of ciprofloxacin can reach 99.97%. In addition, its methane generation from photoreduction of CO 2 is 12.9 times than that of pure TiO 2 . These results are attributed to the well-designed catalyst including the combination of TiO 2 and FeO x as photocatalysts and oxygen buffers, and the dispersion of single-atom Fe clusters as cocatalysts and electron trap sites. The effect mechanism of Fe species on TiO 2 was verified by PBE DFT calculation. Finally, following a concept of thermodynamic-kinetic synergy, a new design strategy for photocatalysts is accordingly proposed, as such, the prepared catalyst is expected to be applied in the environmental remediation.
✓ 已验证
产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）