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Excellent long-term reactivity of inhomogeneous nanoscale Fe-based metallic glass in wastewater purification

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  • ReceivedAug 19, 2019
  • AcceptedOct 10, 2019
  • PublishedNov 7, 2019

Abstract


Funding

This work was financially supported by the National Natural Science Foundation of China(NSFC,51871129,51571127)

the National Key Basic Research and Development Programme(2016YFB0300502)

and the Natural Science Foundation of Jiangsu Province(BK20190480)


Acknowledgment

This work was financially supported by the National Natural Science Foundation of China (NSFC, 51871129 and 51571127), the National Key Basic Research and Development Programme (2016YFB0300502), and the Natural Science Foundation of Jiangsu Province (BK20190480). The author Chen SQ appreciates the help from Heng-Wei Luan, Jia-Cheng Ge, Si-Nan Liu and Dr. Sudheer Kumar Yadav.


Interest statement

The authors declare that they have no conflict of interest.


Contributions statement

Chen SQ designed and performed most of the experiments and wrote the manuscript with support from Hahn H, Shao Y, Yao KF and Zhao W. Hui KZ and Dong LZ performed the experiments of degradation of azo dyes. Li Z prepared the ribbons. Zhang QH and Gu L performed the TEM experiments. Lan S and Ke Y conducted the SANS experiments. Shao Y, Hahn H and Yao KF conceived and supervised the study. All authors contributed to the general discussion.


Author information

Shuang-Qin Chen received her PhD degree in materials science from Tsinghua University under the supervision of Prof. Kefu Yao in 2018. Currently, she is working at Nanjing University of Science and Technology as an assistant professor. Her present research interests focus on the catalytic properties of metallic glasses.


Yang Shao is an associate professor of the School of Materials Science and Engineering at Tsinghua University. He received his BE degree in 2002 and Master degree in 2004 from Tsinghua University, and received his PhD degree in 2009 from McMaster University. After postdoc research in the Canadian Centre for Electron Microscopy, he joined in Tsinghua University in 2010. Dr. Shao’s research interests mainly focus on the fundamentals and applications of advanced metallic alloys.


Supplementary data

Supplementary information

Supporting information is available in the online version of the paper.


References

[1] Safdar M, Khan SU, Jänis J. Progress toward catalytic micro- and nanomotors for biomedical and environmental applications. Adv Mater, 2018, 301703660 CrossRef PubMed Google Scholar

[2] Li WW, Yu HQ, He Z. Towards sustainable wastewater treatment by using microbial fuel cells-centered technologies. Energy Environ Sci, 2013, 7911-924 CrossRef Google Scholar

[3] Zhang F, Zhang WB, Shi Z, et al. Nanowire-haired inorganic membranes with superhydrophilicity and underwater ultralow adhesive superoleophobicity for high-efficiency oil/water separation. Adv Mater, 2013, 254192-4198 CrossRef PubMed Google Scholar

[4] Zhu Z, Wang W, Qi D, et al. Calcinable polymer membrane with revivability for efficient oily-water remediation. Adv Mater, 2018, 301801870 CrossRef PubMed Google Scholar

[5] Chen B, Bi H, Ma Q, et al. Preparation of graphene-MoS2 hybrid aerogels as multifunctional sorbents for water remediation. Sci China Mater, 2017, 601102-1108 CrossRef Google Scholar

[6] Ding L, Zhang Z, Li Y. Synthesis and catalytic property of urania-palladium-graphene nanohybrids. Sci China Mater, 2017, 60399-406 CrossRef Google Scholar

[7] Li K, Jiao T, Xing R, et al. Fabrication of tunable hierarchical mxene@aunps nanocomposites constructed by self-reduction reactions with enhanced catalytic performances. Sci China Mater, 2018, 61728-736 CrossRef Google Scholar

[8] Ling L, Huang XY, Zhang WX. Enrichment of precious metals from wastewater with core-shell nanoparticles of iron. Adv Mater, 2018, 301705703 CrossRef PubMed Google Scholar

[9] Wang Q, Tian S, Long J, et al. Use of Fe(II)Fe(III)-LDHs prepared by co-precipitation method in a heterogeneous-Fenton process for degradation of methylene blue. Catal Today, 2014, 22441-48 CrossRef Google Scholar

[10] Singh P, Raizada P, Kumari S, et al. Solar-Fenton removal of malachite green with novel Fe0-activated carbon nanocomposite. Appl Catal A-General, 2014, 4769-18 CrossRef Google Scholar

[11] Chen J, Liu W, Li Z, et al. Thermally-assisted photodegradation of lignin by TiO2/H2O2 under visible/near-infrared light irradiation. Sci China Mater, 2017, 61382-390 CrossRef Google Scholar

[12] Miklos DB, Remy C, Jekel M, et al. Evaluation of advanced oxidation processes for water and wastewater treatment–A critical review. Water Res, 2018, 139118-131 CrossRef PubMed Google Scholar

[13] Iskandar F, Nandiyanto A  , Yun K , et al. Enhanced photocatalytic performance of brookite TiO2 macroporous particles prepared by spray drying with colloidal templating. Adv Mater, 2007, 191408-1412 CrossRef Google Scholar

[14] Kumar A, Sharma G, Naushad M, et al. Spion/β-cyclodextrin core–shell nanostructures for oil spill remediation and organic pollutant removal from waste water. Chem Eng J, 2015, 280175-187 CrossRef Google Scholar

[15] Zhang X, Wei W, Zhang S, et al. Advanced 3D nanohybrid foam based on graphene oxide: Facile fabrication strategy, interfacial synergetic mechanism, and excellent photocatalytic performance. Sci China Mater, 2019, 621888-1897 CrossRef Google Scholar

[16] Gillham RW, O'Hannesin SF. Enhanced degradation of halogenated aliphatics by zero-valent iron. Ground Water, 1994, 32958-967 CrossRef Google Scholar

[17] Guan X, Sun Y, Qin H, et al. The limitations of applying zero-valent iron technology in contaminants sequestration and the corresponding countermeasures: The development in zero-valent iron technology in the last two decades (1994–2014). Water Res, 2015, 75224-248 CrossRef PubMed Google Scholar

[18] Wang JQ, Liu YH, Chen MW, et al. Rapid degradation of azo dye by Fe-based metallic glass powder. Adv Funct Mater, 2012, 222567-2570 CrossRef Google Scholar

[19] Qin XD, Zhu ZW, Liu G, et al. Ultrafast degradation of azo dyes catalyzed by cobalt-based metallic glass. Sci Rep, 2015, 518226 CrossRef PubMed ADS Google Scholar

[20] Jia Z, Duan X, Qin P, et al. Disordered atomic packing structure of metallic glass: Toward ultrafast hydroxyl radicals production rate and strong electron transfer ability in catalytic performance. Adv Funct Mater, 2017, 271702258 CrossRef Google Scholar

[21] Wang Q, Chen M, Lin P, et al. Investigation of FePC amorphous alloys with self-renewing behaviour for highly efficient decolorization of methylene blue. J Mater Chem A, 2018, 610686-10699 CrossRef Google Scholar

[22] Tang Y, Shao Y, Chen N, et al. Rapid decomposition of Direct Blue 6 in neutral solution by Fe–B amorphous alloys. RSC Adv, 2015, 56215-6221 CrossRef Google Scholar

[23] Tang Y, Shao Y, Chen N, et al. Insight into the high reactivity of commercial Fe–Si–B amorphous zero-valent iron in degrading azo dye solutions. RSC Adv, 2015, 534032-34039 CrossRef Google Scholar

[24] Wang PP, Wang JQ, Huo JT, et al. Fast degradation of azo dye by nanocrystallized Fe-based alloys. Sci China-Phys Mech Astron, 2017, 60076112 CrossRef Google Scholar

[25] Debenedetti PG, Stillinger FH. Supercooled liquids and the glass transition. Nature, 2001, 410259-267 CrossRef PubMed Google Scholar

[26] Chen SQ, Shao Y, Cheng MT, et al. Effect of residual stress on azo dye degradation capability of Fe-based metallic glass. J Non-Crystalline Solids, 2017, 47374-78 CrossRef ADS Google Scholar

[27] Chen S, Chen N, Cheng M, et al. Multi-phase nanocrystallization induced fast degradation of methyl orange by annealing Fe-based amorphous ribbons. Intermetallics, 2017, 9030-35 CrossRef Google Scholar

[28] Chen S, Yang G, Luo S, et al. Unexpected high performance of Fe-based nanocrystallized ribbons for azo dye decomposition. J Mater Chem A, 2017, 514230-14240 CrossRef Google Scholar

[29] Liang SX, Jia Z, Liu YJ, et al. Compelling rejuvenated catalytic performance in metallic glasses. Adv Mater, 2018, 301802764 CrossRef PubMed Google Scholar

[30] Ke Y, He C, Zheng H, et al. The time-of-flight small-angle neutron spectrometer at China spallation neutron source. Neutron News, 2018, 2914-17 CrossRef Google Scholar

[31] Matsuura M, Nishijima M, Takenaka K, et al. Evolution of fcc Cu clusters and their structure changes in the soft magnetic Fe85.2Si1B9P4Cu0.8 (NANOMET) and FINEMET alloys observed by X-ray absorption fine structure. J Appl Phys, 2015, 11717A324 CrossRef ADS Google Scholar

[32] Sharma P, Zhang X, Zhang Y, et al. Competition driven nanocrystallization in high Bs and low coreloss Fe–Si–B–P–Cu soft magnetic alloys. Scripta Mater, 2015, 953-6 CrossRef Google Scholar

[33] Abaidia SEH, Wiedenmann A. Thermal stability of the bulk metallic glass Zr46.75Ti8.25Cu7.5Ni10Be27.5 studied by SANS. Physica B-Condensed Matter, 2000, 276-278454-455 CrossRef ADS Google Scholar

[34] Jia Z, Zhang WC, Wang WM, et al. Amorphous Fe78Si9B13 alloy: An efficient and reusable photo-enhanced Fenton-like catalyst in degradation of cibacron brilliant red 3B-A dye under UV–vis light. Appl Catal B-Environ, 2016, 19246-56 CrossRef Google Scholar

[35] Xie S, Huang P, Kruzic JJ, et al. A highly efficient degradation mechanism of methyl orange using Fe-based metallic glass powders. Sci Rep, 2016, 621947 CrossRef PubMed ADS Google Scholar

[36] Wang JQ, Liu YH, Chen MW, et al. Excellent capability in degrading azo dyes by MgZn-based metallic glass powders. Sci Rep, 2012, 2418 CrossRef PubMed ADS Google Scholar

[37] Wang P, Wang JQ, Li H, et al. Fast decolorization of azo dyes in both alkaline and acidic solutions by Al-based metallic glasses. J Alloys Compd, 2017, 701759-767 CrossRef Google Scholar

[38] Li C, Zhuang Z, Huang F, et al. Recycling rare earth elements from industrial wastewater with flowerlike nano-Mg(OH)2. ACS Appl Mater Interfaces, 2013, 59719-9725 CrossRef PubMed Google Scholar

[39] Liu M, Wang Y, Chen L, et al. Mg(OH)2 supported nanoscale zero valent iron enhancing the removal of Pb(II) from aqueous solution. ACS Appl Mater Interfaces, 2015, 77961-7969 CrossRef PubMed Google Scholar

[40] Jia Z, Wang Q, Sun L, et al. Attractive in situ self-reconstructed hierarchical gradient structure of metallic glass for high efficiency and remarkable stability in catalytic performance. Adv Funct Mater, 2019, 291807857 CrossRef Google Scholar

[41] Mielczarski JA, Atenas GM, Mielczarski E. Role of iron surface oxidation layers in decomposition of azo-dye water pollutants in weak acidic solutions. Appl Catal B-Environ, 2005, 56289-303 CrossRef Google Scholar

[42] Cai C, Zhang H, Zhong X, et al. Ultrasound enhanced heterogeneous activation of peroxymonosulfate by a bimetallic Fe–Co/SBA-15 catalyst for the degradation of Orange II in water. J Hazard Mater, 2015, 28370-79 CrossRef PubMed Google Scholar

[43] Liang SX, Jia Z, Zhang WC, et al. Rapid malachite green degradation using Fe73.5Si13.5B9Cu1Nb3 metallic glass for activation of persulfate under UV–vis light. Mater Des, 2017, 119244-253 CrossRef Google Scholar

[44] Deng Z, Zhang XH, Chan KC, et al. Fe-based metallic glass catalyst with nanoporous surface for azo dye degradation. Chemosphere, 2017, 17476-81 CrossRef PubMed ADS Google Scholar

[45] Jia Z, Duan X, Zhang W, et al. Ultra-sustainable Fe78Si9B13 metallic glass as a catalyst for activation of persulfate on methylene blue degradation under UV-vis light. Sci Rep, 2016, 638520 CrossRef PubMed ADS Google Scholar

[46] Fujita T, Guan P, McKenna K, et al. Atomic origins of the high catalytic activity of nanoporous gold. Nat Mater, 2012, 11775-780 CrossRef PubMed ADS Google Scholar

[47] Detsi E, Cook JB, Lesel BK, et al. Mesoporous Ni60Fe30Mn10-alloy based metal/metal oxide composite thick films as highly active and robust oxygen evolution catalysts. Energy Environ Sci, 2016, 9540-549 CrossRef PubMed Google Scholar

[48] Tan Y, Wang H, Liu P, et al. 3D nanoporous metal phosphides toward high-efficiency electrochemical hydrogen production. Adv Mater, 2016, 282951-2955 CrossRef PubMed Google Scholar

[49] Paschalidou EM, Celegato F, Scaglione F, et al. The mechanism of generating nanoporous Au by de-alloying amorphous alloys. Acta Mater, 2016, 119177-183 CrossRef Google Scholar

[50] Gupta G, Thorp JC, Mara NA, et al. Morphology and porosity of nanoporous Au thin films formed by dealloying of AuxSi1−x. J Appl Phys, 2012, 112094320 CrossRef ADS Google Scholar

[51] Lu X, Bischoff E, Spolenak R, et al. Investigation of dealloying in Au–Ag thin films by quantitative electron probe microanalysis. Scripta Mater, 2007, 56557-560 CrossRef Google Scholar

[52] Parida S, Kramer D, Volkert CA, et al. Volume change during the formation of nanoporous gold by dealloying. Phys Rev Lett, 2006, 97035504 CrossRef PubMed ADS Google Scholar

[53] Suryanarayana C, Inoue A. Iron-based bulk metallic glasses. Int Mater Rev, 2013, 58131-166 CrossRef Google Scholar

[54] Jafari S, Beitollahi A, Yekta BE, et al. Atom probe analysis and magnetic properties of nanocrystalline Fe84.3Si4B8P3Cu0.7. J Alloys Compd, 2016, 674136-144 CrossRef Google Scholar

[55] Hono K, Inoue A, Sakurai T. Atom probe analysis of Fe73.5Si13.5B9Nb3Cu1 nanocrystalline soft magnetic material. Appl Phys Lett, 1991, 582180-2182 CrossRef ADS Google Scholar

[56] Hono K, Ping DH, Ohnuma M, et al. Cu clustering and Si partitioning in the early crystallization stage of an Fe73.5Si13.5B9Nb3Cu1 amorphous alloy. Acta Mater, 1999, 47997-1006 CrossRef Google Scholar

[57] Ayers JD, Harris VG, Sprague JA, et al. The local atomic order of Cu and Fe in heat treated Fe73.5Nb3Cu1Si13.5B9 ribbons. IEEE Trans Magn, 1993, 292664-2666 CrossRef ADS Google Scholar

[58] Ayers JD, Harris VG, Sprague JA, et al. On the role of Cu and Nb in the formation of nanocrystals in amorphous Fe73.5Nb3Cu1Si13.5B9. Appl Phys Lett, 1994, 64974-976 CrossRef ADS Google Scholar

  • Figure 1

    (a) XRD pattern, (b) DSC curve, (c) HRTEM image and (d) HAADF image and its corresponding EDS images of Fe-MGI.

  • Figure 2

    (a) Degradation curves of Fe-MGI, Fe-MG and C-ZVI. UV-vis absorption spectra of Orange II by Fe-MGI (b) and the decomposition products of Orange II degraded by Fe-MGI (c). Experimental conditions: C0 of 25 mg L−1, solution volume of 250 mL, ribbon dosage of 10 g L−1, temperature of 25°C, pH value of 6.

  • Figure 3

    (a) OCP curves and (b) potentio-dynamic polarization curves of Fe-MGI and Fe-MG before and after the degradation of Orange II.

  • Figure 4

    SEM images of Fe-MGI’s surface morphologies after degradation of Orange II: (a) at low magnefication, (b) enlarged reacted region, (c) and (d) enlarged flowerlike structure corrosion products, and (e) further enlarged nanoporous reacted regions. Experimental conditions: C0 of 25 mg L−1, solution volume of 250 mL, ribbon dosage of 10 g L−1, temperature of 25°C, pH value of 6.

  • Figure 5

    Degradation curves of Fe-MGI under different environments: (a) various C0s of Orange II, (b) environment temperatures, (c) the Arrhenius plot for the estimation of the activation energy in degradation of Orange II by Fe-MGI, and (d) different pH values. Experimental conditions: C0 of 25 mg L−1, solution volume of 250 mL, ribbon dosage of 10 g L−1, temperature of 25°C, pH value of 6, except for noted variates.

  • Figure 6

    SEM images of the surface morphology of Fe-MGI after degradation of Orange II solution at pH 10, (a) low enlarged scale SEM image, (b) enlarged reacted region corresponded B region in (a), (c) enlarged cracks in precipitated products corresponded C region in (b), and (d) enlarged precipitated products corresponded D region in (c). Experimental conditions: C0 of 25 mg L−1, solution volume of 250 mL, ribbon dosage of 10 g L−1, temperature of 25°C.

  • Figure 7

    Catalytic properties of Fe-MGI evaluated by degradation of MB in Fenton-like process using various treatment parameters: (a) dosages of Fe-MGI, (b) concentrations of H2O2, (c) C0s of MB, (d) initial pH values and (e) temperatures. (f) The Arrhenius plot for the estimation of the activation energy. If not mentioned, experimental conditions are C0 of 20 mg L−1, solution volume of 250 mL, ribbon dosage of 0.5 g L−1, temperature of 25°C and pH value of 3.

  • Figure 8

    (a) Cyclic degradation curves of Orange II solution with C0 of 100 mg L−1 by Fe-MGI, and (b) degradation efficiency within 50 min (η50min), half-life (t1/2) and the observed degradation rate (kobs) as a function of cycles. Experimental condition: C0 of 100 mg L−1, solution volume of 250 mL, ribbon dosage of 10 g L−1, temperature of 25°C, pH value of 6.

  • Figure 9

    Available cycling data of different reported ZVIs compared with the Fe-MGI prepared in this work.

  • Figure 10

    (a) The optical photographs of Fe-MGI before and after cycle experiment, (b) optical microscope image, (c) and (d) SEM images of Fe-MGI after cycle experiment, (e) and (f) further enlarged SEM images of the main reacted region. Inset of (f) is pore size distribution of the nanoporous structures. (g) Corresponding EDS images of (e).

  • Figure 11

    (a) SEM images of the cross-section of Fe-MGI after the fifteenth cycle experiment, the cracks are highlighted by yellow arrows, (b) SEM images of the cross-section of Fe-MGI before and after different cycles, (c) SEM images of the surfaces of Fe-MGI before and after different cycles.

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