JOURNAL OF MATERIALS SCIENCE & TECHNOLOGY
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2024
·
IF 11.2
Tao Zhao,Dazhong Zhong,Qiang Fang,Xin Zhao,Runxin Du,Genyan Hao,Guang Liu,Jinping Li,Qiang Zhao
The rational design of metal-organic frameworks (MOFs) provides potential opportunities for improving energy conversion efficiency. However, developing efficient MOF-based electrocatalysts remains highly challenging. Herein, a strategy involving strain engineering is developed to promote the electrocatalytic performance of MOFs by optimizing electronic configuration and improving the active site. As expected, the optimized CoFe–BDC NO 2 exhibits a low overpotential of 292 mV at 10 mA cm –2 and a small Tafel slope of 31.6 mV dec –1 as oxygen evolution reaction (OER) electrocatalyst. Notably, when CoFe–BDC NO 2 is prepared on Nickel foam (NF), the overpotential is only 345 mV at 1 A cm –2 , which ensures efficient water oxidation properties. Integrating CoFe–BDC NO 2 /NF anode in membrane electrode assembly (MEA) for overall water splitting and CO 2 reduction reaction (CO 2 RR) tests, the results show that the cell voltages of CoFe–BDC NO 2 /NF are 3.14 and 3.09 V at 300 mA cm –2 (25 °C), respectively, indicating that MOFs have various practical application prospects. The research of the structure-performance relationship reveals the lattice oxygen oxidation mechanism (LOM) where the Co-O-Fe bond is formed during the OER process by changing the electronic environment and coordination structure of CoFe–BDC NO 2 , and with high valence Co as active center, which provides a deep understanding of the structure design of MOFs and their structural transformation during OER.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2024
·
IF 9.4
Yanyu Song,Xianbo Sun,Long D. Nghiem,Jun Duan,Wen Liu,Yongdi Liu,Zhengqing Cai
Building a heterojunction is a fascinating option to guarantee sufficient carrier separation and transfer efficiency, but the mechanism of charge migration at the heterojunction interface has not been thoroughly studied. Herein, MIL-53(Fe)/Bi 4 O 5 I 2 photocatalyst with a Z-scheme heterojunction structure is constructed, which achieves efficient photocatalytic decontamination under solar light. Driven by the newly-built internal electric field (IEF), the formation of Fe-O-Bi electron migration channel allows for rapid separation and transfer of charge carriers at the heterojunction interface, confirmed by the material characterization and density functional theory (DFT) calculation. The narrower band gap and improved visible light response also contribute to the enhanced photocatalytic activity of composite materials. With levofloxacin as the target pollutant, the optimal MIL-53(Fe)/Bi 4 O 5 I 2 achieves complete removal of pollutant within 150 min, the photocatalysis rate of which is ca. 4.4 and 26.0 times that of pure Bi 4 O 5 I 2 and MIL-53(Fe), respectively. Simultaneously, the optimal composite material exhibits satisfactory photodegradation of seven fluoroquinolones, and the photocatalysis rates are as follows: lomefloxacin > ciprofloxacin > enrofloxacin > norfloxacin > pefloxacin > levofloxacin > marbofloxacin. DFT calculations reveal a positive relationship between degradation rate and Fukui index (ƒ 0 ) of main carbon atoms in seven fluoroquinolones. This study sheds light on the existence of electron migration channels at Z-scheme heterojunction interface to ensure sufficient photoinduced carrier transfer, and reveals the influence of pollutant structure on photolysis rate.
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CHEMICAL ENGINEERING JOURNAL
·
2025
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IF 13.2
Ting Zhou,Wenyi Dong,Xuechuan Li,Weigang Liu,Mengke Qiang,Hongjie Wang
High-valent ferric oxide species (HV-Fe(IV)) has been increasingly explored to selectively and efficiently remove pollutants from wastewater owing to its high reduction potential, long lifetime, and valuable resistance to anions. However, the directional production of HV-Fe(IV) and its mechanism remain challenging. Herein, a biochar-based catalyst with monoatomic Fe-trans-N 2 O 2 configuration and rich COOH group (SAFe-NKBC) was rationally constructed via KOH and supramolecular organic framework co-pyrolysis. As a result, the SAFe-NKBC/PMS system exhibited exceptional catalytic performance, achieving rapid sulfamethoxazole degradation (97.4% within 10 min) and TOC removal (73.1%). Mechanistic investigations revealed the cooperative catalytic role of single-atom Fe-trans-N 2 O 2 and COOH in biochar support via surface-confinement effect in boosting peroxymonosulfate activation and directional HV-Fe(IV) generation, mediating spatially coupled electron transfer and promoting selective oxidation pathways. Furthermore, a structure–activity relationship for various para-substituted anilines was systematically established via quantitative structure–activity relationship modeling based on different adsorption and oxidation descriptors. The valid descriptors were confirmed to predict reactivity, offering a molecular-level framework for water purification. Meanwhile, the catalyst demonstrated excellent resistance to matrix interference, long-term stability in flow-through systems, and significantly reduced toxicity of degradation byproducts, underscoring its potential in sustainable and precision-oriented water remediation. This work offered new insights into rational SAC design and reactivity prediction for sustainable water remediation.
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Environmental Science-Processes & Impacts
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2025
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IF 3.9
Rong Peng,Qi Zhu,Shuang Li,Hui Liu
The bacterium Comamonas terrigena strain HJ-2 has been reported as a nitrate-dependent iron-oxidizing bacterium, surprisingly with Fe(III) reduction ability. The control of iron redox cycling by the strain HJ-2 in the Fe(II)-Fe(III) co-existing system is mysterious and worthy of exploration. The present study demonstrates that HJ-2 utilizes nitrate as an electron acceptor to rapidly oxidize Fe(II), with negligible Fe(III) reduction, under neutral anaerobic conditions in a co-existing Fe2+ and ferrihydrite system. Nitrate significantly influences the iron transformation mediated by HJ-2. The final conversion ratio of Fe(II) increased from 27.94% to 96.67%, and the bio-oxidation rate of Fe(II) escalated from 0.000143 to 0.013 h⁻¹ as nitrate concentrations rose from 0.1 to 10 mM. X-ray diffraction results indicated that in the absence of HJ-2, goethite was the sole product, regardless of the nitrate concentration. While in the presence of HJ-2, the minerals formed transitioned from crystalline goethite and lepidocrocite to amorphous or weakly crystalline minerals with increasing nitrate concentration. Scanning electron microscopy and energy-dispersive X-ray spectroscopy showed that the morphology of the final mineral formed under high nitrate conditions resembled ferrihydrite, with higher carbon content on the mineral surface at elevated nitrate concentrations, suggesting enhanced production of bio-iron oxides and increased adsorption capacity for aqueous Fe(II). X-ray photoelectron spectroscopy results confirmed higher Fe(II) content on the amorphous minerals surface than goethite. This work provides new insights into microbial-mediated Fe-N cycling in natural environments, highlighting the significance of nitrate in driving iron redox processes and the iron mineral transformation by strain HJ-2.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2023
·
IF 22.1
Zixuan Zhang,Chenying Zhou,Yiming Sun,Peng Zhou,Yang Liu,Heng Zhang,Ye Du,Chuanshu He,Zhaokun Xiong,Bo Lai
Fenton oxidation technology is a widely-used advanced oxidation technology. However, the generation of hydroxyl radicals is restrained by the sluggish recovery of Fe(II), thus affecting its long-lasting performance for water decontamination. Here, a novel niobium carbide (Nb 2 C) MXene material was applied as a green co-catalyst. Nb 2 C MXene can significantly promote Fenton reactions to produce hydroxyl radicals for degrading dimethyl phthalate (DMP) with high efficiency and high stability for long-term operation, which outperforms than various reported co-catalysts. Meanwhile, the Nb 2 C/Fe(III)/H 2 O 2 system is capable of non-selectively degrading a wide spectrum of refractory pollutants. Mechanism investigation reveals that Nb 2 C MXene as an electron donor can straight reduce Fe(III), meanwhile mediate electron shuttle from Fe(II) to H 2 O 2 to strongly expedite the generation of hydroxyl radicals. In addition, four main degradation routes of DMP were proposed. Therefore, this study offers an updated and valid strategy for the refractory organic pollutants elimination by coupling Nb 2 C MXene and Fenton oxidation.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2024
·
IF 8.1
Xianfa Zhang,Mingzhao Huang,Zuoming Zhou,Xiaodan Zhao,Guohua Jing
Sulfite activation with iron-based heterogeneous activators is a promising technology for the removal of organic contaminants from water. However, the slow valence transformation of >Fe(II)/>Fe(III) compromises sulfite activation efficiency. Regarding that the oxygen vacancy (Vo) can modulate the charge distribution and thus enhance >Fe(II)/>Fe(III) valence transformation via rapid electron transfer, Vo-enriched γ-Fe 2 O 3 is constructed for sulfite activation (simplified as the γ-Fe 2 O 3 -Vo/sulfite system). The γ-Fe 2 O 3 -Vo/sulfite system exhibits excellent abatement performance for iohexol (IOX) with the efficiency as high as 90.2 % within 1 h of reaction at pH 8.5, in which sulfate radicals (SO 4 •− ) and hydroxyl radicals (HO • ) are the major species. Electrochemical and DFT calculations reveal that Vo-enriched γ-Fe 2 O 3 possesses lower electrical impedance and the concomitant higher electron transfer efficiency. According to a series of characterizations, the enhance >Fe(II)/>Fe(III) valence transformation is confirmed to contribute to sulfite activation via the regulation of the electronic structure by the Vo. In addition, the degradation pathways of IOX are proposed by analyzing the degradation products of IOX by UPLC-QTOF-MS. Finally, the effects of different influencing factors on the degradation of IOX and the cyclic performance suggest the system shows strong resistance to interference and reusability, exhibiting superior application potential.
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Journal of Environmental Sciences
·
2024
·
IF 5.9
Zheng Qi,Zaihui Huang,Chunguang Liu
Advanced oxidation processes (AOPs) exhibit significant potential for water disinfection due to their generation of large quantities of highly oxidizing free radicals. However, the neglect of viable but nonculturable (VBNC) cells obscures their true disinfection efficacy and potential environmental health risks. Therefore, the study evaluated the disinfection effectiveness and mechanisms of typical AOPs, including Fe/H 2 O 2 , Fe/persulfate (PS), and O 3 , from the perspective of the production of VBNC bacteria. The results indicate that Fe/PS exhibits the strongest bacterial inactivation rate (99.94%), and the cells lose their ability to reactivate. Fe/H 2 O 2 and O 3 induce more cells to enter the VBNC state compared to Fe/PS. Moreover, different AOPs result in varying levels of free radical production and utilization efficiency, with SO 4 •− and O 3 exhibiting greater selectivity in deactivating bacteria compared to HO • . The inhibition of VBNC bacteria production by Fe/PS treatment may be attributed to the combined action of HO • and SO 4 •− on microorganisms, leading to oxidative stress and metabolic disruption in bacteria through the inhibition of biofilm formation and aminoacyl-tRNA biosynthesis ( p < 0.05), thereby causing direct bacterial death rather than entry into the VBNC state. In contrast, Fe/H 2 O 2 and O 3 result in the upregulation of the metabolism of alanine, aspartate, and glutamate, as well as styrene degradation capacity by the bacteria, leading to the production of more VBNC bacteria. Overall, the study offers insights into mitigating potential biological risks in water disinfection and developing environmentally friendly and efficient disinfection technologies.
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Scientific Reports
·
2015
·Vol. 5
·期 1
·1-13
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IF 5.578
Ye Yi Quan,Jin Chong Wei,Fan Shi Kai,Mao Qian Qian,Sun Cheng Liang,Yu Yan,Lin Xian Yong
Cell wall is the major component of root apoplast which is the main reservoir for iron in roots, while nitric oxide (NO) is involved in regulating the synthesis of cell wall. However, whether such regulation could influence the reutilization of iron stored in root apoplast remains unclear. In this study, we observed that iron deficiency elevated NO level in tomato ( Solanum lycopersicum ) roots. However, application of S-nitrosoglutathione, a NO donor, significantly enhanced iron retention in root apoplast of iron-deficient plants, accompanied with a decrease of iron level in xylem sap. Consequently, S-nitrosoglutathione treatment increased iron concentration in roots, but decreased it in shoots. The opposite was true for the NO scavenging treatment with 2-(4-carboxyphenyl)-4,4,5,5-tetramethylimidazoline-1-oxyl-3-oxide (cPTIO). Interestingly, S-nitrosoglutathione treatment increased pectin methylesterase activity and decreased degree of pectin methylation in root cell wall of both iron-deficient and iron-sufficient plants, which led to an increased iron retention in pectin fraction, thus increasing the binding capacity of iron to the extracted cell wall. Altogether, these results suggested that iron-deficiency-induced elevation of NO increases iron immobilization in root apoplast by decreasing pectin methylation in cell wall.
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FOOD CHEMISTRY
·
2020
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IF 6.306
Xiamin Lv,Huasheng Man,Lijuan Dong,Jianying Huang,Xiangyang Wang
Carbon dots (CDs) have been a new class of fascinating carbon-based fluorescent nanomaterials. In the present work, new N -doped CDs with highly crystalline graphite structures are prepared from renewable precursors, chitosan and tartaric acid, and are well characterized. The prepared CDs are applied as a biocompatible fluorescent sensor for the sequential detection of Fe 3+ and AA. Among various transition metal ions, Fe 3+ can selectively quench the fluorescence of CDs. Upon the further addition of AA, the quenched fluorescence of CDs is then restored as Fe 3+ is reduced to Fe 2+ by AA, which can be utilized for the fluorescent determination of AA. A good linear relationship in the range of 0–150 μM of AA concentration is established with a low detection limit of 0.02 µM. Moreover, the practical applications of this fluorescent sensing method in measurement of AA in food samples are successfully realized with satisfactory results.
研究领域:
材料科学
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分析化学
·
生物医学
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Water
·
2019
·Vol. 11
·期 12
·2532
·
IF 2.524
Md. Nahid Pervez,Felix Y. Telegin,Yingjie Cai,Dongsheng Xia,Tiziano Zarra,Vincenzo Naddeo
In this study, a Fenton-activated persulfate (Fe2+/PS) system was introduced for the efficient degradation of Mordant Blue 9 (MB 9) as a textile dye in an aqueous solution. Results showed that the degradation of MB 9 was markedly influenced by operational parameters, such as initial pH, PS concentration, Fe2+concentration, and initial dye concentration. Optimal reaction conditions were then determined. Inorganic anions, such as Cl−and HCO3−, enhanced the degradation efficiency of MB 9 under optimal conditions. Addition of HCO3−reduced the degradation performance of MB 9, whereas the addition of Cl−increased the degradation percentage of MB 9. In addition, quenching experiments were conducted using methanol and tert-butyl alcohol as scavengers, and methanol was identified as an effective scavenger. Thus, the degradation of MB 9 was attributed to SO4•−and•OH radicals. The degradation and mineralization efficiency of MB 9 was significantly reduced using the conventional Fenton process i.e., Fe2+/ hydrogen peroxide (HP) because of the formation of a Fe complex during degradation. Meanwhile, the Fe2+/persulfate (PS) system improved the degradation and mineralization performance.Keywords:Fenton-activated;Fe-complex;persulfate;mordant dyes;scavengers
研究领域:
环境科学
·
化学工程
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JOURNAL OF ALLOYS AND COMPOUNDS
·
2023
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IF 6.2
Xiaofang Cao,Mingkai He,Baopeng Ma,Shixuan Liu,Xiaohui Pang,Mingzhen Song,Fudong Zhang,Xiaolian Chao,Zupei Yang,Di Wu
The band degeneracy thus thermoelectric performance of (Fe, Co)Sb 3 based p -type skutterudites can be well modulated by adjusting Co/Fe ratio. Combining systematic experiments and density function theory (DFT) calculations, we revealed in this work that the variation of Co/Fe ratio could result in complicated and mutually coupled effects on the individual thermoelectric parameters (band degeneracy, band gap, Fermi level , filling limit of fillers, phonon spectrum, etc.) and that using Co/Fe ratio to improve the overall thermoelectric figure of merit is nontrivial. We eventually found that the optimal Co/Fe ratio for Mm (Misch metal) filled (Fe, Co)Sb 3 lies at 1.3:2.7, which is somewhat off the Co/Fe = 1:3 point where the largest valence band degeneracy appears. Extra Sb was then introduced to compensate Sb volatilization for improved electrical transport performance. An overall peak figure of merit ZT max of 1.06 was eventually achieved in the sample Mm 0.8 Fe 2.7 Co 1.3 Sb 12.60 , which is among the highest ones for all reported (Fe, Co)Sb 3 based p -type skutterudites so far.
研究领域:
材料科学
·
热电学
·
凝聚态物理
·
能源材料
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Inorganic Chemistry Frontiers
·
2026
·
IF 6.2
Shi-Yu Lu,Chuan Li,Longyu Qiu,Yan Zhang,Jiaming He,Minqi Liang,Xin Peng,Jun Zhang,Yin Liu,Juan Liu,Chuan Tan,Menggang Li,Meng Jin
Targeted regulation of electrocatalyst reconstruction during the oxygen evolution reaction (OER) under alkaline conditions proves essential to achieving highly efficient hydrogen production via electrochemical water splitting. Yet this remains a considerable challenge. Herein, we prepare an iron nickel phosphate (Fe-NPO) catalyst, which possesses substantial oxygen vacancies and an asymmetric Fe-O(P)-Ni coordination structure. This structural merit facilitates the effective deep reconstruction of Fe-NPO, which then transforms into the highly active Fe-Vo-P-NiOOH active phase during OER. For the reconstructed Fe-Vo-P-NiOOH, it effectively tunes the d-band center, bringing it notably closer to the Fermi level. This type of electronic modulation not only strengthens the water adsorption capacity but also optimizes the rate-determining step (RDS) in the OER pathway. The anion-exchange membrane water electrolyzer (AEMWE) integrated with the Fe-NPO catalyst as an anode catalyst achieved high industrial current densities of 500, 1000, 1500 and 2000 mA cm-2 at low applied voltages of 1.68, 1.76, 1.84 and 1.92 V, respectively. This work presents a strategy to realize the deep and efficient conversion of OER catalysts into highly active components through defect engineering and asymmetric coordination regulation, while also confirming Fe-NPO’s considerable potential for practical hydrogen production scenarios.
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