CHEMICAL ENGINEERING JOURNAL
·
2018
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IF 6.735
Shanshan Yang,Pingxiao Wu,Junqin Liu,Meiqing Chen,Zubair Ahmed,Nengwu Zhu
For eliminating organic pollutants from wastewater, Fe 0 or Fe 0 -composites as catalyst for peroxymonosulfate (PMS) activation have attracted increasing attention in advanced oxidation processes. In this work, a novel Fe 0 -montmorillonite composites (Fe-Mt-C-H 2 ) have been prepared by thermal reduction and used as an activator for PMS to remove bisphenol A (BPA). The removal efficiency of BPA (25 mg·L −1 ) and total organic carbon (TOC) were 99.3% and 70.6%, respectively, in the presence of Fe-Mt-C-H 2 (0.4 g·L −1 ) and PMS (1 mM) at pH of 3. Electron paramagnetic resonance (EPR) spectroscopy and radical scavenger studies demonstrated that superoxide radical (O 2 − ) and singlet oxygen ( 1 O 2 ) were the crucial reactive oxygen species (ROS) in the Fe-Mt-C-H 2 /PMS system rather than sulfate (SO 4 − ) and hydroxyl radical (·OH). Besides, it was found that pH had a great influence on the catalytic oxidation rate of BPA and the Fe-Mt-C-H 2 exhibited best catalytic performance and reusability at initial pH of 3. Furthermore, the constituents of the iron surface oxidation layer at different initial pH were investigated with X-ray photoelectron spectroscopy studies, which indicated that the major constituents were Fe 3 O 4 in acidic solution and contained α-Fe 2 O 3 , FeO and FeSO 4 (s) in alkaline or neutral solution. The findings of this study provide new insights into the activation mechanism of PMS by Fe 0 -composites and exhibit a promising application of Fe-Mt-C-H 2 in wastewater treatment.
研究领域:
环境科学
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化学工程
✓ 已验证
产品关联
DOI
高影响因子
Journal of Cleaner Production
·
2021
·
IF 9.297
Wuming Xie,Zijun Huang,Fengping Zhou,Yuhui Li,Xiaolin Bi,Qiushi Bian,Shuiyu Sun
The presence of the antibiotics in wastewater and drinking water is causing increasing concern around the world, thereby an advanced sustainable technology needs to be developed to remove the antibiotics from water resources. In this study, Metal-organic frameworks (MOFs) derived zero-valent iron embedded in the carbon matrix structure named FMC is prepared by a direct pyrolysis of Fe-based metal organic framework. FMC is used as a heterogeneous Fenton-like catalyst to degrade amoxicillin (AMX) based on the oxidation and degradation reactions. FMC had the strengthened catalytic performance for amoxicillin elimination with high mineralization efficiency (60.41%), which was evaluated over various experimental conditions. The role of reaction in FMC/H 2 O 2 system was identified, suggesting amoxicillin was eliminated by the attack of hydroxyls radicals (·OH). The carbon structures can facilitate the passage of electrons and boost the contact of zero valent iron and Fe 2+ species on FMC surface with H 2 O 2 , resulting in the accelerated production of ·OH and high removal efficiency of amoxicillin. By defining reactive oxidizing species and degradation intermediates, the plausible degradation pathways of amoxicillin have been inferred. This study revealed that FMC/H 2 O 2 system has high AMX degradation efficiency and decent recyclability .
研究领域:
环境科学
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材料科学
✓ 已验证
产品关联
DOI
高影响因子
Journal of Environmental Chemical Engineering
·
2021
·
IF 5.909
Yanping Zhang,Peng Xiangshi,Jiayu Tian,Fen Li,Xuteng Fan,Liran Ma,Ruijun Zhang
Waste waterworks sludge and walnut shell were employed to synthesize a composite catalyst consisting of Fe 0 /Fe 3 O 4 /biochar using a one-step pyrolysis process . The synthesized catalyst was applied to active peroxymonosulfate (PMS) for studying the degradation of methylene blue (MB). Various characterization results confirmed that Fe 0 and Fe 3 O 4 were distributed on the surface of composite catalyst, which had a porous structure and large specific surface area of 109.87 m 2 /g. Owning to these structural properties, the composite catalyst presented desirable catalytic capability and reusability. When 0.4 g/L PMS and 0.3 g/L composite catalyst were added into the MB solution (pH 7), 99.9% MB could be degraded within 60 min at a high reaction rate of 0.1550 min −1 , which was much better than that of zero valent iron (ZVI)/PMS system. After the three cycles, the catalyst could still maintain an MB degradation of over 68.0%. The free radical quenching experiments and electron paramagnetic resonance experiments demonstrated that SO 4 − ∙ and HO ∙ were generated during the activation of PMS. The X-ray photoelectron spectrometer analysis revealed that Fe 3 O 4 and various functional groups, such as C O were formed on the composite catalyst, and the Fe 2+ was oxidized to Fe 3+ . Furthermore, the iron leaching experiments indicated that both the homogeneous and heterogeneous reactions occurred during the catalysis of PMS using the synthesized composite catalyst. Acidity and higher temperature were conducive to the catalytic reaction . This study offers a green and sustainable route for simultaneously degrading contaminants and reusing wastes.
研究领域:
环境科学
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材料科学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF HAZARDOUS MATERIALS
·
2022
·
IF 14.224
Jie Chen,Jiafeng Wan,Chi Li,Yuhan Wei,Haolin Shi
Fe 0 -Fe 3 O 4 nanoparticles and cerium dioxide hollow spheres as efficient heterogeneous electro-Fenton reagents were rationally designed to be embedded in porous carbon derived from skimmed cotton for the electrocatalytic degradation of ceftriaxone sodium. Skimmed cotton porous carbon material has a hollow tubular structure, and cerium dioxide is dispersed on the surface of the carbon material in a hollow sphere structure of uniform size. Fe 0 -Fe 3 O 4 nanoparticles were wrapped in irregular particle shapes on the surface of cerium dioxide hollow spheres, and the remaining part was laid flat on the surface of porous carbon material. The as-synthesized Fe 0 -Fe 3 O 4 /CeO 2 /C showed excellent degradation efficiency of 95.59 % for ceftriaxone sodium within 120 mins and obtained a COD removal rate of 95.21 % at 240 mins. The zero-valent iron as a reducing agent effectively accelerated the Fe 3+ /Fe 2+ cycle, allowing the composites to exhibit higher catalytic activity and further reducing the possibility of secondary contamination. Moreover, the existence of cerium dioxide further promoted the redox cycle of Ce 4+ /Ce 3+ and accelerated the electron transfer in the interface of the catalyst. The synergistic effect of iron and cerium greatly facilitated the production of hydroxyl radicals and increased the yield of hydroxyl radicals in the reaction system.
研究领域:
环境科学
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材料科学
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化学工程
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Theranostics
·
2020
·
IF 8.579
Wen Liu,Jinpei Wu,Xin Ji,Yandong Ma,Lamei Liu,Xiaoqing Zong,Haiyuan Yang,Jian Dai,Xiaoyuan Chen,Wei Xue
Although the enzyme catalytic nanoreactors reported so far have achieved excellent therapeutic efficacy, how to accurately exert enzyme activity in the tumor microenvironment to specifically kill tumor cells and avoid systemic oxidative damage would be an inevitable challenge for catalytic nanomedicine. At the present study, we fabricate an advanced biomimetic nanoreactor, SOD-Fe 0 @Lapa-ZRF for tumor multi-enzyme cascade delivery that combined specifically killing tumor cells and protect cells from oxidative stress. Methods : We first synthesized the FeNP-embedded SOD (SOD-Fe 0 ) by reduction reaction using sodium borohydride. Next, SOD-Fe 0 and Lapa cargo were encapsulated in ZIF-8 by self-assembly. In order to protect the cargo enzyme from digestion by protease and prolong blood circulating time, SOD-Fe 0 @Lapa-Z was further cloaked with RBC membrane and functionalized with folate targeting, resulting in the final advanced biomimetic nanoreactor SOD-Fe 0 @Lapa-ZRF. Results : Once internalized, ZIF-8 achieves pH-triggered disassembly in weakly acidic tumor microenvironment. The released SOD-Fe 0 and Lapa were further endocytosed by tumor cells and the Lapa produces superoxide anion (O 2 -• ) through the catalysis of NQO1 that is overexpressed in tumor cells, while O 2 -• is converted to H 2 O 2 via SOD. At this time, the released ferrous ions from SOD-Fe 0 and H 2 O 2 are further transformed to highly toxic hydroxyl radicals (•OH) for specifically killing tumor cells, and there was no obvious toxicological response during long-term treatment. Importantly, SOD-Fe 0 @Lapa-ZRF enhanced the normal cell's anti-oxidation ability, and thus had little effect on the secretion of TNF-α, IL-6 and IL-1β pro-inflammatory cytokines, while effectively reversed the decreased activity of T-SOD and GSH-Px and remained stable MDA content after tumor treatment. In vitro and in vivo results indicate that the tumor microenvironment-responsive release multi-enzyme cascade have high tumor specificity and effective anti-tumor efficacy, and can protect cells from oxidative stress damage. Conclusion : The biomimetic nanoreactor will have a great potential in cancer nanomedicine and provide a novel strategy to regulate oxidative stress.
研究领域:
癌症纳米医学
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酶催化
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生物材料
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药物递送系统
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肿瘤学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ENVIRONMENTAL RESEARCH
·
2022
·
IF 8.431
Jin Zhang,Hao Yu,Weijian Xu,Hongyu Shi,Xiaohong Hu,Jiang Xu,Liping Lou
Sulfidized nanoscale zerovalent iron (S-nZVI) was a promising material for degrading halogenated contaminants, but the easy aggregation limits its application for in-situ groundwater remediation . Hence, S-nZVI was decorated onto modified biochar (mBC) to obtain better dispersity and reactivity with florfenicol (FF), a widely used antibiotic. Uniform dispersion of S-nZVI particles were achieved on the mBC with plentiful oxygen-containing functional groups and negative surface charge. Thus, the removal rate of FF by [email protected] was 2.5 and 3.1 times higher than that by S-nZVI and [email protected] , respectively. Adsorption and dechlorination of FF showed synergistic effect under appropriate mBC addition (e.g., C/Fe mass ratio = 1:3, 1:1), probably due to the enrichment of FF facilitates its reduction. In contrast, the contact between FF and S-nZVI could be hindered under more mBC addition, significantly decrease the reduction rate of FF and the reduction capacity of per unit Fe 0 . In addition, sulfur dose altered the surface species of surface Fe and S, and removal rates of FF correlated well with surface reductive species, i.e., FeS ( r = 0.90, p < 0.05) and Fe 0 ( r = 0.98, p < 0.01). These mechanistic insights indicate the importance of rational design for biochar supported S-nZVI, which can lead to more efficient FF degradation.
研究领域:
环境科学
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材料科学
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化学工程
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水处理
✓ 已验证
DOI
PubMed
高影响因子
WATER ENVIRONMENT RESEARCH
·
2025
·Vol. 97
·期 2
·e70022
·
IF 1.9
Guonan Zhao,Ke Feng
The Fenton-like process, utilizing zero-valent iron (Fe 0 ) and hydrogen peroxide (H 2 O 2 ), is employed to degrade refractory organic matter in membrane bioreactor (MBR) effluent derived from landfill leachate. However, the rate-limiting Fe 2+ /Fe 3+ redox step diminishes treatment efficacy and generates substantial iron sludge. This study elucidates the mechanism by which ultraviolet (UV) irradiation augments the Fe 0 /H 2 O 2 process for the removal of refractory organic matter in MBR effluent. The results show that the UV- enhanced H 2 O 2 process effectively disrupts the aromatic structure of organic compounds, reducing molecular weight, degree of polymerization, and humification. Compared with the Fe 0 /H 2 O 2 process, the removal efficiency of UV 254 , color number, and total organic carbon in the effluent treated by the UV/Fe 0 /H 2 O 2 process increased by 24.16%, 14.62%, and 57.46%, respectively. Concurrently, the generation of iron sludge was reduced by 21.6%. This enhancement is primarily attributed to UV's ability to intensify the Fe 2+ /Fe 3+ redox cycle and expedite the surface corrosion of Fe 0 , yielding more iron oxides. This accelerates the decomposition of H 2 O 2 , generating a higher quantity of • OH through both homogeneous and heterogeneous Fenton-like reactions. The refractory organic matter is removed through the oxidation by • OH, as well as the adsorption and precipitation facilitated by iron-based colloids. Practitioner Points UV promotes Fe 0 /H 2 O 2 process to degrade refractory organic matter in MBR effluent. UV promotes Fe 0 to dissolve more Fe 2+ and the redox cycle of Fe 2+ and Fe 3+ . The dosage of H 2 O 2 or Fe 0 influences the treatment effect of the process. Graphical UV can enhance the degradation of refractory organic matter in MBR effluent from landfill leachate by Fe 0 /H 2 O 2 process.
研究领域:
环境科学
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水处理工程
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产品关联
DOI
PubMed
高影响因子
JOURNAL OF HAZARDOUS MATERIALS
·
2019
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IF 7.65
Zhe Yang,Xiaowen Ma,Chao Shan,Xiaohong Guan,Weiming Zhang,Lu Lv,Bingcai Pan
To activate zero-valent iron (ZVI) for efficient nitrobenzene (NB) reduction, a hybrid Fe 0 /Fe 3 O 4 /FeCl 2 microcomposite (hZVI bm ) was synthesized via simple ball-milling of the ternary mixture of ZVI, Fe 3 O 4 , and FeCl 2 ·4H 2 O (hZVI). SEM-EDX and time-of-flight secondary ion mass spectroscopy (ToF-SIMS) indicated the hZVI bm microcomposite (10–20 μm) consisted of Fe 0 core covered by ∼3.3 μm-thick shell decorated with Fe 3 O 4 /FeCl 2 fine particles (0.1–2 μm). Efficient removal (>95%) of NB (200 mg/L) was achieved by hZVI bm (2.0 g Fe/L) in 30 min over a wide pH range from 3 to 9. Notably, the NB removal efficiency of hZVI bm was over 30 times higher than the virgin ZVI or over three times higher than hZVI. The enhanced reactivity synergistically resulted from both chemical and physical aspects. Chemically, the Fe 3 O 4 /FeCl 2 -inlaid shell and the Fe(II) components played significant activation roles, as observed from the comparative experiments in their absence via pretreatments of hZVI bm by sonication and rinsing, respectively, with direct evidence of depassivation effect by XRD analysis. Physically, the ball-milling-induced inter-particle compaction effect was considered crucial to facilitate the interfacial mass/electron transfer processes during the reduction. The reduction pathway from NB to aniline via two intermediates was analyzed by liquid chromatography.
研究领域:
环境科学
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化学工程
✓ 已验证
DOI
高影响因子
Journal of Environmental Chemical Engineering
·
2026
·Vol. 14
·期 6
·125412
·
IF 7.5
Huaqing Liu,Yujian Hu,Wenjuan Liu,Mengcheng Zhang,Wenrui Zhang,Yanlong Wang
A spatially regulated Fe⁰@SiO₂@nCaO₂ nanocomposite was rationally designed. • A multifunctional material integrates oxidation, precipitation, and flocculation. • Fe loading regulates ROS generation and pollutant-specific removal pathways. • Sequential activation of oxidation, precipitation, and flocculation pathways was revealed. The simultaneous removal of coexisting organic and inorganic contaminants remains a major challenge for wastewater treatment because conventional technologies fail to integrate oxidative degradation with inorganic immobilization in a single reaction system. Herein, a spatially regulated Fe 0 @SiO 2 @nCaO 2 multifunctional nanocomposite was developed to achieve synergistic purification of representative organic pollutants (sulfamethoxazole and atrazine) and inorganic contaminants (As(III) and phosphate). Batch experiments showed that the optimized Fe 0 @SiO 2 @nCaO 2 composite (Fe loading of 170.2 mg g −1 , 1 g L −1 ) removed 97.9% of sulfamethoxazole and 99.9% of atrazine, As(III), and phosphate within 24 h at an initial concentration of 20 mg L −1 for each contaminant. Radical–quenching experiments combined with electron paramagnetic resonance analysis revealed the involvement of 1 O 2 and •O 2 - , with a possible contribution from •OH. Notably, 1 O 2 showed the strongest apparent influence on sulfamethoxazole oxidation under the present alkaline conditions. Arsenic removal involved an initial As(III) oxidation step, followed by adsorption onto Fe-based sites and final immobilization through Fe/Ca–Si flocculation, rather than direct precipitation. Phosphate was primarily immobilized through rapid calcium-induced precipitation followed by incorporation into Fe/Ca–Si flocs. In the ternary sulfamethoxazole–As(III)–phosphate system, phosphate precipitation, organic oxidation, and arsenic immobilization exhibited distinct temporal separation. Matrix-effect experiments further showed that humic acid mainly inhibited As immobilization. Nevertheless, in a real-water matrix, 24-h removal efficiencies remained 92.1%, 99.5%, and 97.0% for SMX, phosphate, and As, respectively. These results demonstrated that Fe 0 @SiO 2 @nCaO 2 integrated complementary oxidation, precipitation, and immobilization pathways while maintaining effective performance under complex water-matrix conditions.
✓ 已验证
DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2025
·
IF 21.1
Teng Zong,Ming Tian,Chaojie Wang,Nanxin Wang,Jiachen Yang,Lin Li,Yujia Han,Xiaodong Wang
It is of great significance but challenge to achieve superior H 2 O splitting performance by tailoring active sites in novel Fe-based mixed oxides in order to boost H 2 O activation to achieve the oxidation of metallic Fe to Fe 3+ back into parent substrate rather than thermodynamically more favourable Fe 2+ (Fe-O v ) usually exhibiting low H 2 O activation in chemical looping water splitting (CLWS). Herein, we for the first time reported the performance of Ga-doped garnets (Y 3 Fe 2 Ga x Al 3-x O 12 abbreviated as YF 2 G x Al 3-x , x = 1 and 2) for CLWS which surpassed most of the state-of-the-art Fe-based oxides by virtue of marvelous peak H 2 production rate of 195.3 mL min −1 g −1 , H 2 productivity of 60.7 mL g −1 , 100 % H 2 purity and outstanding redox stability for YF 2 G 2 A 1 . It was clarified that Ga doping led to the formation of an interface with Fe 0 and Ga δ+ -O v in garnets, which synergistically improved H 2 O dissociation, leading to the direct oxidation of Fe 0 to Fe 3+ back into garnets and thus accounting for its prominent performance.
研究领域:
材料科学
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能源化学
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无机化学
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催化化学
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清洁能源技术
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF HAZARDOUS MATERIALS
·
2021
·
IF 10.588
Yiqiong Yang,Wenqing Ji,Xingyu Li,Huidong Lin,Hongjia Chen,Fukun Bi,Zenghui Zheng,Jingcheng Xu,Xiaodong Zhang
Tetracycline (TC) is a commonly used antibiotic that has gained wide spread notoriety owing to its high environmental risks. In this study, rich carbonyl-modified carbon-coated Fe 0 was obtained by pyrolysis of MIL-100(Fe) in an Ar atmosphere, and used to activate peroxymonosulfate (PMS) for the degradation of tetracycline in water. The roles of Fe 0 , carbon and surface carbonyl on PMS activation were investigated. Fe 0 continuously activated PMS, acted as a sustained-release source of Fe 2+ , and could effectively activate PMS to produce SO 4 •− , O 2 •− and •OH. Carbon was found to do responsible for electron transportation during the activation of PMS and slow down the oxidation of Fe 0 . The carbonyl group on the carbon surface layer was the active site of 1 O 2 , which explains the enhanced performance for TC degradation . When Ca = 0.1 g/L and C 0 = 0.4 mM, TC degradation rate reached 96%, which was attributed to the synergistic effect of radicals (i.e., SO 4 •− , O 2 •− , •OH) and non-radical (i.e., 1 O 2 ). Finally, the degradation pathway was proposed by combining density functional theory (DFT) calculations with liquid chromatography-mass spectrometry (LC-MS), toxicities of the intermediate products were also evaluated. All results show that carbonyl-modified carbon-coated Fe 0 possesses promising capacity for the removal of antibiotics from water.
研究领域:
环境科学
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材料科学
✓ 已验证
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2022
·
IF 16.744
Yanlong Wang,Jiang Xu,Kun Yang,Daohui Lin
Water scarcity is one of the most pressing global challenges and limits economic and social development. Multiple processes of current technologies for water purification are needed to meet water quality objectives due to their contaminant-specific removal capability. Here, we developed Fe 0 @SiO 2 @CaO 2 nanocomposite with three layers of core–shell structure that could achieve an array of water contaminants removal by oxidation, reduction, and flocculation. >99 % of 50 mg/L tetracycline, 20 mg/L pentachlorophenol, 450 mg/L Cd(Ⅱ), 20 mg/L Cr(Ⅵ), or 80 mg/L P (in form of PO 4 3− ) was removed by 2 g/L Fe 0 @SiO 2 @CaO 2 in 24 h. Moreover, Fe 0 @SiO 2 @CaO 2 (2 g/L) showed an excellent performance in turbidity removal (239 mg/L kaolinite suspension, removal rate > 99 %) and water decolorization (50 mg/L humic acid, removal rate > 93 %). Cd(II) and Cr(VI) could be reduced to Cd(0) and Cr(III), respectively, through electronic reduction reactions using Fe 0 and •H, which is formed during the reaction Fe 0 + 2H + →2•H + Fe 2+ ; Cd(Ⅱ) and the formed Cr(III) could coprecipitate with the formed orthosilicic acid and OH − . The removal of P was mainly resulted from the coordination with released Ca 2+ and iron compounds. Charge neutralization by nanocomposite and coagulation with the products from nanocomposite transformation were responsible for the kaolinite removal. Reduction by •H and Fe 0 , oxidation by •OH derived from the Fenton reaction, and/or coagulation accounted for the organic contaminant removal. This work provides a novel material that can be used to simultaneously remove a range of contaminants in wastewater treatment.
研究领域:
环境科学
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材料科学
✓ 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）