JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2021
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IF 8.128
Di Chen,Guofu Li,Xing Chen,Qian Zhang,Jing Sui,Chengjie Li,Yingchao Zhang,Jing Hu,Jianhua Yu,Liyan Yu,Lifeng Dong
Rational construction of advanced bifunctional catalysts with dual-active-sites is still challenging for both oxygen reduction (ORR) and oxygen evolution reactions (OER). Herein, metal-doped dicyandiamide formaldehyde resin is innovatively exploited to synthesize N/Co/Fe/Ni multi-doped carbon nanotubes (denoted as CoFeNi@CNT) with metal-nitrogen-carbon (M N C) and CoFeNi nanoparticles as the ORR and OER active sites, respectively. Abundant active sites and high degree of graphitization enable CoFeNi@CNT with a high ORR half-wave potential of 0.82 V and a low OER overpotential of 440 mV at 10 mA cm −2 , which are comparable or superior to noble-metal catalysts. Particularly, the CoFeNi@CNT air electrode of rechargeable Zn-air batteries shows remarkable open circuit potential (1.46 V), discharge power density (152.3 mW cm −2 ), specific capacity (814 mAh g −1 ), and cycling stability for more than 250 h. It is worth emphasizing that this synthesis strategy is rather simple, low-cost, high yield, and the proportion and amount of doped metal ions can be easily adjusted according to the needs for different applications.
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高影响因子
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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Nano Research
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2021
·Vol. 14
·期 11
·4304-4313
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IF 8.897
Zhai Yi,Wang Fumin,Zhang Xubin,Lv Guojun,Wu Yuzhou,Jiang Tao,Zhang Qing,Li Mengyue,Li Mengyao,Liu Yongkui
How to directionally design the hollow zeolite via a green route is of great significance. Here, we successfully synthesized the hollow Fe-silicate-1 encapsulated ultra-small Fe 2 O 3 nanoparticles (2.5 nm) with higher yield (85.2%) by mother liquid than traditional dissolution-recrystallization for the first time, which was achieved by precisely regulating the number and distribution of defects in zeolite and cleverly utilizing the TPAOH and nuclei in mother liquor. The effects of synthetic temperature, synthetic period and addition amount of parent zeolite on the formation of hollow zeolite have been investigated and the effect of synthetic conditions on the defects in parent zeolite has been also firstly quantified. The corresponding formation mechanism has been proposed. The abundant inner defects provided by the zeolite synthesized at 130 °C for 1 day and large amount of TPAOH remaining in mother liquid are conducive to the formation of hollow zeolite. Meanwhile, both parent zeolite and nuclei (4-, 5-member rings and structure units) in mother liquid obtained at 130 °C play the crucial roles in enhancing the zeolite yield. Notably, Fe 2 O 3 nanoparticles could decompose into small fragments by the interaction with nuclei in mother liquid. Partial ultra-small Fe 2 O 3 nanoparticles would be encapsulated in cavity and the rest could be inserted in the zeolite framework, which is significantly different from the conventional dissolution-recrystallization mechanism. The obtained encapsulated catalyst shows the superior catalytic performance and stability in phenol and tetracycline degradation reactions.
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JOURNAL OF ENVIRONMENTAL MANAGEMENT
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2021
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IF 6.789
Qiang Zeng,Hui Zhong,Zhiguo He,Liang Hu
Developing materials from natural minerals to efficiently remove arsenite (As(Ⅲ)) from solution is vital important for resources comprehensive utilization and environment protection. In this study, biotite containing minerals was used to prepare a novel composite of amino modified silica supported MnO 2 /Fe–Al hydroxide (SNMFA composite), which was then applied to remove arsenite. Scanning electron microscope (SEM), X-ray diffraction (XRD) and X-ray photoelectron spectroscopy (XPS) results indicated that many amorphous MnO 2 and Fe–Al hydroxide nano sheets were loaded on the surface of layered silica structure. Batch experiments showed that this composite could efficiently remove As(Ⅲ) from aqueous solution, and the maximal removal capacity was identified as 46.11 mg/g. As(Ⅲ) adsorption behaviours of SNMFA composite were confirmed by the pseudo-second-order kinetic model and Langmuir model, indicating that As(Ⅲ) adsorption on its surface was monolayer adsorption. The adsorption process was a pH and temperature dependent process, and increasing pH and temperature have facilitated the removal of As(Ⅲ). Thermodynamic analysis showed that As(Ⅲ) adsorption process was a spontaneous endothermic reaction . The As(Ⅲ) removal was mainly relied on the stable inner-sphere coordination model, and the corresponding mechanisms were involved in chelation, precipitation, oxidation-adsorption and electrostatic interaction.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2021
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IF 7.312
Li Li,Qian Zhang,Yuecheng She,Yongbo Yu,Junming Hong
Mn–Fe bimetal catalyst possesses excellent activation properties, and the enhancement of Mn/Fe redox cycle for electron transfer is related to the crystalline structure and surface functional groups. Therefore, material structure optimization is an effective strategy to improve its activation performance in advanced oxidation . In this study, Mn–Fe LDO catalyst with strong Mn/Fe synergistic effect was synthesized, and used for bisphenol A degradation. Under the condition of 0.4 g/L Mn-Fe LDO, 1.5 mM PMS and pH 7.0, Mn-Fe LDO/PMS system exhibited excellent degradation performance that 100% of BPA (20 mg/L) and 72.0% of COD could effective be degraded within 50 min. Five-run recycle and metal ions leaching experiments proved the excellent reusability and stability of Mn-Fe LDO. To deepen the understanding of catalytic mechanism, the synergistic effect and electron transfer between Mn and Fe were confirmed via XPS and CVs results. Moreover, the indispensable role of surface hydroxyl groups were clarified via phosphate masking experiment, ATR-FTIR and LSV analysis. The presence of Mn and Fe active sites and hydroxyl groups on Mn-Fe LDO surface could efficiently promote electron transfer, thus accelerating the redox cycles of Mn 3+ /Mn 2+ and Fe 3+ /Fe 2+ . The generation of SO 4 ·− and HO· as the main radicals was occurred on the surface of Mn-Fe LDO, and SO 4 ·− played a major role during the reaction. On the basis of these experimental conclusions, the mechanisms of Mn–Fe LDO/PMS system for high-efficiency BPA degradation were proposed. GC-MS analysis was performed to detect the BPA degradation intermediates and propose the possible degradation pathways.
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Journal of Environmental Chemical Engineering
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2021
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IF 5.909
Peng Liu,Dengjie Zhong,Yunlan Xu,Nianbing Zhong,Guangjun He
Co/Fe co-doped porous graphite carbon (Co/Fe-PGC) nanocomposites were successfully prepared by one-step pyrolysis with CoFe-MOF, in which the Co/Fe nanoparticles were uniformly coated on porous graphite carbon derived from MOF. It was used to microelectrolysis-Fenton degrade rhodamine B through the main active substance ∙OH. The color and TOC removal rate of 100 mg/L rhodamine B reached 99.41% and 64.6%, respectively, for 30 min. Rhodamine B was degraded into small molecular organic acids, alcohols and lipids by N-demethylation and chromophore cleavage, until it was finally degraded into CO 2 and H 2 O, and no new colored organics were produced in the degradation process. The degradation process follows the first-order reaction kinetics, and its rate constant is much higher than that of the previous similar studies. The excellent catalytic performance of Co/Fe-PGC catalyst is attributed to the coupling effect of micro-electrolysis and Fenton reaction, and the acceleration of cobalt on electron transport and Fe 2+ reduction. Co 0 /Fe 0 undergoes galvanic corrosion to generate Co 2+ /Fe 2+ and H 2 O 2 , and then these products undergo Fenton reaction to generate Co 3+ /Fe 3+ and ∙OH, thus forming a circulating system of Co 3+ /Fe 3+ and Co 2+ /Fe 2+ , enhancing the activation of H 2 O 2 and ensuring the efficient degradation of RhB.
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Sustainable Environment Research
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2021
·Vol. 31
·期 1
·1-12
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IF 4.98
Liang Dongxu,Chen Yu,Zhu Suiyi,Gao Yidi,Sun Tong,Ri Kyonghun,Xie Xinfeng
Herein, a KFeS2 whisker was formed in mass production at a low temperature, with waste cold-rolling sludge as Fe source, which exhibited good performance in the removal of Zn/Ni from real electroplating effluent. At laboratory scale, KFeS2 was generated at 80 °C by the hydrothermal method, and KFeS2 whisker grew radially with the extension of the reaction time. This method was applied at pilot scale, where a similar KFeS2 whisker was also produced with waste cold-rolling sludge as Fe source, and a residual brownish supernatant was observed after the reaction and then completely recycled in the next round for KFeS2 synthesis. After recycling five times, the produced KFeS2 whisker did not change. The drying and storage of KFeS2 have also been verified. Freeze drying and vacuum drying were applicable, whereas air drying was not profitable. Moreover, the efficiency of Zn/Ni removal using undried KFeS2 was similar to that of dried KFeS2. The efficiencies of Zn/Ni removal using KFeS2 were apparently higher those of common reagents for wastewater treatment.
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CHEMICAL ENGINEERING JOURNAL
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2021
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IF 13.273
Yuanfeng Wei,Weijian Yang,Zhimin Wang,Kai Yin,Tao Chen,Chengbin Liu
Iron oxide-modified biochars are increasingly recognized as a promising arsenic adsorbent. However, most of them face serious challenges in the rapid and efficient removal of As(III). Herein, we integrated the iron oxide nanoneedles vertically covered biochar fibers (Fe-BFs) with H 2 O 2 and Hydroxylamine (HA) to construct a heterogeneous catalytic system for the rapid oxidation and deep removal of As(III) from water. The system oxidized the As(III) to As(V) with high efficiency, and then the generated As(V) could be rapidly removed by adsorption onto Fe-BFs. The removal efficiency of As(III) by Fe-BFs/H 2 O 2 /HA at 120 min reached up to 98.93%, which is much higher than that of by Fe-BFs (69.20%) and Fe-BFs/H 2 O 2 (92.32%). The system could work reliably in a wide pH range (4–10). Moreover, fixed-bed column experiments demonstrated that the addition of H 2 O 2 and HA could increase the effective treatment volume from ~350 bed volume (BV) to ~700 BV to meet the drinking water standard (<10 μg/L). The introduction of HA induced the reduction of surface Fe(III) of Fe-BFs to surface Fe(II), which reacted with H 2 O 2 to produce OH. The OH played a very important role in promoting the removal of As(III). This study offers a new strategy to enhance the applicability of Fe modified biochar for As(III) removal.
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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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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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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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APPLIED CATALYSIS B-ENVIRONMENTAL
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2021
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IF 19.503
Chen Chen,Yongxiao Tuo,Qing Lu,Han Lu,Shengyang Zhang,Yan Zhou,Jun Zhang,Zhanning Liu,Zixi Kang,Xiang Feng,De Chen
Metal-organic frameworks (MOFs) have recently emerged as promising precursors to construct efficient non-noble metal electrocatalyst for oxygen evolution reaction (OER). Herein, a Co-Ni-Fe spinel oxide-carbonitrides hybrids (CoNiFeO x -NC) electrocatalyst with hierarchical structure was synthesized from Fe-MIL-101-NH 2 through a unique ion-exchange based strategy. The ion exchange of Fe-MIL-101-NH 2 with both Ni and Co ions induced a hierarchically structured 2-D ternary metal MOF shell layer encapsulated 3-D octahedral MOF crystals as a core. This prevents the collapse of MOF frameworks during the air calcination process and affords highly porous structure and large surface area. Additionally, the unique combination of Co-Ni-Fe in spinel oxides derived from calcination of the hierarchically structured core-shell MOF provides a favorable electronic environment for the adsorption of OER intermediates, which was further verified by the XPS characterizations and DFT calculations. DFT study revealed the Ni-Co coordinated O h sites in the MFe 2 O 4 reverse spinel structures as the main active sites, which tuned the binding strength of oxygen species with a catalyst through electron transfer of Fe→Co→Ni, thereby lowered the energy barriers for OER. As a result, the rationally designed CoNiFeO x -NC catalyst manifests superior OER performance with a low overpotential of 265 mV at 50 mA cm −2 and a decent Tafel slope of 64.1 mV dec -1 . The ion-exchange based strategy may serve as a versatile platform for rational design and synthesis of multi-metallic MOF derived electrocatalysts.
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