APPLIED SURFACE SCIENCE
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2023
·
IF 6.7
Xiaoqi Zhao,Yingxiao Li,Xue Zhang,Yanfang Gao,Ling Liu
Surface oxygen vacancy increases active site numbers, and multidimensional cross-linked structure improves the exposure of active sites. Thereby, they can enhance the oxygen reduction reaction (ORR) performance of Fe-N-C catalysts effectively. Herein, Fe(NO 3 ) 3 ·9H 2 O and carbon nanotubes (CNTs) were introduced into zeolitic imidazolate framework nano leaves (ZIF-L) to prepare multidimensional cross-linked Fe-N-CNTs with surface oxygen vacancies through co-pyrolysis at the high-temperature. As expected, the synthesized multidimensional cross-linked Fe-N-CNTs-900-0.2 composite rich in oxygen vacancies increased the conduction band potential and improved the reducing capacity. Thus, Fe-N-CNTs-900-0.2 possessed a better ORR electrochemical performance (half-wave potential = 0.892 V vs. RHE) that surpass the Pt/C catalysts. Moreover, the Al-air batteries containing Fe-N-CNTs-900-0.2 displayed a higher maximum power density than those of Pt/C catalysts. The electronic band structure shows that Fe-N-CNTs-900-0.2 rich in oxygen vacancy concentration has higher conduction band potential and effectively improves the activity of ORR catalysts. This work innovatively proposes that the joint work of multidimensional cross-linked structure and oxygen defects is an effective method to enhance the ORR performance and clarifies its internal reaction mechanism, which provides a new idea to design and preparer Fe-N-C catalysts.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2023
·
IF 9.9
Lixia Wang,Yanjing Qin,Huatong Li,Zhiyang Huang,Mingcheng Gao,Tayirjan Taylor Isimjan,Xiulin Yang
Designing multi-channel mesoporous structure and introducing oxygen vacancies to synergistically enhance oxygen reduction reaction (ORR) activity is crucial for the practical application of zinc-air batteries (ZABs) in the field of energy storage and conversion. Herein, a novel multi-channel mesoporous Bi-Fe 2 O 3 microsphere with abundant oxygen vacancies supported on nitrogen-doped carbon (denoted as Bi-Fe 2 O 3 @NC) is constructed and the designated catalyst demonstrates a higher half-wave potential (0.88 V), large limiting current density (5.8 mA cm −2 @0.4 V), and superior stability. Besides, the aqueous ZAB utilizing Bi-Fe 2 O 3 @NC cathode achieves a high power density of 198.6 mW cm −2 and maintains exceptional stability for 459 h at 5 mA cm −2 , superior to most previously reported catalysts. Furthermore, a solid-state ZAB assembled with Bi-Fe 2 O 3 @NC shows a power density of 55.9 mW cm −2 , highlighting its potential for flexible ZAB applications. The prominent ORR performance of Bi-Fe 2 O 3 @NC can be ascribed to its unique multi-channel mesoporous structure and abundant oxygen vacancies, which increase the exposure of active sites and facilitate efficient electron/mass transport. This work provides valuable insights for the rational design of advanced ORR catalysts for the practical requirements of aqueous/flexible ZABs in energy storage and conversion.
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ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH
·
2023
·Vol. 30
·期 27
·70260-70276
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IF 5.8
Yang Guoliang,Jiang Yan,Yin Bingjie,Liu Guocheng,Ma Dong,Zhang Guangshan,Zhang Guodong,Xin Yanjun,Chen Qinghua
Polycyclic aromatic hydrocarbons (PAHs) in soil have potential harm on human health. However, remediation of PAH-contaminated soils through photocatalytic technology remains a challenge. Therefore, the photocatalyst g-C 3 N 4 /α-Fe 2 O 3 was synthesized and applied to photocatalytic degradation of fluoranthene in soil. The physicochemical properties of g-C 3 N 4 /α-Fe 2 O 3 and various degradation parameters, such as catalyst dosage, the ratio of water/soil, and initial pH, were investigated in detail. In soil slurry reaction system (water/soil=10:1, w/w), the optimal degradation efficiency on fluoranthene was 88.7% after simulated sunlight irradiation for 12 h (contaminated soil=2 g, initial fluoranthene concentration=36 mg/kg, catalyst dosage=5%, and pH=6.8), and the photocatalytic degradation followed pseudo-first-order kinetics. The degradation efficiency of g-C 3 N 4 /α-Fe 2 O 3 was higher compared with P25. Degradation mechanism analysis showed that •O 2 - and h + are the main active species in photocatalytic degradation process of fluoranthene by g-C 3 N 4 /α-Fe 2 O 3 . Coupling g-C 3 N 4 and α-Fe 2 O 3 enhances the interfacial charge transport capacity via Z-scheme charge transfer route and inhibits the recombination of photogenerated electrons and holes of g-C 3 N 4 and α-Fe 2 O 3 , then significantly improves the production of active species and photocatalytic activity. Results showed that photocatalytic treatment of soil by g-C 3 N 4 /α-Fe 2 O 3 is an effective strategy for remediation of soils contaminated by PAHs.
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ENVIRONMENTAL RESEARCH
·
2023
·
IF 8.3
Chunyan Hu,Jinke He,Jianjun Liang,Tao Lin,Qiuliang Liu
A novel photo-Fenton catalyst α-Fe 2 O 3 @g-C 3 N 4 @NH 2 -MIL-101(Fe) (FGN) with dual Z-scheme heterojunction was successfully prepared by hydrothermal method to degrade tetracycline (TC). The preparation conditions were optimized by orthogonal test, and the successful synthesis was confirmed by characterization analyses. The prepared FGN showed better light absorption performance, higher photoelectrons-holes separation efficiency, lower photoelectrons transfer resistance, and higher specific surface area and pore capacity compared with α-Fe 2 O 3 @g-C 3 N 4 and α-Fe 2 O 3 . The effects of experimental conditions on the catalytic degradation of TC were investigated. The degradation rate of 10 mg/L TC could reach 98.33% within 2 h when the dosage of FGN was 200 mg/L, and the degradation rate could remain 92.27% after 5 times of reuse. Furthermore, the XRD spectra and XPS spectra of FGN before and after reuse were compared to explore the structural stability and catalytic active sites of FGN, respectively. According to the identification of oxidation intermediates, three degradation pathways of TC were proposed. Through H 2 O 2 consumption experiment, radical-scavenging experiments, EPR results, the mechanism of the dual Z-scheme heterojunction was proved. The improved performance of FGN was attributed to the dual Z-Scheme heterojunction effectively promoting the separation of photogenerated electrons from the holes and accelerating the electrons transfer , and the increase of the specific surface area.
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
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2023
·
IF 5.2
Yifang Mi,Sen Zhang,Yufeng Zhao,Guojin Sun,Zhihai Cao
Fe-based activated biochar composites are promising catalysts for environmental remediation. However, the limited efficiency of Fe(III)/Fe(II) cycling reaction of commercial Fe 2 O 3 at neutral conditions still impeded the catalytic performance of the heterogeneous Fenton-like catalysts. In this work, high-performance Fe 2 O 3 /activated biochar Fenton-like catalysts with Taihu blue algae (hazardous algae to aquatic ecosystems) as carbon precursors were synthesized and used for the degradation of methylene blue (MB). The physicochemical properties of Fe 2 O 3 /activated biochar composites including pore structure , the generated N species, and persistent free radicals (PFRs) were effectively tailored by activation temperatures. ACK-7-Fe (prepared under the activation temperature, 700 °C) showed a stronger adsorption ability while ACK-8-Fe (800 °C) exhibited superior MB degradation performance (∼99.97% in 30 min at neutral pH). The former was ascribed to the formation of more mesopores with suitable size which was beneficial for MB adsorption. The latter is due to the promoting effect of pyrrolic N and PFRs on the Fe(III)/Fe(II) cycle, responsible for the high catalytic efficiency of ACK-8-Fe. The hydroxyl radicals were the dominant active radicals evidenced by scavenging experiments and electron spin resonance. Moreover, the. The ACK-8-Fe exhibited superior reusability, which was crucial for its practical applications.
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CHEMICAL ENGINEERING JOURNAL
·
2018
·
IF 6.735
Liwei Chen,Xu Zuo,Shengjiong Yang,Tianming Cai,Dahu Ding
Rational design and synthesis of efficient catalyst for the generation of sulfate radicals (SO 4 − ) through heterogeneous approach is highly desirable. In the present study, a magnetic cobalt-based catalyst, Co 3 O 4 @Fe 2 O 3 was successfully synthesized by using metal-organic frameworks (MOFs) as a template. A hollow core-shell structure possessing moderate specific surface area (22.8 m 2 g −1 ) and pore volume (0.18 cm 3 g −1 ) was obtained. The catalyst performed high efficiency for the degradation of norfloxacin (NOR) by coupling with peroxymonosulfate (PMS). And the process was kinetically favorable in neutral (0.43 min −1 at pH of 7.5) and weak acidic/basic conditions, whilst significantly inhibited at acidic condition (0.12 min −1 at pH of 4.5). Catalyst loading showed a more remarkable effect on the degradation process than PMS dose. Interestingly, chloride, phosphate and bicarbonate ions clearly promoted the degradation process while humic acid showed a detrimental effect. Cl 2 /HOCl oxidation system was demonstrated when massive Cl − was added into the reaction system. As evidenced by electron paramagnetic resonance (EPR) analysis, both hydroxyl and sulfate radicals contributed to the degradation and the latter one played a crucial role. Eventually, degradation pathway was tentatively proposed based on the HPLC-ESI-MS/MS analysis of the detected intermediates. This study would be very meaningful to promote the applications of sulfate radical based advanced oxidation processes (SR-AOPs) for the environmental remediation.
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ACS Applied Materials & Interfaces
·
2019
·
IF 8.456
Qiao Yang,Xuhao Wu,Xuankai Huang,Shuang Liao,Kaijie Liang,Xueang Yu,Kuan Li,Chunyi Zhi,Haiyan Zhang,Na Li
Penetrating into the inner surface of porous metal-oxide nanostructures to encapsulate the conductive layer is an efficient but challenging route to exploit high-performance lithium-ion battery electrodes. Furthermore, if the bonding force on the interface between the core and shell was enhanced, the structure and cyclic performance of the electrodes will be greatly improved. Here, vertically aligned interpenetrating encapsulation composite nanoframeworks were assembled from Cl–/SO32–-codoped poly(3,4-ethylenedioxythiophene) (PEDOT) that interpenetrated and coated on porous Fe2O3 nanoframeworks (PEDOT-IE-Fe2O3) via a one-step Fe3+-induced in situ growth strategy. Compared with conventional wrapped structures and methods, the special PEDOT-IE-Fe2O3 encapsulation structure has many advantages. First, the codoped PEDOT shell ensures a high conductive network in the composites (100.6 S cm–1) and provides interpenetrating fast ion/electron transport pathways on the inner and outer surface of a single composite unit. Additionally, the pores inside offer void space to buffer the volume expansion of the nanoscale frameworks in cycling processes. In particular, the formation of Fe–S bonds on the organic–inorganic interface (between PEDOT shell and Fe2O3 core) enhances the structural stability and further extends the cell cycle life. The PEDOT-IE-Fe2O3 was applied as lithium-ion battery anodes, which exhibit excellent lithium storage capability and cycling stability. The capacity was as high as 1096 mA h g–1 at 0.05 A g–1, excellent rate capability, and a long and stable cycle process with a capacity retention of 89% (791 mA h g–1) after 1000 cycles (2 A g–1). We demonstrate a novel interpenetrating encapsulation structure to highly enhance the electrochemical performance of metal-oxide nanostructures, especially the cycling stability, and provide new insights for designing electrochemical energy storage materials.
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JOURNAL OF ANALYTICAL AND APPLIED PYROLYSIS
·
2019
·
IF 3.47
Adel Baimoldina,Konstantinos Papadikis,Elena Yu. Konysheva
The feasibility of α-Fe 2 O 3 catalyst addition in the in-situ catalytic fast pyrolysis of Pinewood was considered with the focus on the variation in its shape: nano-sized non-ideal spheres, nanotubes, hollow nano/microtubes, and octadecahedral crystals. Nano-sized spheres strongly promoted the formation of acetaldehyde, something that was also observed for the octadecahedral crystals. The formation of acids was primarily facilitated through the addition of nanotube catalysts and octadecahedral crystals. Newly formed alicyclic ketonic compounds were promoted through the addition of nano-sized spheres, hollow nano/microtubes, and octadecahedral crystals. The latter two catalysts also showed a moderate selectivity in the formation of furfural. All applied catalysts showed loss of activity, though at different degrees, on the formation of lignin derived phenolic compounds, which can be primarily attributed to favoring the formation of char with simultaneous release of CO 2 . All used α-Fe 2 O 3 catalysts with different shapes maintained their original morphology after the rapid heating with the rate of 20 K/ms followed by catalytic fast pyrolysis at 500 °C, indicating that nanomaterials with targeted dimensions can be applied as catalysts in the catalytic fast pyrolysis of biomass to enhance conversion of undesired oxygenated compounds to higher quality bio-oil and valuable chemicals.
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COMPOSITES PART B-ENGINEERING
·
2019
·
IF 6.864
Jiangtao Xu,Songmin Shang,Shouxiang Jiang
Conventionally, the surface-enhanced Raman spectroscopy (SERS) measurement is performed by dispersing noble metal nanoparticles onto the target sample directly or assembling noble metal nanoparticles onto a micro-sized substrate. Despite it is flourishing, this method is not adequate for various samples, mainly limited by either a defined confinement of the test position or the complex extraction process of the target sample on the irregularly shaped surface, besides the costive materials, complex and uncontrollable fabricating processes. Herein, we demonstrate that the α-Fe 2 O 3 thin film is decorated with Ag nanoparticles constructed on SiO 2 fibers as a flexible SERS-active substrate, which yields a functional optical enhancement of the signal at 532 nm laser excitation . It shows a high enhancement factor of 4.71 × 10 5 , ultrahigh sensitivity of 10 −15 M, and excellent signal stability with a relative standard deviation (RSD) of 1.22% and reproducibility with a RSD of 0.258%.
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JOURNAL OF CHEMICAL TECHNOLOGY AND BIOTECHNOLOGY
·
2018
·Vol. 93
·期 9
·2552-2563
·
IF 2.587
Yi Yang,Huiping Zhang,Ying Yan
BACKGROUND A novel iron-loaded microfibrous entrapped carbon-nanotube catalyst (Fe 2 O 3 -MF-CNT) was synthesized by wet lay-up papermaking, sintering and metal organic chemical vapor deposition (MOCVD) processes. The catalysts were characterized by N 2 adsorption–desorption isotherm, mercury porosimetry, scanning electron microscopy (FE-SEM), energy dispersive spectroscopy (EDS) and NH 3 temperature program desorption (NH 3 -TPD), and the catalytic performance was tested by catalytic wet peroxide oxidation (CWPO) of m-cresol in a fixed-bed reactor. Finally, the probable multistep reaction pathway for CWPO degradation of m-cresol over Fe 2 O 3 -MF-CNT catalyst in a fixed-bed reactor is presented. RESULTS Characterization results conclude that the prepared catalysts are acid catalysts containing macropores and mesopores. Active components Fe 2 O 3 are evenly loaded on the support by the MOCVD method. CWPO results show that higher temperature and higher space time promote the catalyst performance. Meanwhile, the Fe 2 O 3 -MF-CNT catalyst shows perfect reusability with nearly no iron leaching concentration and high m-cresol conversion (above 95.0%) after four successive runs (24 h). Two possible pathways during degradation of m-cresol are presented. The hydroxyl radicals turn m-cresols into aromatic by-products such as p-toluquinone, 4-methylpyrocatechol and methylhydroquinone, followed by evolution to organic acids, and finally to carbon dioxide and water. During the reaction, more m-cresols are degraded through the pathway in which m-cresols are first converted into 4-methylpyrocatechol. CONCLUSION The novel Fe 2 O 3 -MF-CNT catalyst presented herein owns the advantages of both CNTs and stainless steel fibers, and it shows promising performance in CWPO of m-cresol. © 2018 Society of Chemical Industry
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Frontiers of Environmental Science & Engineering
·
2018
·Vol. 12
·期 1
·1-8
·
IF 1.961
Gao Pan,Song Yuan,Wang Shaoning,Descorme Claude,Yang Shaoxia
The Fe 2 O 3 -CeO 2 -Bi 2 O 3 /γ-Al 2 O 3 catalyst, a novel environmental-friendly material, was used to investigate the catalytic wet air oxidation (CWAO) of cationic red GTL under mild operating conditions in a batch reactor. The catalyst was prepared by wet impregnation, and characterized by special surface area (BET measurement), X-ray diffraction (XRD) and X-ray photoelectron spectroscopy (XPS). The Fe 2 O 3 -CeO 2 -Bi 2 O 3 /γ-Al 2 O 3 catalyst exhibited good catalytic activity and stability in the CWAO under atmosphere pressure. The effect of the reaction conditions (catalyst loading, degradation temperature, solution concentration and initial solution pH value) was studied. The result showed that the decolorization efficiency of cationic red GTL was improved with increasing the initial solution pH value and the degradation temperature. The apparent activation energy for the reaction was 79 kJ·mol –1 . Hydroperoxy radicals (HO 2 ·) and superoxide radicals (O 2 – ·) appeared as the main reactive species upon the CWAO of cationic red GTL.
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JOURNAL OF MATERIALS SCIENCE-MATERIALS IN ELECTRONICS
·
2018
·Vol. 29
·期 13
·11178-11186
·
IF 2.324
Cheng Yali,He Yue,Li Shuo,Wang Yifang,Zhao Yan,Li Yu,Li Haiying,Liu Li
In the present work, the acetone gas sensing material based on pure α-Fe 2 O 3 nanotubes, pure and Cu-doped α-Fe 2 O 3 porous nanotubes were fabricated by electrospinning and annealing processes. Different Cu dopant concentrations are introduced to investigate the dopant’s role in sensing performance. The structures and chemical compositions of the as-prepared products were examined using a series of material characterization methods including XRD, EDS, SEM and nitrogen adsorption–desorption analysis. And the acetone sensing results demonstrate that the gas sensitivity of porous nanotubes is better than nanotubes. Moreover, compared with pure samples, the sensor based on 3.0 wt% Cu-doped α-Fe 2 O 3 porous nanotubes exhibits higher response (99.43/100 ppm) and excellent selectivity towards acetone at 164 °C. Meanwhile, the detection limit can extend down to ppb level (2.2/100 ppb). Additionally, the sensor also shows fast response and recovery time (5/18 s) and good repeatability to acetone. The enhancement of gas sensitivity is ascribed to not only the effective utility of hollow and porous structures, but also the high catalytic activity of the Cu additive.
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