Chemical Gradients in Polymer-Modified Paper Sheets — Towards Single-Layer Biomimetic Soft Robots

Biomimetic actuators are typically constructed as functional bi- or multilayers, where actuating and resistance layers together dictate bending responses upon triggering by environmental stimuli. Inspired by motile plant structures, like the stems of the false rose of Jericho (Selaginella lepidophylla), we introduce polymer-modified paper sheets that can act as soft robotic single-layer actuators capable of hygro-responsive bending reactions. A tailored gradient modification of the paper sheet along its thickness entails increased dry and wet tensile strength and allows at the same time for hygro-responsiveness. For the fabrication of such single-layer paper devices, the adsorption behavior of a cross-linkable polymer to cellulose fiber networks was first evaluated. By using different concentrations and drying procedures fine-tuned polymer gradients throughout the thickness can be achieved. Due to the covalent cross-linking of polymer with fibers, these paper samples possess significantly increased dry and wet tensile strength properties. We furthermore investigated these gradient papers with respect to a mechanical deflection during humidity cycling. The highest humidity sensitivity is achieved using eucalyptus paper with a grammage of 150 g m⁻² modified with the polymer dissolved in IPA (~13 wt%) possessing a polymer gradient. Our study presents a straightforward approach for the design of novel hygroscopic, paper-based single-layer actuators, which have a high potential for diverse soft robotic and sensor applications

Humidity Influence on Mechanics and Failure of Paper Materials: Joint Numerical and Experimental Study on Fiber and Fiber Network Scale

Paper materials are natural composite materials and well-known to be hydrophilic unless chemical and mechanical processing treatments are undertaken. The relative humidity impacts the fiber elasticity, the fiber-fiber bonds and the failure mechanism. In this work, we present a comprehensive experimental and computational study on the mechanical and failure behaviour of the fiber and the fiber network under humidity influence. The manually extracted cellulose fiber is exposed to different levels of humidity, and then mechanically characterized using Atomic Force Microscopy, which delivers the humidity dependent longitudinal Young's modulus. The obtained relationship allows calculation of fiber elastic modulus at any humidity level. Moreover, by using Confoncal Laser Scanning Microscopy, the coefficient of hygroscopic expansion of the fibers is determined. On the other hand, we present a finite element model to simulate the deformation and the failure of the fiber network. The model includes the fiber anisotropy and the hygroscopic expansion using the experimentally determined constants. In addition, it regards the fiber-fiber bonding and damage by using a humidity dependent cohesive zone interface model. Finite element simulations on exemplary fiber network samples are performed to demonstrate the influence of different aspects including relative humidity and fiber-fiber bonding parameters on the mechanical features such as force-elongation curves, wet strength, extensiability and the local fiber-fiber debonding. In meantime, fiber network failure in a locally wetted region is revealed by tracking of individually stained fibers using in-situ imaging techniques. Both the experimental data and the cohesive finite element simulations demonstrate the pull-out of fibers and imply the significant role of the fiber-fiber debonding in the failure process of the wet paper.Comment: 21 pages,10 figure

Mechanistic Understanding and Three‐Dimensional Tuning of Fluid Imbibition in Silica‐Coated Cotton Linter Paper Sheets

Paper‐based microfluidic devices are used in point of care diagnostic, sensor technology or lab‐on‐a‐chip devices. Although a number of studies has been reported, only relatively few paper‐based diagnostic tools are available on the market. A remaining challenge is the mechanistic understanding and precise design of capillary flow in paper. Here, silica coatings are applied to control paper wettability, fiber swelling, and thus fluid transport in all three dimensions of a paper sheet via a simple dip‐coating and post‐treatment process. By adjusting the three‐dimensional silica coating distribution, a three‐dimensional asymmetric wettability gradient within the paper sheet is obtained which controls the fluid distribution and imbibition. The correlation between silica coating amount and silica distribution with the resulting fluid behavior is systematically elaborated by analyzing the interaction between fiber and fluid as well as the fiber swelling by applying confocal microscopy. Three different silica‐amount dependent fluid distribution states are demonstrated. These new insights into the mechanism of fluid imbibition using simple silica coatings enable the specific design of different imbibition mechanisms and thus the adjustment of the microfluidic properties in paper‐based microfluidic devices with control over all three spatial dimensions of a paper sheet in one fabrication step

Fluid Flow Programming in Paper-Derived Silica–Polymer Hybrids

In paper-based devices, capillary fluid flow is based on length-scale selective functional control within a hierarchical porous system. The fluid flow can be tuned by altering the paper preparation process, which controls parameters such as the paper grammage. Interestingly, the fiber morphology and nanoporosity are often neglected. In this work, porous voids are incorporated into paper by the combination of dense or mesoporous ceramic silica coatings with hierarchically porous cotton linter paper. Varying the silica coating leads to significant changes in the fluid flow characteristics, up to the complete water exclusion without any further fiber surface hydrophobization, providing new approaches to control fluid flow. Additionally, functionalization with redox-responsive polymers leads to reversible, dynamic gating of fluid flow in these hybrid paper materials, demonstrating the potential of length scale specific, dynamic, and external transport control

Deutsche Außenpolitik und Östliche Partnerschaft: Positionspapier der Expertengruppe Östliche Partnerschaft

In dem sieben Punkte umfassenden Positionspapier fordern acht hochrangige Persönlichkeiten aus der Politik ein stärkeres Engagement Deutschlands in Osteuropa und dem Kaukasus. "Die Östliche Partnerschaft ist von zentraler Bedeutung" für die deutsche und die EU-Außenpolitik. Die Bundesregierung solle einen Sonderbeauftragten ernennen, der dazu die deutsche Position einbringt

Carbohydrate binding module-fused antibodies improve the performance of cellulose-based lateral flow immunoassays

Since the pandemic outbreak of Covid-19 in December 2019, several lateral flow assay (LFA) devices were developed to enable the constant monitoring of regional and global infection processes. Additionally, innumerable lateral flow test devices are frequently used for determination of different clinical parameters, food safety, and environmental factors. Since common LFAs rely on non-biodegradable nitrocellulose membranes, we focused on their replacement by cellulose-composed, biodegradable papers. We report the development of cellulose paper-based lateral flow immunoassays using a carbohydrate-binding module-fused to detection antibodies. Studies regarding the protein binding capacity and potential protein wash-off effects on cellulose paper demonstrated a 2.7-fold protein binding capacity of CBM-fused antibody fragments compared to the sole antibody fragment. Furthermore, this strategy improved the spatial retention of CBM-fused detection antibodies to the test area, which resulted in an enhanced sensitivity and improved overall LFA-performance compared to the naked detection antibody. CBM-assisted antibodies were validated by implementation into two model lateral flow test devices (pregnancy detection and the detection of SARS-CoV-2 specific antibodies). The CBM-assisted pregnancy LFA demonstrated sensitive detection of human gonadotropin (hCG) in synthetic urine and the CBM-assisted Covid-19 antibody LFA was able to detect SARS-CoV-2 specific antibodies present in serum. Our findings pave the way to the more frequent use of cellulose-based papers instead of nitrocellulose in LFA devices and thus potentially improve the sustainability in the field of POC diagnostics