Materials Today Chemistry
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2022
·
IF 7.613
W. Li,M. Gan,L. Ma,W. Zhao,W. Zhan,S. Deng,F. Xie
A highly active and stable anode catalyst for direct methanol fuel cells is critical to commercialization. Therefore, we have synthesized a unique Fe-doped catalyst Fe–PtBi 2 /Bi 2 O 2 CO 3 -NC through the classical hydrothermal method and sodium borohydride reduction. Physical characterizations confirm the existence of Bi 2 O 2 CO 3 nanosheets and successful loading of PtBi nanocages. It is the alternating layer arrangement of Bi 2 O 2 CO 3 , the bifunctional mechanism of PtBi alloy and the synergistic effect of each component that make the synthesized Fe–PtBi 2 /Bi 2 O 2 CO 3 -NC possess such remarkable methanol oxidation reaction activity (a mass activity of 9345 mA/mg Pt in alkaline electrolyte). Moreover, electrochemical measurements also indicate that 51.7% of the mass activity was retained after 1 h durable operation, which is approximately 4.1 times than that of commercial Pt black. Fe–PtBi 2 /Bi 2 O 2 CO 3 -NC may be applied as a promising alkaline anode catalyst for direct methanol fuel cells due to its outstanding structure and performance. The specific work provides a reference for designing reliable structures and selection of doping elements to enhance the sluggish kinetics of methanol electrooxidation.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2022
·
IF 24.319
Dong-Hua Xie,Pu-Can Guo,Keng-Qiang Zhong,Guo-Ping Sheng
A self-assembly strategy was presented for the synthesis of highly dispersed Co/Fe bimetallic carbon cages (CoFe50@C) through thermal morphology-controlled transformation of Fe doping dual metal-organic frameworks (MOFs). Taking advantage of the well dispersibility, synergetic effects between Fe and Co species, and enhanced graphitization degree of carbon, CoFe50@C exhibited a high removal efficiency of 98% in 180 min for sulfamethoxazole (SMX). The synergistic effect between Co and Fe species played an important role in promoting the reduction of Co(III) to Co(II) and the adsorption of H 2 O 2 molecules, thus enhancing the generation of hydroxyl radicals (HO•), which had been demonstrated by density functional theory (DFT) calculations. Meanwhile, the graphitized carbon cages could prevent the loss of bimetallic active component and promote the electron transfer during catalytic reaction . This work provides a new type of highly dispersed Co/Fe bimetal carbon cages as heterogeneous Fenton nanocatalyst for the degradation of organic contaminants.
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CHEMOSPHERE
·
2022
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IF 8.943
Tao Zhang,Pan Wu,Gary Owens,Zuliang Chen
Since ofloxacin (OFX) is one of many common antibiotics, which effluxes into aquatic environment in relatively high concentration, it has become of significant environmental concern due to the potential for increased antibiotic resistance. In this study, an innovative functional Fe/Ni@ZIF-8 composite was successfully used for the Fenton-like oxidation of OFX, with a OFX removal efficiency >98% under optimal conditions. FTIR analysis confirmed that OFX removal occurred via adsorption to Fe/Ni@ZIF-8 by a combination of π-π bond intercalation and electrostatic interaction, while XPS revealed that the Fe/Ni NPs in Fe/Ni@ZIF-8 were also involved in oxidation. Furthermore, LC-MS analysis identified the presence of several OFX degradation products post exposure, which indicted that Fe/Ni NPs in Fe/Ni@ZIF-8 reacted with H 2 O 2 to form •OH, leading to Fenton-like oxidation of OFX. Thus overall, OFX removal by Fe/Ni@ZIF-8 involved both adsorption to ZIF-8 and Fenton-like oxidation by Fe/Ni NPs. A synergistic mechanism for OFX removal by Fe/Ni@ZIF-8 was thus proposed. The removal efficiency of the synthesized catalysts remained high (above 65%) even after a 5th reuse cycle, which reflected the high stability of Fe/Ni@ZIF-8. Overall, this study demonstrated that Fe/Ni@ZIF-8 had significant potential for the removal of OFX from wastewaters with a removal efficiency >90%.
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International Journal of Applied Ceramic Technology
·
2022
·Vol. 20
·期 1
·24-38
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IF 2.328
Cong Zhou,HaiPeng Feng,GuangAo Liu,Feng Tao,Qi Liu
SiFeCO ceramic nanocomposites with porous structure have been successfully prepared via pyrolysis of novel iron-containing precursors, which were synthesized by modification of polycarbosilane with different contents of MIL-101(Fe), a kind of metal-organic framework made by our laboratory. Iron-containing precursors were pyrolyzed at relatively low temperatures ranging from 500 to 900°C under nitrogen atmosphere, the polymer-to-ceramic conversion process were investigated by Fourier transform infrared spectroscopy, X-ray diffraction (XRD), and thermo gravimetric analysis (TGA) measurements. SiFeCO ceramics with different iron contents were intensively studied with respect to their crystallization behavior, microstructure evolution, and porous morphology influenced by additive amount of MIL-101(Fe). The results of XRD and Transmission electron microscopy revealed that MIL-101(Fe)-modified precursors converted into amorphous SiFeCO ceramics when pyrolyzed below 700°C under nitrogen, extremely small Fe 3 O 4 and α-Fe crystallites with grain size of only 2–5 nm were in situ generated and dispersed uniformly in the SiCO ceramic matrix. Simultaneously, interconnected porous structure was created in the matrix by the decomposition of MIL-101(Fe). The as-obtained SiFeCO ceramics could serve as heterogeneous Fenton-like catalysts for the degradation of xylene orange and exhibit outstanding catalytic properties.
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JOURNAL OF PHYSICS AND CHEMISTRY OF SOLIDS
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2022
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IF 4.383
Yujie Zhang,Qin Yang,Jie Liang,Yongsong Luo,Qian Liu,Yingchun Yang,Xuping Sun
Sulfate radical-based advanced oxidation processes (SR-AOPs) have emerged as an attractive technology in organic dye wastewater treatment. In this study, hydrothermally synthesized Fe-glycerate microspheres is successfully applied as a heterogeneous catalyst to degrade methylene blue (MB) via activating peroxymonosulfate (PMS). The experimental results suggest that MB degradation efficiency and total organic carbon (TOC) removal can arrive at 99.7% and 37.1% in 60 min by the Fe-glycerate/PMS system, indicating that Fe-glycerate microspheres has an excellent catalytic degradation performance. In addition, the effects of PMS concentration, catalyst dosage, initial pH and coexisting ions on MB degradation efficiency were studied. Radical quenching and electron paramagnetic resonance (EPR) tests confirm that the major active species are sulfate radical (SO 4 ·– ) and singlet oxygen ( 1 O 2 ) for MB degradation, followed by superoxide radical (O 2 ·– ) and hydroxyl radical (·OH). Furthermore, the possible mechanism of MB degradation by Fe-glycerate/PMS system was inferred. This work shows Fe-glycerate microspheres can be considered as a new and promising pathway to activate PMS for treating organic dye wastewater.
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Environmental Science-Nano
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2022
·Vol. 9
·期 8
·3081-3093
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IF 9.473
Yuqi Wan,Huaizhi Yang,Qigao Shang,Qingrong Cheng,Hong Zhou,Zhiquan Pan
A novel metal–organic framework@covalent organic framework (MOF@COF) heterojunction was synthesized based on post-synthetic covalent modification. In the present work, aldehyde-modified MOFs (NH2–MIL-101(Fe)) were covalently bonded with covalent organic frameworks (Schiff base network-1, SNW-1) forming the NH2–MIL-101(Fe)@SNW-1 (MS-x) heterojunction by using this strategy. The MS-x heterojunction showed excellent photodegradation ability for pollutants and photocatalytic hydrogen production under simulated sunlight. The superior photocatalytic performance of the MS-x heterojunction can be attributed to the formation of –CN– bonds between NH2–MIL-101(Fe) and SNW-1, which enhances the charge separation efficiency and improves the stability of the photocatalyst. It is worth mentioning that SNW-1 on the surface of the catalyst had a hollow structure which can promote the photoelectric charge migration. Furthermore, the results verified that the matched band structure of NH2–MIL-101(Fe) and SNW-1 could induce a type II heterojunction, which could well explain the improved photocatalytic performance of the photocatalytic system. This work not only provides a new idea to construct highly efficient and stable MOF@COF heterojunctions but also broadens the applications of COF-based materials.
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CHEMICAL ENGINEERING JOURNAL
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2022
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IF 16.744
Shaoxia Yang,Qing Wang,Huazhang Zhao,Daoqing Liu
The intrinsic properties of metal-based adsorbents originate from multiples factors such as surface functional groups, electronic and dimensional structures. However, the synthetic strategies are limited to top-down methods, which inhibited the improvement of adsorbent performance. Herein, Fe-Ce bimetal oxide composites are prepared by a bottom-up modified MOF template method. MOF template-directed nano rod-like morphology can expose more active sites and facilitate phosphate access to active sites. The introduction of citric acid effectively increased the amount of surface –OH groups and greatly improved the phosphate adsorption capacity. Furthermore, the Fe dopant enables the high Ce(III) fraction and generate magnetic property for Fe-Ce bimetal oxide composites, which are capable of enhancing the intrinsic phosphate adsorption performance. The results show that the optimized Fe-Ce bimetal adsorbent showed remarkably high phosphate adsorption capacity, achieving a maximum phosphate adsorption capacity of 357 mg g −1 by Langmuir model. High adsorption capacity and high magnetic separation efficiency characteristics make this adsorbent a promising material for phosphate treatment. The above results further prove the effectiveness of the bottom-up strategy in the design process of environmental functional materials.
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JOURNAL OF ENVIRONMENTAL MANAGEMENT
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2022
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IF 8.91
Xiaoying Jin,Heng Li,Xiuduan Zhu,Na Li,Gary Owens,Zuliang Chen
The integration of metal–organic frameworks with other functional materials has recently emerged as a promising approach for creating innovative materials for environmental remediation. Here, a nano-sized iron/nickel (Fe/Ni) functionalized zeolitic imidazolate framework-8 (ZIF-8-Fe/Ni) was fabricated for oxytetracycline (OTC) removal from wastewater. Cyclic voltammetry and amperometric I-t measurements indicated that OTC was degraded by ZIF-8-Fe/Ni. X-ray diffraction spectroscopy (XRD), transmission electron microscopy mapping (TEM-mapping) and X-ray photoelectron spectroscopy (XPS) indicated that Fe/Ni was evenly dispersed throughout ZIF-8 and partially oxidized after reaction with OTC. OTC adsorption isotherms and kinetics best fitted the Langmuir isotherm ( R 2 > 0.982) and pseudo-second-order model ( R 2 > 0.997), respectively. Reduction kinetics data followed the pseudo-first-order model ( R 2 > 0.905), where the apparent activation energy ( E a) was 22.9 kJ mol −1 , demonstrating that OTC degradation was mainly via a chemical process. The practical removal efficiency of OTC from real wastewater by ZIF-8-Fe/Ni was 92.6%, where even after application of ZIF-8-Fe/Ni for 5 consecutive removal cycles, a high OTC removal of 74.9% was maintained. Thus ZIF-8-Fe/Ni exhibited both high removal efficiency and good recyclability .
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Energies
·
2022
·Vol. 15
·期 16
·5851
·
IF 3.252
Yong Yao,Shizhu Li,Chuangting Chen,Dongchen Zheng,Zhichao Wu,Chi Yu,Shuying Pu,Fa-Qian Liu
MIL-53(Fe) was prepared and modified with benzoic acid to prepare MIL-53(Fe)-BA additive, which was used to improve the catalytic oxidation rate of sulfite, prevent the scaling of the desulfurization tower, and improve the desulfurization efficiency during the wet flue gas desulfurization (WFGD) process of power plants. MIL-53(Fe)-BA exhibits abundant Lewis acid sites because of the appearance of coordination unsaturated Fe atoms. Due to the excellent sorption capacity, Ca(OH)2was used as the main SO2desulfurizer. The composite desulfurizers were prepared by mixing MIL-53(Fe)-based additives and Ca(OH)2, and were characterized by SEM, XRD, and FT-IR. A desulfurization unit was set up at laboratory scale to study the effect of catalytic oxidation additives on sulfite oxidation and desulfurization efficiency. The results showed that the addition of MIL-53(Fe)-BA can increase the oxidation capacity of sulfite by 159%, and greatly improve the desulfurization efficiency. These composite desulfurizers broaden the adaptability of the desulfurizing system to high-sulfur coals, and provide support for improving the desulfurizing efficiency of power plants.Keywords:catalytic oxidation;oxidative desulfurization;wet flue gas desulfurization;calcium hydroxide;MIL-53(Fe);Lewis acid sites
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RENEWABLE ENERGY
·
2022
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IF 8.634
Yuewen Shao,Jie Wu,Zhiyuan Zheng,Mengjiao Fan,Kai Sun,Félix Mérimé Bkangmo Kontchouo,Lijun Zhang,Shu Zhang,Guangzhi Hu,Xun Hu
Production of cyclopentanone (CPO) from biomass-derived furfural is attractive but challenging, as deep hydrogenation or ring-opening of furan ring in furfural over Co-based catalysts hinders the formation of the targeting products. In this study, alloying Co with Fe species in Co–Fe–Al catalysts is proposed for selective conversion of furfural to CPO in water. The formation of CoFe alloy in Co–Fe–Al catalyst weakened the interaction between Co species and the alumina carrier, lowered the adsorption/activation of H 2 , suppressed the formation of especially Brønsted acidic sites, facilitated the electron transfer from Co 0 to Fe species, increased the activation energy for hydrogenation of furfural (from 17.2 kJ mol −1 over Co–Al to 33.4 kJ mol −1 over 1.5Co-1.5Fe-1.0Al), and weakened the adsorption of C C and C–O–C functionalities in furan ring of furfuryl alcohol (FA) on metallic sites. These factors together suppressed deep hydrogenation of furan ring in FA or ring-opening of FA to diols, producing CPO and CPL with total yield of 91.5%, which was attributed to the synergy between hydrogenation and Brønsted acidic sites. In addition, the presence of Fe in Co–Fe–Al catalysts also enhanced the structural stability of Co species, preventing the phase transformation and aggregation of Co species, and rendering the catalyst with superior reusability .
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Journal of Environmental Chemical Engineering
·
2022
·
IF 7.968
Kailin Wang,Songyu Yang,Yan Wu
Dual cocatalysts play an important role in photocatalytic water splitting to hydrogen production . In this paper, Fe-doped Co 3 O 4 (Fe-Co 3 O 4 ) and Pt were loaded on the surface of g -C 3 N 4 to enhance the water photocatalytic splitting, in which Fe-Co 3 O 4 was used as an oxidation cocatalyst to capture the photo-generated holes of g -C 3 N 4 , and Pt was used as a reduction cocatalyst to transfer photo-generated electrons. Under the irradiation of visible light, its hydrogen production rate reaches up to 3.015 mmol g −1 h −1 , which is 3.01 times higher than that of g -C 3 N 4 loaded with Pt. Pt and Fe-Co 3 O 4 dual cocatalysts not only promote the migration rate of photo-generated electrons and holes on the surface of g -C 3 N 4 , but also improve the light absorption capacity of visible light. The interfacial electric field built from the p-n heterojunction of Fe-Co 3 O 4 / g -C 3 N 4 drives photo-generated electrons in Fe-Co 3 O 4 flowing to the holes of g -C 3 N 4 , which further inhibiting the recombination of g -C 3 N 4 photo-generated carriers. This work provides a reference for the development of high-efficiency photocatalyst and an effective support for the development of semiconductor cocatalyst.
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INORGANIC CHEMISTRY
·
2022
·
IF 5.436
Si-Jia Guan,Peng Zhang,Shen-Jing Ji,Yu Cao,Nian-Tzu Suen
It is well known that the “iron” impurity will influence the oxygen evolution reaction (OER) in an alkaline electrolyte, especially for the Ni-based electrocatalyst. Many research studies have investigated the function of Fe in the OER active phase, such as M(OH)2/MOOH (M = Ni and/or Fe), while, surprisingly, very few studies have examined the function of Fe in the “precatalyst” system. Accordingly, in this work, the Ni3–xFexP (x = 0, 0.5, 1) series as an Ni-based precatalyst was employed to inspect the function of internal and external Fe in the Ni-based precatalyst system. It was realized that the sample with internal Fe (i.e., Ni2.5Fe0.5P and Ni2FeP) exhibits efficient OER activity compared to that of the Fe-free one (i.e., Ni3P) owing to the large amount of active M(OH)2/MOOH formed on the surface. This indicates that the internal Fe in the present system may have the ability to facilitate the phase transformation; it was later rationalized from electronic structural calculations that the d band center of the internal Fe (middle transition metal) and Ni (late transition metal) holds the key for this observation. Adding excessive ferrous chloride tetrahydrate (FeCl2·4H2O) as the external Fe in the electrolyte will greatly improve the OER performances for Ni3P; nevertheless, that the OER activity of Ni2FeP is still much superior than that of Ni3P corroborates the fact that the Fe impurity is not the only reason for the elevated OER activity of Ni2FeP and that internal Fe is also critical to the phase transformation as well as OER performance.
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