CHEMISTRY OF MATERIALS
·
2022
·
IF 10.508
Jie Xue,Ziyu Wang,Andrew Comstock,Zhiyu Wang,Herman H. Y. Sung,Ian D. Williams,Dali Sun,Junwei Liu,Haipeng Lu
Recent discoveries of novel physics in two-dimensional (2D) magnetic materials have sparked the search of new layered magnetic semiconductors. Compared to the traditional inorganic 2D van der Waals crystals, hybrid organic–inorganic metal–halide frameworks offer significantly enhanced chemical and structural versatility, where their optical, electronic, and magnetic properties can be readily modulated with both organic and inorganic components. Here, we reported a series of new Fe–Cl-based layered double perovskites LnMIMIIICl8, [n = 4, L = phenylethylammonium or chiral R-(+)-β-methylphenethylammonium and n = 2, L = 1,4-butanediammonium; MI = Ag/Na; MIII = Fe/In]. UV–vis measurements show that their optical band gaps are highly tunable by varying the organic cations, MI ion, and MIII ion. Magnetic susceptibility measurements suggest an antiferromagnetic coupling between the nearest FeIII–FeIII, where the Curie–Weiss temperature, Néel temperature, and frustration factors can be easily modulated with their compositions and dimensionality. Our study demonstrates the rich and interesting magnetic properties in these layered transition-metal–halide double perovskites and paves the way for design of multifunctional magnetic materials.
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iScience
·
2026
·Vol. 29
·期 10
·117733
·
IF 4.5
Yanlin Wu,Wenyu Yang,Yilan Zeng,Dingfeng Huang,Wenbo Dong,Olivier Monfort,Martin Motola
Natural resveratrol can assist Fe(III)-mediated PDS activation • RES promotes Fe(III) reduction and supports Fe(III)/Fe(II) cycling • Balanced RES concentration improves redox cycling while limiting radical competition • Near-neutral OFL degradation is achieved without additional pH adjustment Summary Iron-mediated peroxydisulfate (PDS) activation is limited by slow Fe(III)/Fe(II) redox cycling under circumneutral conditions. Here, resveratrol (RES), a natural stilbene polyphenol, was introduced as a low-dose redox mediator to promote Fe(II) formation from Fe(III) for enhanced PDS activation. The Fe(III)/RES/PDS system showed higher ofloxacin (OFL) degradation than the corresponding single-reagent and binary systems and achieved approximately 90% OFL degradation at pH 6.5. Chemical quenching and competition-kinetic analysis indicated that sulfate radical (SO 4 ·− ) was the major contributor to OFL degradation, while hydroxyl radical ( · OH) played a secondary role. Matrix experiments showed that Cl − and NO 3 − had minor effects, whereas NO 2 − strongly inhibited OFL degradation. This work provides a case study of RES-mediated Fe(III)/PDS activation for antibiotic degradation under near-neutral conditions. Download: Download high-res image (83KB) Download: Download full-size image
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JOURNAL OF POWER SOURCES
·
2023
·
IF 9.2
Xiaocan Wang,Zhangtang Jiang,Yichang Ma,Xiangyu Su,Xikang Zhao,Aimei Zhu,Qiugen Zhang
Anion exchange membrane water electrolysis (AEMWE) is a feasible pathway to industrial-scale production of hydrogen due to the use of low cost, non-precious metal catalysts . In this study, we demonstrate a stable NiFe 2 O 4 anodic oxygen evolution reaction (OER) catalyst to achieve durable and efficient AEMWE via a simple strategy combining hydrothermal and thermal reduction reactions. The prepared NiFe 2 O 4 -50 catalyst, with polyhedral-sphere hybrid morphology and abundant oxygen vacancies , exhibits an overpotential of 280 mV at 50 mA cm −2 and a Tafel slope of only 44.6 mV dec −1 for OER. Moreover, its use as oxygen evolution electrode in AEMWE cell assembled with a Pt/C cathode show excellent water electrolysis performance with a current density of high to 4 A cm −2 at 1.89 V, a cell voltage of only 1.64 V at 1 A cm −2 , as well as good long-term stability over >1000 h of continuous water electrolysis under a current density of 1 A cm −2 . The newly developed NiFe 2 O 4 catalyst demonstrates excellent AEMWE performance and has a potential application for practical large-scale hydrogen production .
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CERAMICS INTERNATIONAL
·
2023
·
IF 5.2
Liyuan Liu,Guanfu Liu,Shibo Wu,Jiahao He,Yang Zhou,Muslum Demir,Ruona Huang,Zijin Ruan,Guohua Jiang,Pianpian Ma
Sr-based perovskites represent enormous potential as supercapacitor electrode materials. However, the wide-temperature supercapacitor application for perovskite-based electrodes has not been studied yet. Thus, there is a pressing need for comprehensive research and investigation in the wide-temperature range to unlock the full capabilities of Sr-based perovskite and pave the way for its successful integration into versatile supercapacitor systems. In this study, SrCo 1- x Fe x O 3-δ ( x = 0.05, 0.10, 0.15 and 0.20) were synthesized by solid-state sintering method, as oxygen-intercalated electrode materials for wide temperature-tolerant supercapacitors. SrCo 1- x Fe x O 3-δ contains orthogonal and monoclinic phases for x = 0.05 and x = 0.10, and a stable monoclinic phase can be obtained when the substitution amount is at least 15 %. The best electrochemical performance was obtained in x = 0.10, with a specific capacitance of 526.6 F g −1 at 1 A g −1 . This can be attributed to the lowest resistance and richest oxygen vacancies of SrCo 0.9 Fe 0.1 O 3-δ , which are conducive to oxygen-intercalated energy storage. The SrCo 0.9 Fe 0.1 O 3-δ @CC//AC@CC supercapacitor device displays a working voltage of 1.6 V and a stable long-term cycle life with 85.71 % capacity retention after 5000 cycles. Furthermore, the temperature-dependent electrochemical characterization indicates an improvement of electrochemical performance for both electrode and device as temperature increases, which may be ascribed to the enhanced ion migration in the electrolyte. From 0 to 85 °C, the specific capacitance of SrCo 0.9 Fe 0.1 O 3-δ @CC electrode increases from 91.8 to 1035.9 F g −1 at 1A g −1 , and the energy density of the device also increases from 7.6 to 26.2 Wh kg −1 when the power density is 800 W kg −1 .
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CHEMOSPHERE
·
2023
·
IF 8.8
Zhenda Liang,Zhiquan Chen,Yongtao Xu,Haiqing Wang,Li Zhou,Bing Yan
Manganese dioxide (MnO 2 ) has been recognized as one of the natural systems' most active mineral oxidants. However, when it comes to catalytic oxidation of antibiotic applications, pure MnO 2 falls short in delivering satisfactory performance. Hence, a set of Fe 3+ -doped porous MnO 2 (0.02Fe–MnO 2 , 0.1Fe–MnO 2 , and 0.14Fe–MnO 2 ) nanoparticles were synthesized here via a convenient and energy-efficient one-step reaction method. A series of experiments revealed that Fe-doping strategy enhances the properties of MnO 2 host by suppressing the crystalline structure, increasing the amount of surface oxygen defects, and modifying the Mn 3+ /Mn 4+ ratio. Specifically, the tetracycline (TC) removal efficiency of 0.14Fe–MnO 2 reaches 92% without the need for any additional co-oxidant, representing a 20% improvement over pristine MnO 2 nanoparticles . Moreover, this process shows a fast dynamic (achieving 70% of TC removal in just 5 min) and demonstrates pH-resistance, maintaining high TC removal efficiency (≥90%) over a wide pH range of 3.0–9.0. Mechanical studies reveal that the degradation of TC can be attributed to the oxidation by reactive oxygen radicals and Mn 3+ , with 1 O 2 being the primary radical involved in the reaction, accounting for 55% of TC removal. Importantly, cytotoxicity testing indicates that the biotoxicity of TC toward organisms can be effectively mitigated using 0.14Fe–MnO 2 nanomaterial . This study presents a readily applicable candidate for economically and conveniently eliminating of environmental TC pollution, thereby reducing the threat posed by TC pollution to the ecosystem.
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APPLIED CLAY SCIENCE
·
2023
·
IF 5.6
Haibin Yang,Junzhen Guo,Liang Chu,Zhi Huang,Zhaohui Liu,Liyan Wang,Zhaokun Wang,Mu Yang,Ge Wang
Utilizing natural, abundant, and eco-friendly materials to facilitate the industrial application of nano-sized MOF particles is of utmost importance, since these nanoparticles possess high activity but difficult to recovery. Herein, benefiting from the negatively charged vermiculite , dispersed nano-sized Fe-MOF particles were successfully in-situ grown on the surface of vermiculite nanosheets (VNs) via a simple solvothermal method. The construction of the composites improved the exposure of organic dye to active sites, resulting in a remarkable performance of Fe-MOF@VNs-4 towards photo-Fenton degradation of RhB , with a k value of 0.096 min −1 and an activity of 0.581 mmol g −1 h −1 , significantly higher than that of pure VNs and Fe-MOF, surpassing most reported MOF composite catalysts. The excellent adsorption ability of Fe-MOF@VNs, along with the presence of divalent iron in vermiculite, greatly enhanced catalytic performance. Mechanistic investigations revealed that VNs facilitate the separation of photoinduced carriers excited from Fe-MOF, indicating a synergy effect between Fe-MOF and VNs. Overall, this work provides a simple and effective strategy to design large-scale and commercially available catalysts for water treatment , and also offers a promising alternative for the industrial application of nano-sized MOF particles.
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JOURNAL OF POROUS MATERIALS
·
2021
·Vol. 28
·期 5
·1315-1324
·
IF 2.496
Cai Qiang,Yue Xiaoyang,Dong Wen-Sheng
Bimetallic modified Fe–Sn/Beta was synthesized and examined as a solid acid catalyst for the transformation of glucose into methyl lactate in methanol. The catalysts were characterized by a combined characterization techniques i.e. X-ray fluorescence spectroscopy, N 2 physisorption, powder X-ray diffraction, X-ray photoelectron spectroscopy, NH 3 temperature-programmed desorption, and pyridine adsorption Fourier transform infrared spectroscopy. A high yield of methyl lactate of 67% was achieved upon conversion of 0.3 g glucose in 24 g methanol over 0.15 g catalyst at 220 ℃ under 2 MPa N 2 for 6 h. The recyclability of the catalyst was also investigated, and the conversion of glucose remained constant; conversely, the yield of methyl lactate decreased slightly in five catalytic runs. The excellent catalytic performance of Fe–Sn/Beta was attributed to the presence of large amounts of Lewis acid sites. Besides, the rich mesoporosity in Fe–Sn/Beta improved mass transfer rates in the conversion of glucose to alkyl lactates.
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Sustainable Energy & Fuels
·
2021
·Vol. 5
·期 8
·2228-2233
·
IF 6.367
Xinyue Zhang,Yanling Qiu,Wenxiu Zhang,Xuqiang Ji,Jingquan Liu
Ingeniously designing a water-oxidation catalyst with advantages of a large surface area, multicomponent synergy, and optimized electronic structure, especially utilizing a one-step reaction system to achieve these dominant characteristics is pivotal to high-performance electrochemical water splitting. Here, flower-like multiphase nickel hydroxide catalysts doped with Fe (Fe-α,β-Ni(OH)2) are fabricated through a one-pot solvothermal-coordination methodology. The resulting Fe-α,β-Ni(OH)2 presents excellent oxygen production activity. An overpotential of 267 mV is required to drive a current density of 30 mA cm−2. Fe-α,β-Ni(OH)2 achieves stable operation for over 20 h. The considerable OER performance should result from the unique bionic flower structure, large surface area, and Fe-doping as well as the unique phase interfaces between the α- and β-Ni(OH)2 components. Our study provides a new trial of combining several favorable structural features into one material system that benefits efficient OER catalysis based on earth-abundant Fe and Ni elements.
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RSC Advances
·
2021
·Vol. 11
·期 17
·9977-9984
·
IF 3.361
Fuhua Wei,Qinhui Ren,Huan Zhang,Lili Yang,Hongliang Chen,Zhao Liang,Ding Chen
Zirconium-iron metal–organic frameworks (Zr/Fe-MOFs) and Zr/Fe-MOF/graphene oxide (GO) composites were prepared via solvothermal synthesis using ferrous sulfate heptahydrate, zirconium acetate, and 1,3,5-benzenetricarboxylic acid. The MOFs and composites were measured using scanning electron microscopy (SEM), infrared spectrometry (IR), and thermogravimetric analysis (TGA). In this study, we explored the ability of Zr/Fe-MOFs and Zr/Fe-MOF/GO composites to adsorb tetracycline hydrochloride from an aqueous solution. Additionally, we optimized the adsorption performance by varying the ratio of MOFs and MOF composites to tetracycline hydrochloride solution, the concentration of tetracycline hydrochloride solution, and the pH of the solution. The results were investigated and fit to both pseudo-first-order and pseudo-second-order kinetic models. The results of the Freundlich and Langmuir isotherm models indicate that Zr/Fe-MOFs and Zr/Fe-MOF/GO composites have heterogeneous adsorption surfaces and that tetracycline hydrochloride is adsorbed over Zr/Fe-MOFs and Zr/Fe-MOF/GO by multilayer adsorption. Overall, our findings indicate that Zr/Fe-MOFs and Zr/Fe-MOF/GO composites can effectively treat wastewater, providing an inexpensive alternative to other methods.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2021
·
IF 7.312
Jia Deng,Xiang Zhan,Feng Wu,Shuxian Gao,Li-Zhi Huang
Trichloroethylene (TCE), one of the most frequently detected chlorinated organic pollutants (COPs) in groundwater, has potential risks to human health. The bimetallic system consisting of zero-valent iron (ZVI) and a second catalytic metal has been widely investigated for reductive dechlorination of COPs. However, the passivation layer of ZVI inhibits the electron transfer causing a low dechlorination efficiency. In this work, we designed a novel bimetallic system using Fe(OH) 2 and Ni for fast dechlorination of TCE. The reduction efficiency of TCE reaches 94.8 % after 5 h of reaction in the Fe(OH) 2 /Ni system. TCE was completely dechlorinated to nontoxic gas products including ethylene and ethane, which was attributed to the generation of active hydrogen species (H*) in the system. The Ni 2+ cations undergo the process of hydroxylation and olation. Subsequently, electrons of Fe(OH) 2 were transferred to Ni(II) causing the formation of Ni(0). The catalytic Ni(0) sites generate H* for TCE dechlorination via catalytic reduction of H 2 O/H + . A part of Fe(II) in the Fe hydroxide layer of Fe(OH) 2 was oxidized to Fe(III) leading to the formation of green rust with a hexagonal structure. Our work demonstrates Fe(OH) 2 /Ni is a promising composite material for the remediation of TCE-contaminated groundwater.
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Journal of Materials Chemistry B
·
2021
·Vol. 9
·期 23
·4726-4734
·
IF 6.331
Wenli Zhao,Guangpu Zhang,Yang Du,Shuangqin Chen,You Fu,Fan Xu,Xiangyun Xiao,Wei Jiang,Qingmin Ji
The proportion of Fe2+ and Fe3+ in Fe-based nanozymes is a key point in determining their catalytic activity. However, it is hard to adjust the Fe2+/Fe3+ ratio in nanozyme systems to achieve the best catalytic performance. In this work, we successfully regulate Fe2+/Fe3+ ratios in a wide range of 0.81–1.45 based on a novel porous platform of Fe doped silica hollow spheres. The homogeneous distribution and stable fixation of Fe components in Fe doped silica hollow spheres facilitate the valence regulation of Fe in the reduction heating in H2/Ar. When the Fe doped spheres (FeOx@SHSs) were used as nanozymes, different Fe2+/Fe3+ ratios have shown to influence the peroxidase-like catalytic activity greatly. The highest activity at the ratio of 1.41 should be due to the combined effects of the accelerated reaction rate by Fe2+ and the enhanced catalytic cycle efficiency by Fe3+. The FeOx@SHSs-based nanozyme is further applied to construct a facile colorimetric biosensing system, which exhibited extremely sensitive determination of glucose. This work presents an effective platform for controlling Fe valences and optimizing the peroxidase-like activity for catalytic processes or sensing systems.
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WATER RESEARCH
·
2021
·
IF 11.236
Shi-Qi Tian,Jing-Yao Qi,Yun-Peng Wang,Yu-Lei Liu,Lu Wang,Jun Ma
After reaction with permanganate or ferrate, the resulted Mn-loaded and Fe-loaded biochar (MnOx/biochar and FeOx/biochar) exhibited excellent catalytic ozonation activity. O 3 (2.5 mg/L) eliminated 48% of atrazine (ATZ, 5 μM) within 30 min at pH 7.0, while under identical conditions, ozonation efficiency of ATZ increased to 83% and 100% in MnOx/biochar and FeOx/biochar (20 mg/L) heterogeneous catalytic systems, respectively. Radical scavenger experiment and electron paramagnetic resonance (EPR) analysis confirmed that hydroxyl radical (•OH) was the dominant oxidant. Total Lewis acid sites on MnOx/biochar and FeOx/biochar were 3.5 and 4.1 times of that on the raw biochar, which induced enhanced adsorption of O 3 and its subsequent decomposition into •OH. Electron transfer via redox pairs on MnOx/biochar and FeOx/biochar was observed by cyclic voltammetry scans, which also functioned in the improved catalytic capacity. Degradation pathways of ATZ in MnOx/biochar and FeOx/biochar ozonation systems were proposed, with 34.6% and 44.8% of dechlorination effect accomplished within 30 min of reaction, which was improved by 4.1 and 5.3 times compared to pure ozonation. After 12-hour treatment, acute toxicity of ATZ oxidation products was reduced from 38.3% of pure ozonation system to 14.5% and 6.3% of activated ozonation systems with MnOx/biochar and FeOx/biochar, respectively. Mn-loaded biochar and Fe-loaded biochar have great potential for heterogeneous catalytic ozonation of polluted water.
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