APPLIED CATALYSIS B-ENVIRONMENTAL
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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.
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ENVIRONMENTAL SCIENCE & TECHNOLOGY
·
2023
·
IF 11.4
Jinzhao Wang,Di Huang,Fengxia Chen,Jianhua Chen,Hongyu Jiang,Yifan Zhu,Chuncheng Chen,Jincai Zhao
Fe(III) and carboxylic acids are common compositions in atmospheric microdroplet systems like clouds, fogs, and aerosols. Although photochemical processes of Fe(III)–carboxylate complexes have been extensively studied in bulk aqueous solution, relevant information on the dynamic microdroplet system, which may be largely different from the bulk phase, is rare. With the help of the custom-made ultrasonic-based dynamic microdroplet photochemical system, this study examines the photochemical process of Fe(III)–citric acid complexes in microdroplets for the first time. We find that when the degradation extent of citric acid is similar between the microdroplet system and the bulk solution, the significantly lower Fe(II) ratio is present in microdroplet samples due to the rapider reoxidation of photogenerated Fe(II). However, by replacing citric acid with benzoic acid, no much difference in the Fe(II) ratio between microdroplets and bulk solution is observed, which indicates distinct reoxidation pathways of Fe(II). Moreover, the presence of •OH scavenger, namely, methanol, greatly accelerates the reoxidation of photogenerated Fe(II) in both citric acid and benzoic acid situations. Further experiments reveal that the high availability of O2 and the citric acid- or methanol-derived carbon-centered radicals are responsible for the rapider reoxidation of Fe(II) in iron–citric acid microdroplets by prolonging the length of HO2•- and H2O2-involved radical reaction chains. The results in this study may provide a new understanding about iron–citric acid photochemistry in atmospheric liquid particles, which can further influence the photoactivity of particles and the formation of secondary organic aerosols.
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ACS Nano
·
2019
·
IF 13.903
Xiang Ao,Wei Zhang,Zhishan Li,Jian-Gang Li,Luke Soule,Xing Huang,Wei-Hung Chiang,Hao Ming Chen,Chundong Wang,Meilin Liu,Xiao Cheng Zeng
Single-atom catalysts (SACs) have emerged as one of the most promising alternatives to noble metal-based catalysts for highly efficient oxygen reduction reaction (ORR). While SACs can offer notable benefits in terms of lowering overall catalyst cost, there is still room for improvement regarding catalyst activity. To this end, we designed and successfully fabricated an ORR electrocatalyst in which atomic clusters are embedded in an atomically dispersed Fe–N–C matrix (FeAC@FeSA–N–C), as shown by comprehensive measurements using aberration-corrected scanning transmission electron microscopy (AC-STEM) and X-ray absorption spectroscopy (XAS). The half-wave potential of FeAC@FeSA–N–C is 0.912 V (versus reversible hydrogen electrode (RHE)), exceeding that of commercial Pt/C (0.897 V), FeSA–N–C (0.844 V), as well as the half-wave potentials of most reported non-platinum-group metal catalysts. The ORR activity of the designed catalyst stems from single-atom active centers but is markedly enhanced by the presence of Fe nanoclusters, as confirmed by both experimental measurements and theoretical calculations.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2018
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IF 3.927
Haoran Dong,Yujun Cheng,Yue Lu,Kunjie Hou,Lihua Zhang,Long Li,Bin Wang,Yaoyao Wang,Qin Ning,Guangming Zeng
This study examined the toxicities of Fe/Ni and starch-stabilized Fe/Ni (S-Fe/Ni) nanoparticles (NPs) toward Escherichia coli . The inactivation of E. coli by Fe/Ni NPs was concentration- and time-dependent. Fe/Ni NPs exhibited a stronger toxicity than the bare Fe 0 NPs (i.e., Ni = 0 wt%), revealing that the loading of Ni increased the toxicity of Fe 0 NPs. However, there was no positive correlation between Ni content and the toxicity of Fe/Ni NPs when Ni content increased from 1 wt% to 5 wt%. The starch coating could alleviate the toxicity of Fe/Ni NPs, depending on starch concentration. Transmission Electron Microscopy analysis demonstrates that membrane disruption and cellular internalization of NPs occurred for E. coli after exposure to the Fe/Ni NPs. The NPs might have reacted with the carboxyl, ester and amine groups on the cell surface, as indicated by the Fourier Transform Infrared Spectroscopy analysis. However, the S-Fe/Ni NPs did not cause obvious membrane disruption of the cells due to the effect of starch coating, which inhibited the close contact of NPs with cells by providing electrostatic repulsion and steric hindrance. Besides, the addition of N-Acetyl-L-cysteine, as a potent scavenger for reactive oxygen species (ROS), remarkably reduced the toxicities of both Fe/Ni and S-Fe/Ni NPs, which indicated that the ROS-induced oxidative stress should be the primary mechanism for the inactivation of E. coli . The aging experiments evidenced that both Fe/Ni and S-Fe/Ni NPs would lose their toxic potential over time, posing less threat to the environment in the long term.
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Surfaces and Interfaces
·
2024
·
IF 5.7
Pengfei Zhu,Mengrong Geng,Shuang Qin,Heyang Cao,Zhenhong He,Xinhua Gao,Chuanyi Wang
The conversion of CO 2 into chemical products or fuels of great value always remains an outstanding challenge. Here, we report a heterojunction Fe@C/Ni 2 P composite catalyst obtained by preparing MIL-100(Fe) derived Fe@C confined Ni 2 P nanoparticles, which is applied to photothermal catalytic CO 2 hydrogenation with H 2 O. Without adding any sacrificial agents or co-catalysts, the optimal Fe@C/Ni 2 P sample shows higher yields for CO 2 -to-C 2 H 6 and CO 2 -to-CO yield of 5.83 μmol g −1 h −1 and 179.9 μmol g −1 h −1 than that of pristine Fe@C and Ni 2 P, respectively. The experimental results indicated that the obtained Fe@C/Ni 2 P can act as catalytic sites to adsorb, activate, and convert CO 2 under low-intensity LED light irradiation (420 nm) with a temperature of 200 ℃. The physical structure, photochemical properties and energy band structure of the Fe@C/Ni 2 P composite catalysts were investigated by XRD, XPS, FT-IR, TEM, BET, respectively. Furthermore, the reaction pathway of Fe@C/Ni 2 P photothermal catalytic CO 2 hydrogenation with H 2 O to C2 products and CO were systematically analyzed by in situ infrared spectroscopy (DRIFTS).
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CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Haiyang Xie,Dan Tang,Yanjuan Zhang,Zuqiang Huang,Huayu Hu,Qian He,Hongbing Ji,Tao Gan
The design of non-noble metal single-atom catalysts (SACs) with superior performance for semi-hydrogenation of alkynol to alkenol is remarkable but challenging. Herein, fluorine-tuned Fe SACs supported on N, F-codoped carbon (Fe 1 -NFC) with a Fe-N 4 F 1 structure is successfully prepared via a complexation method. The axial F-doping can modulate the electronic structure of the metalloporphyrin-like active sites (Fe-N 4 ), promoting the transfer of electrons from Fe atoms to F atoms to form electron-deficient Fe δ+ species. As a result, the Fe 1 -NFC catalyst shows a remarkable activity for the semi-hydrogenation of 2-methyl-3-butyn-2-ol to 2-methyl-3-buten-2-ol under mild conditions, with a TOF of 9163 h −1 and a selectivity of 96 % at 97 % conversion, both much higher than that of the Fe SACs supported on N-doped carbon (Fe 1 -NC). Density functional theory (DFT) calculations reveal that the excellent catalytic activity is attributed to the interfacial electronic effect of Fe species induced by axial F-doping, thereby enhancing the exothermic adsorption of alkynol on the Fe-N 4 F 1 structures and accelerating the desorption of alkenol to against the overhydrogenation.
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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.
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JOURNAL OF HAZARDOUS MATERIALS
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2023
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IF 13.6
Wen Song,Xinyu Xiao,Guanlong Wang,Xiaoli Dong,Xiufang Zhang
Supporting Fe catalysts on N doped carbon (Fe-N-C) renders a promising way towards peroxymonosulfate (PMS) activation for water decontamination , but constructing high-efficiency Fe-N-C remains challenging due to the insufficient understanding of the structure-performance relationship. Herein, the N doped carbon nanotube supported Fe catalysts (Fe-NCNT) were prepared towards PMS activation for organic pollutants removal, in which the Fe-N coordination number and Fe species were tuned through changing the pyrolysis temperature to study their roles in PMS activation. Results showed increasing the pyrolysis temperature converted the Fe-N 4 structure in Fe-NCNT to low-coordinated Fe-N 3 structure and produced Fe nanoparticles (FeNP, encapsulated in carbon). The Fe-NCNT with Fe-N 3 and FeNP exhibited a remarkably high specific activity (0.119 L min −1 m −2 ), which was 1.8 times higher than that of Fe-NCNT with only Fe-N 4 and obviously outperformed those of the state-of-the-art PMS activators. The low-coordinated structure and FeNP promoted the PMS reduction on Fe 2+ of Fe-N x for •OH and SO 4 •− production, which served as major oxidants for pollutants degradation . The experimental results and theoretical calculation corroborated the low-coordinated structure and FeNP jointly enhanced the PMS adsorption and electron density on Fe center, which accelerated electron transfer from Fe center to PMS for radical production.
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Frontiers of Environmental Science & Engineering
·
2022
·Vol. 16
·期 12
·1-15
·
IF 6.048
Huang Xiaoge,Chen Lihao,Ma Ziqi,Carroll Kenneth C.,Zhao Xiao,Huo Zailin
Cadmium (Cd) is a common toxic heavy metal in the environment. Taking Cd(II) as a target contaminant, we systematically compared the performances of three Fe-based nanomaterials (nano zero valent iron, nZVI; sulfidated nZVI, S-nZVI; and nano FeS, nFeS) for Cd immobilization under anaerobic conditions. Effects of nanomaterials doses, initial pH, co-existing ions, and humic acid (HA) were examined. Under identical conditions, at varied doses or initial pH, Cd(II) removal by three materials followed the order of S-nZVI > nFeS > nZVI. At pH 6, the Cd(II) removal within 24 hours for S-nZVI, nFeS, and nZVI (dose of 20 mg/L) were 93.50%, 89.12% and 4.10%, respectively. The fast initial reaction rate of nZVI did not lead to a high removal capacity. The Cd removal was slightly impacted or even improved with co-existing ions (at 50 mg/L or 200 mg/L) or HA (at 2 mg/L or 20 mg/L). Characterization results revealed that nZVI immobilized Cd through coprecipitation, surface complexation, and reduction, whereas the mechanisms for sulfidated materials involved replacement, coprecipitation, and surface complexation, with replacement as the predominant reaction. A strong linear correlation between Cd(II) removal and Fe(II) dissolution was observed, and we proposed a novel pseudo-second-order kinetic model to simulate Fe(II) dissolution.
研究领域:
环境科学
·
材料科学
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ACS Sustainable Chemistry & Engineering
·
2018
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IF 6.14
Junhui Liu,Anfeng Zhang,Xiao Jiang,Min Liu,Yanwei Sun,Chunshan Song,Xinwen Guo
Conversion of CO2 to sustainable chemical feedstocks and fuels by reacting with renewable hydrogen is considered to be a promising direction in energy research. The selectivity of desired products, such as C2–C4= and C5+, is low over unpromoted iron-based catalysts for CO2 hydrogenation. Therefore, promoters are often used to tailor and optimize the product distribution. In this work, the effect of doping Cu into Fe-based supported catalysts on the catalytic performance for CO2 hydrogenation to hydrocarbons was studied with a particularly focus on the interaction between Fe and Cu. For this purpose, catalysts with different Fe and Cu distribution were prepared by various impregnation methods. It was found that the selectivity of C2–C4= over Cu-promoted catalysts decreased, but a significant improvement was obtained for C5+. This promoting behavior is different from that of other promoters (e.g., K, Mn, Zn, etc.). The secondary conversion of produced olefins on Cu-promoted catalysts, which results from the improvement of olefins adsorption, on Cu-promoted catalysts leads to the decrease of C2–C4= (hydrogenation) but the increase of C5+ (oligomerization). Characterization results demonstrate that the catalytic performance is evidently associated with the strength of the interaction between Fe and Cu in the supported catalysts.
研究领域:
催化化学
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能源研究
·
化学工程
·
可持续化学
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ACS Applied Materials & Interfaces
·
2026
·Vol. 18
·期 34
·46221-46234
·
IF 7.8
Zhou Xiang,Wang Yuyan,Jin Tenghui,Zhou Shan,Tang Zhuoyun,Qu Wei,Chen J. Paul
Nonradical peroxymonosulfate (PMS) activation provides a selective route for micropollutant degradation, yet the orbital-level origin of oxidant speciation at single-atom sites remains unclear. Herein, an asymmetric Fe single-atom catalyst (Fe–N 3 –V N –C) is synthesized via molten-salt-assisted pyrolysis of a zeolitic imidazolate framework precursor, where NaCl etching enriches pyrrolic-N anchors and stabilizes low-coordination Fe centers. Fe–N 3 –V N –C exhibits efficient degradation of electron-rich micropollutants, exemplified by sulfamethoxazole, over a wide pH range of 3.5–9.5 and in wastewater matrices. The study through quenching experiments and electron paramagnetic resonance spectroscopy indicates singlet oxygen ( 1 O 2 ) as the dominant reactive species, with only minor radical contributions. The density functional theory calculations reveal that asymmetric coordination induces Fe 3 d electron delocalization, which reinforces Fe 3 d –O 2 p coupling, strengthens Fe–O covalency, accelerates interfacial charge transfer, and stabilizes Fe–O intermediates. In addition, adjacent pyrrolic N cooperates with Fe to polarize adsorbed pollutants, forming a dual-site center that promotes selective 1 O 2 generation. This work establishes Fe 3 d electron delocalization as a key electronic origin of nonradical PMS activation and provides a mechanistic basis for designing single-atom catalysts for practical water purification.
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ACS Omega
·
2022
·
IF 4.132
Liwei Ma,Guoqiang Li,Youqian Wang,Siqi Chai,Guojie Zhang
Fe2+ complexation wet denitrification technology has become a research hotspot. It is very important to achieve efficient regeneration of the absorbent and increase NO absorption in the Fe2+ complexation system. They are the key to the industrial application of the Fe2+ complexation absorption process. In this paper, 2-phosphonate-butane-1,2,4-tricarboxylic acid and ethylenediamine tetraacetic acid were used as ligands to prepare a composite system for the first time. The characteristics of NO removal were investigated under different temperatures, pHs, Fe2+ concentrations, O2 contents, NO concentrations, CO2 contents, and SO2 concentrations. Compared with the single ligand, the results show that the denitrification performance of the solution with a complex ligand is significantly improved. In this system, pH 9, 40 °C temperature, and 20 mmol/L Fe2+ concentration are the economic ideal conditions for NO removal. The system can realize simultaneous removal of NO and SO2, but SO2 in flue gas has a dual effect on the NO removal reaction.
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