JOURNAL OF HAZARDOUS MATERIALS
·
2025
·
IF 11.3
Qian Guo,Zuxin Xu,Wenhai Chu,Yingying Zhou,Xiaoting Gao,Cheng Ye
Sewer overflows are a potential source of emerging contaminants to urban waters, posing a threat to ecosystems and human health. Herein, the performance and mechanism of ferrate(Ⅵ) (Fe(Ⅵ))/peroxymonosulfate (PMS), Fe(Ⅵ)/peroxydisulfate (PDS), and Fe(Ⅵ)/percarbonate (SPC) for the degradation of ofloxacin (OFL) in overflows were comparatively investigated. These systems achieved efficient degradation of OFL and the removal of conventional pollutants. Particularly, Fe(Ⅵ)/PMS showed better degradation performance for OFL with a degradation efficiency of 98.8 %. The dominant reactive oxygen species for OFL degradation in the Fe(Ⅵ)/PMS, Fe(Ⅵ)/PDS, Fe(Ⅵ)/SPC systems were singlet oxygen ( 1 O 2 ), sulfate radical (SO 4 · - ), and hydroxyl radical (·OH), respectively. High-valent iron species played an important role in the Fe(Ⅵ)/PMS and Fe(Ⅵ)/PDS systems. Notably, the synergistic effect of oxidation and in-situ coagulation played a key role in OFL degradation, which determined the superior performance of Fe(Ⅵ)/PMS. The formed flocs with Fe-O-P bond acted as a highway to promote the electron transfer from OFL to PMS, resulting in the efficient degradation of OFL in Fe(Ⅵ)/PMS system. Moreover, a same degradation pathway of OFL was found, and the toxicity of the degradation products was reduced, especially in the Fe(Ⅵ)/PMS system. This study provided a new strategy for overflows treatment.
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BULLETIN OF THE CHEMICAL SOCIETY OF JAPAN
·
2018
·Vol. 91
·期 6
·998-1007
·
IF 3.526
Zhang Xuezhi,Jia Shaoyi,Song Jia,Wu Songhai,Han Xu
Flocculation using Fe(II) instead of Fe(III) has been considered more efficient in the removal of As. However, excess Fe(II) used in the process always leaves substantial TFe [Fe(II)+Fe(III)] unutilized. We therefore developed three methods [the one-staged process (OS), the one-staged process with H2O2 (OSH) and the two-staged process (TS)] to remove As(III)/As(V) by Fe(II) (Fe:As = 2.0). Our results indicate that pH is an important factor that determines the utilization efficiency of TFe and the removal efficiency of As. In OS, the initial pH was adjusted before the reaction. At the optimal pHs of 10.0 and 11.0, the removal efficiencies of As(V) and TAs [As(III)+As(V)] could reach 84.0% and 66.7%, with only 61.9% and 80.2% TFe being utilized, respectively. In OSH, H2O2 was added after pH adjustment. After OS, pH was re-adjusted to the optimal values before the next 30 min reaction (TS). Compared with OS, the removal efficiencies of As could increase by more than 9% in OSH and TS at the optimal pHs. Besides, there is more than 10% improvement in the utilization efficiencies of TFe except at 12.0. Accelerating oxidation of Fe(II) or re-adjusting pH is therefore highly efficient for a more efficient removal of As from Fe(II)-rich groundwater.
研究领域:
环境科学
·
水处理工程
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KOREAN JOURNAL OF CHEMICAL ENGINEERING
·
2026
·
IF 3.4
Wang Xiaoqi,Yang Pengwei,Yu Linzhu,Jiang Haoxuan,Ma Jingxiang,Ma Xiangshuai,Ma Shuangchen
Electrochemical nitrogen reduction reaction (eN2RR) is a highly promising approach for ammonia synthesis under normal temperature and pressure conditions. However, its practical application is limited by the low activity and selectivity of the catalysts. In this study, a series of Fe-MOFs materials were prepared by hydrothermal method, and further sintered to obtain Fe@C materials. The electrocatalytic performance of these materials in eN2RR was systematically investigated. The results showed that MIL-53(Fe)-2 exhibited excellent catalytic activity at -0.4 V vs. RHE, with an ammonia production rate of 1.443 µg·h⁻¹·mg⁻¹ and a Faradaic efficiency of 5.972%. In contrast, the Fe@C material derived from MIL-53(Fe)-1, although having rapid activation characteristics within a narrow potential window, did not perform as well as the former. This work provides a new material strategy and experimental basis for the design of iron-based eN2RR catalysts.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2026
·
IF 19.7
Lei Wang,Jianpu Xing,Jianqiao Zhang,Weijun Chen,Mingyan Wang,Yan Li,Yongmin Cao,Wenjie Liu,Weibin Li,Yinghe Zhang,Lei Yang
Highly efficient synergistic catalysis is achieved by constructing a dual two-dimensional MoS 2 /ZnFe-layered double hydroxide composite (2D/2D MoS 2 @ZnFe-LDH) and coupling photocatalysis and Fenton-like process to address the drawbacks of the traditional Fenton-like system. The layered structure of ZnFe-LDH enables firm anchoring and uniform dispersion of Fe active sites within the layers without forming clusters, meanwhile enhancing mass transfer efficiency and accelerating both peroxymonosulfate (PMS) adsorption and reactive oxygen species desorption. The constructed 2D/2D heterojunction strengthens interfacial covalent bonding and compatibility, shortens the migration distance of photogenerated carriers, thereby significantly improving the charge separation efficiency, which accelerates the Fe(III)/Fe(II) cycle for sustainable catalysis across a broad pH range without Fe sludge aggregation. Comprehensive analysis of EPR, in-situ XPS, quenching and probe experiments, and DFT indicates that PMS is efficiently adsorbed onto Fe sites and reduced to generate SO 4 •- and •OH. Meanwhile, further characterization combining EPR, determination of surface Fe(II) concentration, in-situ photoelectrochemical and Raman measurements, XPS and DFT confirms that photogenerated electron can simultaneously reduce Fe(III) and promote radical desorption, thereby achieving sustainable catalysis. Hence, the system achieves complete phenol removal with a high synergistic index and figure of merit of 9.69 and 2.62 × 10 −10 mol·L −1 ·h −1 ·g −1 ·J −1 , respectively. It also operates efficiently in various complex water matrices and maintains stable operation over 24 h in the continuous-flow reactor, demonstrating strong anti-interference capability without any biological toxicity. In conclusion, this study proposes a new strategy to develop for developing high-performance and sustainable photo-Fenton-like dual-system.
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Nature Catalysis
·
2022
·Vol. 5
·期 6
·503-512
·
IF 40.706
Xiao Fei,Wang Qi,Xu Gui-Liang,Qin Xueping,Hwang Inhui,Sun Cheng-Jun,Liu Min,Hua Wei,Wu Hsi-wen,Zhu Shangqian,Li Jin-Cheng,Wang Jian-Gan,Zhu Yuanmin,Wu Duojie,Wei Zidong,Gu Meng,Amine Khalil,Shao Minhua
Proton exchange membrane fuel cells convert hydrogen and oxygen into electricity without emissions. The high cost and low durability of Pt-based electrocatalysts for the oxygen reduction reaction hinder their wide application, and the development of non-precious metal electrocatalysts is limited by their low performance. Here we design a hybrid electrocatalyst that consists of atomically dispersed Pt and Fe single atoms and Pt–Fe alloy nanoparticles. Its Pt mass activity is 3.7 times higher than that of commercial Pt/C in a fuel cell. More importantly, the fuel cell with a low Pt loading in the cathode (0.015 mg Pt cm −2 ) shows an excellent durability, with a 97% activity retention after 100,000 cycles and no noticeable current drop at 0.6 V for over 200 hours. These results highlight the importance of the synergistic effects among active sites in hybrid electrocatalysts and provide an alternative way to design more active and durable low-Pt electrocatalysts for electrochemical devices.
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JOURNAL OF HAZARDOUS MATERIALS
·
2019
·
IF 7.65
Binbin Shao,Hongyu Dong,Liying Feng,Junlian Qiao,Xiaohong Guan
Although several groups have made efforts to study micropollutants degradation by Fe(VI)/sulfite process, the mechanism is far from clear and warrants further investigation. Herein, the degradation kinetics and mechanism of selected micropollutants by sulfite (SO 3 2− )-activated Fe(VI) oxidation were systematically investigated. The oxidation rates of enrofloxacin (ENR) and phenol in Fe(VI)/sulfite process ranged from 0.151 s −1 to 6.18 s −1 at pH 6.5 and 8.0. Sulfite applied in multiple-addition mode improved the degradation efficiency of micropollutants with electron-rich moieties compared to the single-addition mode. Based on results of the quenching experiments and kinetic simulation, Fe(V) was identified as the predominant active oxidant at [SO 3 2− ]/[Fe(VI)] molar ratio of 0.1 to 0.3. However, both Fe(V) and SO 4 − / OH contributed to micropollutants oxidation at [SO 3 2− ]/[Fe(VI)] molar ratio ≥ 0.4 and their contributions were strongly dependent on the properties of micropollutants. The different degradation products of ENR in Fe(VI)/sulfite process at different sulfite dosages further supported the contribution of different active oxidants at different [SO 3 2− ]/[Fe(VI)] molar ratios. The toxicity of the reaction products of ENR towards Vibrio qinghaiensis sp.-Q67 decreased dramatically after Fe(VI)/sulfite treatment. The results of this work may promote the application of sulfite-activated Fe(VI) oxidation in water treatment.
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ACS Applied Materials & Interfaces
·
2017
·
IF 7.504
Huayu Chen,Shuxin Ouyang,Ming Zhao,Yunxiang Li,Jinhua Ye
Water splitting has been greatly limited by the sluggish kinetics of the oxygen evolution reaction (OER). High-oxidation-state metal species are required as the favorable active sites in OER. Here, amorphous Cox–Fe–B (x is the molar ratio of Co/Fe), Co–B, and Fe–B compounds were successfully synthesized as the oxygen evolution electrocatalysts. The calculation of turnover frequency (TOF) indicates that both the Co and Fe sites are active for OER. Cyclic voltammetry, X-ray photoelectron spectroscopy, and long-term stability curves were used to demonstrate that Fe can stabilize Co in a higher oxidation level and meanwhile promote the generation of OOH-like species (the key intermediates for OER). The reduced impedance for Co2–Fe–B (compared with that for Fe–B and Co–B) obtained from the electrochemical impedance spectra confirms the enhanced conductivity for the Co2–Fe–B. This optimal sample on Cu substrate shows a low overpotential of 0.298 V at the current density of 10 mA cm–2 with a decreased overpotential of 42 mV compared to that of Co–B. The Co2–Fe–B catalyst also exhibits a small Tafel slope of 62.6 mV/dec and good stability. The enhanced performance could be attributed to the synergistic effect of the increased population of high-oxidation-state metal–OOH species and the promoted conductivity of the catalyst. A solar-to-hydrogen energy conversion efficiency of 4.2% and a Faradaic efficiency of 97.2% can be achieved by connecting the HER and as-prepared OER electrodes to a crystalline silicon solar cell.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2024
·
IF 8.1
Shishun Wang,Shuang Gai,Kui Cheng,Zhuqing Liu,Markus Antonietti,Fan Yang
The degradation efficiency of organic contaminants using Fenton-like system based on Fe(II) and peroxymonosulfate (PMS) has been hindered by the rapid transformation from Fe(II) to Fe(III) and the slow regeneration of Fe(II). To address this challenge, artificial humic acid (AHA) derived from biomass was incorporated into Fe(III)/PMS system to build AHA/Fe(III)/PMS system. The results demonstrated that the degradation rate of atrazine (ATZ) in AHA/Fe(III)/PMS system (98.83%) is significantly superior to those in Fe(III)/PMS (16.51%) and AHA/PMS system (41.76%) within 90 min. Furthermore, Fe(II) measurement experiments revealed that AHA exhibited more significant iron-reducing potential. The analysis of FTIR, 3D-EEM, and liquid NMR indicated that AHA possessed more structures with reductive potential in comparison to commercial humic acid (CHA) and humic acid extracted from lignite (LHA). The results of persistent free radicals indicated that CHA possessed oxidative potential, which also accounted for the lowest Fe(II) concentration in those system containing CHA. Furthermore, quenching experiments, EPR analysis, and PMSO probe analysis have indicated the presence of reactive species such as •OH, SO 4 •- , and Fe(IV) within AHA/Fe(III)/PMS system. The degradation products from ATZ were identified and determined to exhibit reduced toxicity relative to parent compound. Collectively, these findings presented an in-depth understanding to reactivate Fe(III)/PMS system, offering a promising alternative strategy for efficient degradation of organic pollutants in water treatment processes.
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WATER SCIENCE AND TECHNOLOGY
·
2024
·Vol. 89
·期 7
·1682-1700
·
IF 2.5
Zhang Longbin,Gao Jianxiong,Liu Yulong,Zhou Zhengyuan,Sheng Xianxian,Li Dexiao,Chen Yuantian,Lyu Shuguang
View large Download slide View large Download slide Close modal In this research, ascorbic acid (AA) was used to enhance Fe(II)/Fe(III)-activated permonosulfate (PMS) systems for the degradation of fluoranthene (FLT). AA enhanced the production of ROS in both PMS/Fe(II) and PMS/Fe(III) systems through chelation and reduction and thus improved the degradation performance of FLT. The optimal molar ratio in PMS/Fe(II)/AA/FLT and PMS/Fe(III)/AA/FLT processes were 2/2/4/1 and 5/10/5/1, respectively. In addition, the experimental results on the effect of FLT degradation under different groundwater matrixes indicated that PMS/Fe(III)/AA system was more adaptable to different water quality conditions than the PMS/Fe(II)/AA system. was the major reactive oxygen species (ROS) responsible for FLT removal through the probe and scavenging tests in both systems. Furthermore, the degradation intermediates of FLT were analyzed using gas chromatograph-mass spectrometry (GC-MS), and the probable degradation pathways of FLT degradation were proposed. In addition, the removal of FLT was also tested in actual groundwater and the results showed that by increasing the dose and pre-adjusting the solution pH, 88.8 and 100% of the FLT was removed for PMS/Fe(II)/AA and PMS/Fe(III)/AA systems. The above experimental results demonstrated that PMS/Fe(II)/AA and PMS/Fe(III)/AA processes have a great perspective in practice for the rehabilitation of FLT-polluted groundwater. The effect of AA on the circulation between Fe(II) and Fe(III) in the PMS system was investigated. SO 4 •− was the primary ROS in PMS/Fe(II)/AA and PMS/Fe(III)/AA systems. The effect of actual groundwater matrixes on FLT removal was investigated. The possible degradation pathways of FLT were proposed. Effective degradation of FLT in actual groundwater was achieved.
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MATERIALS CHEMISTRY AND PHYSICS
·
2017
·
IF 2.084
Mingming Zou,Fengqiang Xiong,Ayyakannu Sundaram Ganeshraja,Xiaohua Feng,Chuanxi Wang,Tiju Thomas,Minghui Yang
Iron (III) and nitrogen co-doped mesoporous TiO 2 microspheres (Fe-N-TiO 2 ) are prepared using a self-assembly based solvothermal process followed by an ammonothermal method. Among all samples, 1 mol.% of Fe dopants and 500 °C nitridation (for 2 h) gives the highest visible light photoactivity. Results imply that the Fe 3+ /Fe 2+ dopant trap energy level introduced within the band gap in mildly Fe (∼1 at%) doped TiO 2 and the mesoporous nature of the material, both aid in the observed catalytic performance. Subjecting Fe-TiO 2 samples to ammonothermal process induces oxygen vancancies, and substitutional and interstitial N. This reduces optical band gap, and introduces local states. The lower band gap and local states together aid in the absorption of visible light and separation of charge carriers. Co-dopants are distributed uniformly in the best photocatalysts . The active species generated in the photocatalytic system is shown to be singlet molecular oxygen ( 1 O 2 ) using selective radical quenchers.
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ENVIRONMENTAL RESEARCH
·
2025
·
IF 7.7
Ning Liu,Ti-Bo Fang,Ling-Xi Zhao,Na Li,Xiang-Feng Chen,Ru-Song Zhao
Naphthalene acetic acid (NAA) is an auxin plant growth regulator (PGR) and widely used to regulate the growth process of plants. As excessive NAA enter the environment, it damages the ecological environment and endangers human life and health. Layered bimetallic hydroxides (LDHs) are widely used for the adsorption of pollutants due to their large surface area and excellent structural properties. Based on the classical Fe 3 O 4 @MgAl-LDH material, Fe 3 O 4 @FeMgAl-LDHs were synthesized by adding different contents of Fe element to adsorb NAA in water. The morphology and properties of Fe 3 O 4 @FeMgAl-LDHs and the effect of Fe on adsorption efficiency were studied. The adsorption process and adsorption mechanism of NAA were analyzed. The results indicated that the content of Fe element will affect the adsorption effect of NAA by influencing the specific surface area and adsorption sites of Fe 3 O 4 @FeMgAl-LDHs. The maximum adsorption capacity for NAA can reach 330.1 mg/g when the proportion of Fe is 0.50. Exploring the adsorption mechanism, Fe 3 O 4 @FeMgAl-LDHs achieved efficient removal of NAA through hydrogen bonding, van der Waals forces, anion exchange, and electrostatic interactions. The adsorption efficiency of various PGRs were deeply explored. Fe 3 O 4 @FeMgAl-LDH (Fe-0.50) has good adsorption and regeneration ability for various PGRs. Therefore, by exploring the influence of different Fe ratios on the adsorption efficiency of the Fe 3 O 4 @FeMgAl-LDH, the adsorption performance of the material can be improved, making it have greater application advantages in wastewater treatment containing drugs.
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IEEE SENSORS JOURNAL
·
2024
·Vol. 24
·期 23
·38685-38692
·
IF 4.3
Shan Tang,Jingcai Xu,Xinqin Lu,Weijie Chen,Hongwei Chen,Bo Hong,Xinqing Wang
Metal-organic frameworks (MOFs) have potential applications in gas sensing due to their abundant porosity and unique surface properties. In this study, Fe2O3 hexagonal spindles (Hgs) derived from MIL-88B(Fe) were successfully prepared using an oil bath method, followed by calcination treatment at an optimized temperature of
$450~^{\circ }$
C. The high-purity porous Fe2O3 Hgs showed excellent acetone gas-sensing performance in the range of 0.4–50-ppm acetone concentration. The Fe2O3 Hgs-450 obtained the high sensing response (Ra/Rg =23,
$\tau _{\text {res}} =17$
s, and
$\tau _{\text {rec}} =2059$
s), excellent selectivity, and stability over 120 days to 10-ppm acetone at an operating temperature of
$220~^{\circ }$
C. The sensing response value was still 1.88 even at 0.4-ppm acetone and the theoretical detection limit (DL) was calculated to reach 3.59-ppb acetone. These excellent acetone gas-sensing properties were attributed to the uniform porous structure, abundant adsorbed oxygen, and small grain size of Fe2O3 Hgs, making them an excellent candidate for screening diabetic patients through exhaled gas analysis.
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