Andreas Lendlein

Materials are said to show a shape-memory effect if they can be deformed and fixed into a temporary shape, and recover their original, permanent shape only on exposure to an external stimulus. Shape-memory polymers have received increasing attention because of their scientific and technological significance. In principle, a thermally induced shape-...

Critical size defects in bone, which do not heal by themselves, occur after trauma, infection, or tumor resections. Rising awareness of the socioeconomic impact and the lack of adequate treatments has stimulated significant scientific attention on creating therapeutic options for bone regeneration. The growth of pores during degradation corresponds...

The ability of hydrophilic chain segments in polymer networks to strongly interact with water allows the volumetric expansion of the material and formation of a hydrogel. When polymer chain segments undergo reversible hydration depending on environmental conditions, smart hydrogels can be realized, which are able to shrink/swell and thus alter thei...

Shape memory is the capability of a material to be deformed and fixed into a temporary shape. Recovery of the original shape can then be triggered only by an external stimulus. Shape-memory polymers are highly deformable materials that can be programmed to recover a memorized shape in response to a variety of environmental and spatially localized s...

Classic rotating engines are powerful and broadly used but are of complex design and difficult to miniaturize. It has long remained challenging to make large-stroke, high-speed, high-energy microengines that are simple and robust. We show that torsionally stiffened shape memory nanocomposite fibers can be transformed upon insertion of twist to stor...

A layer of laminins, assembled on a thin sheet of collagen type IV (Col‐IV) forms the backbone of the basal lamina, which controls biological processes such as embryogenesis, tissue homeostasis, and development. Here, the dynamic functions of laminin‐111 (Lam‐111) in ultrathin films at the air–water interface are investigated. It is shown that the...

In situ hydrogelation of injectable precursors upon biological stimulus is relevant to generate hydrogels under mild conditions and, potentially, at a biological side of interest. Here, it is shown that hydrolytic enzymes can be used to initiate the formation of covalent hydrogel networks, realizing a cleavage‐leading‐to‐gelation strategy. For this...

The clinical success of orthopedic implants is closely related to their integration in the bone tissue promoted by rough device surfaces. The biological response of precursor cells to their artificial microenvironments plays a critical role in this process. In this study, we elucidated the relation between cell instructivity and surface microstruct...

Abstract The basement membrane (BM) is a biointeractive ultrathin network with distinct composition and organization of its epithelial and stromal sides, which render BMs with asymmetric biofunctions and mechanical properties. There are difficulties in the recapitulation of the highly hierarchical structure and function of BM. Here, the interfacial...

Citation: Farhan, M.; Hartstein, D.S.; Pieper, Y.; Behl, M.; Lendlein, A.; Neffe, A.T. Bio-Inspired Magnetically Controlled Reversibly Actuating Multimaterial Fibers. Polymers 2023, 15, 2233. https://doi. Abstract: Movements in plants, such as the coiling of tendrils in climbing plants, have been studied as inspiration for coiling actuators in robo...

Motile organs have evolved in climbing plants enabling them to find a support and, after secure attachment, to reach for sunlight without investing in a self-supporting stem. Searching movements, the twining of stems, and the coiling of tendrils are involved in successful plant attachment. Such coiling movements have great potential in robotic appl...

Enzymatic hydrolysis holds great promise for plastic waste recycling and upcycling. The interfacial catalysis mode, and the variability of polymer specimen properties under different degradation conditions, add to the complexity and difficulty of understanding polymer cleavage and engineering better biocatalysts. We present a systemic approach to s...

Soft actuator performance can be tuned by chemistry or mechanical manipulation, but this adjustability is limited especially in view of their growing technological relevance. Inspired from textile engineering, we designed and fabricated fiber mesh actuators and introduced new features like anisotropic behavior and soft-tissue like elastic deformabi...

Adaptivity is an essential capability of creatures to develop skills for surviving and reproducing. Mimicking such behavior would enable the design of biologically inspired functions. Hydrogel actuators are promising candidate materials capable of stimuli-responsive movements via water uptake and release. Here, for the first time, the adaptive-like...

Mechanical stress is recognized as a principle for opening enclosed compartments through compression, stretching, or shear, eventually resulting in the onset of a diffusion-controlled release. Here, we hypothesized that the geometrical design of cavities (cut-outs) introduced as containers in elastic polymer substrates and sealed with a brittle coa...

Guidance of postinfarct myocardial remodeling processes by an epicardial patch system may alleviate the consequences of ischemic heart disease. As macrophages are highly relevant in balancing immune response and regenerative processes their suitable instruction would ensure therapeutic success. A polymeric mesh capable of attracting and instructing...

In vivo endothelialization of polymer-based cardiovascular implant materials is a promising strategy to reduce the risk of platelet adherence and the subsequent thrombus formation and implant failure. However, endothelial cells from elderly patients are likely to exhibit a senescent phenotype that may counteract endothelialization. The senescence s...

The degradation of polymers is described by mathematical models based on bond cleavage statistics including the decreasing probability of chain cuts with decreasing average chain length. We derive equations for the degradation of chains under a random chain cut and a chain end cut mechanism, which are compared to existing models. The results are us...

Maximizing the efficiency of nanocarrier-mediated co-delivery of genes for co-expression in the same cell is critical for many applications. Strategies to maximize co-delivery of nucleic acids (NA) focused largely on carrier systems, with little attention towards payload composition itself. Here, we investigated the effects of different payload des...

Collagen-based biomaterials with oriented fibrils have shown great application potential in medicine. However, it is still challenging to control the type I collagen fibrillogenesis in ultrathin films. Here, we report an approach to produce cohesive and well-organized type I collagen ultrathin films of about 10 nm thickness using the Langmuir-Blodg...

Highlights The production and consumption of commodity polymers have been an indispensable part of the development of our modern society. Owing to their adjustable properties and variety of functions, polymer-based materials will continue playing important roles in achieving the Sustainable Development Goals (SDG)s, defined by the United Nations, i...

Tissue reconstruction has an unmet need for soft active scaffolds that enable gentle loading with regeneration‐directing bioactive components by soaking up but also provide macroscopic dimensional stability. Here microporous hydrogels capable of an inverse shape‐memory effect (iSME) are described, which in contrast to classical shape‐memory polymer...

Soft robotics aims at creating systems with improved performance of movement and adaptability in unknown, challenging, environments and with higher level of safety during interactions with humans. This Roadmap on Soft Robotics covers selected aspects for the design of soft robots significantly linked to the area of multifunctional materials, as the...

In vitro transcribed (IVT)-mRNA has been accepted as a promising therapeutic modality. Advances in facile and rapid production technologies make IVT-mRNA an appealing alternative to protein- or virus-based medicines. Robust expression levels, lack of genotoxicity and their manageable immunogenicity benefit its clinical applicability. We postulated...

Insufficient endothelialization of cardiovascular grafts is a major hurdle in vascular surgery and regenerative medicine, bearing a risk for early graft thrombosis. Neither of the numerous strategies pursued to solve these problems were conclusive. Endothelialization is regulated by the endothelial basement membrane (EBM), a highly specialized part...

Among the high-performance and engineering polymers, polyimides and the closely related polyetherimide (PEI) stand out by their capability to react with nucleophiles under relatively mild conditions. By targeting the phthalimide groups in the chain backbone, post-functionalization offers a pathway to adjust surface properties such as hydrophilicity...

Polymeric devices capable of releasing submicron particles (subMP) on demand are highly desirable for controlled release systems, sensors, and smart surfaces. Here, a temperature-memory polymer sheet with a programmable smooth surface served as matrix to embed and release polystyrene subMP controlled by particle size and temperature. subMPs embeddi...

The shape and the actuation capabilty of state of the art robotic devices typically relies on multimaterial systems from a combination of geometry determining materials and actuation components. Here, we present multifunctional 4D-actuators processable by 3D-printing, in which the actuator functionality is integrated into the shaped body. The mater...

Supporting the wound healing of soft tissues requires fixation devices becoming more elastic while degrading. To address this unmet need, we designed a blend of degradable multiblock copolymers, which is cross-linked by PLA stereocomplexation combining two soft segments differing substantially in their hydrolytic degradation rate. The degradation p...

Glycerol-based epoxy networks have great potential for surface functionalization, providing anti-microbial and protein repellant function. However, the synthesis of glycerol glycidyl ether (GGE) monomer often requires excessive epichlorohydrin (ECH). ECH derived organochloride containing byproducts from monomer production maybe present in the eluen...

Functionalization of gelatin with glycidylmethacrylate (GMA-gelatin) enables network formation employing the double bond, so that the reaction is orthogonal to the inherent functional groups in the biomacromolecule. Here, network formation by crosslinking of GMA-gelatin with hexane 1,6-dithiol or nonane 1,9-dithiol to tailor properties and enable a...

Spherical particles from shape-memory polymers (SMP) can be stretched to ellipsoids with high aspect ratio (AR) and temporarily stabilized. They can switch back to low AR upon thermal stimulation. Here, the creation of an alternative shape-switching capability of particles from low to high AR is introduced, where a SMP matrix from polyvinyl alcohol...

Effective temporary shape fixation by strain-induced formation of supramolecular nanostructures enables high energy density one-way shape-memory polymers.

Multiblock copolymers type PDC are polyetheresterurethanes composed of poly(ɛ-caprolactone) and poly(p-dioxanone) segments. They were designed as degradadable shape-memory polymers for medical devices, which can be implanted minimally-invasively. While providing structural support in the initial phase after implantation, they are capable to modulat...

In vitro thrombogenicity test systems require co-cultivation of endothelial cells and platelets under blood flow-like conditions. Here, a commercially available perfusion system is explored using plasma-treated cyclic olefin copolymer (COC) as a substrate for the endothelial cell layer. COC was characterized prior to endothelialization and co-culti...

Human induced pluripotent stem cells (hiPSCs) are a promising cell source to generate the patient-specific lung organoid given their superior differentiation potential. However, the current 3D cell culture approach is tedious and time-consuming with a low success rate and high batch-to-batch variability. Here, we explored the establishment of lung...

Background: Polymeric materials have been widely used as artificial grafts in cardiovascular applications. These polymeric implants can elicit a detrimental innate and adaptive immune response after interacting with peripheral blood. A surface modification with components from extracellular matrices (ECM) may minimize the activation of immune cell...

Sulfated biomolecules are known to influence numerous biological processes in all living organisms. Particularly, they contribute to prevent and inhibit the hypercoagulation condition. The failure of polymeric implants and blood contacting devices is often related to hypercoagulation and microbial contamination. Here, bioactive sulfated biomacromol...

Human induced pluripotent stem cells (hiPSCs) are highly sensitive to extrinsic physical and biochemical signals from their extracellular microenvironments. In this study, we analyzed the effect of cyclic temperature changes on hiPSCs behaviors, especially by means of scanning force microscopy (BIO-AFM). The alternation in cellular mechanics, as we...

Shape-memory polymer micronetworks (MN) are micrometer-sized objects that can switch their outer shape upon external command. This study aims to scale MN sizes to the low micrometer range at very narrow size distributions. In a two-step microfluidic strategy, the specific design of coaxial class capillary devices allowed stabilizing the thread of t...

Biofouling on medical device surfaces, which is initiated by protein adsorption and adhesion of microbes especially the antibiotic-resistant bacteria, attracts global attention for centuries due to its enduring challenges in healthcare. Here, the antifouling effect of hydrophilic poly(glycerol glycidyl ether) (polyGGE) film is explored in compariso...

The Venus flytrap is a fascinating plant with a finely tuned mechanical bi-stable system, which can switch between mono- and bi-stability. Here, we combine geometrical design of compliant mechanics and the function of shape-memory polymers to enable switching between bi- and mono-stable states. Digital design and modelling using the Chained Beam Co...

Complexes from catalysts and initiator can be used to insert a specific number of additional chemical functional groups in (co)polymers prepared by ring-opening polymerization (ROP) of lactones. We report on the synthesis of cooligomers from sec -butyl-morpholine-2,5-dione (SBMD) and para -dioxanone (PDX) by ROP with varied feed ratios in the bulk...

Identification of patterns in chemical reaction pathways aids in the effective design of molecules for specific applications. Here, we report on model reactions with a water-soluble single thiol-thioester exchange (TTE) reaction substrate, which was designed taking in view biological and medical applications. This substrate consists of the thio-dep...

Toll-like receptor (TLR) can trigger an immune response against virus including SARS-CoV-2. TLR expression/distribution is varying in mesenchymal stromal cells (MSCs) depending on their culture environments. Here, to explore the effect of periodic thermomechanical cues on TLRs, thermally controlled shape-memory polymer sheets with programmable actu...

Multifunctionality of electrospun polylactic acid (PLA) nonwovens was generated by the morphological design of nanofibers. Coaxial fibers with a lower number average molar mass M n PLLA core and a higher M n PDLA shell form PDLA–PLLA stereocrystals at the interface, induced by annealing. In tensile tests under physiological conditions, the core–she...

Rapid migration of mesenchymal stem cells (MSCs) on device surfaces could support in vivo tissue integration and might facilitate in vitro organoid formation. Here, polydopamine (PDA) is explored as a biofunctional coating to effectively promote MSC motility. It is hypothesized that PDA stimulates fibronectin deposition and in this way enhances int...

Increasing the surface hydrophilicity of polyetherimide (PEI) through partial hydrolysis of the imide groups while maintaining the length of the main-chain was explored for adjusting its function in biomedical and membrane applications. The outcome of the polymer analogous reaction, i.e., the degree of ring opening and chain cleavage, is difficult...

Near-physiological in vitro thrombogenicity test systems for the evaluation of blood-contacting endothelialized biomaterials requires co-cultivation with platelets (PLT). However, the addition of PLT has led to unphysiological endothelial cell (EC) detachment in such in vitro systems. A possible cause for this phenomenon may be PLT activation trigg...

Active fibers can serve as artificial muscles in robotics or components of smart textiles. Here, we present an origami hand robot, where single fibers control the reversible movement of the fingers. A recovery/contracting force of 0.2 N with a work capacity of 0.175 kJ kg ⁻¹ was observed in crosslinked poly[ethylene- co -(vinyl acetate)] (cPEVA) fi...

Inspired by the interesting functional traits of a climbing cactus, Selenicereus setaceus, found in the forest formations of Southeastern Brazil, we formulated a hypothesis that we can directly learn from the plants to develop multi-functional artificial systems by means of a multi-disciplinary approach. In this context, our approach is to take adv...

The hierarchical design approach provides various opportunities to adjust the structural performance of polymer materials. Electrospinning processing techniques give access to molecular orientation as a design parameter, which we consider here in view of the shape-memory actuation performance. The aim of this work is to investigate how the reversib...

The application of polymers in medicine requires sterilization while retaining material structure and properties. This demands detailed analysis, which we show exemplarily for the sterilization of PLLA/PDLA core–shell nanofibers with ethylene oxide (EtO). The electrospun patch was exposed to EtO gas (6 vol% in CO 2 , 1.7 bar) for 3 h at 45 °C and 7...

The potential of using crystallinity as morphological parameter to control polyester degradation in acidic environments is explored in ultrathin films by Langmuir technique. Films of hydroxy or methacrylate end-capped oligo(ε-caprolactone) (OCL) are prepared at the air–water interface as a function of mean molecular area (MMA). The obtained amorpho...

High crystallization rate and thermomechanical stability make polylactide stereocomplexes effective nanosized physical netpoints. Here, we address the need for soft, form-stable degradable elastomers for medical applications by designing such blends from (co)polyesters, whose mechanical properties are ruled by their nanodimensional architecture and...

Shape-memory hydrogels (SMH) are multifunctional, actively-moving polymers of interest in biomedicine. In loosely crosslinked polymer networks, gelatin chains may form triple helices, which can act as temporary net points in SMH, depending on the presence of salts. Here, we show programming and initiation of the shape-memory effect of such networks...

Shape-memory hydrogels (SMH) are as multifunctional, actively-moving polymers of interest in biomedicine. In loosely crosslinked polymer networks gelatin chains may form triple helices, which can act as temporary netpoints in SMH, depending on the presence of salts. Here, we show programming and initiation of the shape-memory effect of such network...

Climbing plants must reach supports and navigate gaps to colonize trees. This requires a structural organization ensuring the rigidity of so-called ‘searcher’ stems. Cacti have succulent stems adapted for water storage in dry habitats. We investigate how a climbing cactus Selenicereus setaceus develops its stem structure and succulent tissues for c...

Semi-crystalline oligomers are explored as functionalized thermoswitchable coatings for modification of biomaterials surface. Highly crystalline oligo(ε-caprolactone) (OCL) films are prepared at the air–water interface by the Langmuir technique, which consist of tightly packed single crystals. Their morphology and melting temperature can be tuned b...

Langmuir monolayers are introduced as highly efficient model system to investigate the impact of water on crystallization, melting and recrystallization of semi‐crystalline oligomers, in particular oligo(e‐caprolactone). More details can be found in article number 2001940 by Andreas Lendlein and co‐workers.

Back Cover: In article number 2000730 by Andreas Lendlein and co‐workers, a temperature‐controlled micro‐bench vise is applied to program anisotropic PDLCL foams into a temporary shape and to observe their stress‐free recovery upon heating. Differences in the geometry of the pore deformationen along the two axes of the anisotropic system become app...

Bio-interactive hydrogel formation in situ requires sensory capabilities toward physiologically relevant stimuli. Here, we report on pH-controlled in situ hydrogel formation relying on latent cross-linkers, which transform from pH sensors to reactive molecules. In particular, thiopeptolide/thio-depsipeptides were capable of pH-sensitive thiol-thioe...

The capability of a degradable implant to provide mechanical support depends on its degradation behavior. Hydrolytic degradation was studied for a polyesteretherurethane (PEEU70), which consists of poly(p-dioxanone) (PPDO) and poly(ε-caprolactone) (PCL) segments with a weight ratio of 70:30 linked by diurethane junction units. PEEU70 samples prepar...

Isotropic and anisotropic shape‐memory polymer foams are prepared by supercritical carbon dioxide foaming from a multiblock copolymer (PDLCL) consisting of poly(ω‐pentadecalactone) and poly(ε‐caprolactone) segments. Analysis by micro‐computed tomography reveals for the anisotropic PDLCL foam cells a high shape anisotropy ratio of R = 1.72 ± 0.62 wi...

High levels of reactive oxygen species (ROS) during stem cell expansion often lead to replicative senescence. Here, a polydopamine (PDA)-coated substrate was used to scavenge extracellular ROS for mesenchymal stem cell (MSC) expansion. The PDA-coated substrate could reduce the oxidative stress and mitochondrial damage in replicative senescent MSCs....

The thermal behavior of ultrathin, semi‐crystalline films of oligo(ε‐caprolactone)s (OCLs) with hydroxy or methacrylate end groups, is studied by the Langmuir technique in dependence on mean molecular areas and crystallization temperatures. The films on solid substrate as obtained by Langmuir–Schaefer transfer exhibit different lamellar thicknesses...

Enzymes can support the synthesis or degradation of biomacromolecules in natural processes. Here, we demonstrate that enzymes can induce a macroscopic-directed movement of microstructured hydrogels following a mechanism that we call a "Jack-in-the-box" effect. The material's design is based on the formation of internal stresses induced by a deforma...