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The electrostatic attraction between positively charged CL and negatively charged LS led to the formation of insoluble self-organized macromolecule aggregates that align to films. The structures of the formed layers were evaluated by atomic force microscopy (AFM), firstly on glass lamina using dip-coating deposition and then on handsheets and industrial uncoated paper using roll-to-roll coating in a layer-by-layer mode. Coated samples were also characterized by optical microscopy, scanning electron microscopy (SEM) coupled with energy dispersive spectroscopy (SEM\/EDS), and contact angle measurements. It was suggested that the structure of all-lignin aggregates is the result of the interaction of amphiphilic water-soluble lignin molecules leading to their specifically ordered mutual arrangement depending on the order and the mode of their application on the surface. The all-lignin coating of cellulosic fiber imparts lower air permeability and lower free surface energy to paper, mainly due to a decrease in surface polarity, thus promoting the paper\u2019s hydrophobic properties. Moderate loading of lignin coating formulations (5\u20136 g m\u22122) did not affect the mechanical strength of the paper.<\/jats:p>","DOI":"10.3390\/ma15227869","type":"journal-article","created":{"date-parts":[[2022,11,8]],"date-time":"2022-11-08T12:45:47Z","timestamp":1667911547000},"page":"7869","update-policy":"https:\/\/doi.org\/10.3390\/mdpi_crossmark_policy","source":"Crossref","is-referenced-by-count":13,"title":["Modification of Paper Surface by All-Lignin Coating Formulations"],"prefix":"10.3390","volume":"15","author":[{"given":"Patricia I. F.","family":"Pinto","sequence":"first","affiliation":[{"name":"RAIZ\u2014Forest and Paper Research Institute, Quinta de S. Francisco, Apartado 15, 3801-501 Eixo Aveiro, Portugal"},{"name":"CICECO\u2014Aveiro Institute of Materials and Department of Chemistry, University of Aveiro, Campus Universit\u00e1rio de Santiago, 3810-193 Aveiro, Portugal"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-4518-5718","authenticated-orcid":false,"given":"Sandra","family":"Magina","sequence":"additional","affiliation":[{"name":"CICECO\u2014Aveiro Institute of Materials and Department of Chemistry, University of Aveiro, Campus Universit\u00e1rio de Santiago, 3810-193 Aveiro, Portugal"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-5958-466X","authenticated-orcid":false,"given":"Sara","family":"Fateixa","sequence":"additional","affiliation":[{"name":"CICECO\u2014Aveiro Institute of Materials and Department of Chemistry, University of Aveiro, Campus Universit\u00e1rio de Santiago, 3810-193 Aveiro, Portugal"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-1561-4406","authenticated-orcid":false,"given":"Paula C. R.","family":"Pinto","sequence":"additional","affiliation":[{"name":"RAIZ\u2014Forest and Paper Research Institute, Quinta de S. Francisco, Apartado 15, 3801-501 Eixo Aveiro, Portugal"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-8244-8153","authenticated-orcid":false,"given":"Falk","family":"Liebner","sequence":"additional","affiliation":[{"name":"CICECO\u2014Aveiro Institute of Materials and Department of Chemistry, University of Aveiro, Campus Universit\u00e1rio de Santiago, 3810-193 Aveiro, Portugal"},{"name":"Department of Chemistry, Institute of Chemistry of Renewable Resources, University of Natural Resources and Life Sciences, Vienna (BOKU), Konrad Lorenz Strasse 24, A-3430 Tulln, Austria"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-6304-5105","authenticated-orcid":false,"given":"Dmitry V.","family":"Evtuguin","sequence":"additional","affiliation":[{"name":"CICECO\u2014Aveiro Institute of Materials and Department of Chemistry, University of Aveiro, Campus Universit\u00e1rio de Santiago, 3810-193 Aveiro, Portugal"}]}],"member":"1968","published-online":{"date-parts":[[2022,11,8]]},"reference":[{"key":"ref_1","doi-asserted-by":"crossref","first-page":"574","DOI":"10.1016\/j.indcrop.2016.11.012","article-title":"Nanocellulose in packaging: Advances in barrier layer technologies","volume":"95","author":"Ferrer","year":"2017","journal-title":"Ind. 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