Accelerated Engineering of ELP-Based Materials through Hybrid Biomimetic-De Novo Predictive Molecular Design.

Efforts to engineer high-performance protein-based materials inspired by nature have mostly focused on altering naturally occurring sequences to confer the desired functionalities, whereas de novo design lags significantly behind and calls for unconventional innovative approaches. Here, using partially disordered elastin-like polypeptides (ELPs) as initial building blocks this work shows that de novo engineering of protein materials can be accelerated through hybrid biomimetic design, which this work achieves by integrating computational modeling, deep neural network, and recombinant DNA technology. This generalizable approach involves incorporating a series of de novo-designed sequences with α-helical conformation and genetically encoding them into biologically inspired intrinsically disordered repeating motifs. The new ELP variants maintain structural conformation and showed tunable supramolecular self-assembly out of thermal equilibrium with phase behavior in vitro. This work illustrates the effective translation of the predicted molecular designs in structural and functional materials. The proposed methodology can be applied to a broad range of partially disordered biomacromolecules and potentially pave the way toward the discovery of novel structural proteins.

Thermochromic Nanocellulose Films for Temperature-Adaptive Passive Cooling.

Energy efficiency in habitation spaces is a pivotal topic for maintaining energy sufficiency, cutting climate impact, and facilitating economic savings; thus, there is a critical need for solutions aimed at tackling this problem. One viable approach involves complementing active cooling methods with powerless or passive cooling ones. Moreover, considerable scope remains for the development of passive radiative cooling solutions based on sustainable materials. Cellulose, characterized by its abundance, renewability, and biodegradability, emerges as a promising material for this purpose due to its notable radiative cooling potential exploiting the mid-infrared (MIR) atmospheric transmission window (8-13 µm). In this work, we propose the utilization of thermochromic (TC) materials in conjunction with cellulose nanofibrils (CNF) to confer temperature-dependent adaptivity to hybrid CNF films. We employ a concept where high reflection, coupled with MIR emission in the heated state, facilitates cooling, while high visible light absorption in the cold state allows heating, thus enabling adaptive thermal regulation. CNF films were doped with black-to-leuco TC particles, and a thin silver layer was optionally applied to the films. The films exhibited a rapid transition (within 1 s) in their optical properties at ∼22 °C, becoming transparent above the transition temperature. Visible range transmittance of all samples ranged from 60 to 90%, with pronounced absorption in the 8-13 µm range. The cooling potential of the films was measured at 1-4 °C without any Ag layer and ∼10 °C with a Ag layer. In outdoor field testing, a peak cooling value of 12 °C was achieved during bright sunshine, which is comparable to a commercial solar film. A simulation model was also built based on the experimental results. The concept presented in this study extends beyond applications as standalone films but has applicability also in glass coatings. Overall, this work opens the door for a novel application opportunity for green cellulose-based materials.

Carboxymethyl Cellulose (CMC) Optical Fibers for Environment Sensing and Short-Range Optical Signal Transmission.

Optical fibers are a key component in modern photonics, where conventionally used polymer materials are derived from fossil-based resources, causing heavy greenhouse emissions and raising sustainability concerns. As a potential alternative, fibers derived from cellulose-based materials offer renewability, biocompatibility, and biodegradability. In the present work, we studied the potential of carboxymethyl cellulose (CMC) to prepare optical fibers with a core-only architecture. Wet-spun CMC hydrogel filaments were cross-linked using aluminum ions to fabricate optical fibers. The transmission spectra of fibers suggest that the light transmission window for cladding-free CMC fibers was in the range of 550-1350 nm, wherein the attenuation coefficient for CMC fibers was measured to be 1.6 dB·cm-1 at 637 nm. CMC optical fibers were successfully applied in touch sensing and respiratory rate monitoring. Finally, as a proof-of-concept, we demonstrate high-speed (150 Mbit/s) short-distance signal transmission using CMC fibers (at 1310 nm) in both air and water media. Our results establish the potential of carboxymethyl cellulose-based biocompatible optical fibers for highly demanding advanced sensor applications, such as in the biomedical domain.

Thermoresponsive Nanocellulose Films as an Optical Modulation Device: Proof-of-Concept.

Flexible optoelectronic technologies are becoming increasingly important with the advent of concepts such as smart-built environments and wearable systems, where they have found applications in displays, sensing, healthcare, and energy harvesting. Parallelly, there is also a need to make these innovations environmentally sustainable by design. In the present work, we employ nanocellulose and its excellent film-forming properties as a basis to develop a green flexible photonic device for sensing applications. Cellulose nanofibrils (CNFs) and cellulose nanocrystals (CNCs) were used as matrix materials along with a black thermochromic pigment to prepare thermoresponsive hybrid films. Optical properties of nanocellulose films such as transparency and haze were tuned by varying pigment loading. Nearly 90% transparent CNF and CNC films could be tuned to reduce the transmission to as low as 4 and 17%, respectively. However, the films regained transparency to up to 60% when heated above the thermochromic transition temperature (31 °C). The thermoresponsive behavior of the prepared films was exploited to demonstrate an all-optical modulation device. Continuous infrared light (1300 nm) was modulated by using a 660 nm visible diode laser. The laser intensity was sufficient to cause a localized thermochromic transition in the films. The laser was pulsed at 0.3 Hz and a uniform cyclic modulation depth of 0.3 dB was achieved. The demonstrated application of functional nanocellulose hybrid films as a light switch (modulator) could be harnessed in various thermally stimulated sensing systems such as temperature monitoring, energy-saving, and anti-counterfeiting.

Disposable roll-to-roll hot embossed electrophoresis chip for detection of antibiotic resistance gene mecA in bacteria.

We present a high-throughput roll-to-roll (R2R) manufacturing process for foil-based polymethyl methacrylate (PMMA) chips of excellent optical quality. These disposable, R2R hot embossed microfluidic chips are used for the identification of the antibiotic resistance gene mecA in Staphylococcus epidermidis. R2R hot embossing is an emerging manufacturing technology for polymer microfluidic devices. It is based on continuous feeding of a thermoplastic foil through a pressurized area between a heated embossing cylinder and a blank counter cylinder. Although mass fabrication of foil-based microfluidic chips and their use for biological applications were foreseen already some years ago, no such studies have been published previously.

Stimulation of human embryonic stem cell-derived cardiomyocytes on thin-film microelectrodes.

We describe successful long-term stimulation of human embryonic stem cell-derived cardiomyocyte clusters on thin-film microelectrode structures in vitro. Interdigitated electrode structures were constructed using plain titanium on glass as the electrode material. Titanium rapidly oxidizes in atmospheric conditions to produce an insulating TiO(χ) layer with high relative permittivity. Capacitive coupling to the incubation medium and to the cells adherent to the electrodes was still efficient, and the dielectric layer prevented electrolysis, allowing a wider window of possible stimulation amplitudes to be used, relative to conducting surfaces. A common hypothesis suggests that to achieve proper differentiation of electroactive cells from the stem cells electrical stimuli are also needed. Spontaneously beating cardiomyocyte clusters were seeded on the glass-electrode surfaces, and we successfully altered and resynchronized a clearly different beat interval. The new pace was reliably maintained for extended periods of several tens of minutes.

Design and fabrication of integrated solid-phase extraction-zone electrophoresis microchip.

Integrated solid-phase extraction-zone electrophoresis (SPE-ZE) device has been designed and fabricated on microchip. The structures were fabricated by using multiple layers of SU-8 polymer with a novel technique that enables easy alignment and high yield of the chips. SU-8 adhesive bonding has two major advantages: it enables bonding of high aspect ratio pillars and it results in fully SU-8 microchannels with uniform electrokinetic flow properties. The SPE-ZE device has a fluidic reservoir with 15:1 high aspect ratio pillars for bead filters that act as a SPE part in the chip structure. The separation unit is a 25 mm long electrophoresis channel starting from the outlet of SPE reservoir. Argon laser-induced fluorescence (LIF) detector was used to monitor simultaneously the SPE reservoir and the detection site at the end of the electrophoresis channel. Flow characteristics and electric field distributions were simulated with Femlab software. Fluorescein was used as the analyte for detecting the operational performance of the chip. Adsorption, bead rinsing, elution and detection were tested to verify functioning of the chip design.

Isotachophoresis of beta-blockers in a capillary and on a poly(methyl methacrylate) chip.

Analysis of the beta-blockers oxprenolol, atenolol, timolol, propranolol, metoprolol, and acebutolol in human urine by a combination of isotachophoresis (ITP) and zone electrophoresis (ZE) was investigated. Methods were developed with a conventional capillary electrophoresis (CE) apparatus and a poly(methyl methacrylate) (PMMA) microchip system. With CE the separation of oxprenolol, atenolol, timolol, and acebutolol from a standard solution containing 5 microg/mL of each compound was accomplished by performing ZE with transient ITP. The electrolyte system consisted of 10 mM sodium morpholinoethane sulfonate (pH 5.5) and 0.1% methylhydroxyethylcellulose as the leading electrolyte and 30 mM ortho-phosphoric acid (pH 2.0) as both the terminating and the ZE background electrolyte. With the microchip system the separation of oxprenolol and acebutolol from a standard solution containing 10 microg/mL of each compound was accomplished by a coupled-channel ITP-ZE device using the same leading electrolyte solution as the CE system but 5 mM glutamic acid (pH 3.4) as terminating and background electrolytes. The systems were used for analyses of patient urine samples. Water-soluble hydrophilic matrix compounds were removed from the urine samples by solid-phase extraction (SPE). Limits of quantification below 5 microg/mL could be achieved. The PMMA ITP-ZE chip has not earlier been used for analyses of any drugs from urine samples.