Mauricio A. Sarabia-Vallejos

San Sebastián University | USS · Facultad de Ingeniería y Tecnología

The preparation of sophisticated hierarchically structured and cytocompatible hydrogel scaffolds is presented. For this purpose, a photosensitive resin was developed, printability was evaluated, and the optimal conditions for 3D printing were investigated. The design and fabrication by additive manufacturing of tailor-made porous scaffolds were com...

Abstract: Hybrid scaffolds that are based on PLA and PLA/PMMA with 75/25, 50/50, and 25/75 weight ratios and functionalized with 10 wt.% of bioglass nanoparticles (n-BG) were developed using an electrospinning technique with a chloroform/dimethylformamide mixture in a 9:1 ratio for bone tissue engineering applications. Neat PLA and PLA/PMMA hybrid...

Patients with bone diseases often experience increased bone fragility. When bone injuries exceed the body’s natural healing capacity, they become significant obstacles. The global rise in the aging population and the escalating obesity pandemic are anticipated to lead to a notable increase in acute bone injuries in the coming years. Our research de...

Mesenchymal stem cells (MSC) are recognized for their immunomodulatory effects and regenerative properties, being promising therapeutic agents for a wide range of diseases. To ensure a localized effect of MSC in the organism biobased hydrogels have been tested for their ability to act as a matrix-embedded to improve MSC targeted delivery. In this c...

Mesenchymal stem cells (MSC) are recognized for their immunomodulatory effects and regenerative properties, being promising therapeutic agents for a wide range of diseases. To ensure a localized effect of MSC in the organism, biobased hydrogels have been tested for their ability to acting as a matrix-embedded to improves MSC targeted delivery. In t...

This review summarizes the relevant developments in preparing wrinkled structures with variable characteristics. These include the formation of smart interfaces with reversible wrinkle formation, the construction of wrinkles in non-planar supports, or, more interestingly, the development of complex hierarchically structured wrinkled patterns. Smart...

Bone implants or replacements are very scarce due to the low donor availability and the high rate of body rejection. For this reason, tissue engineering strategies have been developed as alternative solutions to this problem. This research sought to create a cellular scaffold with an intricate and complex network of interconnected pores and microch...

This review summarizes the most recent advances from technological and physico-chemical perspectives to improve several remaining issues in polymeric materials’ additive manufacturing (AM). Without a doubt, AM is experimenting with significant progress due to technological innovations that are currently advancing. In this context, the state-of-the-...

This article is devoted to the use of polymers in additive manufacturing (AM), also generally known as 3D printing or rapid prototyping. AM presents essential advantages in comparison to traditional fabrication methodologies since it allows the fabrication of wholly customized 3D parts and objects with astonishing levels of geometrical complexity....

Alveolar architecture plays a fundamental role in the processes of ventilation and perfusion in the lung. Alterations in the alveolar surface area and alveolar cavity volume constitute the pathophysiological basis of chronic respiratory diseases such as pulmonary emphysema. Previous studies based on micro-computed tomography (micro-CT) of lung samp...

Biocompatible smart interfaces play a crucial role in biomedical or tissue engineering applications, where their ability to actively change their conformation or physico-chemical properties permits finely tuning their surface attributes. Polyelectrolytes, such as acrylic acid, are a particular type of smart polymers that present pH responsiveness....

Smart wrinkled hydrogel patterns with modulated chemical composition and wrinkle characteristics (amplitude and period) were formed by taking advantage of surface instabilities using a simple, cost-affordable, and robust method. The microstructured surfaces were prepared by dip coating and were designed to be stimuli-responsive by introducing poly(...

The use of 4D printing is, without any doubt, one of the current challenges and also an exciting opportunity to create customized and perfectly defined 3D structures capable of changing their shape according to a particular external stimulus. This article aims to provide a basic and general overview of 4D printing, providing the characteristics and...

Background: Protective mechanical ventilation (MV) aims at limiting global lung deformation and has been associated with better clinical outcomes in acute respiratory distress syndrome (ARDS) patients. In ARDS lungs without MV support, the mechanisms and evolution of lung tissue deformation remain understudied. In this work, we quantify the progre...

Additive manufacturing (AM), commonly known as three-dimensional (3D) printing, is a widely used methodology that permits to fabricate fully customizable parts and objects with an astonishing level of geometrical complexity in a reduced time and with low costs. Polymers are, by far, the most widely used materials to fabricate 3D-printed parts due t...

This manuscript presents an inkjet-based strategy to fabricate wrinkled hydrogel surfaces with controlled characteristics (period and amplitude). For this purpose, a monomer mixture containing a crosslinking agent, a hydrophilic monomer, and a photoinitiator were deposited onto polycarbonate substrates. Upon UV irradiation and controlled drying und...

Introduction Breathing produces a phenomenon of cyclic deformation throughout life. Biomechanically, deformation of the lung is measured as strain. Regional strain recently started to be recognised as a tool in the study of lung pathophysiology, but regional lung strain has not been studied in healthy subjects breathing spontaneously without volunt...

In this article, a simple protocol based on a multi-step methodology is used to form flat, first-generation (G1) or second-generation (G2) wrinkled patterns. Different concentrations of DMAEMA were used to synthesize hy- drogel films. The multi-step method used to form the wrinkled pattern involves vacuum, argon plasma, and UV exposure. This method...

Alveolar stresses are fundamental to enable the respiration process in mammalians and have recently gained increasing attention due to their mechanobiological role in the pathogenesis and development of respiratory diseases. Despite the fundamental physiological role of stresses in the alveolar wall, the determination of alveolar stresses remains c...

In this work, hydrogels based on HEMA and DMAEMA (pH-sensitive monomer) were used to form biocompatible films which present microwrinkled patterns in their surface, with the focus of exploring the role of chemical composition on cell adhesion and proliferation. Three different pH (5.4, 7.4, and 8.3) were employed to prepare these hydrogels. The pre...

Three-dimensional (3D) printing technologies can be widely used for producing detailed geometries based on individual and particular demands. Some applications are related to the production of personalized devices, implants (orthopedic and dental), drug dosage forms (antibacterial, immunosuppressive, anti-inflammatory, etc.), or 3D implants that co...

Additive manufacturing (AM), also known as additive manufacturing, permits the fabrication of fully customized objects with a high level of geometrical complexity at reduced fabrication time and cost. Besides metals and ceramics, polymers have become a widely researched class of materials for applica- tions in AM. The synthetic versatility and adap...

The generation of microstructured patterns on the surface of a specific polymeric material could radically improve their performance in a particular application. Most of the interactions with the environment occur at the material interface; therefore, increasing the exposed active surface considerably improves their range of application. In this ar...

In a previous chapter of this book, some biological/biomedical polymeric devices in which wrinkled patterns were formed on the surface were fully revised. Particularly, different materials, with interesting thermal, optical, and mechanical properties, which could be used for several applications like generation of ultrasensitive force/pressure sens...

In this chapter, several methodologies used to generate surface instabilities on hydrogel films are reviewed. The main advantage of surface instability usage for generating nano- and micro-patterned surfaces is their low cost, ease of fabrication, and the possibility of methodology scalement for industrial processes. Surfaces instabilities are gene...

Frontal polymerization (FP) or vitrification consists in the generation of a reaction front, in a localized sector of the material, that travels in a particular direction. Their remarkable flexibility permits to controllably polymerize materials with different molecular weights and variable chemical nature. One of the advantages of FP is that it is...

Wrinkling and buckling of multilayered materials are common methodologies used for generating micro- or nano-patterned topographies on the top of the devices. According to the material used and the size and distribution of those patterns, some of these devices can be used for several interesting purposes like aeronautics, force/pressure sensing, or...

In this chapter, the different strategies to fabricate wrinkled surface morphologies are described. The methodologies have been classified as a function of the film structure, i.e., layered films, depth-wise gradient, or homogeneous films. Layered films are formed by different substrates and different top layers. The bilayer systems described in th...

In contrast to conventional patterning methodologies, the use of surface instabilities to pattern polymer surfaces does not require expensive equipment or long and multistep procedures to obtain surface microstructures. In addition, surface instabilities enable the fabrication of intricate and complex multiscale surface features which are difficult...

Traditional approaches to the patterning process of polymer surfaces (lithography, embossing, imprinting) have been largely explored and covered in this book. Parallel, patterns originated by surface instabilities and, in particular, those forming wrinkled surfaces have been also incorporated. The aim of this book is to cover the above-depicted asp...

In this work, we have reviewed the formation of ion beam-induced self-assembled wrinkle pattern on polymer surfaces, especially PDMS. By exposing the surface with a localized ion beam, it is possible to vary the chemical and/or mechanical properties of the material. Oxidation of the sample is procured, which entails the modification of their Young’...

In this article, we explored the selective antibiofouling capacity acquired by functional wrinkled hydrogel films via a fine tuning of their chemical structure through the gradual insertion of hydrophobic radical groups in their network. The hydrogel consists of three main components: hydroxyethyl methacrylate (HEMA, amphiphilic monomer), trifluoro...

Herein, we report the fabrication of wrinkled hydrogel films with tunable pH sensitivity by using tertiary amine methacrylate-based monomers. On the one hand, hydrogels composed of 2-hydroxyethyl methacrylate (HEMA), N,N-diethylaminoethyl methacrylate (DEAEMA), and poly(ethylene glycol) diacrylate (PEGDA575) were synthesized using different monomer...

Six new whole aromatic poly(azomethine)s with different rigidity were prepared from three diamines and two dialdehydes, all of them containing a diphenylsilane moiety as a central structural element. Two amines containing biphenyl moieties were obtained for the first time. Thus, the synthesized polymers contain two silicon atoms in the repeat unit,...

In this study, four new silicon-containing poly(ether-azomethine)s with linear structures were prepared using original silicon and biphenyl moiety-containing monomers: two diamines and two dialdehydes. The oligomeric natures of the samples were established by GPC analysis, which showed chains containing 3 to 5 repetitive units. The monomers and the...

Mechanics plays a key role in respiratory physiology, as lung tissue cyclically deforms to bring air in and out the lung, a life-long process necessary for respiration. The study of regional mechanisms of deformation in lung parenchyma has received great attention to date due to its clinical relevance, as local overstretching and stress concentrati...

In this review, we provide a general and clear overview about the different alternatives reported to fabricate a myriad of polypeptide architectures based on the ring-opening polymerization of N-carbonyanhydrides (ROP NCAs). First of all, the strategies for the preparation of NCA monomers directly from natural occurring or from modified amino acids...

Biomimetic planar artificial membranes have been widely studied due to their multiple applications in several research fields. Their humectation and thermal response are crucial for reaching stability; these characteristics are related to the molecular organization inside the bilayer, which is affected by the aliphatic chain length, saturations, an...

The present work describes oligomeric poly(amide-imide)s (PAIs) containing several l-amino acidic residues and two silicon atoms in their repeat unit, whose carboxylate terminal group was chemisorbed onto metallic particles (Cu, Ag or Au) previously deposited in controlled conditions via physical vapor deposition. Thus, for each prepared polymer-me...

This review describes, in an organized manner, the recent developments in the elaboration of hydrogels that possess antimicrobial activity. The fabrication of antibacterial hydrogels for biomedical applications that permits cell adhesion and proliferation still remains as an interesting challenge, in particular for tissue engineering applications....

Correlation between theoretical and experimental (Infrared and Raman spectroscopies) vibrational spectra of two compounds, both with a silyl group present in their main chain and with an optically active structure (L-valine) as side group, were performed. These compounds are based in a chiral dicarboxylic acid monomer and its respective polyamide-i...

Hydrogel films possess the ability of retain water and deliver it to a phospholipid bilayer mainly composed by DPPC (1,2-dipalmitoyl-sn-glycero-3-phosphocholine); moisture of the medium favors the stability of an artificial biomembrane when it is subjected to repetitive heating cycles. This hypothesis is valid when the hydrogel film, used as scaffo...

Two new aromatic dianhydride monomers containing R,R-diphenylsilane (R = Me or Ph), an ether group and an isobenzofuran-1,3-dione moiety in their structure were prepared and spectroscopically characterized. They were reacted with two silylated aromatic diamines, previously reported, in order to prepare four different aromatic poly(ether-imide)s (PE...

A highly epitaxial delafossite CuFe1 -xGaxO2 film was made with pulse laser deposition in high vacuum. The sample thickness was around 48 nm and it was terminated with CuFeO2. This delafossite sample was exposed to a CO2 atmosphere under controlled conditions and chemisorption of CO2 on the surface was observed. Transmittance and reflectance spectr...

DPPC bilayers were deposited over thin hydrogel scaffolds using the Langmuir-Blodgett technique (with DPPC thickness ∼6.2nm). Wrinkled hydrogels films were used to maintain a moist environment in order to enhance DPPC bilayer stability. Polymer mixtures were prepared using HEMA (as a base monomer) and DEGDMA, PEGDA575, PEGDA700 or AAm (as crosslink...

Organic thin film deposition presents a multiplicity of challenges. Most notably, layer thickness control, homogeneity and subsequent characterization have been not cleared yet. Phospholipid bilayers are frequently used to model cell membranes. Bilayers can be disrupted by changes in mechanical stress, pH and temperature. The strategy presented in...

Thermal behavior of Dipalmitoylphosphatidylcholine (DPPC) bilayers deposited over hydrogel fibers was examined. Thus, membrane stability, water absorption-release, phase transitions and phase transition temperatures were studied through different methods during heating cycles. Hydrogel films were realized using an oligomer mixture (HEMA-PEGDA575/ph...

Block copolymers have been recognized as versatile materials to prepare nanoporous polymer films or mem- branes, but their potential has not been completely explored. This study focuses on the formation and characterization of nanoporous polymer films based on poly(styrene)-block-(methylmethacrylate/methacrylic acid); (PS-b-MMA/MAA) were obtained t...

Oligo(ether-amide)s (PEAs) based on diphenylsilane and oxyphenyl units were synthesized through a Yamazaki–Higashi phosphorylation polyamidation technique. Thus, three new aromatic monomers were synthesized and characterized: a di(ether-amine), bis(4-(4-aminophenoxy)phenyl)dimethylsilane, and two dicarboxylic acids, bis(4-(4-carboxyphenoxy)phenyl)d...

Poly(ethylene glycol) diacrylate (PEGDA) of different molecular weight (Mn = 575 and 700) was used as crosslinking agent for the photopolymerization of 2-hydroxyethyl methacrylate (HEMA) in order to obtain HEMA/PEGDA-based hydrogels. Composites were synthesized in-situ employing a new methodology that implies the addition of different quantities of...

In situ nanoparticle formation embedded into hydrogel matrix, acting as container and stabilizer for nanoparticle reaction was the focus in this research; this method was realized using AgNO3 (0.75 and 1.0 M) as silver source for nanoparticle formation; also, monomers (HEMA), cross-linker agents (DEGDMA) and a photoini- tiator (Irgacure 651) were u...

FT-IR and Raman spectra of bis(4-aminophenyl)diphenylsilane (DIA) and a dicarboxylic acid containing the imide function and a L-alanine moiety (L-ALA) and their resultant polymer (PALA) were recorded in the 500-4000 cm-1 and 400-3800 cm-1 region; respectively. The optically active poly(imide-amide) obtained has two sp3 carbons in the main chain, fa...

A self-assembled diblock copolymer containing styrene (S), methyl methacrylate and a certain percentage of hydrophilic segment of poly(methacrylic acid) (i.e., poly(styrene)-block-poly(methyl methacrylate/methacrylic acid) was synthesized via the ATRP method in two steps. This was followed by a partial hydrolysis of the methyl ester linkages of the...

1,2-dipalmitoyl-sn-3-phosphoglycerocholine membranes were deposited onto a silicon substrate (Si/SiO(2)) using physical vapor deposition with in situ ellipsometric thickness control. Along several heating cycles it was possible to identify well-defined boundaries for gel, ripple, liquid crystalline, and fluid-disordered phases. Particularly, the se...