Abstract
A series of high dielectric composite films based on low-cost and eco-friendly titanium dioxide (TiO2) and cellulose nanofibril (CNF) was prepared under a facile condition. The relative dielectric constants (εr) and dielectric loss (\( \tan\updelta \)) were studied as the function of frequency and filler content. The εr of CNF/TiO2 composite film was 19.51 (at 1 kHz) with a relatively low dielectric loss. Compared with pure CNF films (εr = 6.92 at 1 kHz), the εr of the composite film was improved about three times with the dielectric loss increased slightly. The effects of TiO2 addition and hot-press treatment on microstructure, thermal stability, and dynamic mechanical properties of the composite films were also analyzed. It was found that the addition of TiO2 particles reduces the cellulose–cellulose bonding so generates more pores in the films, which has significant impacts on both dielectric and physical strength properties.
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Abdel-karim AM, Salama AH, Hassan ML (2018) Electrical conductivity and dielectric properties of nanofibrillated cellulose thin films from bagasse. J Phys Org Chem 31(9):e3851. https://doi.org/10.1002/poc.3851
Al-Saygh A, Ponnamma D, AlMaadeed M, Vijayan P, Karim A, Hassan M (2017) Flexible pressure sensor based on PVDF nanocomposites containing reduced graphene oxide–titania hybrid nanolayers. Polymers 9(2):33. https://doi.org/10.3390/polym9020033
Alam MM, Ghosh SK, Sarkar D, Sen S, Mandal D (2017) Improved dielectric constant and breakdown strength of gamma-phase dominant super toughened polyvinylidene fluoride/TiO2 nanocomposite film: an excellent material for energy storage applications and piezoelectric throughput. Nanotechnology 28(1):015503. https://doi.org/10.1088/0957-4484/28/1/015503
Anju V, Narayanankutty SK (2016) Polyaniline coated cellulose fiber/polyvinyl alcohol composites with high dielectric permittivity and low percolation threshold. AIP Adv 6(1):015109
Bonardd S, Robles E, Barandiaran I, Saldias C, Leiva A, Kortaberria G (2018) Biocomposites with increased dielectric constant based on Chitosan and nitrile-modified cellulose nanocrystals. Carbohydr Polym 199:20–30. https://doi.org/10.1016/j.carbpol.2018.06.088
Chang CJ, Tsai MH, Chen GS, Wu MS, Hung TW (2009) Preparation and properties of porous polyimide films with TiO2/polymer double shell hollow spheres. Thin Solid Films 517(17):4966–4969. https://doi.org/10.1016/j.tsf.2009.03.201
Chenampulli S, Unnikrishnan G, Thomas S, Narine SS (2019) Novel ethylene diamine functionalised nanocellulose/poly(ethylene-co-acrylic acid) composites for biomedical applications. Cellulose 26(3):1795–1809. https://doi.org/10.1007/s10570-018-02227-6
Chiang C, Popielarz R (2002) Polymer composites with high dielectric constant. Ferroelectrics 275(1):1–9
Dang Z-M (2018) 1—Introduction. In: Dang Z-M (ed) Dielectric polymer materials for high-density energy storage. William Andrew Publishing, Oxford, pp 1–9. https://doi.org/10.1016/B978-0-12-813215-9.00001-4
Deshmukh K, Ahamed MB, Deshmukh RR, Pasha SKK, Sadasivuni KK, Ponnamma D, AlMaadeed MA (2017) Striking multiple synergies in novel three-phase fluoropolymer nanocomposites by combining titanium dioxide and graphene oxide as hybrid fillers. J Mater Sci: Mater Electron 28(1):559–575. https://doi.org/10.1007/s10854-016-5559-1
Dou Z, Liu W, Lin T, Zhou K, Hang L (2017) High performance capacitors via aligned TiO2 nanowire array. Appl Phys Lett. https://doi.org/10.1063/1.4979407
Du X, Zhang Z, Liu W, Deng Y (2017) Nanocellulose-based conductive materials and their emerging applications in energy devices—a review. Nano Energy 35:299–320. https://doi.org/10.1016/j.nanoen.2017.04.001
Emmert S, Wolf M, Gulich R, Krohns S, Kastner S, Lunkenheimer P, Loidl A (2011) Electrode polarization effects in broadband dielectric spectroscopy. Eur Phys J B 83(2):157–165. https://doi.org/10.1140/epjb/e2011-20439-8
Feng Y, Yin JH, Chen MH, Song MX, Su B, Lei QQ (2013) Effect of nano-TiO2 on the polarization process of polyimide/TiO2 composites. Mater Lett 96:113–116. https://doi.org/10.1016/j.matlet.2013.01.037
Feng Y, Yin JH, Chen MH, Liu XX, Su B, Fei WD, Lei QQ (2014) Influence of interface on the electrical properties of polyimide/TiO2 composite films. IEEE Trans Dielectr Electr Insul 21(4):1501–1508. https://doi.org/10.1109/Tdei.2014.004322
Fujisaki Y et al (2014) Transparent nanopaper-based flexible organic thin-film transistor array. Adv Funct Mater 24(12):1657–1663. https://doi.org/10.1002/adfm.201303024
Fukuzumi H, Saito T, Okita Y, Isogai A (2010) Thermal stabilization of TEMPO-oxidized cellulose. Polym Degrad Stab 95(9):1502–1508. https://doi.org/10.1016/j.polymdegradstab.2010.06.015
Gan WC, Abd Majid WH (2014) Effect of TiO2 on enhanced pyroelectric activity of PVDF composite. Smart Mater Struct. https://doi.org/10.1088/0964-1726/23/4/045026
Gaspar D et al (2014) Nanocrystalline cellulose applied simultaneously as the gate dielectric and the substrate in flexible field effect transistors. Nanotechnology 25(9):094008. https://doi.org/10.1088/0957-4484/25/9/094008
Hassan ML, Ali AF, Salama AH, Abdel-Karim AM (2019) Novel cellulose nanofibers/barium titanate nanoparticles nanocomposites and their electrical properties. J Phys Org Chem 32(2):e3897
Inui T, Koga H, Nogi M, Komoda N, Suganuma K (2014) High-dielectric paper composite consisting of cellulose nanofiber and silver nanowire. In: 14th IEEE international conference on nanotechnology, pp 470–473
Inui T, Koga H, Nogi M, Komoda N, Suganuma K (2015) A miniaturized flexible antenna printed on a high dielectric constant nanopaper composite. Adv Mater 27(6):1112–1116. https://doi.org/10.1002/adma.201404555
Ishmael SA et al (2014) Thermal conductivity and dielectric properties of a TiO2-based electrical insulator for use with high temperature superconductor-based magnets. Supercond Sci Technol 27(9):9. https://doi.org/10.1088/0953-2048/27/9/095018
Isogai A, Saito T, Fukuzumi H (2011) TEMPO-oxidized cellulose nanofibers. Nanoscale 3(1):71–85. https://doi.org/10.1039/c0nr00583e
Jayaramudu T, Ko H-U, Kim H, Kim J, Muthoka R, Kim J (2018a) Electroactive hydrogels made with polyvinyl alcohol/cellulose nanocrystals. Materials 11(9):1615
Jayaramudu T, Ko HU, Kim HC, Kim JW, Muthoka RM, Kim J (2018b) Electroactive hydrogels made with polyvinyl alcohol/cellulose nanocrystals. Materials 11(9):11. https://doi.org/10.3390/ma11091615
Ji S et al (2017) High dielectric performances of flexible and transparent cellulose hybrid films controlled by multidimensional metal nanostructures. Adv Mater 29(24):1700538. https://doi.org/10.1002/adma.201700538
Kafy A, Sadasivuni KK, Akther A, Min S-K, Kim J (2015a) Cellulose/graphene nanocomposite as multifunctional electronic and solvent sensor material. Mater Lett 159:20–23
Kafy A, Sadasivuni KK, Kim HC, Akther A, Kim J (2015b) Designing flexible energy and memory storage materials using cellulose modified graphene oxide nanocomposites. Phys Chem Chem Phys 17(8):5923–5931. https://doi.org/10.1039/c4cp05921b
Kizilkaya C, Dumludag F, Karatas S, Apohan NK, Altindal A, Gungor A (2012) The effect of titania content on the physical properties of polyimide/titania nanohybrid films. J Appl Polym Sci 125(5):3802–3810. https://doi.org/10.1002/app.35292
Koytepe S, Seckin T, Kivrilcim N, Adiguzel HI (2008) Synthesis and dielectric properties of polyimide–titania hybrid composites. J Inorg Organomet Polym Mater 18(2):222–228. https://doi.org/10.1007/s10904-007-9169-5
Kumar V et al (2014) Comparison of nano- and microfibrillated cellulose films. Cellulose 21(5):3443–3456. https://doi.org/10.1007/s10570-014-0357-5
Kumari A, Ghosh BD (2018) La doped barium titanate/polyimide nanocomposites: a study of the effect of La doping and investigation on thermal, mechanical and high dielectric properties. J Appl Polym Sci 135(47):12. https://doi.org/10.1002/app.46826
Lay M, Meng S, Ramli MR, Ahmad Z, Ismail H, Huat TS, Todo M (2018) Interphase volume calculation of polyimide/TiO2 nanofibers nanocomposite based on dielectric constant model and its effect on glass transition. J Mater Sci: Mater Electron 29(24):20742–20749. https://doi.org/10.1007/s10854-018-0215-6
Le Bras D, Stromme M, Mihranyan A (2015) Characterization of dielectric properties of nanocellulose from wood and algae for electrical insulator applications. J Phys Chem B 119(18):5911–5917. https://doi.org/10.1021/acs.jpcb.5b00715
Lee WH, Wang CC (2010) Effect of nanocomposite gate-dielectric properties on pentacene microstructure and field-effect transistor characteristics. J Nanosci Nanotechnol 10(2):762–769. https://doi.org/10.1166/jnn.2010.1817
Lee WH, Wang CC, Ho JC (2009) Improved performance of pentacene field-effect transistors using a nanocomposite gate dielectric. J Vac Sci Technol, B 27(2):601–605. https://doi.org/10.1116/1.3093881
Lee WH, Liu CT, Lee YC (2012) Study on preparation of high-k organic-inorganic thin film for organic-inorganic thin film transistor gate dielectric application. Jpn J Appl Phys 51(6):7. https://doi.org/10.1143/jjap.51.061603
Lin JQ, Wang Y, Yang WL, Lu HW (2017) Balance of mechanical and electrical performance in polyimide/nano titanium dioxide prepared by an in-sol method. J Appl Polym Sci 134(13):9. https://doi.org/10.1002/App.44666
Lizundia E et al (2016) Cu-coated cellulose nanopaper for green and low-cost electronics. Cellulose 23(3):1997–2010
Lu HB, Zhang XY (2006) Influence of the relaxation of Maxwell–Wagner–Sillars polarization and dc conductivity on the dielectric behaviors of nylon 1010. J Appl Phys 100(5):054104. https://doi.org/10.1063/1.2336494
Lu HW, Lin JQ, Yang WL, Liu LZ, Wang Y, Chen GR, Huang W (2017) Effect of nano-TiO2 surface modification on polarization characteristics and corona aging performance of polyimide nano-composites. J Appl Polym Sci 134(29):9. https://doi.org/10.1002/app.45101
Madusanka N, Shivareddy SG, Hiralal P, Eddleston MD, Choi Y, Oliver RA, Amaratunga GA (2016) Nanocomposites of TiO2/cyanoethylated cellulose with ultra high dielectric constants. Nanotechnology 27(19):195402
Madusanka N, Shivareddy SG, Eddleston MD, Hiralal P, Oliver RA, Amaratunga GA (2017) Dielectric behaviour of montmorillonite/cyanoethylated cellulose nanocomposites. Carbohydr Polym 172:315–321
Meena JS et al (2012) Facile synthetic route to implement a fully bendable organic metal–insulator–semiconductor device on polyimide sheet. Org Electron 13(5):721–732. https://doi.org/10.1016/j.orgel.2012.01.007
Milinskii AY, Baryshnikov SV, Thuong NH (2018) Dielectric properties of nanocomposites based on potassium iodate with porous nanocrystalline cellulose. Ferroelectrics 524(1):181–188. https://doi.org/10.1080/00150193.2018.1432830
Milovidova SD, Rogazinskaya OV, Sidorkin AS, Thuong NH, Grohotova EV, Popravko NG (2014) Dielectric properties of composites based on nanocrystalline cellulose and triglycine sulfate. Ferroelectrics 469(1):116–119. https://doi.org/10.1080/00150193.2014.949132
Mohiuddin M, Sadasivuni KK, Mun S, Kim J (2015) Flexible cellulose acetate/graphene blueprints for vibrotactile actuator. RSC Adv 5(43):34432–34438
Novac OC, Maries GRE, Chira D, Novac M (2017) Study concerning the influence of the grinding percentage on some electrical properties of PA 6.6, POM and ABS by methods for determining relative permittivity and the dielectric dissipation factor. Mater Plast 54(3):453–460
Olariu MA, Hamciuc C, Okrasa L, Hamciuc E, Dimitrov L, Kalvachev Y (2017) Electrical properties of polyimide composite films containing TiO2 Nanotubes. Polym Compos 38(11):2584–2593. https://doi.org/10.1002/pc.23851
Osong SH, Norgren S, Engstrand P (2016) Processing of wood-based microfibrillated cellulose and nanofibrillated cellulose, and applications relating to papermaking: a review. Cellulose 23(1):93–123. https://doi.org/10.1007/s10570-015-0798-5
Paniagua SA, Kim Y, Henry K, Kumar R, Perry JW, Marder SR (2014) Surface-initiated polymerization from barium titanate nanoparticles for hybrid dielectric capacitors. ACS Appl Mater Interfaces 6(5):3477–3482. https://doi.org/10.1021/am4056276
Park HH, Choi Y, Park DJ, Cho SY, Yun YS, Jin HJ (2013) Enhanced dielectric properties of electrospun titanium dioxide/polyvinylidene fluoride nanofibrous composites. Fibers Polym 14(9):1521–1525. https://doi.org/10.1007/s12221-013-1521-5
Postek MT, Moon RJ, Rudie AW, Bilodeau MA (2013) Production and applications of cellulose. Tappi Press, Peachtree Corners
Poyraz B (2018) Enzyme treated CNF biofilms: characterization. Int J Biol Macromol 117:713–720. https://doi.org/10.1016/j.ijbiomac.2018.05.222
Poyraz B, Tozluoğlu A, Candan Z, Demir A (2017a) Matrix impact on the mechanical, thermal and electrical properties of microfluidized nanofibrillated cellulose composites. J Polym Eng 37(9):921–931. https://doi.org/10.1515/polyeng-2017-0022
Poyraz B, Tozluoglu A, Candan Z, Demir A, Yavuz M (2017b) Influence of PVA and silica on chemical, thermo-mechanical and electrical properties of Celluclast-treated nanofibrillated cellulose composites. Int J Biol Macromol 104(Pt A):384–392. https://doi.org/10.1016/j.ijbiomac.2017.06.018
Prabakaran K, Mohanty S, Nayak SK (2014) Influence of surface modified TiO2 nanoparticles on dielectric properties of PVdF–HFP nanocomposites. J Mater Sci: Mater Electron 25(10):4590–4602. https://doi.org/10.1007/s10854-014-2209-3
Qi FW, Chen N, Wang Q (2017) Preparation of PA11/BaTiO3 nanocomposite powders with improved processability, dielectric and piezoelectric properties for use in selective laser sintering. Mater Design 131:135–143. https://doi.org/10.1016/j.matdes.2017.06.012
Qi FW, Chen N, Wang Q (2018) Dielectric and piezoelectric properties in selective laser sintered polyamide11/BaTiO3/CNT ternary nanocomposites. Mater Design 143:72–80. https://doi.org/10.1016/j.matdes.2018.01.050
Raghunathan SP, Narayanan S, Poulose AC, Joseph R (2017) Flexible regenerated cellulose/polypyrrole composite films with enhanced dielectric properties. Carbohydr Polym 157:1024–1032
Rajala S et al (2016) Cellulose nanofibril film as a piezoelectric sensor material. ACS Appl Mater Interfaces 8(24):15607–15614. https://doi.org/10.1021/acsami.6b03597
Rekik H, Ghallabi Z, Royaud I, Arous M, Seytre G, Boiteux G, Kallel A (2013) Dielectric relaxation behaviour in semi-crystalline polyvinylidene fluoride (PVDF)/TiO2 nanocomposites. Compos Part B Eng 45(1):1199–1206. https://doi.org/10.1016/j.compositesb.2012.08.002
Ribeiro C et al (2018) Electroactive poly(vinylidene fluoride)-based structures for advanced applications. Nat Protoc 13(4):681–704. https://doi.org/10.1038/nprot.2017.157
Sacui IA et al (2014) Comparison of the properties of cellulose nanocrystals and cellulose nanofibrils isolated from bacteria, tunicate, and wood processed using acid, enzymatic, mechanical, and oxidative methods. ACS Appl Mater Interfaces 6(9):6127–6138. https://doi.org/10.1021/am500359f
Saito T, Hirota M, Tamura N, Kimura S, Fukuzumi H, Heux L, Isogai A (2009) Individualization of nano-sized plant cellulose fibrils by direct surface carboxylation using tempo catalyst under neutral conditions. Biomacromolecules 10(7):1992–1996. https://doi.org/10.1021/bm900414t
Samet M, Levchenko V, Boiteux G, Seytre G, Kallel A, Serghei A (2015) Electrode polarization vs. Maxwell–Wagner–Sillars interfacial polarization in dielectric spectra of materials: characteristic frequencies and scaling laws. J Chem Phys 142(19):194703. https://doi.org/10.1063/1.4919877
Shi L et al (2018) Dielectric gels with ultra-high dielectric constant, low elastic modulus, and excellent transparency. NPG Asia Mater 10(8):821
Shimizu M, Saito T, Isogai A (2016) Water-resistant and high oxygen-barrier nanocellulose films with interfibrillar cross-linkages formed through multivalent metal ions. J Membr Sci 500:1–7. https://doi.org/10.1016/j.memsci.2015.11.002
Stelte W, Sanadi AR (2009) Preparation and characterization of cellulose nanofibers from two commercial hardwood and softwood pulps. Ind Eng Chem Res 48(24):11211–11219. https://doi.org/10.1021/ie9011672
Su R et al (2016) High energy density performance of polymer nanocomposites induced by designed formation of BaTiO3@sheet-IikeTiO2 hybrid nanofillers. J Phys Chem C 120(22):11769–11776. https://doi.org/10.1021/acs.jpcc.6b01853
Tanaka T (2005) Dielectric nanocomposites with insulating properties. IEEE Trans Dielectr Electr Insul 12(5):914–928. https://doi.org/10.1109/TDEI.2005.1522186
Tanaka T, Kozako M, Fuse N, Ohki Y (2005) Proposal of a multi-core model for polymer nanocomposite dielectrics. IEEE Trans Dielectr Electr Insul 12(4):669–681. https://doi.org/10.1109/TDEI.2005.1511092
Tang R, Liggat JJ, Siew WH (2018) Filler and additive effects on partial discharge degradation of PET films used in PV devices. Polym Degrad Stab 150:148–157. https://doi.org/10.1016/j.polymdegradstab.2018.02.003
Thomas S, Deepu VN, Mohanan P, Sebastian MT (2008) Effect of filler content on the dielectric properties of PTFE/ZnAl2O4-TiO2 composites. J Am Ceram Soc 91(6):1971–1975. https://doi.org/10.1111/j.1551-2916.2008.02365.x
Topala I, Dumitrascu N, Pohoata V (2007) Influence of plasma treatments on the hemocompatibility of PET and PET + TiO2 films. Plasma Chem Plasma Process 27(1):95–112. https://doi.org/10.1007/s11090-006-9046-y
Wang D, Dang Z-M (2018) Processing of polymeric dielectrics for high energy density capacitors. In: Dielectric polymer materials for high-density energy storage. Elsevier, Amsterdam, pp 429-446
Wang SF, Wang YR, Cheng KC, Chen SH (2010a) Physical and electrical properties of polyimide/ceramic hybrid films prepared via non-hydrolytic sol–gel process. J Mater Sci: Mater Electron 21(1):104–110. https://doi.org/10.1007/s10854-009-9876-5
Wang Y, Zhou X, Chen Q, Chu BJ, Zhang QM (2010b) Recent development of high energy density polymers for dielectric capacitors. IEEE Trans Dielectr Electr Insul 17(4):1036–1042. https://doi.org/10.1109/Tdei.2010.5539672
Wang JC, Long YC, Sun Y, Zhang XQ, Yang H, Lin BP (2018) Fabrication and enhanced dielectric properties of polyimide matrix composites with core-shell structured CaCu3Ti4O12@TiO2 nanofibers. J Mater Sci: Mater Electron 29(9):7842–7850. https://doi.org/10.1007/s10854-018-8783-z
Wu GL, Li JL, Wang KK, Wang YQ, Pan C, Feng AL (2017) In situ synthesis and preparation of TiO2/polyimide composite containing phenolphthalein functional group. J Mater Sci: Mater Electron 28(9):6544–6551. https://doi.org/10.1007/s10854-017-6343-6
Wypych A et al (2014) dielectric properties and characterisation of titanium dioxide obtained by different chemistry methods. J Nanomater. https://doi.org/10.1155/2014/124814
Yagyu H, Ifuku S, Nogi M (2017) Acetylation of optically transparent cellulose nanopaper for high thermal and moisture resistance in a flexible device substrate. Flex Print Electron 2(1):7. https://doi.org/10.1088/2058-8585/aa60f4
Yang L, Ji HL, Zhu KJ, Wang J, Qiu JH (2016) Dramatically improved piezoelectric properties of poly(vinylidene fluoride) composites by incorporating aligned TiO2@MWCNTs. Compos Sci Technol 123:259–267. https://doi.org/10.1016/j.compscitech.2015.11.032
Yang J, Xie H, Chen H, Shi Z, Wu T, Yang Q, Xiong C (2018a) Cellulose nanofibril/boron nitride nanosheet composites with enhanced energy density and thermal stability by interfibrillar cross-linking through Ca 2+. J Mater Chem A 6(4):1403–1411. https://doi.org/10.1039/C7TA08188J
Yang Q, Zhang C, Shi Z, Wang J, Xiong C, Saito T, Isogai A (2018b) Luminescent and transparent nanocellulose films containing europium carboxylate groups as flexible dielectric materials. ACS Appl Nano Mater 1(9):4972–4979. https://doi.org/10.1021/acsanm.8b01112
Yin J et al (2014) Effect of MMT content on structure of polyimide/(TiO2 + MMT) nanocomposite films. In: 2014 9th international forum on strategic technology (IFOST), pp 475–478. https://doi.org/10.1109/IFOST.2014.6991167
Yuan Y, Cui YR, Wu KT, Huang QQ, Zhang SR (2014) TiO2 and SiO2 filled PTFE composites for microwave substrate applications. J Polym Res 21(2):6. https://doi.org/10.1007/s10965-014-0366-y
Yuan Y, Wang J, Yao MH, Tang B, Li EZ, Zhang SR (2018) Influence of SiO2 addition on properties of PTFE/TiO2 microwave composites. J Electron Mater 47(1):633–640. https://doi.org/10.1007/s11664-017-5826-9
Zeng XL, Deng LB, Yao YM, Sun R, Xu JB, Wong CP (2016) Flexible dielectric papers based on biodegradable cellulose nanofibers and carbon nanotubes for dielectric energy storage. J Mater Chem C 4(25):6037–6044. https://doi.org/10.1039/c6tc01501h
Zha JW, Dang ZM, Song HT, Yin Y, Chen G (2010a) Dielectric properties and effect of electrical aging on space charge accumulation in polyimide/TiO2 nanocomposite films. J Appl Phys 108(9):6. https://doi.org/10.1063/1.3506715
Zha JW, Dang ZM, Zhou T, Song HT, Chen G (2010b) Electrical properties of TiO2-filled polyimide nanocomposite films prepared via an in situ polymerization process. Synth Metals 160(23–24):2670–2674. https://doi.org/10.1016/j.synthmet.2010.10.024
Zhou Y, Huang X, Huang J, Zhang L, Zhou Z (2018) Predicting the dielectric properties of nanocellulose-modified presspaper based on the multivariate analysis method. Molecules 23(7):1507. https://doi.org/10.3390/molecules23071507
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Tao, J., Cao, Sa., Liu, W. et al. Facile preparation of high dielectric flexible films based on titanium dioxide and cellulose nanofibrils. Cellulose 26, 6087–6098 (2019). https://doi.org/10.1007/s10570-019-02495-w
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DOI: https://doi.org/10.1007/s10570-019-02495-w