Regenerated Silk Nanofibers for Robust and Cyclic Adsorption-Desorption on Anionic Dyes.

In recent years, adsorption-based membranes have been widely investigated to remove and separate textile pollutants. However, cyclic adsorption-desorption to reuse a single adsorbent and clear scientific evidence for the adsorption-desorption mechanism remains challenging. Herein, silk nanofibers were used to assess the adsorption potential for the typical anionic dyes from an aqueous medium, and they show great potential toward the removal of acid dyes from the aqueous solution with an adsorption rate of ∼98% in a 1 min interaction. Further, we measured the filtration proficiency of a silk nanofiber membrane in order to propose a continuous mechanism for the removal of acid blue dye, and a complete rejection was observed with a maximum permeability rate of ∼360 ± 5 L·m-2·h-1. The Fourier transform infrared spectroscopy and X-ray photoelectron spectroscopy studies demonstrate that this fast adsorption occurs due to multiple interactions between the dye molecule and the adsorbent substrate. The as-prepared material also shows remarkable results in desorption. A 50-time cycle exhibits complete adsorption and desorption ability, which not only facilitates high removal aptitude but also produces less solid waste than other conventional adsorbents. Additionally, fluorescent 2-bromo-2-methyl-propionic acid (abbreviated as EtOxPY)-silk nanofibers can facilitate to illustrate a clear adsorption and desorption mechanism. Therefore, the above-prescribed results make electrospun silk nanofibers a suitable choice for removing anionic dyes in real-time applications.

Immobilization of Pt Nanoparticles via Rapid and Reusable Electropolymerization of Dopamine on TiO2 Nanotube Arrays for Reversible SERS Substrates and Nonenzymatic Glucose Sensors.

Inspired by mussel-adhesion phenomena in nature, polydopamine (PDA) coatings are a promising route to multifunctional platforms for decorating various materials. The typical self-polymerization process of dopamine is time-consuming and the coatings of PDA are not reusable. Herein, a reusable and time-saving strategy for the electrochemical polymerization of dopamine (EPD) is reported. The PDA layer is deposited on vertically aligned TiO2 nanotube arrays (NTAs). Owing to the abundant catechol and amine groups in the PDA layer, uniform Pt nanoparticles (NPs) are deposited onto the TiO2 NTAs and can effectively prevent the recombination of electron-hole pairs generated from photo-electrocatalysis and transfer the captured electrons to participate in the photo-electrocatalytic reaction process. Compared with pristine TiO2 NTAs, the as-prepared Pt@TiO2 NTA composites exhibit surface-enhanced Raman scattering sensitivity for detecting rhodamine 6G and display excellent UV-assisted self-cleaning ability, and also show promise as a nonenzymatic glucose biosensor. Furthermore, the mussel-inspired electropolymerization strategy and the fast EPD-reduced nanoparticle decorating process presented herein can be readily extended to various functional substrates, such as conductive glass, metallic oxides, and semiconductors. It is the adaptation of the established PDA system for a selective, robust, and generalizable sensing system that is the emphasis of this work.

A Review of Structure Construction of Silk Fibroin Biomaterials from Single Structures to Multi-Level Structures.

The biological performance of artificial biomaterials is closely related to their structure characteristics. Cell adhesion, migration, proliferation, and differentiation are all strongly affected by the different scale structures of biomaterials. Silk fibroin (SF), extracted mainly from silkworms, has become a popular biomaterial due to its excellent biocompatibility, exceptional mechanical properties, tunable degradation, ease of processing, and sufficient supply. As a material with excellent processability, SF can be processed into various forms with different structures, including particulate, fiber, film, and three-dimensional (3D) porous scaffolds. This review discusses and summarizes the various constructions of SF-based materials, from single structures to multi-level structures, and their applications. In combination with single structures, new techniques for creating special multi-level structures of SF-based materials, such as micropatterning and 3D-printing, are also briefly addressed.

Structuring and Shaping of Mechanically Robust and Functional Hydrogels toward Wearable and Implantable Applications.

Hydrogels possess unique features such as softness, wetness, responsiveness, and biocompatibility, making them highly suitable for biointegrated applications that have close interactions with living organisms. However, conventional man-made hydrogels are usually soft and brittle, making them inferior to the mechanically robust biological hydrogels. To ensure reliable and durable operation of biointegrated wearable and implantable devices, mechanical matching and shape adaptivity of hydrogels to tissues and organs are essential. Recent advances in polymer science and processing technologies have enabled mechanical engineering and shaping of hydrogels for various biointegrated applications. In this review, polymer network structuring strategies at micro/nanoscales for toughening hydrogels are summarized, and representative mechanical functionalities that exist in biological materials but are not easily achieved in synthetic hydrogels are further discussed. Three categories of processing technologies, namely, 3D printing, spinning, and coating for fabrication of tough hydrogel constructs with complex shapes are reviewed, and the corresponding hydrogel toughening strategies are also highlighted. These developments enable adaptive fabrication of mechanically robust and functional hydrogel devices, and promote application of hydrogels in the fields of biomedical engineering, bioelectronics, and soft robotics.

PLCL-TPU bi-layered artificial blood vessel with compliance matching to host vessel.

Compliance mismatch between the artificial blood vessel and the host vessel leads to abnormal hemodynamics and is a major mechanical trigger of intimal hyperplasia. Efforts have been made to achieve higher compliance of artificial blood vessels. However, the preparation of artificial blood vessels with compliance matching to host vessels has not been realized. A bi-layered artificial blood vessel was successfully prepared by dip-coating and electrospinning composite method using poly(L-Lactide-co-caprolactone) (PLCL) and thermoplastic poly(ether urethane) (TPU). In the case of a certain wall thickness (200 µm), thickness ratios of the PLCL inner layer (dip-coating method) and TPU outer layer (electrospinning method) were controlled at 0:1, 1:9, 3:7, 5:5, 7:3, and 1:0 respectively and the compliance, radial tensile properties, burst pressure, and suture retention strength were investigated. Results showed compliance value of the artificial blood vessel decreased with the increase of the thickness ratio, which suggested the compliance of the bi-layered artificial blood vessel can be regulated by adjusting the ratio of the inner and outer layer thicknesses. In the six different artificial blood vessels, the one with thickness ratio of 1:9 not only had high compliance (8.768 ± 0.393%/100 mmHg) but also can guarantee the other mechanical properties, such as the radial breaking strength (6.333 ± 0.689 N/mm), burst pressure (534.473 ± 20.899 mmHg), and suture retention strength (300.773 ± 9.351 cN). The proposed artificial blood vessel preparation method is expected to achieve compliance matching with the host vessel. It is beneficial for eliminating abnormal hemodynamics and reducing intimal hyperplasia.

Pseudotripoconidium, a new anamorph genus connected to Orbilia.

A new anamorphic fungus is described based on four isolates from ascospores of Orbilia aff. luteorubella. This fungus differs from previously known Orbilia anamorphs in producing inversely pyramidal, unicellular conidia with several protuberances at their distal end. Conidia produce 1-7 prominent denticles that emerge from a node at the conidiophore apex. Conidiogenesis is holoblastic. Because phylogenetic analysis indicated greater than 90% ITS sequence similarities among the four isolates they are treated here as a single species. In the sequence analysis of the internal transcribed spacer region (ITS) these isolates and other sequences identified as O. aff. luteorubella were nested within Orbilia and formed a clade with 99% bootstrap support. This clade is separated from nematode-trapping species of Orbilia. Based on both morphological and molecular analyses, we propose a new genus, Pseudotripoconidium.

Plasticizing Silk Protein for On-Skin Stretchable Electrodes.

Soft and stretchable electronic devices are important in wearable and implantable applications because of the high skin conformability. Due to the natural biocompatibility and biodegradability, silk protein is one of the ideal platforms for wearable electronic devices. However, the realization of skin-conformable electronic devices based on silk has been limited by the mechanical mismatch with skin, and the difficulty in integrating stretchable electronics. Here, silk protein is used as the substrate for soft and stretchable on-skin electronics. The original high Young's modulus (5-12 GPa) and low stretchability (<20%) are tuned into 0.1-2 MPa and > 400%, respectively. This plasticization is realized by the addition of CaCl2 and ambient hydration, whose mechanism is further investigated by molecular dynamics simulations. Moreover, highly stretchable (>100%) electrodes are obtained by the thin-film metallization and the formation of wrinkled structures after ambient hydration. Finally, the plasticized silk electrodes, with the high electrical performance and skin conformability, achieve on-skin electrophysiological recording comparable to that by commercial gel electrodes. The proposed skin-conformable electronics based on biomaterials will pave the way for the harmonized integration of electronics into human.

Recent advances on smart TiO2 nanotube platforms for sustainable drug delivery applications.

To address the limitations of traditional drug delivery, TiO2 nanotubes (TNTs) are recognized as a promising material for localized drug delivery systems. With regard to the excellent biocompatibility and physicochemical properties, TNTs prepared by a facile electrochemical anodizing process have been used to fabricate new drug-releasing implants for localized drug delivery. This review discusses the development of TNTs applied in localized drug delivery systems, focusing on several approaches to control drug release, including the regulation of the dimensions of TNTs, modification of internal chemical characteristics, adjusting pore openings by biopolymer coatings, and employing polymeric micelles as drug nanocarriers. Furthermore, rational strategies on external conditions-triggered stimuli-responsive drug release for localized drug delivery systems are highlighted. Finally, the review concludes with the recent advances on TNTs for controlled drug delivery and corresponding prospects in the future.

TiO2 nanotube platforms for smart drug delivery: a review.

Titania nanotube (TNT) arrays are recognized as promising materials for localized drug delivery implants because of their excellent properties and facile preparation process. This review highlights the concept of localized drug delivery systems based on TNTs, considering their outstanding biocompatibility in a series of ex vivo and in vivo studies. Considering the safety of TNT implants in the host body, studies of the biocompatibility present significant importance for the clinical application of TNT implants. Toward smart TNT platforms for sustainable drug delivery, several advanced approaches were presented in this review, including controlled release triggered by temperature, light, radiofrequency magnetism, and ultrasonic stimulation. Moreover, TNT implants used in medical therapy have been demonstrated by various examples including dentistry, orthopedic implants, cardiovascular stents, and so on. Finally, a future perspective of TNTs for clinical applications is provided.

Tuning the surface microstructure of titanate coatings on titanium implants for enhancing bioactivity of implants.

Biological performance of artificial implant materials is closely related to their surface characteristics, such as microtopography, and composition. Therefore, convenient fabrication of artificial implant materials with a cell-friendly surface structure and suitable composition was of great significance for current tissue engineering. In this work, titanate materials with a nanotubular structure were successfully fabricated through a simple chemical treatment. Immersion test in a simulated body fluid and in vitro cell culture were used to evaluate the biological performance of the treated samples. The results demonstrate that the titanate layer with a nanotubular structure on Ti substrates can promote the apatite-inducing ability remarkably and greatly enhance cellular responses. This highlights the potential of such titanate biomaterials with the special nanoscale structure and effective surface composition for biomedical applications such as bone implants.

Bioinspired porous octacalcium phosphate/silk fibroin composite coating materials prepared by electrochemical deposition.

The biomimetic structure and composition of biomaterials are recognized as critical factors that determine their biological performance. A bioinspired nano-micro structured octacalcium phosphate (OCP)/silk fibroin (SF) composite coating on titanium was achieved through a mild electrochemically induced deposition method. Findings indicate that SF plays a critical role in constructing the unique biomimetic hierarchical structure of OCP/SF composite coating layers. In vitro cell culture tests demonstrate that the presence of OCP/SF composite coatings, with highly ordered and hierarchically porous structure, greatly enhance cellular responses. The coatings developed in this study have considerable potential for various hard tissue engineering and applications.

Highly flexible and lightweight organic solar cells on biocompatible silk fibroin.

Organic electronics have gained widespread attention due to their flexibility, lightness, and low-cost potential. It is attractive due to the possibility of large-scale roll-to-roll processing. However, organic electronics require additional development before they can be made commercially available and fully integrated into everyday life. To achieve feasibility for commercial use, these devices must be biocompatible and flexible while maintaining high performance. In this study, biocompatible silk fibroin (SF) was integrated with a mesh of silver nanowires (AgNWs) to build up flexible organic solar cells with maximum power conversion efficiency of up to 6.62%. The AgNW/SF substrate exhibits a conductivity of ∼11.0 Ω/sq and transmittance of ∼80% in the visible light range. These substrates retained their conductivity, even after being bent and unbent 200 times; this surprising ability was attributed to its embedded structure and the properties of the specific SF materials used. To contrast, indium tin oxide on synthetic plastic substrate lost its conductivity after the much less rigid bending. These lightweight and silk-based organic solar cells pave the way for future biocompatible interfaces between wearable electronics and human skin.