CHEMICAL GEOLOGY
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2024
·
IF 3.6
Kuan Cheng,Yunlu Yin,Ying Wang,Guoyong Huang,Dandan Pan,Milan Wang,Xuxin Song,Tongxu Liu,Xiaomin Li
Microbial Fe(II) oxidation is mainly mediated by the outer-membrane proteins that contain c -type cytochromes ( c- Cyts), and the widespread Fe(II)-oxidizing bacteria are usually subjected to fluctuations between oxic and anoxic conditions. However, it remains unclear how oxygen affects the redox dynamics of c- Cyts by Fe(II), particularly in the presence of organic ligands that are widely distributed in the environment. Here, the reduction of a model heme-containing c- Cyts by Fe(II) was investigated in the absence and presence of organic ligands (i.e., citrate and acetate) at pH 5.5 under anoxic and oxic conditions . The kinetic results showed that c- Cyts reduction was enhanced by citrate and acetate under anoxic conditions, and the enhancement by citrate was more pronounced than that by acetate. The speciation calculation and cyclic voltammetry results suggested that the proportions of Fe(II)-Citrate complexes were much higher than those of Fe(II)-Acetate complex, but the addition of acetate and citrate caused minor changes in redox potential of Fe(II)/Fe(III) species. Further analysis using quantum chemical computation demonstrated that the formation of Fe(II)-Heme complexes via lateral binding to the carboxyl group of c- Cyts was more stable than those via replacing the S-linked axial ligand of heme, with the recombination energy with Heme ranking as Fe(II)-Citrate < Fe(II)-Acetate < Fe(II). Therefore, the stronger complexation of Fe(II)-Citrate and its lower recombination energy with c- Cyts drive the enhanced c- Cyts reduction under anoxic conditions. By contrast, the c- Cyts reduction by Fe(II) and Fe(II)-ligand was inhibited under oxic conditions. The electron spin resonance characterization indicated that both O 2 − • and OH• radicals were produced in the system of c- Cyts with Fe(II) or Fe(II)-ligand under oxic conditions and the signals were higher with Fe(II)-ligand than those with Fe(II). These reactive oxygen species were proposed to enable a re-oxidation of the c- Cyts that was reduced by Fe(II) or Fe(II)-ligand, causing an inhibitory effect on the observed c- Cyts reduction and forming more reactive oxygen species . Our findings shed light on the important roles of Fe(II)-ligand-heme complexation and reactive oxygen species in the interaction between Fe(II) and c- Cyts, which deepen the understanding of microbial/enzymatic Fe(II) oxidation under oxic conditions at the molecular level.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2024
·
IF 20.2
Yuan Qin,Zihao Ou,Chaozhong Guo,Yao Liu,Rong Jin,Chuanlan Xu,Haifeng Chen,Yujun Si,Honglin Li
Regulating the electronic structure by phosphor-doping is a preferred strategy to boost the performance of carbon-based catalysts for oxygen reduction reaction (ORR). Here, a porous Fe, P, N-codoped carbon catalyst (PCF-FeTz-900) is designed by a phytic acid-assisted thermal etching strategy, in which P atoms are first doped into the carbon matrix to form a stable P C bond, and then FeN 4 sites are produced from Fe-2,4,6-Tris(2-pyridyl)-s-triazine complex (Fe-TPTz). Theoretical calculations suggest that the electrons are transferred from the doped P atom to the neighboring FeN 4 sites, which facilitates the ORR at the Fe sites by reducing the energy barrier and the adsorption energy of intermediates. Additionally, the P-doped FeN 4 (FeN 4 P) structure manifests a lower free energy difference than that of FeN 4 and the d -band center of Fe is also lowered, which further ensures its higher ORR catalytic ability. As a result, the PCF-FeTz-900 catalyst exhibits superior ORR activity and stability in alkaline electrolyte, and the assembled primary zinc-air battery shows greater performances compared to the commercial Pt/C catalyst. This work can provide an effective pathway for modulating the performance of doped-carbon materials in energy conversion devices.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2020
·
IF 7.489
Xuanxuan Jia,Hao Liu,Yu Zhang,Wei Chen,Qing Tong,Guangxia Piao,Chuanzhi Sun,Lin Dong
In recent years, Fe-based catalysts for the selective catalytic reduction of NO with NH 3 (NH 3 -SCR) have been attracting more attention. In this work, a novel Fe-Sb binary metal oxide catalyst was synthesized using the ethylene glycol assisted co-precipitation method and was characterized using a series of techniques. It was found that the catalyst with a molar ratio of 7:3 (Fe:Sb) displayed the best NH 3 -SCR activity with 100% conversion of NO x (nitrogen oxides) over a wide temperature window and with good resistance to H 2 O + SO 2 at 250 °C. The X-ray photoelectron spectroscopy (XPS) and in situ diffused reflectance infrared Fourier transform spectroscopy ( in situ DRIFTS) of NO x adsorption results suggested that strong electron interactions between Fe and Sb in Fe-O-Sb species existed and electrons of Sb could be transferred to Fe through the 2Fe 3+ + Sb 3+ ↔ 2Fe 2+ + Sb 5+ redox cycle. The introduction of Sb significantly improved the adsorption behaviour of NO x species on the Fe 0.7 Sb 0.3 O x surface, which benefitted the adsorption/transformation of NO x , thereby facilitating the NH 3 -SCR reaction. In addition, the Fe 0.7 Sb 0.3 O x catalyst demonstrated a good tolerance of H 2 O and SO 2 , since the decomposition of NH 4 HSO 4 on the catalyst surface was promoted by the introduction of Sb.
研究领域:
催化
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环境科学
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材料科学
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JOURNAL OF BIOLOGICAL INORGANIC CHEMISTRY
·
2023
·Vol. 28
·期 4
·379-391
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IF 3
Chen Chan,Tang Weikang,Chen Qinfei,Han Mengqi,Shang Qi,Liu Wenbin
Hydroxytyrosol, one of the most powerful natural antioxidants, exhibits certificated benefits for human health. In this study, a biomimetic approach to synthesize hydroxytyrosol from the hydroxylation of tyrosol was established. EDTA-Fe 2+ coordination complex served as an active center to simulate tyrosine hydroxylase. H 2 O 2 and ascorbic acid were used as oxygen donor and hydrogen donor, respectively. Hydroxy radical and singlet oxygen contributed to active species. The biomimetic system displayed analogous component, structure, and activity with TyrH. Hydroxytyrosol titer of 21.59 mM, and productivity of 9985.92 mg·L −1 ·h −1 was achieved with 100 mM tyrosol as substrate. The proposed approach provided efficient and convenient route to quickly produce high amount of hydroxytyrosol. Graphical abstract
研究领域:
生物化学
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合成生物学
·
抗氧化研究
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REACTIVE & FUNCTIONAL POLYMERS
·
2024
·
IF 4.5
Yi Sun,Guqing Xiao,Zijun Liu,Dan Wu,Li Xia
There are inorganic salts in glyphosate production liquor and natural water bodies coexisting with glyphosate. It is imperative to develop a salt-tolerant adsorbent for glyphosate in water. Industrial D113 resin undergone two-step transformation to optimize the preparation of D113 in-situ loaded with Fe 3+ (D113-Fe 3+ ) as salt-resistance glyphosate adsorbent. The loading amount of Fe 3+ on D113-Fe 3+ is 3.5 mmol/g. The adsorption mechanism revealed that Fe 3+ in D113-Fe 3+ formed Fe-O-P bond with the phosphonate group of glyphosate. At 293 K, the maximum complex ratio of the adsorbed glyphosate to Fe 3+ in D113-Fe 3+ was 2.4:1. At 293 K, the remarkable saturated glyphosate adsorption capacity of D113-Fe 3+ reached 1420.2 mg/g. In pK 2 state of glyphosate, D113-Fe 3+ featured its maximum adsorption capacity at the zero charge point 2.43 of D113-Fe 3+ and 293 K. In glyphosate solution coexisting 0–16 % NaCl, D113-Fe 3+ exhibited stable glyphosate adsorption capacity and salt-resistance compared with D201, D301 and 330 resin. The endothermic and spontaneous adsorption of glyphosate on D113-Fe 3+ can fit Freundlich model and pseudo-second-order model. 2 mol/L NH 3 ·H 2 O, 2 mol/L FeCl 3 and 2 mol/L H 2 SO 4 could all regenerate D113-Fe 3+ . The characteristics of salt-resistance and the remarkable saturated adsorption capacity made D113-Fe 3+ comparable to all reported glyphosate adsorbents.
研究领域:
环境科学
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材料科学
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ACS Applied Electronic Materials
·
2026
·Vol. 8
·期 15
·6545-6553
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IF 4.7
Liu Qianzuo,Sun Sifan,Li Jiawei,Yang Haoran,Xiang Xinyue,Hao Ying,Yan Xuehua,Zhang Ting,Li Tie
Hydrogen peroxide (H 2 O 2 ), a key reactive oxygen species in physiological and pathological processes, demands highly sensitive detection for biological and biomedical research, yet developing electrocatalytic materials with high sensitivity, low detection limit, and excellent stability remains a challenge. Herein, a Fe−C@Fe/Ce−C bilayer heterojunction composite was fabricated for H 2 O 2 detection. Benefiting from its unique heterojunction architecture and synergistic Fe/Ce/carbon interactions, the as-prepared nanocomposite exhibits the exceptional H 2 O 2 sensing performance, with a wide linear range of 0.5−6000 µM, a high sensitivity of 490.5 μA·mM −1 ·cm −2 , a low detection limit of 0.12 µM, excellent anti-interference selectivity against common biological interferents, and outstanding long-term stability with no obvious performance variation after 11 days of continuous testing. The robust built-in electric field arising from the heterojunction facilitates interfacial charge transfer and accelerates H 2 O 2 activation, boosting sensing behavior. Furthermore, the flexible electrochemical sensor was fabricated via the screen-printing technology, which enables reliable real-time monitoring of intracellular H 2 O 2 released from HeLa cells, showing great potential for biological sensing. This work provides a promising design strategy for high-performance flexible electrochemical sensors and deepens the understanding of heterojunction and built-in electric field roles in electrocatalytic sensing systems.
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Journal of Environmental Chemical Engineering
·
2026
·Vol. 14
·期 3
·122408
·
IF 7.5
Shan Huang,Jiangxue Luo,Tianren Zhan,Yubo Wu,Jiankun Li,Yanjuan Zhang,Zuqiang Huang,Huayu Hu,Tao Gan
Iron-based catalysts have been widely used to activate peroxymonosulfate (PMS) for the treatment of carbamazepine (CBZ) wastewater. However, the development of efficient and stable pyrite (FeS 2 )-based catalysts to mitigate the consumption of Fe 3 + /Fe 2+ and S 2 2– is still challenging. Herein, FeS 2 /nitrogen-doped carbon (FeS 2 /NC) composite was synthesized using hydrothermal combined with pyrolytic strategy, wherein FeS 2 and NC connected by Fe−N x and Fe−C x bonds. In the photo-PMS system, FeS 2 /NC achieved a removal rate of 98.2 % for CBZ within 6 min, and the total organic carbon (TOC) removal was 83.4 %, which exceeded FeS 2 and most of the results reported in the previous literature. The electron paramagnetic resonance results and quenching experiments confirmed that 1 O 2 played a critical role in the FeS 2 /NC + PMS + visible light system, while h + , SO 4 • − , and •O 2 − were secondary. The excellent performance stemmed from that the Fe−N x and Fe−C x bonds between FeS 2 and NC enhanced the photogenerated electron transport efficiency, resulting in efficiently circulating Fe 3+ to Fe 2+ and minimizing the S 2 2– consumption. Meanwhile, the electron-deficient graphitic-N could facilitate the 1 O 2 generation. Moreover, FeS 2 /NC exhibited good stability and satisfactory universality, providing the potential for actual wastewater treatment. This work offers a novel strategy for enhancing the Fe 3+ /Fe 2+ cycle and reducing the S 2 2– consumption of FeS 2 -based catalyst for the effective treatment of CBZ wastewater.
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RSC Advances
·
2026
·Vol. 16
·期 18
·16505-16511
·
IF 6.1
Cong Gao,Houfen Li,Jize Liu,Wenchao Yang,Hong Chen,Jianbo Han
The heterogeneous Fenton-like reaction is a promissing technology for removing organic pollutants in water. The reduction of Fe(III) to Fe(II), as the rate-limiting step for generating ˙OH, is crucial in heterogeneous Fenton-like reactions and may be improved using organic pollutants with lower redox potential than that of Fe(III)/Fe(II). In this work, the rapid reduction of Fe(III) to Fe(II) on the MIL-100-Fe catalyst was achieved by degrading methylene blue (MB, E0 = 0.01 V), which has the desired lower redox potential than that of MIL-100-Fe(III)/Fe(II) (E0 = 0.76 V). By contrast, organic pollutants with higher redox potentials than that of MIL-100-Fe, such as phenol (E0 = 0.97 V) and p-nitrophenol (E0 = 1.23 V), were incapable of reducing Fe(III) to Fe(II). As a result, the degradation rate constant of MB was one order of magnitude higher than those of phenol and p-nitrophenol. Notably, MB could also promote the reduction of Fe(III) to Fe(II) in the presence of phenol or p-nitrophenol; thus, the degradation rate constants of phenol and p-nitrophenol were significantly enhanced by 50 and 30 times, respectively. The results revealed that organic pollutants with lower redox potential than that of Fe(III)/Fe(II) could facilitate the reduction of Fe(III) to Fe(II), which is beneficial for producing more ˙OH, thus improving the heterogeneous Fenton-like catalytic performance.
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PubMed
高影响因子
Environmental Science-Nano
·
2023
·Vol. 10
·期 8
·2066-2076
·
IF 7.3
Jiahui Zhou,Xuesong Li,Qiuying Yi,Zhiwei Wang
Heterogeneous Fenton-like processes based on Fe-based catalysts are effective technology to degrade emerging organic pollutants in water and wastewater such as tetracycline (TC). However, the kinetically limited redox cycling between Fe2+ and Fe3+ is still a persistent challenge for their widespread application. To address this issue, we designed a novel Fe-based catalyst by coating reduced iron powder (RIP) with ferroferric oxide nanoparticles (FONP@RIP) using a simple chemical co-precipitation method. The reduced iron could rapidly reduce Fe(III) to Fe(II) and accelerate the cycle of Fe(II)/Fe(III) in the heterogeneous Fenton-like system. Benefiting from the accelerated cycle of Fe(II)/Fe(III), TC could be efficiently degraded in the FONP@RIP/H2O2 system over a wide pH range of 3–6, with a removal efficiency of 94.5% within 60 min (TC0 = 150 ppm). The predominant reactive oxygen species were identified as ˙OH and HO2˙. Based on the identified intermediates, the possible pathway of TC degradation was deduced and the toxicity of pollutants could also be significantly reduced during the degradation process. Moreover, FONP@RIP exhibited stable catalytic performance during multiple cyclic tests with only a marginal loss of catalytic components. This study presents a new catalyst design strategy for heterogeneous Fenton-like processes, which provides a promising way for the degradation of residual antibiotics in water and wastewater.
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Journal of Water Process Engineering
·
2022
·
IF 7.34
Junjie Su,Han Hao,Jingran Li,Zhilin Yang,Qi Yang
Nanometer zero-valent iron (nZVI), Fe 2+ and H 2 were potential electron donors for CT removal by nZVI. However, the action of these electron donors in CT reduction was often ambiguous. In this study, the actual catalytic activity of Ni 4 /Fe@Fe 3 O 4 under common ions and humic acid (HA) was investigated. The results showed that Na + and K + had no effect on CT removal, Cl ‐ , SO 4 2 ‐ and low concentration of Mg 2+ was beneficial to CT removal, while NO 3 ‐ , HCO 3 ‐ , Ca 2+ and HA exhibited the negative effects. According to the analysis results of gas chromatography (GC) and ion chromatography (IC), a possible dechlorination pathway of CT was proposed. Furthermore, the action mechanism of nZVI, Ni 0 and magnetite (Fe 3 O 4 ) on CT removal were explored. Among the three possible nZVI reducing mechanism, the use of H 2 by Ni 0 for the hydrodechlorination was dominant, while the direct reduction of nZVI was secondary. Fe 2+ , the product of nZVI corrosion, contributed little to CT degradation and required longer reaction time. Ni 0 could not only utilize H 2 but also form galvanic cells with nZVI to accelerate CT dechlorination. In addition, the support Fe 3 O 4 significantly improved the dispersion of Ni/Fe nanoparticles and its corrosion product Fe 2+ also promoted the CT removal. These findings were significant for comprehending the mechanisms of bimetallic nanocomposites in reducing CT, and might guide to the development of nZVI based technology for repairing polluted water or soil with organochlorine pollutants.
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WATER RESEARCH
·
2023
·
IF 12.8
Bin Liu,Yin Jun,Changrong Zhao,Chu Zhou,Tingting Zhu,Senlin Shao
Ultrafiltration (UF) is a technology commonly used to treat secondary effluents in wastewater reuse; however, it faces two main challenges: 1) membrane fouling and 2) inadequate nitrogen (N), phosphorus (P), and organic micropollutants (OMPs) removal. To address these two issues, in this study, we applied peracetic acid (PAA), Fe(VI)/PAA, and Fe(II)/PAA as UF pretreatments. The results showed that the most effective pretreatment was Fe(II)/200 μM PAA, which reduced the total fouling resistance by 90.2%. In comparison, the reduction was only 29.7% with 200 μM PAA alone and 64.3% with Fe(VI)/200 μM PAA. Fe(II)/200 μM PAA could effectively remove fluorescent components and hydrophobic organics in effluent organic matter (EfOM), and enhance the repulsive force between foulants and membrane (according to XDLVO analysis), and consequently, mitigate pore blocking and delay cake layer formation. Regarding pollutant removal, Fe(II)/200 μM PAA effectively degraded OMPs (>85%) and improved P removal by 58.2% via in-situ Fe(Ⅲ) co-precipitation. The quencher and probe experiments indicated that Fe IV O 2+ , •OH, and CH 3 C(O)OO•/CH 3 C(O)O• all played important roles in micropollutant degradation with Fe(II)/PAA. Interestingly, PAA oxidation produced highly biodegradable products such as acetic acid, which significantly elevated the BOD 5 level and increased the BOD 5 /total nitrogen (BOD 5 /TN) ratio from 0.8 to 8.6, benefiting N removal with subsequent denitrification. Overall, the Fe(II)/PAA process exhibits great potential as a UF pretreatment to control membrane fouling and improve water quality during secondary effluent treatment.
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高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2020
·
IF 10.652
Yong Sun,Muhammad Danish,Meesam Ali,Ali Shan,Ming Li,Yanchen Lyu,Zhaofu Qiu,Qian Sui,Xueke Zang,Shuguang Lyu
The performance of trichloroethene (TCE) degradation was significantly improved with the addition of FeS in nanoscale calcium peroxide (nCP) environment and the enhancement of HO generation in nCP/Fe(II)/FeS system was confirmed by comparison with nCP/Fe(II) and nCP/FeS systems. The role of FeS in nCP/Fe(II)/FeS system demonstrated that the majority of reactive oxygen radicals (ROSs) was generated on the catalyst surface due to the heterogeneous reaction through FeS activated nCP in one hand, and the reductive FeS could promote TCE degradation by regenerating Fe(II) from Fe(III) in the other hand. The probe as well as scavenger test results suggested that the major ROSs was HO rather than O 2 − . Over 91.5% TCE could be degraded at the molar ratio of 2/2/4/1 of nCP/Fe(II)/FeS/TCE, in which more than 95.5% TCE was dechlorinated. The effect of surfactants on TCE degradation was evaluated. In contrast, further investigation found that BTEX removal was inhibited with the addition of FeS. In conclusion, this study revealed the well function and fundamental synergistic mechanism of FeS. Moreover, the degradation of TCE in actual groundwater confirmed that nCP/Fe(II)/FeS technique has a great advantage and potential in TCE contaminated groundwater remediation in ISCO practice.
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