Hydrogel Probe Research Articles

Controllable Preparation of a Cu NCs@Zn-MOF Hybrid with Dual Emission Induced by an Ion Exchange Strategy for the Detection of Explosives.

The precise synthesis of Cu NCs is a highly desirable and controllable route for the preparation of desired structures and properties, which facilitates the rational design of valuable probes for fluorescence sensing and the understanding of structure-property relationships. Herein, an ion-exchange strategy combined with a bottom-up synthetic approach was utilized in the synthesis process of Cu NCs for the first time, which achieved the controllable synthesis of Cu NCs and in situ anchoring of Cu NCs on the support material HPU-14. The as-prepared Cu NCs@HPU-14-4h not only had a good peroxidase-like property but also exhibited stable dual-emitting fluorescence at 470 and 620 nm. Notably, the peroxidase-like property endowed Cu NCs@HPU-14-4h with the capability of highly sensitive colorimetric detection of H2O2 in a linear concentration from 0.1 to 140 μM (detection limit of 86.7 nM), and a change in the fluorescent color from red to blue could be observed by the naked eye. Furthermore, due to the large overlap between the absorption of 2,4,6-trinitrophenol (TNP) and the excitation band of Cu NCs@HPU-14-4h, TNP could also be detected from 27 types of analogs and common ions with a limit of detection of 68 nM. Finally, a portable hydrogel probe with efficient wipe sampling was fabricated by polyvinyl alcohol (PVA) comprising Cu NCs@HPU-14-4h with the aim of on-site visualization of different explosives. Consequently, the current study not only provides a new idea for the precise synthesis of Cu NCs and their controllable anchoring on support materials but also offers an effective method for predicting H2O2 and TNP.

Targeting tumour surface collage with hydrogel probe: a new strategy to enhance intraoperative imaging sensitivity and stability of bladder cancer.

The incomplete resection of non-muscle invasive bladder cancer (NMIBC) augments the risk of disease recurrence. Imaging-guided surgery by molecular probes represents a pivotal strategy for mitigating postoperative recurrence. Traditional optical molecular probes, primarily composed of antibodies/peptides targeting tumour cells and fluorescent groups, are challenged by the high heterogeneity of NMIBC cells, leading to inadequate probe sensitivity. We have developed a collagen-adhesive probe (CA-P) to target the collagen within the tumour microenvironment, aiming to address the issue of insufficient imaging sensitivity. The distribution characteristics of collagen in animal bladder cancer models and human bladder cancer tissues were explored. The synthesis and properties of CA-P were validated. In animal models, the imaging performance of CA-P was tested and compared with our previously reported near-infrared probe PLSWT7-DMI. The clinical translational potential of CA-P was assessed using human ex vivo bladder tissues. The distribution of collagen on the surface of tumour cells is distinct from its expression in normal urothelium. In vitro studies have demonstrated the ability of the CA-P to undergo a "sol-gel" transition upon interaction with collagen. In animal models and human ex vivo bladder specimens, CA-P exhibits superior imaging performance compared to PLSWT7-DMI. The sensitivity of this probe is 94.1%, with a specificity of 81%. CA-P demonstrates the capability to overcome tumour cell heterogeneity and enhance imaging sensitivity, exhibiting favorable imaging outcomes in preclinical models. These findings provide a theoretical basis for the application of CA-P in intraoperative navigation for NMIBC.

Bioinspired Lubricity from Surface Gel Layers.

Surface gel layers on commercially available contact lenses have been shown to reduce frictional shear stresses and mitigate damage during sliding contact with fragile epithelial cell layers in vitro. Spencer and co-workers recently demonstrated that surface gel layers could arise from oxygen-inhibited free-radical polymerization. In this study, polyacrylamide hydrogel shell probes (7.5 wt % acrylamide, 0.3 wt % N,N'-methylenebisacrylamide) were polymerized in three hemispherical molds listed in order of decreasing surface energy and increasing oxygen permeability: borosilicate glass, polyether ether ketone (PEEK), and polytetrafluoroethylene (PTFE). Hydrogel probes polymerized in PEEK and PTFE molds exhibited 100× lower elastic moduli at the surface ( = 80 ± 31 and = 106 ± 26 Pa, respectively) than those polymerized in glass molds ( = 31,560 ± 1,570 Pa), in agreement with previous investigations by Spencer and co-workers. Biotribological experiments revealed that hydrogel probes with surface gel layers reduced frictional shear stresses against cells (τPEEK = 35 ± 15 and τPTFE = 22 ± 16 Pa) more than those without (τglass = 68 ± 15 Pa) and offered greater protection against cell damage when sliding against human telomerase-immortalized corneal epithelial (hTCEpi) cell monolayers. Our work demonstrates that the "mold effect" resulting in oxygen-inhibition polymerization creates hydrogels with surface gel layers that reduce shear stresses in sliding contact with cell monolayers, similar to the protection offered by gradient mucin gel networks across epithelial cell layers.

Multifunctional hydrogels simultaneously featuring ultrahigh stretchability, remarkable tearing resistance, and reusable fluorescence for information encoding–decoding and smart anticounterfeiting

Fluorescent hydrogels with fluorescent dyes are widely used for anti-counterfeiting encryption. However, developing highly stretchable and remarkable tear-resistant hydrogels with reusable fluorescence for anti-counterfeiting purposes remains challenging. In this study, we fabricated and characterized double network (DN) hydrogels comprising polyvinyl alcohol-borax (PVA-borax) as the first network and poly(methacrylamide-co-polyethylene glycol-co-pyrenylmethyl acrylate) (P(MAM-co-PEGMA-co-PyMA)) as the second network with varying MAM to PEGMA ratios. SEM images showed the hydrogels had 3D porous structures. FT-IR and thermal properties analysis (DSC and TGA) indicated the presence of hydrogen bonds between PVA-borax and P(MAM-co-PEGMA-co-PyMA) without any chemical bonds. The red shift in characteristic absorption bands at 841 and 710 cm−1 further confirmed the presence of π-π* interactions between pyrene moieties. XRD analysis revealed no significant changes in crystalline phase of the hydrogels, which facilitated the formation of a 3D network due to abundant hydrogen bond presence. When the MAM to PEGMA ratio was adjusted to 9:2, the resulting hydrogels exhibited remarkable properties such as ultra-high stretchability (strain over 3300 %), excellent notch-insensitivity, and exceptional tear resistance (tearing energy over 3.25 × 105 J/m2). Importantly, the hydrogel's fluorescence intensity could be reversibly changed by alternatively adding Fe3+ and EDTA-2Na. It could be reused more than 10 times while maintaining a fluorescence intensity of around 80 %, demonstrating its reliability as a versatile hydrogel probe for Fe3+ detection with “ON-OFF-ON” fluorescence behavior. Furthermore, the hydrogels demonstrated exceptional 2D encryption and decryption capabilities, highlighting their potential applications in information storage and data security. To improve the level of anti-counterfeiting, multiple encryption approaches such as QR codes and ASCII binary codes were rationally designed. Overall, this study successfully developed a universal DN hydrogel platform with ultra-high stretchability and remarkable tear resistance, capable of rapid encoding and decoding of complex information for smart anti-counterfeiting.

Fabrication of 1,8-naphthalimide modified cellulose derivative composite fluorescent hydrogel probes and their application in the detection of Cr(VI)

The design and development of a rapid and quantitative method for the detection of heavy metal ions is of great importance for environmental protection. We have prepared a 1,8-Naphthalimide modified cellulose composite fluorescent hydrogel (CENAEA/PAA) with a stereo double network structure. Characterized by excellent hydrogel functional structure and fluorescence detection performance, it can efficiently and selectively identify and detect Cr(VI) with linear quenching in the range of 0–400 μmol/L and detection limit of 0.58 μmol/L for Cr(VI). The results show that the CENAEA/PAA can effectively adsorb Cr(VI) with a maximum adsorption capacity of 189.04 mg/g. Finally, the morphological characteristics, chemical structure, fluorescence properties and adsorption behavior of CENAEA/PAA were analyzed and fitted well with the pseudo-second-order model and Freundlich model. Thus, the present work provides a green and sustainable approach for the synthesis of a functional material that can be used for the detection and adsorption of heavy metal ions.

Aggregation-Induced Emission Luminogen-Encapsulated Fluorescent Hydrogels Enable Rapid and Sensitive Quantitative Detection of Mercury Ions.

Hg2+ contamination in sewage can accumulate in the human body through the food chains and cause health problems. Herein, a novel aggregation-induced emission luminogen (AIEgen)-encapsulated hydrogel probe for ultrasensitive detection of Hg2+ was developed by integrating hydrophobic AIEgens into hydrophilic hydrogels. The working mechanism of the multi-fluorophore AIEgens (TPE-RB) is based on the dark through-bond energy transfer strategy, by which the energy of the dark tetraphenylethene (TPE) derivative is completely transferred to the rhodamine-B derivative (RB), thus resulting in intense photoluminescent intensity. The spatial networks of the supporting hydrogels further provide fixing sites for the hydrophobic AIEgens to enlarge accessible reaction surface for hydrosoluble Hg2+, as well create a confined reaction space to facilitate the interaction between the AIEgens and the Hg2+. In addition, the abundant hydrogen bonds of hydrogels further promote the Hg2+ adsorption, which significantly improves the sensitivity. The integrated TPE-RB-encapsulated hydrogels (TR hydrogels) present excellent specificity, accuracy and precision in Hg2+ detection in real-world water samples, with a 4-fold higher sensitivity compared to that of pure AIEgen probes. The as-developed TR hydrogel-based chemosensor holds promising potential as a robust, fast and effective bifunctional platform for the sensitive detection of Hg2+.

Rapid skin biomarker discovery using hydrogel-phase sampling followed by semi-automated liquid-phase re-extraction high-resolution mass spectrometry

A facile and rapid skin metabolomics protocol is proposed. The liquid microjunction-surface sampling probe system has been partly automated, and used in conjunction with hydrogel probes for skin metabolite analysis. A control device was built to precisely control the segmented solvent flow and analyte re-extraction into the liquid microjunction. This mode provides rapid online re-extraction of the analytes from hydrogel probes. Humectant was added to the hydrogel, and moist heat treatment was used to make the hydrogel probes rugged for sampling in the clinical setting. The developed method was validated for the analysis of choline – a putative biomarker of psoriasis. A linear relationship over six calibration levels from 3.18 × 10−5 to 3.18 × 10−4 mol m−2 has been obtained. The limit of detection was 6.6 × 10−6 mol m−2, while the recoveries range from 92 to 109%. The within-run and between-run precision were evaluated and the coefficients of variation range from 1.84 to 7.13%. Furthermore, the developed method has been used to screen patients (n = 10) and healthy participants (control group; n = 10) for psoriasis-related skin metabolites. Metabolomic profiling of the skin excretion-related signals identified potential biomarkers of psoriasis: choline, pipecolic acid, ornithine, urocanic acid, and methionine.

In vitro models of soft tissue damage by implant-associated frictional shear stresses.

Silicone elastomer medical implants are ubiquitous in medicine, particularly for breast augmentation. However, when these devices are placed within the body, disruption of the natural biological interfaces occurs, which significantly changes the native energy-dissipation mechanisms of living systems. These new interfaces can introduce non-physiological contact pressures and tribological conditions that provoke inflammation and soft tissue damage. Despite their significance, the biotribological properties of implant-tissue and implant-extracellular matrix (ECM) interfaces remain poorly understood. Here, we developed an in vitro model of soft tissue damage using a custom-built in situ biotribometer mounted onto a confocal microscope. Sections of commercially-available silicone breast implants with distinct and clinically relevant surface roughness (Ra = 0.2 ± 0.03 μm, 2.7 ± 0.6 μm, and 32 ± 7.0 μm) were mounted to spherically-capped hydrogel probes and slid against collagen-coated hydrogel surfaces as well as healthy breast epithelial (MCF10A) cell monolayers to model implant-ECM and implant-tissue interfaces. In contrast to the "smooth" silicone implants (Ra < 10 μm), we demonstrate that the "microtextured" silicone implant (10 < Ra < 50 μm) induced higher frictional shear stress (τ > 100 Pa), which led to greater collagen removal and cell rupture/delamination. Our studies may provide insights into post-implantation tribological interactions between silicone breast implants and soft tissues.

Facile method to synthesize fluorescent chitosan hydrogels for selective detection and adsorption of Hg2+/Hg+

Fluorescent chitosan-based hydrogel for the selective detection and adsorption of Hg2+/Hg+ in aqueous environment was prepared through three-step synthesis strategy. NO2-Boron-dipyrrolemethene (BODIPY) was prepared firstly, and then the -NO2 group was reduced to -NH2 group. Finally, the NH2-BODIPY was introduced to chitosan by Schiff base formation reaction through bi-aldehyde. Eventually, fluorescent chitosan hydrogel was obtained. The as-prepared fluorescent hydrogel probe could detect Hg2+/Hg+ through PET mechanism with the detection limit of 0.3 μM. The recognition site which combines Hg2+/Hg+ is CN, it is just formed in the reaction with chitosan and the amino group on BODIPY. Adsorption capacity of the fluorescent hydrogel is 121 mg·g−1, which is almost seven times of the original chitosan. The isotherm and kinetics of Hg2+/Hg+ removal follows Langmuir isotherm and pseudo-second order kinetics, respectively. Besides, a series of fluorescent hydrogels were prepared to compare the elasticity, hydropHilicity, fluorescence intensity and adsorption capacity.

A Pre-Gelled EEG Electrode and Its Application in SSVEP-Based BCI.

Electroencephalogram (EEG) electrodes are critical devices for brain-computer interface and neurofeedback. A pre-gelled (PreG) electrode was developed in this paper for EEG signal acquisition with a short installation time and good comfort. A hydrogel probe was placed in advance on the Ag/AgCl electrode before wearing the EEG headband instead of a time-consuming gel injection after wearing the headband. The impedance characteristics were compared between the PreG electrode and the wet electrode. The PreG electrode and the wet electrode performed the Brain-Computer Interface (BCI) application experiment to evaluate their performance. The average impedance of the PreG electrode can be decreased to 43 [Formula: see text] or even lower, which is higher than the wet electrode with an impedance of 8 [Formula: see text]. However, there is no significant difference in classification accuracy and information transmission rate (ITR) between the PreG electrode and the wet electrode in a 40 target BCI system based on Steady State Visually Evoked Potential (SSVEP). This study validated the efficiency of the proposed PreG electrode in the SSVEP-based BCI. The proposed PreG electrode will be an excellent substitute for wet electrodes in an actual application with convenience and good comfort.

A tough fluorescent nanocomposite hydrogel probe based on graphene quantum dots for the selective detection of Fe3+ ions

A tough fluorescent nanocomposite hydrogel probe crosslinked by graphene quantum dots for the selective detection of Fe3+ ions.

Hydrothermal synthesis of nanocellulose-based fluorescent hydrogel for mercury ion detection

Cellulose nanofibers (CNF) possess excellent hydrophilicity, biocompatibility, high specific surface area and biodegradability, and the application of CNF to fluorescent hydrogels is one of the hotspots in the field of functional hydrogels. However, the rapid and efficient preparation of them remains a challenge, and it is necessary to explore its application in the detection of heavy metal ions. In this study, a hydrothermal method was adopted to investigate the one-pot synthesis of CNF-based fluorescent hydrogel (CFH) for mercury ion detection, which synchronously enabled CFH formation and in-situ carbon quantum dots synthesis. The as-prepared CFH had a complete 3D network structure, and epichlorohydrin showed positive effects on the mechanical properties of CFH. Moreover, excellent fluorescence performance can be achieved through regulating the synthesis process of carbon quantum dots. The as-prepared CFH showed different quenching effects in the Hg2+ solution with different concentrations, and the fluorescence intensity of CFH was closely related to the Hg2+ concentration in the range of 0–300 mmol/L, which showed great development potential and prospects in the fields of fluorescence probes on Hg2+ sensing and detection. This study provided a promising method for the rapid preparation of biocompatible and environment-friendly fluorescent hydrogel probes and ion detection materials.

Photothermal-Induced Electrochemical Interfacial Region Regulation Enables Signal Amplification for Dual-Mode Detection of Ovarian Cancer Biomarkers.

Detection sensitivity of an electrochemical immunosensor mainly depends on the accessible distance toward the sensing interface; regulating the electrochemical interfacial region thereon is an effective strategy for signal amplification. Herein, a photothermal-regulated sensing interface was designed based on a near-infrared (NIR)-responsive hydrogel probe for ultrasensitive detection of human epididymis protein 4 (HE4). Silver nanoparticle-deposited graphene oxide nanosheet (AgNPs@GO) hybrids as electrochemical signal tags and a photothermal transducer, which were encapsulated in the poly(N-isopropylacrylamide) (pNIPAM) hydrogel, were used to develop the NIR-responsive GO@AgNPs-pNIPAM hydrogel probe. Under NIR light irradiation, the excellent photothermal effect of AgNPs@GO hybrids not only rapidly converted NIR light into heat for temperature readout but also triggered the shrinkage behavior of the hydrogel for electrochemical signal amplification. Compared with the conventional sandwich immunoassay, the shrinkage behavior of the hydrogel signal probe endowed itself with interface regulation capability to improve the electrochemical reaction efficiency; on the basis of ensuring the extended outer Helmholtz plane (OHP) region, the proposed photothermal-induced interface regulation also shortened the OHP, leading to higher sensitivity. Moreover, the obtained dual-mode signals provided satisfactory accuracy for the detection of tumor markers. Therefore, this detection scheme provided an opportunity for the broad applications of the photothermal effect in clinical diagnosis.

Rational shaping of hydrogel by electrodeposition under fluid mechanics for electrochemical writing on complex shaped surfaces at microscale

• “Electrodeposition + Pulling” is proposed for processing and shaping hydrogel. • The process synergistically combines electrochemistry with fluid mechanics. • Rational control relies on electrodeposition kinetics and meniscus evolution. • Sharp hydrogel probes of width < 1 µm are obtained for local electrochemistry. • Electrochemical writing on complex 3D structures is achieved at tunable resolution. The precise control of hydrogel shaping at high resolution is an intrinsic engineering challenge due to the low solid content of the material. Most of the approaches are based on lithographic mold, which becomes tricky to demold when the precision rises to micron and sub-micron range. In this work, a novel automated “electrodeposition + pulling” approach for rationally shaping chitosan hydrogel in 3D is reported. Taking advantage of the transient meniscus generated while pulling a sharpened metal wire out from a viscous solution, the process confines the electrodeposition of hydrogel simultaneously in it. Considering that the electrodeposition of hydrogel is driven by electrochemically generated OH − ions, the reaction engineering rationally and synergistically combines the mass transport of OH − ions, the gelification and the fluid mechanics in a dynamic process. With automation and mastering the process, the shape of hydrogel can be tuned, and it can be sharpened to below 1 µm at the tip with a desired length. Thus, it is demonstrated for electrochemical writing on 3D printed complex shaped surfaces. The sharpened hydrogel is in soft contact with the sample, allowing electrochemical deposition or etching reactions to be spatially localized in the contact area. By precisely pressing or stretching the hydrogel, the resolution can be tuned from a few to tens of microns just like traditional ink brushes, which may significantly improve the efficiency of writing. The work shows the power of electrochemical reaction engineering towards spatial control in 3D at micro and nano scale.

Mapping cellular-scale internal mechanics in 3D tissues with thermally responsive hydrogel probes

Local tissue mechanics play a critical role in cell function, but measuring these properties at cellular length scales in living 3D tissues can present considerable challenges. Here we present thermoresponsive, smart material microgels that can be dispersed or injected into tissues and optically assayed to measure residual tissue elasticity after creep over several weeks. We first develop and characterize the sensors, and demonstrate that internal mechanical profiles of live multicellular spheroids can be mapped at high resolutions to reveal broad ranges of rigidity within the tissues, which vary with subtle differences in spheroid aggregation method. We then show that small sites of unexpectedly high rigidity develop in invasive breast cancer spheroids, and in an in vivo mouse model of breast cancer progression. These focal sites of increased intratumoral rigidity suggest new possibilities for how early mechanical cues that drive cancer cells towards invasion might arise within the evolving tumor microenvironment.

Friction-Induced Inflammation

Friction-induced inflammation is a new hypothesis that implicates interfacial shear stress as a trigger for the production of pro-inflammatory signals, which in severe cases may lead to chronic inflammation and pain. If frictional shear stresses at the interface exceed physiological norms, a likely cellular response may involve the release of pro-inflammatory signals (e.g., proteins, cytokines, chemokines, and enzymes). Ocular lubricity and comfort are critically dependent on the stability of the tear film and the health of the corneal and conjunctival epithelium. The insertion of a contact lens may increase contact pressures and shear stresses on the epithelia, but these are difficult to measure in vivo. Epithelial cells are known to sense and respond to mechanical strains and deformations through a process called mechanotransduction. The effects of frictional shear stress on cellular responses were experimentally measured in vitro by sliding soft, spherical shell hydrogel probes against human corneal epithelial (hTCEpi) cell monolayers with two different normal forces: 500 and 1000 µN, giving ~ 30 and ~ 60 Pa shear stresses, respectively. Molecular biology assays (quantitative reverse transcription—polymerase chain reaction, RT-qPCR, and enzyme-linked immunosorbent assay, ELISA) followed friction experiments. Compared to control populations, RT-qPCR revealed frictional shear stresses of 60 Pa were sufficient to increase gene expression of the pro-inflammatory genes Interleukin-1β (IL-1β), Interleukin-6 (IL-6), Matrix Metalloproteinase 9 (MMP9), and pro-apoptotic genes DNA Damage-Inducible Transcript 3 (DDIT3) and FAS Cell Surface Death Receptor (FAS). An ELISA of growth media sampled after sliding revealed IL-6 cytokine release increased by 100% following shear stress experiments. These results suggest that frictional shear stress may be at least partly responsible for inducing inflammatory responses in corneal epithelial cells in vitro.

Polymeric lithography editor: Editing lithographic errors with nanoporous polymeric probes.

A new lithographic editing system with an ability to erase and rectify errors in microscale with real-time optical feedback is demonstrated. The erasing probe is a conically shaped hydrogel (tip size, ca. 500 nm) template-synthesized from track-etched conical glass wafers. The "nanosponge" hydrogel probe "erases" patterns by hydrating and absorbing molecules into a porous hydrogel matrix via diffusion analogous to a wet sponge. The presence of an interfacial liquid water layer between the hydrogel tip and the substrate during erasing enables frictionless, uninterrupted translation of the eraser on the substrate. The erasing capacity of the hydrogel is extremely high because of the large free volume of the hydrogel matrix. The fast frictionless translocation and interfacial hydration resulted in an extremely high erasing rate (~785 μm2/s), which is two to three orders of magnitude higher in comparison with the atomic force microscopy-based erasing (~0.1 μm2/s) experiments. The high precision and accuracy of the polymeric lithography editor (PLE) system stemmed from coupling piezoelectric actuators to an inverted optical microscope. Subsequently after erasing the patterns using agarose erasers, a polydimethylsiloxane probe fabricated from the same conical track-etched template was used to precisely redeposit molecules of interest at the erased spots. PLE also provides a continuous optical feedback throughout the entire molecular editing process-writing, erasing, and rewriting. To demonstrate its potential in device fabrication, we used PLE to electrochemically erase metallic copper thin film, forming an interdigitated array of microelectrodes for the fabrication of a functional microphotodetector device. High-throughput dot and line erasing, writing with the conical "wet nanosponge," and continuous optical feedback make PLE complementary to the existing catalog of nanolithographic/microlithographic and three-dimensional printing techniques. This new PLE technique will potentially open up many new and exciting avenues in lithography, which remain unexplored due to the inherent limitations in error rectification capabilities of the existing lithographic techniques.

Spherically capped membrane probes for low contact pressure tribology

Low contact pressure measurements are needed for biotribology studies on cells, cell layers, and tissues. Such studies typically require low forces to achieve kPa range contact pressures, but such methods frequently come at the expense of contact area and, in turn, relevance. In seeking lower contact pressures, the corresponding contact areas can become too small to be physiologically relevant or important. The recently developed method creates probes that are thin spherical shells, specifically designed to create low contact pressures. These polyethylene glycol and polyacrylamide hydrogel probes were polymerized with embedded fluorescent nanoparticles, and indentation experiments were performed in situ on a confocal microscope to determine the deformation mechanics. The indentation load versus contact width behavior revealed that this design has the ability to achieve pressures in the kPa range at macroscopic contact areas that are independent of the applied load (i.e., the area grows linearly with the applied load, leading to a constant contact pressure).

Corneal cell friction: Survival, lubricity, tear films, and mucin production over extended duration in vitro studies

The tear film is a thin, aqueous, mucin-rich layer on the ocular surface that provides hydration and lubrication for healthy vision. The ability of the tear film to provide a highly lubricious interface during ocular movement is largely attributed to its entangled network of mucins secreted from the corneal and conjunctival epithelia. However, the extent to which these mucin networks can provide lubricity and protect the epithelia over extended durations of contact lens interactions is unknown. In vitro tribological experiments were performed against a monolayer of mucin-producing human corneal epithelial cells (hTCEpi) for 10,000 reciprocating cycles at physiologically-relevant contact pressures and deliberately low and tribologically-challenging sliding speeds. The use of a polyacrylamide hydrogel probe with a spherically-capped shell geometry enabled average normal forces of FN ~200μN and contact pressures on the order of 1kPa, resulting in an average friction coefficient of μ=0.058±0.008 over 10,000 reciprocating cycles. Cell survival after extended duration tribological experimentation was approximately 99.8%. Mucin was observed to accumulate during the experiment. From these in vitro studies, we postulate that mucin production may be a cellular process driven in part by frictional shear stress.

Multifunctional hydrogel nano-probes for atomic force microscopy.

Since the invention of the atomic force microscope (AFM) three decades ago, there have been numerous advances in its measurement capabilities. Curiously, throughout these developments, the fundamental nature of the force-sensing probe—the key actuating element—has remained largely unchanged. It is produced by long-established microfabrication etching strategies and typically composed of silicon-based materials. Here, we report a new class of photopolymerizable hydrogel nano-probes that are produced by bottom-up fabrication with compressible replica moulding. The hydrogel probes demonstrate excellent capabilities for AFM imaging and force measurement applications while enabling programmable, multifunctional capabilities based on compositionally adjustable mechanical properties and facile encapsulation of various nanomaterials. Taken together, the simple, fast and affordable manufacturing route and multifunctional capabilities of hydrogel AFM nano-probes highlight the potential of soft matter mechanical transducers in nanotechnology applications. The fabrication scheme can also be readily utilized to prepare hydrogel cantilevers, including in parallel arrays, for nanomechanical sensor devices.