WATER RESEARCH
·
2021
·
IF 11.236
Chenying Zhou,Peng Zhou,Minglu Sun,Yang Liu,Heng Zhang,Zhaokun Xiong,Juan Liang,Xiaoguang Duan,Bo Lai
The sluggish kinetics of Fe(II) recovery strongly impedes the scientific progress of Fenton reaction (Fe(II)/H 2 O 2 ) towards practical application. Here, we propose a novel mechanism that metal-free nitrogen-doped carbon nanotubes (NCNT) can enhance Fenton chemistry with H 2 O 2 as electron donors by elevating the oxidation potential of Fe(III). NCNT remarkably promotes the circulation of Fe(III)/Fe(II) to produce hydroxyl radical ( • OH) with excellent stability for multiple usages (more than 10 cycles) in the NCNT/Fe(III)/H 2 O 2 system. Although carbonyl on NCNT can act as the electron supplier for Fe(III) reduction, the behavior of NCNT is distinct from common reductants such as hydroxylamine and boron. Electrochemical analysis and density functional theory calculation unveil that nitrogen sites of NCNT can weakly bind with Fe(III) to elevate the oxidation potential of Fe(III) (named near-free Fe(III), primarily FeOH 2+ ) at pH ranging from 2.0 to 4.0. Without inputs of external stimulations or electron sacrificers, near-free Fe(III) can promote H 2 O 2 induced reduction of Fe(III) to initiate Fenton chain reactions for long-lasting generation of • OH. To our delight, it is a common property of N-doped carbon materials (e.g., graphene, carbon nanofibers, and acetylene black), our research thus provides a novel, sustainable, and green strategy for promoting Fenton chemistry.
研究领域:
环境科学
·
材料科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2022
·
IF 16.744
Huihui Liu,Jie Zhao,Yu Wang,Yanlin Wu,Wenbo Dong,Minghua Nie,Xiaoning Wang
Peroxymonosulfate (PMS) is more cost-effective than peroxydisulfate (PDS) and has drawn great attention presently. Low efficiency of Fe(III)/Fe(II) cycle is a great intrinsic drawback of Fenton-like system, which extremely limits its widespread application. In this study, sinapic acid (SA) as a natural and environmental-friendly reductant, was applied to enhance Fe(III)/Fe(II) cycle in PMS/Fe(III) system. The removal efficiency of methyl paraben (MEP) was 98.3% (7.2 × 10 −4 s −1 ) within 90 min in the modified system, and the k obs was 18 times higher than in PMS/Fe(II) system. For the active species identification, SO 4 − , HO and Fe(Ⅳ) were all responsible for MEP degradation, while SO 4 − was the dominant radical. The role of SA in SA/PMS/Fe(III) system was investigated, Fe(III) was reduced to Fe(II) and SA was oxidized to quinone species in this reaction process. The concentration of Fe(II) and the activation efficiency of PMS were all improved with SA concentration increasing from 5 to 20 μM, and the contribution of active species for MEP degradation were estimated. The effect of initial pH and common anions were also investigated. For the effect of anions, HCO 3 − and SO 4 2− presented inhibition effect on MEP removal, and with the HCO 3 − concentration increasing 1–10 mM the inhibition decreased. Low concentration Cl − promoted MEP degradation while Cl − with higher concentration exhibited inhibition. And NO 3 − was almost no effect on MEP degradation.
研究领域:
环境科学
·
化学
✓ 已验证
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2024
·
IF 8.1
Xinyu Wang,Shiqi Chen,Can Liu,Jiapeng Yue,Zhiwei Yang,Qian Ye,Hao Xu,Yujian Zhang,Xinyi Xing,Jing Zhang
In this study, the charge transfer capability of MoO 2 materials was significantly improved by introducing carbon materials in situ. The resulting MoO 2 -C material could accelerate the Fe(III)/Fe(II) redox cycle and promote the continuous generation of reactive oxygen species in Fenton-like system. The results suggested that MoO 2 -C exhibited significant co-catalytic activity against a variety of pollutants. Meanwhile, the mechanisms behind the Fe(III)/Fe(II) cycle and reactive oxygen species generation were clarified. Analysis indicated that the incorporation of carbon material provided a reduction active site for the reduction of Fe(III) to Fe(II) on the surface of molybdenum oxide, and also reduced the thermodynamic energy barrier associated with Fe(III) reduction. Furthermore, quenching experiments and electron paramagnetic resonance (EPR) technology demonstrated that hydroxyl radicals ( ∙ O H ) and singlet oxygen ( 1 O 2 ) rapidly degrade the target pollutants. Fe(II) was verified as the primary component responsible for peroxymonosulfate (PMS) and peroxydisulfate (PDS) activation. Additionally, the main generation pathway for 1 O 2 differed between the MoO 2 -C/Fe(III)/PDS and MoO 2 -C/Fe(III)/PMS systems. This study provides a new strategy to improve the iron reduction properties of metal oxide materials.
研究领域:
环境科学
·
催化化学
✓ 已验证
产品关联
DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2019
·
IF 14.229
Peng Zhou,Jing Zhang,Zhaokun Xiong,Yang Liu,Xiaowei Huo,Xin Cheng,Wenshu Li,Feng Cheng,Yongli Zhang
Hydroxylated C 60 Fullerene (Fullerol) induced photochemical production of reactive oxygen species (ROS, e.g. singlet oxygen ( 1 O 2 ) and hydroxyl radical ( OH)) is a slow process, and the role of its surface groups other than high water-solubility is still lack of investigation. In this study, we demonstrate Fullerol can promote Fe(III)/Fe(II) cycles to degrade dimethyl phthalate (DMP) in Fe(III)/H 2 O 2 Fenton system as both an electron donor and an electron-transfer mediator. At acidic condition, the formation of carbonyl and carboxyl via pinacol rearrangement and subsequent keto-enol isomerization can produce cage-opened structure of Fullerol, resulting in the pH-dependent formation of Fe(III)-Fullerol complex. Two pathways of Fe(II) recovery via intramolecular electron transfer of Fe(III)-Fullerol complex to enhance Fe(III)/H 2 O 2 Fenton oxidation were proposed: 1) Fullerol direct reduces Fe(III) into Fe(II) as an electron donor in dark, and it was strongly enhanced under visible light irradiation; 2) Fullerol mediates electron transfer from electron donor (e.g. hydrogen peroxide and organics) to Fe(III) in visible light condition. Furthermore, DMP degradation pathway was proposed based on variation of main intermediates.
研究领域:
环境科学
·
化学
✓ 已验证
产品关联
DOI
高影响因子
Journal of Environmental Chemical Engineering
·
2023
·
IF 7.7
Zhongmou Liu,Pan Zhang,Xiangyu Zhao
Reduced graphene oxide supported with ferric ion (Fe(III)-rGO) was successfully prepared, and performed as an excellent catalyst to activate hydrogen peroxide (H 2 O 2 ) and peroxymonosulfate (PMS) for isoprothiolane (IPT) degradation. IPT removal efficiency was proven to be better in the Fe(III)-rGO/H 2 O 2 /PMS system (96.2%) than in the Fenton-like reaction (72.6%) and PMS-AOP (80.0%) individually. X-ray photoelectron spectroscopy showed that Fe(III) was reduced in Fenton-like reaction, and the reduced Fe(II) played a crucial role in the subsequent PMS-AOP. The combination of the Fenton-like reaction and PMS-AOP involved the valence state conversion of Fe, which consequently improved Fe(III)-rGO utilization rate and IPT removal efficiency. Fe(III)-rGO remarkably boosted the Fe(III)/Fe(II) cycle and generated superoxide radical (O 2 − •) and singlet oxygen ( 1 O 2 ) in the Fe(III)-rGO/H 2 O 2 /PMS system. Fe(III)-rGO acts as the electron transfer mediator; thus, promoting electron transfer from IPT to H 2 O 2 and PMS and accelerating the generation of active species. Fe(IV) with high oxidation performance was formed in PMS-AOP and efficiently removed some of the IPT. IPT removal efficiency was more than 90% at a pH range of 3–11; this efficiency could be maintained above 50% even after five consecutive degradation experiments, exhibiting excellent stability and reusability of Fe(III)-rGO. Additionally, iron sludge formation was greatly reduced because of the stable chemical bonding of iron ions to the rGO surface. Therefore, this study provides a new multisystem and synergistic approach for the efficient removal of organic micro-pollutants from water.
研究领域:
环境科学
·
化学工程
✓ 已验证
产品关联
DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2022
·
IF 24.319
Xianhu Long,Zhaokun Xiong,Rongfu Huang,Yahan Yu,Peng Zhou,Heng Zhang,Gang Yao,Bo Lai
Herein, an electrochemical (EC) system was applied as “co-catalyst” to enhance the activation of peroxymonosulfate (EC/Fe(III)/PMS) for efficient Sulfamethoxazole (SMX) degradation. The cathodic reduction reaction can facilitate electron transfer to Fe(III) and trigger the sustainable Fe(III)/Fe(II) redox cycle. Unexpectedly, in addition to hydroxyl radical ( OH) and sulfate radical (SO 4 •− ), non-radicals mechanism including singlet oxygen ( 1 O 2 ) and Fe(IV) were also found involved in EC/Fe(III)/PMS system. The degradation of SMX in EC/Fe(III)/PMS system was accomplished by the collaboration of radicals and non-radicals oxidation . The generation routes and mechanisms of involved reactive oxygen species (ROS) were explored. The relative contributions of OH, SO 4 •− , and nonradical species for the degradation of SMX were calculated to 4.75 %, 25.31 %, and 69.94 %, respectively. Besides, multiple degradation pathways of SMX were proposed by identifying the formed byproducts. The EC/Fe(III)/PMS process could efficiently degrade SMX under the influence of co-existing ions and inactivate pathogens in the wastewater.
研究领域:
环境科学
·
化学
✓ 已验证
产品关联
DOI
高影响因子
Environmental Technology & Innovation
·
2024
·
IF 6.7
Binbin Wu,Zheng Wang,Yannan Jia,Nannan Xu,Lisha Liao,Chenyue Zhang,Zhiwei Wang,Yuanxiang Shan,Wanting Feng,Hongqin Xue
Biochar loaded with bimetallic Fe/Mo (Fe/Mo-BC) was prepared as a cost-effective catalyst for the degradation of organic matter by activated peroxydisulfate, in which MoO 2 was used as a co-catalyst to enhance Fe 2+ /Fe 3+ cycling. The tetracycline-degradation efficiency of the system reached 74.49 % within 10 min, and it showed high removal rates over a wide pH range (3–9). Quenching experiments and electron paramagnetic resonance analyses showed that 1 O 2 , •OH, O 2 • - , and SO 4 • − produced by the Fe/Mo-BC/PDS system are involved in tetracycline degradation, with 1 O 2 and •OH being the dominant active substances. X-ray photoelectron spectroscopy analysis revealed that Mo(IV) reduces Fe 3+ to Fe 2+ and oxidizes itself to Mo(VI). In addition, the Fe/Mo-BC remained stable and could be recycled three times, indicating the feasibility of this system for practical applications. The possible pathways of TC degradation by this system were investigated by LC-MS and DFT calculations. Thus, the present study provides a feasible strategy for the use of biochar-loaded bimetallic materials and PDS for the degradation of organic matter.
研究领域:
环境科学
·
污染控制
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2021
·
IF 19.503
Leiduo Lai,Peng Zhou,Hongyu Zhou,Minglu Sun,Yue Yuan,Yang Liu,Gang Yao,Bo Lai
Coupling dithionite (DNT) with FeVO 4 induced PMS activation (FeVO 4 /PMS/DNT) effectuates fast heterogeneous Fe(III) reduction to generate multitudinous reactive oxygen species (ROS) for fast degradation of carbamazepine (2.5 mg/L, >90 % degradation efficiency within 300 s) in batch mode. The Fe(III)/Fe(II) circulation propelled by DNT and reduced V species experiences two stages. DNT induces SO 2 − generation, which is a highly active species with strong reducibility for Fe and V reduction. The reduced V species donate electrons to ≡Fe(III) via Fe-O-V bond rather than directly react with PMS, implying introducing polyvalent V to modulate Fe-based materials intensifies DNT utilization and alleviates ROS quenching effects. Moreover, FeVO 4 crystalline form regains after reaction, and FeVO 4 /PMS/DNT system has an excellent reutilization and strong resistance to natural waters. Our discovery sheds new light on acceleration of heterogenous Fe(III)/Fe(II) circulation to promote Fenton-like oxidation , it may be a long-lasting strategy for water remediation.
研究领域:
环境科学
·
化学工程
✓ 已验证
DOI
高影响因子
APPLIED ORGANOMETALLIC CHEMISTRY
·
2021
·Vol. 36
·期 3
·e6556
·
IF 4.105
Wen-Jing Qiu,Ming-Wu Gao,Qi Chen,Ao Zheng,Yi-Jia Shi,Xin Liu,Juan-Hong Li,Guo-Liang Dai,Yang Hu,Zi-Xia Lin
Under normal temperature and pressure, a novel improved Fenton system that was named MHACF-MOF-808(Zr) was constructed after the introduction of Pd/MOF-808(Zr) and H 2 to solve the inherent problem of the production of iron sludge in the classic Fenton system. Only trace amount of Fe II was required during the whole reaction because Fe III could be rapidly reduced by the active hydrogen derived from the adsorption and activation of H 2 on the surface of Pd/MOF-808(Zr) composite. The concentration of Fe II could be maintained more than 10 μM. The removal of target pollutant sulfamethazine in this system was mainly relied on the degradation of ·OH verified by both of the direct detection and indirect inhibition (using methanol). By using the calculation of Laplacian bond order, the degradation pathway of sulfamethazine followed by the cleavage of N S bond. This prediction was verified by the detection of intermediate products. Only 21% sulfamethazine could be degraded after 3-h reaction in the classic Fenton reaction system, while it could be thoroughly degraded in 1.5 h in the MHACF-MOF-808(Zr) system. The influence of main parameters on the degradation effect of sulfamethazine, such as initial pH, the flow of H 2 , dosage of Pd/MOF-808(Zr), concentration of sulfamethazine, ferrous, and hydrogen peroxide, were systematically studied. Based on the relative stability of Pd/MOF-808(Zr) confirmed by the morphological characterization, sulfamethazine could be efficiently degraded in the MHACF-MOF-808(Zr) system.
研究领域:
环境科学
·
化学工程
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 13.2
Zhipeng Zhang,Rui Liu,Wei Zheng,Yaqiong Lan,Yongmei Li,Lujun Chen
In this study, a ternary co-fermentation system was developed using iron-phosphorus precipitates (FePs)-bearing sludge, peroxydisulfate (PDS), and corn gluten meal (CGM) to activate PDS through a microbe-mediated endogenous iron cycle, thereby promoting phosphorus (P) release and acidogenesis. Fe(II) was released along with P via the dissolution of Fe(II)Ps, resulting from Fe(III)Ps bioreduction. Subsequently, the released Fe(II) induced PDS activation, which avoided the negative impact of external activators on P release by precipitation with P. The optimal PDS dosage for ternary co-fermentation was 0.2 mM/g TSS. At this dosage, P release efficiency increased from 27.3 % (sludge-only group) to 71.6 % and volatile fatty acids (VFAs) production increased from 41.0 (sludge-only group) to 158.5 mg COD/g VSS. SO 4 ·− and ·OH generated through PDS activation disintegrated sludge flocs to promote encapsulated Fe(II)Ps dissolution and organics release. The concentration of soluble chemical oxygen demand in the sludge-CGM-PDS group was 4.4 times greater than that in the sludge-only group. The increased content and biodegradability of hydrolysates (e.g., protein-like, tryptophan-like, and tyrosine-like substances) contributed to the enrichment of hydrolytic-acidogenic bacteria, resulting in a relative abundance of 40.7 %. Unclassified_c__Ignavibacteria , Clostridium , and Rubrivivax were the dominant hydrolytic-acidogenic biomarkers, which enhanced the intracellular metabolisms of glycolysis, amino acid degradation, and acetogenesis, leading to notable increases in VFAs yields. The relative abundance of phosphate acetyltransferase, a key enzyme in acetate biosynthesis, increased by 8.9 %, thus facilitating acetogenesis. In addition, unclassified_c__Ignavibacteria , as putative iron reducers, were the primary microbes mediating endogenous iron reduction. This study provides valuable insights into the PDS self-activation mechanism and microfloral traits during ternary co-fermentation, contributing to the valorization of FePs-bearing sludge waste.
研究领域:
环境工程
·
微生物学
·
废水处理
✓ 已验证
产品关联
DOI
高影响因子
Catalysts
·
2025
·Vol. 15
·期 7
·680
·
IF 4
Jiayi He,Ge Song,Akhtar Islam,Minghua Zhou
Sulfamethazine (SMT) is an antibiotic with good antimicrobial effect and is widely used to treat human and livestock diseases. Though the degradation of SMT by the conventional Fenton and electro-Fenton (EF) processes is efficient, it is limited by a narrow pH and iron sludge generation. Herein, we constructed a cost-effective EF system with the synergistic effect of zero-valent iron (Fe0) and sulfite (Fe0-EF/Sulfite), and key parameters such as applied current, catalyst dosing, sulfite dosage, and initial pH were optimized. Under the optimal conditions (Fe0dosing of 50 mg/L, sulfite dosage of 1.5 mM, current of 40 mA, and pH of 3), the removal efficiency of 10 mg/L SMT reached 100% within 30 min, and the degradation rate constant reached 0.194 min−1. Electron paramagnetic resonance (EPR) analysis and quenching experiments confirmed the generation of various reactive oxygen species (ROS), such as•OH, SO4−, O2−, and1O2, which significantly improved the pollutant removal efficiency. Sulfite accelerated iron cycling and inhibited the formation of iron sludge, thus broadening the pH range of the reaction from three to eight and overcoming the limitations of the conventional EF process. The Fe0-EF/Sulfite system performs cost-effectively at a wide pH range, providing an efficient and low-carbon solution for environmental pollution remediation with broad application prospects.
研究领域:
环境科学
·
环境工程
·
水污染治理
·
高级氧化技术
·
药物代谢
·
环境化学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF HAZARDOUS MATERIALS
·
2025
·
IF 11.3
Yiqiao Zhang,Yanshi Zhang,Huan Cheng,Chunhua Xu
Slow iron cycling is an important factor limiting the reactivity of zero-valent iron (ZVI). Developing novel strategies to facilitate iron cycling is vital for the ZVI practical application. This study reports a novel interfacial slow-release reduction strategy for synthesizing L-ZVI with excellent performance by adding L-ascorbic acid 2-phosphate sesquimagnesium salt hydrate (AAPS). Experiments revealed that AAPS slowly released ascorbic acid via acid-catalyzed hydrolysis, thereby using reduction to promote Fe(III)/Fe(II) cycling, a process that regulates iron cycling while preventing low utilization by direct adding reductants. The enhanced content of Fe(II) and self-corrosion of L-ZVI facilitated the release of Fe(II) into the solution. Electrochemical experimental and comparisons of hydrogen production demonstrated that L-ZVI exhibited exceptional electron transfer and selectivity capacity. The strategy alters the electronic structure of L-ZVI, lowers work function, and shifts the band center upward. Cr (VI) was chosen as the model contaminant to investigate the reactivity of L-ZVI. L-ZVI can remove Cr (VI) within 7 min completely, exhibiting a reaction rate constant ( k obs ) of 0.6809 min⁻¹ , which was 154.75-fold higher than that of ZVI (0.0044 min⁻¹) and significantly surpassing the performance of other reported water treatment materials. This article presents a novel strategy for developing efficient iron-based materials.
研究领域:
环境科学
·
材料科学
·
化学工程
·
水处理技术
✓ 已验证
DOI
PubMed
高影响因子
危险品化学品经营许可证（带存储）