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Funding Information: The financial support of the Austrian Federal Ministry of Digital and Economic Affairs and the National Foundation for Research, Technology and Development , Austria, is gratefully acknowledged. We also thank the industrial partners Mondi, Canon Production Printing, Kelheim Fibres, and SIG Combibloc for their support. Publisher Copyright: © 2021 Copyright: Copyright 2021 Elsevier B.V., All rights reserved. Hydrophobization of cellulosic materials and particularly paper products is a commonly used procedure to render papers more resistant to water and moisture. Here, we explore the hydrophobization of unsized paper sheets via the gas phase. We employed three different compounds, namely palmitoyl chloride (PCl), trifluoroacetic anhydride/acetic anhydride (TFAA/Ac2O)) and hexamethyldisilazane (HMDS) which were vaporized and allowed to react with the paper sheets via the gas phase. All routes yielded hydrophobic papers with static water contact angles far above 90° and indicated the formation of covalent bonds. The PCl and TFAA approach negatively impacted the mechanical and optical properties of the paper leading to a decrease in tensile strength and yellowing of the sheets. The HMDS modified papers did not exhibit any differences regarding relevant paper technological parameters (mechanical properties, optical properties, porosity) compared to the non-modified sheets. XPS studies revealed that the HMDS modified samples have a rather low silicon content, pointing at the formation of submonolayers of trimethylsilyl groups on the fiber surfaces in the paper network. This was further investigated by penetration dynamic analysis using ultrasonication, which revealed that the whole fiber network has been homogeneously modified with the silyl groups and not only the very outer surface as for the PCl and the TFAA modified papers. This procedure yields a possibility to study the influence of hydrophobicity on paper sheets and their network properties without changing structural and mechanical paper parameters.

In this study we have evaluated the suitability of laboratory testing methods to predict inkjet printing results. We have developed and used testing liquids that are spanning the operational window of industrial High Speed Inkjet (HSI) printers while still covering the maximum possible range of viscosity and surface tension. First we correlated liquid penetration measured with ultrasound (ULP) and direct absorption (ASA) to print through from HSI prints. The best correlation ( R 2 ≈ 0.7 {R^{2}}\approx 0.7 ) was found for the sized paper. For papers with increasing liquid penetration speed we found a decreasing ability of both testing methods to predict print through, for the strong absorbing paper the correlation drops to R 2 ≈ 0.2 {R^{2}}\approx 0.2 . Second we correlated contact angle and drop diameter to the dot area from HSI prints. Contact angle turned out to be a better predictor for printed dot area than drop diameter. Evaluating the change in contact angle over time we found the highest correlation to the dot area in the print when measuring the contact angle as soon as possible, in our case 1 ms after deposition of the drop on the paper. We also compared contact angle with microliter drops to picoliter drops, which are in the size scale of the actual inkjet droplet. To our great surprise correlations for microliter drops were equal or better than for picoliter drops, particularly for highly absorbing papers. Thus in order to predict dot spreading on paper our results suggest to measure the contact angle with microliter drops. Overall we found that, using laboratory testing methods, print through and dot spreading for HSI printing can be quite well predicted for slow absorbing papers but not very well for fast absorbing papers.

In this study, we investigated the effect of liquid viscosity and surface tension for inkjet printing on porous cellulose sheets. We used five model liquids, representing the operational field of an industrial high speed inkjet printer, as specified by Ohnesorge- and Reynolds number. Drops with 30 pl and 120 pl drop size were jetted with a commercial HSI printhead. We printed on four uncoated papers representing the most relevant grades on the market in terms of hydrophobisation and surface treatment. We are presenting a quantitative analysis of viscosity and surface tension on the print outcome, evaluating dot size, liquid penetration (print through) and surface coverage of the printed dots. The most important finding is that for liquids within the jetting window the variation of the liquid viscosity typically has a 2–3 times higher impact on the print outcome than variation of the liquid surface tension. Increased viscosity in all cases reduces dot area, liquid penetration and liquid surface coverage. Surface tension plays a smaller role for liquid spreading and penetration, except for hydrophobised substrates, where both are reduced for higher surface tension. Interestingly, higher surface tension consistently increases liquid surface coverage for all papers and drop sizes. A detailed analysis on the competing effect of dot spreading and liquid penetration is presented, in terms of viscosity, surface tension and surface coverage of the liquid.

The contact angle Θ measured on rough, absorbing substrates is known to decrease with proceeding imbibition of the drop. We demonstrate that the impact of three absorption related parameters (absorption rate, drop size and residence time) on the measured contact angle is comprehensively captured by the relative absorbed drop volume, i.e. the percentage of the drop volume penetrated into the substrate. We analyzed a wide range of drop volumes (30 pl to 4 μl, spanning a factor 105) on substrates with very different liquid absorption rates (6 ml m−2s−1 to 710 ml m−2s−1). Also the effect of liquid surface tension (26.8 mN m−1 to 73 mN m−1) and the effect of evaporation have been evaluated. Analyzing the development of drop volume and contact angle over time one can identify the regimes of (1) surface roughness filling and (2) bulk penetration. Independent of drop size, absorption rate and drop residence time the contact angle decreases between ~ 0. 5∘ to ~ 1. 2∘ for each percentage point of drop volume penetrated into the substrate. Thus, the relative amount of absorbed drop volume fully captures the combined effect of drop size, contact time and substrate absorption rate on the contact angle measurement, it can be used to estimate the effect of liquid penetration on the measured contact angle. The effect of evaporation was negligible for most water based liquids. In conclusion contact angle values measured on absorbing substrates can only be compared for the same percentage of absorbed drop volume, e.g. when 30% of the drop volume has been absorbed.