JOURNAL OF MEMBRANE SCIENCE
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2021
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IF 8.742
Yixuan Gao,Siming Yan,Yi He,Yi Fan,Liyun Zhang,Jing Ma,Ruitong Hou,Li Chen,Jingyu Chen
Herein, a novel membrane with polyacrylic acid (PAA), NH 2 -MIL-88B(Fe) (NM88B), and graphene oxide (GO) was fabricated via a simple vacuum filter method equipped with the nylon membrane substrate. The composite membrane (PAA@NM88B/GO membrane) retained the laminated structure of GO, and PAA@NM88B was used as the photo-Fenton catalytic nano-filler to intercalate GO. Through a series of material characterization and membrane separation performance tests, the results showed that by introducing porous NM88B and PAA cross-linking modification, PAA@NM88B/GO membrane had excellent hydrophilicity, water flux and dye rejection performance. The flux of the PAA@NM88B/GO membrane was 68.21 L m −2 h −1 bar −1 , which is about 15 times higher than that of GO membrane. In addition, the composite membrane had a high rejection (over 97%) for methylene blue (MB), crystal violet (CV) and Congo red (CR). More importantly, PAA@NM88B/GO membrane can also be used to degrade textile wastewater in real life. The membrane can be used as a catalyst to degrade contaminants, and had a high removal of MB in 40 min (98.79%) under the synergistic effect of membrane adsorption and photocatalysis . Therefore, the results indicated that this new type of PAA@NM88B/GO membrane had potential applications in water purification and actual textile wastewater treatment .
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SEPARATION AND PURIFICATION TECHNOLOGY
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2021
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IF 7.312
Langming Bai,Zihan Liu,Haorui Wang,Guibai Li,Heng Liang
Ferrous-activated peroxymonosulfate (PMS) is regarded as a promising technology to treat organic pollutants. However, the excessive sulfate anions generated in the oxidation process need to be considered with respect to their potential harm to the environment and human health. The removal of organic compounds and sulfate anions by Fe(II)/PMS oxidation coupled with nanofiltration (NF) was studied in this research. The mechanism of Fe(II)/PMS coupled with NF in natural organic matter (NOM) and sulfamethoxazole (SMX) removal were systematically investigated by comparison with single Fe(II)/PMS and NF treatments. The results demonstrated that the hybrid system showed better performance than the single treatments for both pollutants. High-performance size exclusion chromatography (HPSEC) analysis indicated that macromolecular organic matter in Songhua River water was broken down and converted into small fragments with a size of approximately hundreds of Da by Fe(II)/PMS oxidation. Zeta potential analysis showed that the zeta potential of the effluent decreased under the effect of Fe(III) and that some small organic molecules generated in the process of oxidation were negatively charged. The SMX removal experiment showed that Fe(II)/PMS oxidation played a leading role in SMX removal in the hybrid system. Moreover, a radical quenching experiment was conducted to explore the effects of SO 4 ·− and HO · on SMX degradation. Fe(II)/PMS treatment effectively alleviated membrane fouling and improved the flux behaviour, with a stable sulfate anion rejection rate of approximately 90% achieved by NF in the long term. These results suggested that Fe(II)/PMS coupled with NF could control membrane fouling, intercept sulfate anions and improve effluent quality, which provides a new strategy for water treatment.
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ACS Sustainable Chemistry & Engineering
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2020
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IF 7.632
Haidong Yang,Yang Liu,Yutong Luo,Shiqing Lu,Bitao Su,Jiantai Ma
Electrocatalytic nitrogen reduction reaction (NRR) represents a highly promising process to ammonia synthesis for artificial N2 fixation. However, the yield rate for NH3 production and Faradaic efficiency (FE) are still low, which greatly hinder its widespread applications. Until now, although a variety of catalysts, including single-atom catalysts, have been developed for NRR in the pursuit of suppressing hydrogen evolution reaction (HER) and the corresponding higher FE, the limited NH3 yield rate makes them uncompetitive for the synthesis of ammonia. Herein, we report a Fe single-atom catalyst anchoring on a nitrogen-doped carbon substrate (Fe SAC/N–C) as a highly efficient NRR catalyst. The catalyst achieves a high FE of 39.6% in 0.1 M KOH under room temperature, particularly a dramatically enhanced NH3 yield rate of 53.12 μgNH3 h–1 mgcat–1. The isotopic labeling (15N2) experiment confirms that the NH3 production completely originates from N2 reduction. Meanwhile, theoretical calculations and X-ray fine structure analysis reveal that the Fe–N3 coordination of Fe SAC/N–C is indeed responsible for the suppression of HER, particularly resulting in a maximum activation of NRR intermediates to produce ammonia with a high yield rate.
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Catalysis Science & Technology
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2020
·Vol. 10
·期 19
·6583-6598
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IF 5.721
Jialing Chen,Gang Peng,Wei Zheng,Wenbo Zhang,Li Guo,Xiaoqing Wu
A superior Fe-containing MCM-22 zeolite prepared by a one-pot synthesis method (OP-Fe/M22) showed excellent NH3 selective catalytic reduction (NH3-SCR) activity and almost 100% N2 selectivity in a wide temperature window (200–500 °C). To investigate the effects of preparation strategies on the NH3-SCR reaction, other three Fe/MCM-22 zeolites with similar iron content (4.4–4.8 wt%) were prepared by solid-state ion exchange (SSIE-Fe/M22), incipient wetness impregnation (IM-Fe/M22) and mechanical mixing (MM-Fe/M22) methods, respectively. Catalytic results in NH3-SCR demonstrate that OP-Fe/M22 gives significantly higher activity in the whole temperature range (100–550 °C) than the other three post-synthesized catalysts. As revealed by XRD, UV-vis, H2-TPR, NH3-TPD, and Py-IR experiments, OP-Fe/M22 has the highest concentrations of isolated Fe3+ species and acid sites, and the lowest concentration of Fe2O3 nanoparticles among the four catalysts, which ensures its highest activity in the NH3-SCR reaction. Besides, OP-Fe/M22 exhibits the higher activity both in NH3 oxidation and NO oxidation reactions than IM-Fe/M22, indicating the better NO oxidation ability and NH3 storage capacity of OP-Fe/M22 which also facilitates the NH3-SCR process. In contrast with Cu-based MCM-22 zeolite obtained from the incipient wetness impregnation method at similar metal content (5% Cu/M22), OP-Fe/M22 shows comparable activity with 5% Cu/M22 in the low-temperature range (100–300 °C) while obviously higher activity at high temperatures (300–550 °C). Moreover, by removing part of undesired iron oxides in OP-Fe/M22 through mild acid post-treatments, the NH3-SCR activity of OP-Fe/M22 in the medium and high temperature ranges (200–550 °C) can be further improved, suggesting that OP-Fe/M22 is a potential catalyst with highly-efficient NH3-SCR activity in a wide temperature window.
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JOURNAL OF CHEMICAL TECHNOLOGY AND BIOTECHNOLOGY
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2021
·Vol. 96
·期 6
·1523-1532
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IF 3.174
Shiting Xu,Xixi Chen,Shujuan Zhan,Shuanghong Tian,Ya Xiong
BACKGROUND To strengthen the treatment efficiency of photocatalytic ozonation, it is necessary to develop a stable bifunctional catalyst active in both processes of photocatalysis and catalytic ozonation. RESULTS A series of Fe doped CeO 2 nanocubes with the main exposure of active (100) crystal facets were simply synthesized by a one-pot hydrothermal method and applied in photocatalytic ozonation for the first time. It was found that doping did not change the morphology of nanocubes but it decreased the crystal size, induced abundant defects of oxygen vacancies and Ce 3+ , and shifted the optical absorption edge to the visible region. Due to these structure modifications, Fe doped CeO 2 nanocubes enhanced the mineralization rate of 4-chlorophenol by 55.4–74.7% and reduced the formation of carcinogenic bromate by 60.2–85.4%, depending on the doping content. Due to the simultaneous occurrence of photocatalysis, catalytic ozonation, and their synergy in 5%Fe-CeO 2 mediated photocatalytic ozonation under solar irradiation, 4-chlorophenol almost completely degraded within 9 min, 74.7% of mineralization rate was achieved within 45 min, and the first order kinetics reaction constant reached 2.97 × 10 −2 ·min −1 , about 4.1 times that of photo ozonation without any catalysts. Moreover, the introduction of 5%Fe-CeO 2 to the ozonation, photolysis, and photo ozonation decreased the corresponding energy consumption by 60.2%, 84.2%, and 62.5%, respectively. CONCLUSION In this study, an efficient and economical Fe doped CeO 2 nanocubes-mediated photocatalytic ozonation process was successfully developed for the refractory organics-containing wastewater treatment under solar light irradiation. © 2021 Society of Chemical Industry
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CHEMICAL ENGINEERING JOURNAL
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2020
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IF 10.652
Huili Zheng,Baoxin Ma,Yesi Shi,Qixuan Dai,Dongsheng Li,En Ren,Jing Zhu,Jianming Liu,Hu Chen,Zhenyu Yin,Chengchao Chu,Xiaomin Wang,Gang Liu
We report the preparation of gallic acid (GA)-modified MoS 2 nanosheets (MoS 2 @GA) with high Fe(III) loading. The MoS 2 @GA-Fe can function as a “Fenton Nanoreactor” in the tumor microenvironment (TME), in which GA-Fe(III) can be reduced to GA-Fe(II) by glutathione (GSH) and amounts of reactive hydroxyl radicals (•OH) are generated during the Fenton reaction. Notably, the MoS 2 degrades into small fragments during the process, and more Mo(IV) reaction sites are exposed on the surface, resulting in a “snowball effect” and enhanced •OH production. Furthermore, unsaturated S atoms can capture protons in the TME and form hydrogen sulfide (H 2 S). We combined the photoacoustic imaging and magnetic resonance imaging contrast properties of MoS 2 @GA-Fe and constructed an imaging-guided chemodynamic treatment, featuring excellent antitumor efficiency and biosafety. The TME-responsive “Fenton Nanoreactor” provides a promising strategy with enhanced translational potency for tumor therapy.
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Journal of Food Measurement and Characterization
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2021
·Vol. 15
·期 2
·1747-1753
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IF 2.431
Li Yi-Fang,Lin Zheng-Zhong,Hong Cheng-Yi,Huang Zhi-Yong
A facile colorimetric method for rapid detection of putrescine (Put) and cadaverine (Cad) based on the peroxidase-like activity of (Fe,Co) codoped-CDs was developed. With the enzymatic hydrolysis by diamine oxidase (EC 1.4.3.6, DAO), Biogenic amines (BAs) were decomposed to produce H 2 O 2 which oxidizes 3,3',5,5'-tetramethyl-benzidine with the catalysis of (Fe,Co)-codoped CDs. By means of principal component analysis, Put and Cad were differentiated from BAs and their total amounts were detected by measuring the spectral absorption at 652 nm with a linear range from 0.25 to 10 mg kg −1 . The colorimetric method was applied to the detection of Put and Cad in various fish samples with a detection limit ((3σ/k, n = 9)) of 0.06 mg kg −1 . Besides verifying with HPLC, the recoveries of the colorimetric method were also tested by spiking standards at three levels with the range of 98.2%–115.7%, indicating that the established colorimetric method was accurate and sensitive.
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ELECTROCHIMICA ACTA
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2020
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IF 6.215
Wenqiang Yang,Qibo Zhang,Samarjeet Singh Siwal,Yixin Hua,Cunying Xu
Herein, S-doped Co-Fe hybrid films with unique 3D porous microsphere arrays stacked by ultrathin nanoflakes directly grown on nickel foam (Co-Fe-S NFs@MS/NF) are synthesized via a single-step co-electrodeposition strategy. The synergistic effects among Fe, S and Co enable superior oxygen evolution reaction (OER) catalytic activity in basic environments. Impressively, this hybrid material can achieve further enhanced OER catalytic performance with surface self-assembly through in-situ electrochemical oxidation activation in both gentle alkaline (GA: 1.0 M KOH at 298 K) and industrial alkaline (IA: 30 wt.% KOH at 353 K) water electrolysis conditions. The transition processes are revealed in detail regarding the chemical, structural, and catalytic properties of the catalysts served in the GA and IA conditions. The pristine quasi-amorphous Co-Fe-S is found to partially transform into crystallized Co(Fe)OOH in the GA condition, while it remains amorphous nature in the IA condition. The enhanced OER activity is attributed to the formation of active Co(Fe)OOH species with massively proliferated specific surface area, optimized electronic structure, and accelerated kinetics. The activated Co-Fe-S NFs@MS/NF exhibits excellent OER activity, achieving 10 and 500 mA cm −2 at ultralow potentials of 1.453 (iR corrected) and 1.517 V with outstanding durability in the GA and IA conditions, respectively. For full water splitting, the assembled two-electrode system based on the Co-Fe-S NFs@MS/NF anode and a Co-S based cathode affords voltages of only 1.518 and 1.685 V to robustly deliver 10 and 500 mA cm −2 in GA and IA conditions over 200 h, respectively.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
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2020
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IF 3.573
Chaofeng Zhang,Yaozong Yang,Linfeng Li,Jiandong Zhang,Shuangping Huang,Ruifeng Li
Polyoxymethylene dimethyl ether (PODEn) is a promising ether fuel. Especially PODE3–5 can be directly mixed into diesel without modification of the diesel engine’s infrastructure for improving thermal efficiency, and significant reduction in particulate matter (PM) and nitrogen oxides (NOx) emissions. In this paper, a series of heterogeneous catalysts, the imidazole sulfonate ionic liquids (ILs) encapsulated in the cages of metal–organic frameworks (MOFs) MIL-100(Fe), were used successfully and efficiently in the synthesis of polyoxymethylene dimethyl ethers (PODEn) from methanol and trioxane (TOX). These catalysts have exhibited excellent catalytic properties because of strong Brønsted acid sites. MIL-100(Fe)@[BSO3HIm][CF3SO3] shows the best catalytic activity with 96.98% conversation of TOX and 47.49% selectivity of the desired product PODE3–5 under a mild reaction condition. Of importance is that the catalyst is recovered easily and reused.
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CANADIAN JOURNAL OF CHEMICAL ENGINEERING
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2020
·Vol. 99
·期 9
·1962-1975
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IF 1.687
Haoran Du,Zhaoping Zhong,Bo Zhang,Jimin Fu,Zhaoying Li
To obtain high-value bio-oil, pure ceria (CeO 2 ) and a series of Ce/Fe composite metal oxides were synthesized via precipitation method and were used to enhance hydrocarbons and ketones production during catalytic pyrolysis of bamboo sawdust. The characterization results were comprehensively analyzed and revealed that doping CeO 2 with Fe promoted the formation of a solid solution structure, which further increased the surface area and number of oxygen vacancies of the catalyst for deoxygenation. Experimental consequences demonstrated that, compared to non-catalytic trial, the catalytic pyrolysis over CeO 2 generated lower amounts of acids and aldehydes, and enhanced the conversion of large oxygenates to monofunctional hydrocarbon precursors via decarboxylation, deoxidation, and ketonization. The concentrations of hydrocarbons and ketones obtained over Ce/Fe catalysts were significantly higher than those obtained over CeO 2 , and that was attributed to the higher surface area and oxygen storage capacity of Ce/Fe catalysts. Particularly, the composite catalyst with the Ce/Fe molar ratio of 4 (Ce 0.8 Fe 0.2 ) presented the most optimal deoxidation capacity in this study. The relative concentration of hydrocarbons generated over Ce 0.8 Fe 0.2 was the highest, and monocyclic aromatics and short-chain aliphatic hydrocarbons accounted for 47.13% and 29.72%, respectively, of the total hydrocarbons. Simultaneously, the amount of ketones, the main hydrocarbon precursors, obtained over Ce 0.8 Fe 0.2 was significantly higher than that obtained over CeO 2 , and the fraction of linear and cyclic ketones of the total ketones increased from 45.96% for the non-catalytic pyrolysis to 97.57%. This further confirmed that the mesoporous Ce/Fe composite catalysts efficiently catalyzed the aldol condensation and ketonization reactions.
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Molecular Catalysis
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2020
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IF 3.687
Wei Wu,Wei Zhang,Yu Long,Jiaheng Qin,Jiantai Ma
In this work, by the simple pyrolysis of Fe 2+ , Co 2+ or Ni 2+ and 1,10-phenanthroline (Phen) complexes under the presence of activated carbon and dicyandiamide in nitrogen atmosphere, different nonprecious transition metal-based species that well confined in nitrogen doped carbon (M-N-C, M = Fe, Co or Ni) were prepared. The Fe-N-C showed the best catalytic performance for the transfer hydrogenation of halogenated nitrobenzenes. More importantly, through the catalytic results comparison of the three catalysts estimated by gas chromatography-mass spectrometer, two speculations might be presented for the reaction pathway depending on the catalyst used. The transfer hydrogenation reaction route over Fe-N-C might follow the indirect way like the Co-N-C and Ni-N-C. Another assumption was the Fe-N-C might go through the direct pathway in contrast to the Co-N-C and Ni-N-C which resulted in formation of azoxybenzene and azobenzene intermediates before complete conversion to aniline. Those differences were found to be correlated with the different valence states and active metal components in different catalysts. In addition, the optimal Fe-N-C could be efficiently recovered by using an applied magnetic field and reused without significant decrease of activity. Therefor the catalyst may possess important potential for the industrial application in the selective hydrogenation of halogenated nitrobenzenes.
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ACS Sustainable Chemistry & Engineering
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2020
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IF 7.632
Qingqing Zha,Mingxia Li,Zihao Liu,Yonghong Ni
Metal–organic frameworks (MOFs) have attracted much interest in electrocatalysis as promising catalysts in recent years. However, it still remains a challenge to directly use MOF-based materials as bifunctional electrocatalysts for overall water splitting. Herein, a hierarchical Co,Fe-MOF-74/Co/carbon cloth (CC) three-layer hybrid electrode is synthesized by a simple electrochemical deposition technology with subsequent solvothermal treatment. Electrochemical performance investigations show that the as-constructed Co,Fe-MOF-74/Co/CC electrode exhibits impressive electrocatalytic activity for full water splitting, which only requires a low overpotential of 226 mV@20 mA cm–2 for the oxygen evolution reaction (OER) and 94 mV@–10 mA cm–2 for the hydrogen evolution reaction (HER), respectively. Employing the as-constructed electrode as the anode and cathode in a two-electrode setup simultaneously, only 1.65 V of the voltage is needed to deliver the current density of 20 mA cm–2. The above excellent electrochemical performances should be attributed to the specific architecture, the synergistic effect of the Co and Fe species, and the superhydrophilic surface of the catalyst. More importantly, further investigations uncover that metal hydroxides and oxyhydroxides produced in situ during electrochemical tests are the veritable active species, which promote the high catalytic activity of the present catalyst.
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