Biomimetic Non-ergodic Aging by Dynamic-to-covalent Transitions in Physical Hydrogels.

Hydrogels are soft materials engineered to suit a multitude of applications that exploit their tunable mechanochemical properties. Dynamic hydrogels employing noncovalent, physically cross-linked networks dominated by either enthalpic or entropic interactions enable unique rheological and stimuli-responsive characteristics. In contrast to enthalpy-driven interactions that soften with increasing temperature, entropic interactions result in largely temperature-independent mechanical properties. By engineering interfacial polymer-particle interactions, we can induce a dynamic-to-covalent transition in entropic hydrogels that leads to biomimetic non-ergodic aging in the microstructure without altering the network mesh size. This transition is tuned by varying temperature and formulation conditions such as pH, which allows for multivalent tunability in properties. These hydrogels can thus be designed to exhibit either temperature-independent metastable dynamic cross-linking or time-dependent stiffening based on formulation and storage conditions, all while maintaining structural features critical for controlling mass transport, akin to many biological tissues. Such robust materials with versatile and adaptable properties can be utilized in applications such as wildfire suppression, surgical adhesives, and depot-forming injectable drug delivery systems.

AAV eluting lenses for single-step targeted expression of genetically-encoded activity sensors for in vivo microendoscopic calcium imaging.

Optical methods for studying the brain offer powerful approaches for understanding how neural activity underlies complex behavior. These methods typically rely on genetically encoded sensors and actuators to monitor and control neural activity. For microendoscopic calcium imaging, injection of a virus followed by implantation of a lens probe is required to express a calcium sensor and enable optical access to the target brain region. This two-step process poses several challenges, chief among them being the risks associated with mistargeting and/or misalignment between virus expression zone, lens probe and target brain region. Here, we engineer an adeno-associated virus (AAV)-eluting polymer coating for gradient refractive index (GRIN) lenses enabling expression of a genetically encoded calcium indicator (GCaMP) directly within the brain region of interest upon implantation of the lens. This approach requires only one surgical step and guarantees alignment between GCaMP expression and lens in the brain. Additionally, the slow virus release from these coatings increases the working time for surgical implantation, expanding the brain regions and species amenable to this approach. These enhanced capabilities should accelerate neuroscience research utilizing optical methods and advance our understanding of the neural circuit mechanisms underlying brain function and behavior in health and disease. Significance Statement: We engineered a polymer coating for gradient refractive index (GRIN) lenses that provides controlled release of adeno-associated viruses (AAVs). This technology enables expression of a genetically encoded calcium indicator (GCaMP) directly at the brain region of interest upon implantation of the lens. Compared to current methods, our coating offers two important improvements. First, it simplifies surgery by combining GCaMP expression and lens placement in one step, saving time and ensuring alignment. Second, controlled release of AAV from these coatings extends the time available for surgery, making it possible to implant lenses in deeper parts of the brain and in more species. These advances accelerate neuroscience research and deepen our understanding of how neural circuits impact both health and disease.

Continuous carbon capture in an electrochemical solid-electrolyte reactor.

Electrochemical carbon-capture technologies, with renewable electricity as the energy input, are promising for carbon management but still suffer from low capture rates, oxygen sensitivity or system complexity1-6. Here we demonstrate a continuous electrochemical carbon-capture design by coupling oxygen/water (O2/H2O) redox couple with a modular solid-electrolyte reactor7. By performing oxygen reduction reaction (ORR) and oxygen evolution reaction (OER) redox electrolysis, our device can efficiently absorb dilute carbon dioxide (CO2) molecules at the high-alkaline cathode-membrane interface to form carbonate ions, followed by a neutralization process through the proton flux from the anode to continuously output a high-purity (>99%) CO2 stream from the middle solid-electrolyte layer. No chemical inputs were needed nor side products generated during the whole carbon absorption/release process. High carbon-capture rates (440 mA cm-2, 0.137 mmolCO2 min-1 cm-2 or 86.7 kgCO2 day-1 m-2), high Faradaic efficiencies (>90% based on carbonate), high carbon-removal efficiency (>98%) in simulated flue gas and low energy consumption (starting from about 150 kJ per molCO2) were demonstrated in our carbon-capture solid-electrolyte reactor, suggesting promising practical applications.

Fluorinated Multi-Walled Carbon Nanotubes Coated Separator Mitigates Polysulfide Shuttle in Lithium-Sulfur Batteries.

Li-S batteries still suffer from two of the major challenges: polysulfide shuttle and low inherent conductivity of sulfur. Here, we report a facile way to develop a bifunctional separator coated with fluorinated multiwalled carbon nanotubes. Mild fluorination does not affect the inherent graphitic structure of carbon nanotubes as shown by transmission electron microscopy. Fluorinated carbon nanotubes show an improved capacity retention by trapping/repelling lithium polysulfides at the cathode, while simultaneously acting as the "second current collector". Moreover, reduced charge-transfer resistance and enhanced electrochemical performance at the cathode-separator interface result in a high gravimetric capacity of around 670 mAh g-1 at 4C. Unique chemical interactions between fluorine and carbon at the separator and the polysulfides, studied using DFT calculations, establish a new direction of utilizing highly electronegative fluorine moieties and absorption-based porous carbons for mitigation of polysulfide shuttle in Li-S batteries.

Symptomatic and asymptomatic infections of rotavirus, norovirus, and adenovirus among hospitalized children in Xi'an, China.

Rotavirus (RV), norovirus (NoV), and adenovirus (AdV) have been reported as the common viral pathogens of acute gastroenteritis in children. To determine the prevalence of RV, NoV, and AdV infections among hospitalized children with and without symptoms of acute gastroenteritis, fecal specimens, and data on clinical symptoms were collected from 201 children with diarrhea and 53 children without diarrhea admitted to the Xi'an Children's Hospital in Xi'an, China between March 2009 and May 2010. RV, NoV, and AdV were identified in 68.7% (138/201), 20.4% (41/201), and 5.0% (10/201), respectively, of children with diarrhea. These three viruses were also detected in 13.2% (7/53), 35.9% (19/53), and 9.4% (6/53), respectively, of children without diarrhea. Diarrheal children infected with RV alone showed the average severity score of 6.5, statistically significant higher than the average score of 5.3 in children with unidentifiable viruses. GII.3 and GII.4 were the only two NoV genotypes identified, and the GII.4 sequences were genetically close to GII.4 2006b cluster. These findings highlight the importance of NoV as a causative agent of pediatric diarrhea after RV based on the clinical and epidemiological characteristics of NoV infection, and particularly convey information of asymptomatic infections of enteric viruses in young children.