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Unravelling the Mechanism of Stabilization and Microstructure of Oil-in-Water Emulsions by Native Cellulose Microfibrils in Primary Plant Cells Dispersions

  • Emma M. Nomena*
    Emma M. Nomena
    Unilever R&D Vlaardingen, Olivier van Noortlaan 120, Vlaardingen 3133 AT, The Netherlands
    Institute of Physics, University of Amsterdam, Science Park 904, Amsterdam 1098 XH, The Netherlands
    *Email: [email protected]
  • Caroline Remijn
    Caroline Remijn
    Unilever R&D Vlaardingen, Olivier van Noortlaan 120, Vlaardingen 3133 AT, The Netherlands
  • Faranaaz Rogier
    Faranaaz Rogier
    Unilever R&D Vlaardingen, Olivier van Noortlaan 120, Vlaardingen 3133 AT, The Netherlands
  • Micah van der Vaart
    Micah van der Vaart
    Unilever R&D Vlaardingen, Olivier van Noortlaan 120, Vlaardingen 3133 AT, The Netherlands
  • Panayiotis Voudouris
    Panayiotis Voudouris
    Unilever R&D Vlaardingen, Olivier van Noortlaan 120, Vlaardingen 3133 AT, The Netherlands
  • , and 
  • Krassimir P. Velikov*
    Krassimir P. Velikov
    Unilever R&D Vlaardingen, Olivier van Noortlaan 120, Vlaardingen 3133 AT, The Netherlands
    Institute of Physics, University of Amsterdam, Science Park 904, Amsterdam 1098 XH, The Netherlands
    Soft Condensed Matter, Debye Institute for Nanomaterials Science, Utrecht University, Princetonplein 5, Utrecht 3584 CC, The Netherlands
    *Email: [email protected]
Cite this: ACS Appl. Bio Mater. 2018, 1, 5, 1440–1447
Publication Date (Web):October 31, 2018
https://doi.org/10.1021/acsabm.8b00385
Copyright © 2018 American Chemical Society

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Abstract

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It is long known that oil-in-water emulsions can be stable against coalescence in homogenized plant cell wall dispersions because of the presence of surface-active biopolymers. When plant cell wall material is homogenized to the extent of deagglomeration of the cellulose microfibrils (CMFs), a much more complex dispersed system is obtained. Here we show that in such complex systems both surface active soluble polymers and individual CMFs are at the origin of this stabilization against coalescence, as they form a shell around the oil droplets providing Pickering-like stabilization. Individual CMFs and bundles of them in the presence of soluble biopolymers form a hybrid network in the continuous phase linking the droplets, creating a viscoelastic network that prevents the droplets from coalescing. Depletion induced attraction caused by soluble biopolymers and dispersed CMFs induces the formation of oil droplet clusters at low CMF concentrations leading to a highly heterogeneous distribution of oil droplets. This effect diminishes at high CMF concentrations at which the strong viscoelastic network arrests the droplets. These findings are important steps toward controlling complex dispersed systems comprising CMF–polymers mixtures with a second liquid or solid dispersed phase.

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The Supporting Information is available free of charge on the ACS Publications website at DOI: 10.1021/acsabm.8b00385.

  • Confocal images and cryo-SEM of the plant cell wall dispersion after deagglomeration, AFM image of the supernatant, interfacial tension between the supernatant and the oil, measurement of the molecular weight, and zeta potential (PDF)

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Cited By

This article is cited by 17 publications.

  1. Hanaé Dupont, Valentin Maingret, Véronique Schmitt, Valérie Héroguez. New Insights into the Formulation and Polymerization of Pickering Emulsions Stabilized by Natural Organic Particles. Macromolecules 2021, 54 (11) , 4945-4970. https://doi.org/10.1021/acs.macromol.1c00225
  2. Qi Li, Quan Ma, Yilan Wu, Yan Li, Bin Li, Xiaogang Luo, Shilin Liu. Oleogel Films Through the Pickering Effect of Bacterial Cellulose Nanofibrils Featuring Interfacial Network Stabilization. Journal of Agricultural and Food Chemistry 2020, 68 (34) , 9150-9157. https://doi.org/10.1021/acs.jafc.0c03214
  3. Xin Wang, Ye Zhou, Viviana Palacio-Betancur, Young-Ki Kim, Lily Delalande, Michael Tsuei, Yu Yang, Juan J. de Pablo, Nicholas L. Abbott. Reconfigurable Multicompartment Emulsion Drops Formed by Nematic Liquid Crystals and Immiscible Perfluorocarbon Oils. Langmuir 2019, 35 (49) , 16312-16323. https://doi.org/10.1021/acs.langmuir.9b02864
  4. Luis Valencia, Emma M. Nomena, Aji P. Mathew, Krassimir P. Velikov. Biobased Cellulose Nanofibril–Oil Composite Films for Active Edible Barriers. ACS Applied Materials & Interfaces 2019, 11 (17) , 16040-16047. https://doi.org/10.1021/acsami.9b02649
  5. Zhiheng Yuan, Xinyue Xu, Jiaxin Xu, Danshi Zhu, Jun Liu, He Liu. Emulsifying properties of homogenised soybean hull suspensions as stabilisers for oil/water emulsions. International Journal of Food Science & Technology 2023, 58 (7) , 3946-3957. https://doi.org/10.1111/ijfs.15932
  6. Nithin Madhavan, Manas Mukherjee, Madivala G. Basavaraj. Exploiting kaolinite-alumina heteroaggregation in Pickering emulsion stabilisation and porous mullite fabrication. Applied Clay Science 2023, 236 , 106881. https://doi.org/10.1016/j.clay.2023.106881
  7. Zhiheng Yuan, Danshi Zhu, Xinyue Xu, Jiaxin Xu, Lina Yang, Hong Song, Shengnan Wang, Jun Liu, He Liu. Homogenized soybean hull suspension as an emulsifier for oil/water emulsions: Synergistic effect of the insoluble fiber and soluble polysaccharide. International Journal of Biological Macromolecules 2023, 237 , 123950. https://doi.org/10.1016/j.ijbiomac.2023.123950
  8. Annelies E. Blok, Dieuwerke P. Bolhuis, Luben N. Arnaudov, Krassimir P. Velikov, Markus Stieger. Influence of thickeners (microfibrillated cellulose, starch, xanthan gum) on rheological, tribological and sensory properties of low-fat mayonnaises. Food Hydrocolloids 2023, 136 , 108242. https://doi.org/10.1016/j.foodhyd.2022.108242
  9. Shu-Ming Cui, Saud Hashmi, Wen-Qiang Li, Stephan Handschuh-Wang, Cheng-Tian Zhu, Shi-Chang Wang, Pian-Pian Yang, Yan-Fei Huang, Guang-Ming Zhu, Florian J. Stadler. Influence of Cellulose Nanofibers on the Behavior of Pickering Emulsions. Part 1. Microscopy and Startup Flow Test. Materials 2022, 15 (23) , 8285. https://doi.org/10.3390/ma15238285
  10. Shao Hui Teo, Ching Yern Chee, Mochamad Zakki Fahmi, Satya Candra Wibawa Sakti, Hwei Voon Lee. Review of Functional Aspects of Nanocellulose-Based Pickering Emulsifier for Non-Toxic Application and Its Colloid Stabilization Mechanism. Molecules 2022, 27 (21) , 7170. https://doi.org/10.3390/molecules27217170
  11. Annelies E. Blok, Dieuwerke P. Bolhuis, Heleen V.M. Kibbelaar, Daniel Bonn, Krassimir P. Velikov, Markus Stieger. Comparing rheological, tribological and sensory properties of microfibrillated cellulose dispersions and xanthan gum solutions. Food Hydrocolloids 2021, 121 , 107052. https://doi.org/10.1016/j.foodhyd.2021.107052
  12. Nasim Ghavidel, Pedram Fatehi. Recent Developments in the Formulation and Use of Polymers and Particles of Plant‐based Origin for Emulsion Stabilizations. ChemSusChem 2021, 14 (22) , 4850-4877. https://doi.org/10.1002/cssc.202101359
  13. Emma M. Nomena, Micah van der Vaart, Panayiotis Voudouris, Krassimir P. Velikov. Rheology of oil-in-water emulsions stabilised by native cellulose microfibrils in primary plant cells dispersions. Food Structure 2021, 30 , 100239. https://doi.org/10.1016/j.foostr.2021.100239
  14. Jun-ru Qi, Li-wen Song, Wei-qi Zeng, Jin-song Liao. Citrus fiber for the stabilization of O/W emulsion through combination of Pickering effect and fiber-based network. Food Chemistry 2021, 343 , 128523. https://doi.org/10.1016/j.foodchem.2020.128523
  15. Shasha Guo, Xia Li, Yishan Kuang, Jianming Liao, Kai Liu, Jun Li, Lihuan Mo, Shuaiming He, Wenyuan Zhu, Junlong Song, Tao Song, Orlando J. Rojas. Residual lignin in cellulose nanofibrils enhances the interfacial stabilization of Pickering emulsions. Carbohydrate Polymers 2021, 253 , 117223. https://doi.org/10.1016/j.carbpol.2020.117223
  16. Emma M. Nomena, Krassimir P. Velikov. Drying of pickering emulsions in a viscoelastic network of cellulose microfibrils. Colloids and Surfaces A: Physicochemical and Engineering Aspects 2019, 568 , 271-276. https://doi.org/10.1016/j.colsurfa.2019.01.075
  17. Juntao Tang, Ning Lin, Zhen Zhang, Chunyue Pan, Guipeng Yu. Nanopolysaccharides in Emulsion Stabilization. 2019, 221-254. https://doi.org/10.1007/978-981-15-0913-1_6

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