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The synthesis of polycyclic aromatic hydrocarbon (PAH) data allows us to quantify and gain insights into the spatiotemporal dynamics of PAH contamination in marine bays. Here, a data synthesis framework was developed to understand data-driven insights into the spatiotemporal levels, compositional profiles, and potential sources of PAHs in water and sediment of marine bays. PAHs were detected in 69 bays worldwide, with contamination hotspots located in Asian bays. PAH concentrations in pre-2000 were significantly lower than those in the 2000s and post-2010, while the dominant species in water and sediment were 2-3 ring and 4-6 ring PAHs, respectively. The composition patterns of PAHs included 2-3 ring, 3-5 ring, and 4-5 ring dominant categories, but no significant distance decay relationship was found in the composition similarity due to international energy trade. Temporal dynamic patterns of concentrations included Descending-, Ascending-, and Inverted V-type, whereas over longer time spans, the pattern is more similar to the Inverted V-type owing to the reductions in emission intensity. PAHs were derived from both petrogenic and pyrolytic sources, with combustion from both coal and petroleum being the dominant source. These data-driven discoveries provide quantitative insights into the spatiotemporal patterns in the concentration and composition of PAHs, contributing to the mitigation of PAH contamination.

Continuous monitoring of physiological signals from the human body is critical in health monitoring, disease diagnosis, and therapeutics. Despite the needs, the existing wearable medical devices rely on either bulky wired systems or battery-powered devices needing frequent recharging. Here, we introduce a wearable, self-powered, thermoelectric flexible system architecture for wireless portable monitoring of physiological signals without recharging batteries. This system harvests an exceptionally high open circuit voltage of 175-180 mV from the human body, powering the wireless wearable bioelectronics to detect electrophysiological signals on the skin continuously. The thermoelectric system shows long-term stability in performance for 7 days with stable power management. Integrating screen printing, laser micromachining, and soft packaging technologies enables a multilayered, soft, wearable device to be mounted on any body part. The demonstration of the self-sustainable wearable system for detecting electromyograms and electrocardiograms captures the potential of the platform technology to offer various opportunities for continuous monitoring of biosignals, remote health monitoring, and automated disease diagnosis.

Photocatalytic covalent organic frameworks (COFs) are typically constructed with rigid aromatic linkers for crystallinity and extended π-conjugation. However, the essential hydrophobicity of the aromatic backbone can limit their performances in water-based photocatalytic reactions. Here, we for the first time report the synthesis of hydrophilic COFs with aliphatic linkers [tartaric acid dihydrazide (TAH) and butanedioic acid dihydrazide] that can function as efficient photocatalysts for H 2 O 2 and H 2 evolution. In these hydrophilic aliphatic linkers, the specific multiple hydrogen bonding networks not only enhance crystallization but also ensure an ideal compatibility of crystallinity, hydrophilicity, and light harvesting. The resulting aliphatic linker COFs adopt an unusual ABC stacking, giving rise to approximately 0.6 nm nanopores with an improved interaction with water guests. Remarkably, both aliphatic linker-based COFs show strong visible light absorption, along with a narrow optical band gap of ∼1.9 eV. The H 2 O 2 evolution rate for TAH-COF reaches up to 6003 μmol h -1 g -1 , in the absence of sacrificial agents, surpassing the performance of all previously reported COF-based photocatalysts. Theoretical calculations reveal that the TAH linker can enhance the indirect two-electron oxygen reduction reaction for H 2 O 2 production by improving the O 2 adsorption and stabilizing the *OOH intermediate. This study opens a new avenue for constructing semiconducting COFs using nonaromatic linkers.

The development of a catalytic method for stereogenic carbon center formation holds immense significance in organic synthesis. Transition-metal-catalyzed cross-coupling reaction has been regarded as a straightforward and efficient tool for stereoselectively forging C-C bond. Nevertheless, the creation of acyclic all-carbon quaternary-containing vicinal stereocenters remains notoriously challenging within the domain of cross-coupling chemistry despite their prominence in various bioactive small molecules. Herein, we describe a palladium-catalyzed asymmetric multicomponent cross-coupling of trisubstituted alkene with aryl diazonium salts and arylboronic acids to realize the formation of tertiary-quaternary carbon centers with high regio-, distereo-, and enantioselectivity. Specifically, the precise manipulation of the stereoconfiguration of trisubstituted alkenes enables the divergent stereoselective cross-coupling reaction, thus allowing for the facile construction of all four enantiomers. Harnessing the ligand-swap strategy involving a chiral bisoxazoline and an achiral fumarate individually accelerates the enantioselective migratory insertion and reductive elimination step in the cross-coupling process, as supported by density functional theory (DFT) calculations, thus obviating the requirement for a neighboring directing group within the internal olefin skeleton.

Fundamentally suppressing Li dendrite growth is known to be critical for realizing the potential high energy density for Li-metal batteries (LMBs). Inspired by the ionic transport function of proteins, we previously discovered that utilizing natural proteins was able to stabilize the Li anode but have not demonstrated how a specific amino acid of the protein enabled the function. In this study, we decorate the separator with Leucine ( Leu ) amino acid assisted by poly(acrylic acid) (PAA) for effectively stabilizing the Li-metal anode, so as to dramatically improve the cycling performance of LMBs. The decorated separator improves electrolyte wettability and effectively suppresses Li dendrite growth. As a result, the amino acid-enabled separator prolongs the cycle life of the symmetrical Li|Li cells, exhibits higher Coulombic efficiency in the Li|Cu cells, and improves the cycling performance in LMBs with the LiFePO 4 cathode. This work is an initial study on applying a specific amino acid of proteins to enhance the performance of batteries, providing a new strategy on guiding Li + deposition, and laying an important foundation for functional separator design of high-energy-density batteries.

This study provides a systematic analysis of the transport and magnetophoretic behavior of nanoscale zerovalent iron (nZVI) particles, both bare and surface functionalized by poly(ethylene glycol) (PEG) and carboxymethyl cellulose (CMC), after undergoing a chemical reaction. Here, a simple and well-investigated chemical reaction of methyl orange (MO) degradation by nZVI was used as a model reaction system, and the sand column transport and low-gradient magnetophoretic profiles of the nanoparticles were measured before and after the reaction. The results were compared over time and analyzed in the context of extended Derjaguin-Landau-Verwey-Overbeek (DLVO) theory to understand the particle interactions involved. The colloidal stability of both bare and functionalized nZVI particles was enhanced after the reaction due to the consumption of metallic Fe content, resulting in a significant drop in their magnetic properties. As a result, they exhibited improved mobility across the sand column and a slower magnetophoretic collection rate compared to the unreacted particles. Here, the colloidal filtration theory (CFT) was employed to analyze the transport behavior of nZVI particles across the packed sand column. It has been observed that the surface properties of the reacted functionalized particles changed, possibly due to the entrapment of degraded products within the polymer adlayer. Moreover, quartz crystal microbalance with dissipation (QCM-D) measurements were performed to reveal the viscoelastic contribution of the adlayer formed by both bare and functionalized nZVI particles after the reaction on influencing their transport behavior across the sand column. Finally, we proposed the implementation of a high-gradient magnetic trap (HGMT) to reduce the transport distance of the colloidally stable CMC-nZVI, both before and after the reaction. This study sheds light on the behavioral changes of iron nanoparticles after the reaction and highlights environmental concerns regarding the presence of reacted nanoparticles.

The skin secretion of Andrias davidianus (SSAD) is a novel biological adhesive raw material under development. This material exhibits robust adhesion while maintaining the flexibility of the wound. It also has the potential for large-scale production, making it promising for practical application explore. Hence, in-depth research on methods to fine-tune SSAD properties is of great importance to promote its practical applications. Herein, we aim to enhance the adhesive and healing properties of SSAD by incorporating functional components. To achieve this goal, we selected 3,4-dihydroxy-l-phenylalanine and vaccarin as the functional components and mixed them with SSAD, resulting in a new bioadhesive, namely, a formulation termed "enhanced SSAD" (ESSAD). We found that the ESSAD exhibited superior adhesive properties, and its adhesive strength was improved compared with the SSAD. Moreover, ESSAD demonstrated a remarkable ability to promote wound healing. This study presents an SSAD-based bioadhesive formulation with enhanced properties, affirming the feasibility of developing SSAD-based adhesive materials with excellent performance and providing new evidence for the application of SSAD. This study also aims to show that SSAD can be mixed with other substances, and addition of effective components to SSAD can be studied to further adjust or improve its performance.

Single-molecule localization microscopy (SMLM) enables the visualization of cellular nanostructures in vitro with sub-20 nm resolution. While substructures can generally be imaged with SMLM, the structural understanding of the images remains elusive. To better understand the link between SMLM images and the underlying structure, we developed a Monte Carlo (MC) simulation based on experimental imaging parameters and geometric information to generate synthetic SMLM images. We chose the nuclear pore complex (NPC), a nanosized channel on the nuclear membrane which gates nucleo-cytoplasmic transport of biomolecules, as a test geometry for testing our MC model. Using the MC model to simulate SMLM images, we first optimized our clustering algorithm to separate >10 6 molecular localizations of fluorescently labeled NPC proteins into hundreds of individual NPCs in each cell. We then illustrated using our MC model to generate cellular substructures with different angles of labeling to inform our structural understanding through the SMLM images obtained.

Light has profoundly impacted modern medicine and healthcare, with numerous luminescent agents and imaging techniques currently being used to assess health and treat diseases. As an emerging concept in luminescence, aggregation-induced emission (AIE) has shown great potential in biological applications due to its advantages in terms of brightness, biocompatibility, photostability, and positive correlation with concentration. This review provides a comprehensive summary of AIE luminogens applied in imaging of biological structure and dynamic physiological processes, disease diagnosis and treatment, and detection and monitoring of specific analytes, followed by representative works. Discussions on critical issues and perspectives on future directions are also included. This review aims to stimulate the interest of researchers from different fields, including chemistry, biology, materials science, medicine, etc., thus promoting the development of AIE in the fields of life and health.

A redox-neutral copper-catalyzed cascade reaction involving alkoxyl radical-mediated ring expansion/1,4-difunctionalization of 1,3-enynes was developed, offering a straightforward approach to the tetra-substituted allenes with macrolactone, CN, and CF 3 functional groups. Remarkably, incorporation of the NH 2 group onto the 1,3-enyne moiety enabled further cyclization to give a unique scaffold containing a lactone and an indole moiety.

Circularly polarized luminescence (CPL) is attracting much interest because it can carry extensive optical information. CPL shows left- or right-handedness and can be regarded as part of high-level visual perception to supply an extra dimension of information with regard to regular light. A key to meeting the needs for practical applications is to develop the emerging field of ultra-dissymmetric CPL. Chiral liquid crystal (LC) assemblies─otherwise referred to as cholesteric liquid crystals (CLCs)─are essentially organized helical superstructures with a highly ordered one-dimensional orientation, and distinctly superior to regular helical supramolecules. CLCs can achieve a perfect equilibrium of molecular short-range interaction and long-range orientational order, enabling molecule-scale chirality on a helical pitch and observable scale. LC assembly could be an ideal strategy for amplifying chirality, making it accessible to ultra-dissymmetric CPL. Herein, we focused on some basic but important issues regarding CPL: (i) How can CPL be created from chiral dyes? (ii) Is the chirality of luminescent dyes an essential factor for the generation of CPL? That is, can all chiral dyes emit CPL and vice versa? (iii) How can CPL be transferred within intermolecular systems, and what principles of CPL transmission should be followed? Given these queries and our work, in this Perspective we discuss the generation, transmission, and modulation of CPL with chiral LC assembly, aiming to design and build up novel chiroptical materials. Recent applications of CPL-active LC microstructures in three-dimensional displays, circularly polarized lasers, and asymmetric catalysis are also discussed.

Plant bioactive metabolites such as flavonoids are usually present in glycosylated forms by the attachment of various sugar groups. In this study, a catalytically flexible and reversible glycosyltransferase (HtUGT72AS1) was cloned and characterized from Helleborus thibetanus . HtUGT72AS1 could directly accept six sugar donors (UDP-glucose/-arabinose/-galactose/-xylose/- N -acetylglucosamine/-rhamnose) to catalyze the 3-OH glycosylation of flavonols. It also catalyzed the 4' and 7-OH glycosylation of other types of flavonoids, which lacked the 3-OH group. Additionally, the HtUGT72AS1-catalyzed reaction was highly reversible when using 2-chloro-4-nitrophenyl glycosides as substrates, which could be used for one-pot or coupled production of bioactive glycosides. It is the first reported UGT for the synthesis of arabinosides and galactosides using a transglycosylation platform. Based on structural modeling and mutagenetic analysis, the mutation of Tyr377 to Ara enhanced the catalytic efficiency of HtUGT72AS1 toward UDP- N -acetylglucosamine, and the V146S mutant gained an improvement in the regioselectivity toward 7-OH of flavonoids.

Postsynthetic chemical transformation provides a powerful platform for creating heteronanostructures (HNs) with well-defined materials and interfaces that generate synergy or enhancement. However, it remains a synthetic bottleneck for the precise construction of HNs with increased degrees of complexity and more elaborate functions in a predictable manner. Herein, we define a general transformative protocol for metal phosphosulfide HNs based on tunable hexagonal Cu 1.81 S frameworks with corner-, edge- and face-controlled growth of Co 2 P domains. The region-controlled Cu 1.81 S-Co 2 P framework interfaces can serve as "kinetic barriers" in mediating the direction and rate between P and S anion exchange reactions, thus leading to a family of morphology and phase designed Cu 3 P 1- x S x -Co 2 P HNs with hollow (branched, dotted and crown), porous and core-shell architectures. This study reveals the internal transformation mechanism between metal sulfide and phosphide nanocrystals, and opens up a new way for the rational synthesis of metastable HNs that are otherwise inaccessible.

The possible magnetophoretic migration of iron oxide nanoparticles through the cellulosic matrix within a single layer of paper is challenging with its underlying mechanism remained unclear. Even with the recent advancements of theoretical understanding on magnetophoresis, mainly driven by cooperative and hydrodynamics phenomena, the contributions of these two mechanisms on possible penetration of magnetic nanoparticles through cellulosic matrix of paper have yet been proven. Here, by using iron oxide nanoparticles (IONPs), both nanospheres and nanorods, we have investigated the migration kinetics of these nanoparticles through grade 4 Whatman filter paper with a particle retention of 20-25 μm. By performing droplet tracking experiments, the real-time stained area growth of the particle droplet on the filter paper, under the influences of a grade N40 NdFeB magnet, were recorded. Our results show that the spatial and temporal expansion of the IONP stain is biased toward the magnet and such an effect is dependent on (i) particle concentration and (ii) particle shape. The kinetics data were first analyzed by treating it as a radial wicking fluid, and later the IONP distribution within the cellulosic matrix was investigated by optical microscopy. The macroscopic flow front velocities of the stained area ranged from 259 μm/s to 16 040 μm/s. Moreover, the microscopic magnetophoretic velocity of nanorod cluster was also successfully measured as ∼214 μm/s. Findings in this work have indirectly revealed the strong influence of cooperative magnetophoresis and the engineering feasibility of paper-based magnetophoretic technology by taking advantage of magnetoshape anisotropy effect of the particles.

Controlling the optical properties of metal plasma nanomaterials through structure manipulation has attracted great attention for solar steam generation. However, realizing broadband solar absorption for high-efficiency vapor generation is still challenging. In this work, a free-standing ultralight gold film/foam with a hierarchical porous microstructure and high porosity is obtained through controllably etching a designed cold-rolled (NiCoFeCr) 99 Au 1 high-entropy precursor alloy with a unique grain texture. During chemical dealloying, the high-entropy precursor went through anisotropic contraction, resulting in a larger surface area compared with that from the Cu 99 Au 1 precursor although the volume shrinkage is similar (over 85%), which is beneficial for the photothermal conversion. The low Au content also results in a special hierarchical lamellar microstructure with both micropores and nanopores within each lamella, which significantly broadens the optical absorption range and makes the optical absorption of the porous film reach 71.1-94.6% between 250 and 2500 nm. In addition, the free-standing nanoporous gold film has excellent hydrophilicity, with the contact angle reaching zero within 2.2 s. Thus, the 28 h dealloyed nanoporous gold film (NPG-28) exhibits a rapid evaporation rate of seawater under 1 kW m -2 light intensity, reaching 1.53 kg m -2 h -1 , and the photothermal conversion efficiency reaches 96.28%. This work demonstrates the enhanced noble metal gold using efficiency and solar thermal conversion efficiency by controlled anisotropic shrinkage and forming a hierarchical porous foam.

Recent advances in wearable technologies have enabled ways for people to interact with external devices, known as human-machine interfaces (HMIs). Among them, electrooculography (EOG), measured by wearable devices, is used for eye movement-enabled HMI. Most prior studies have utilized conventional gel electrodes for EOG recording. However, the gel is problematic due to skin irritation, while separate bulky electronics cause motion artifacts. Here, we introduce a low-profile, headband-type, soft wearable electronic system with embedded stretchable electrodes, and a flexible wireless circuit to detect EOG signals for persistent HMIs. The headband with dry electrodes is printed with flexible thermoplastic polyurethane. Nanomembrane electrodes are prepared by thin-film deposition and laser cutting techniques. A set of signal processing data from dry electrodes demonstrate successful real-time classification of eye motions, including blink, up, down, left, and right. Our study shows that the convolutional neural network performs exceptionally well compared to other machine learning methods, showing 98.3% accuracy with six classes: the highest performance till date in EOG classification with only four electrodes. Collectively, the real-time demonstration of continuous wireless control of a two-wheeled radio-controlled car captures the potential of the bioelectronic system and the algorithm for targeting various HMI and virtual reality applications., Competing Interests: The authors declare the following competing financial interest(s): Georgia Tech has a US patent pending technology., (© 2023 The Authors. Published by American Chemical Society.)

Recent advances in soft materials and nano-microfabrication have enabled the development of flexible wearable electronics. At the same time, printing technologies have been demonstrated to be efficient and compatible with polymeric materials for manufacturing wearable electronics. However, wearable device manufacturing still counts on a costly, complex, multistep, and error-prone cleanroom process. Here, we present fully screen-printable, skin-conformal electrodes for low-cost and scalable manufacturing of wearable electronics. The screen printing of the polyimide (PI) layer enables facile, low-cost, scalable, high-throughput manufacturing. PI mixed with poly(ethylene glycol) exhibits a shear-thinning behavior, significantly improving the printability of PI. The premixed Ag/AgCl ink is then used for conductive layer printing. The serpentine pattern of the screen-printed electrode accommodates natural deformation under stretching (30%) and bending conditions (180°), which are verified by computational and experimental studies. Real-time wireless electrocardiogram monitoring is also successfully demonstrated using the printed electrodes with a flexible printed circuit. The algorithm developed in this study can calculate accurate heart rates, respiratory rates, and heart rate variability metrics for arrhythmia detection.

Ruthenium (Ru)-based materials, as a class of efficient hydrogen evolution reaction (HER) catalysts, play an important role in hydrogen generation by electrolysis of water in an alkaline solution for clean hydrogen energy. Hybrid nanostructure (HN) materials, which include two or more components with distinct functionality, show better performance than their individual materials, since HN materials can potentially integrate their advantages and overcome the weaknesses. However, it remains a challenge to construct Ru-based HN materials with desired crystal phases for enhanced HER performances. Herein, a series of new Ru-based HN materials (t-Ru-RuS 2 , S-Ru-RuS 2 , and T-Ru-RuS 2 ) through phase engineering of nanomaterials (PEN) and chemical transformation are designed to achieve highly efficient HER properties. Owing to the plentiful formation of heterojunctions and amorphous/crystalline interfaces, the t-Ru-RuS 2 HN delivers the most outstanding overpotential of 16 mV and owns a small Tafel slope of 29 mV dec -1 at a current density of 10 mA cm -2 , which exceeds commercial Pt/C catalysts (34 mV, 38 mV dec -1 ). This work shows a new insight for HN and provides alternative opportunities in designing advanced electrocatalysts with low cost for HER in the hydrogen economy.

Amyloid protein cross-seeding is a peculiar phenomenon of cross-spreading among different diseases. Unlike traditional infectious ones, diseases caused by amyloid protein cross-seeding are spread by misfolded proteins instead of pathogens. As a consequence of the interactions among misfolded heterologous proteins or polypeptides, amyloid protein cross-seeding is considered to be the crucial cause of overlapping pathological transmission between various protein misfolding disorders (PMDs) in multiple tissues and cells. Here, we briefly review the phenomenon of cross-seeding among amyloid proteins. As an interesting example worth mentioning, the potential links between the novel coronavirus pneumonia (COVID-19) and some neurodegenerative diseases might be related to the amyloid protein cross-seeding, thus may cause an undesirable trend in the incidence of PMDs around the world. We then summarize the theoretical models as well as the experimental techniques for studying amyloid protein cross-seeding. Finally, we conclude with an outlook on the challenges and opportunities for basic research in this field. Cross-seeding of amyloid opens up a new perspective in our understanding of the process of amyloidogenesis, which is crucial for the development of new treatments for diseases. It is therefore valuable but still challenging to explore the cross-seeding system of amyloid protein as well as to reveal the structural basis and the intricate processes.

Active engineering and modulation of optical spectra in a remote and fully reversible light is urgently desired in photonics, chemistry, and materials. However, the real-time regulation of multiple optical information such as wavelength, bandwidth, reflectance, and polarization is still a longstanding issue due to the lack of an appropriate photoresponsive candidate. Herein, we propose an additional "degree-of-freedom (DOF)" in a photo-modulated soft helix, and build up an unprecedented inhomogeneous helical pitch length with light-reconfiguring property, fatigue resistance, and reversibility. For the working model, the intrinsic chiral photoswitch LBC5 is employed as an actuator to modulate the helical pitch length, which is proportional to the irradiation intensity, and the unique broadband absorbance photo-modulator BTA-C5 is incorporated as an attenuator of the transmitted light to decrease its intensity along the sample thickness, therefore successfully adding another controlled DOF on the pitch length distribution (i.e., homogeneous or inhomogeneous) apart from the common soft helix with only a single DOF on the pitch length. The absorbance photo-modulator BTA-C5 with a unique variable broadband absorption enables the light to reconfigure the helical pitch from homogeneous to inhomogeneous, thereby achieving the robust fatigue-resistance establishment of reversible spectral programming. The established light-reconfigurable inhomogeneous helical pitch with the photoresponsive modulator BTA-C5 can provide a breakthrough to control absorbance and chirality, especially for dynamically broadening and narrowing the bandwidth on demand, and further enable the ever-desired broadband NIR circularly polarized luminescence (CPL) with a high dissymmetry factor g lum of up to 1.88. The cutting-edge photoswitchable inhomogeneous soft helical pitch provides access to multi-freedom control in soft materials, optics, biophotonics, and other relevant fields.

ConspectusPhotochromic diarylethenes featuring reversible regulation by external light irradiation have attracted increasing attention in versatile applications such as logic gates, supramolecular systems, liquid crystals, and super-resolution imaging because of their outstanding bistability and fatigue resistance. However, for typical diarylethene systems, there always exist three typical unsolved issues. The first is how to modulate the bistability between the open and closed forms from the viewpoint of ethene bridge aromaticity. The second is how to decrease and avoid the photoinactive parallel conformer in order to achieve a high quantum yield, since the open form possesses the photoactive antiparallel ( ap ) conformation and the photoinactive parallel ( p ) conformation. Because of the typical rapid rotation of the flexible side aryl groups, the two conformers cannot be separated efficiently, thereby resulting in a relatively low photocyclization quantum yield. The third is how to fulfill the enantiospecific transformation with reversibility to photomodulate the chirality. Stereochemically, the ap conformer with C 2 symmetry can be further subdivided into a pair of enantiomers with P and M helicity originating from the central hexatriene moiety. Similarly, the rapid rotation can also lead to the loss of intrinsic chirality, restricting the development and application of light-driven chiroptical switches. Accordingly, it is desirable to construct a specific diarylethene system to break through these bottlenecks for real versatile applications.Our group has recently developed a unique sterically hindered diarylethene system based on benzobis(thiadiazole) as the ethene bridge for completely solving these issues. We introduce a low-aromaticity benzobis(thiadiazole) unit into the diarylethene as a central ethene bridge with incomparably high bistability. To block or freeze the rotation of flexible side aryls, we further incorporate a large bulky benzothiophene unit to induce a large steric hindrance, or rotation barrier, between the ethene bridge and side aryls, thereby successfully separating multiple conformers of the diarylethenes with high photocyclization quantum yields and enantiospecific photoreaction. Consequently, given such a fantastic building block, we enhance its performance by means of supramolecular self-assembly, thereby realizing unique conformer-dependent self-assembly as well as unprecedented concerted isomerization and enantiospecific photoreaction of photoresponsive metallacycles. In addition, decoration of the intrinsically chiral diarylethenes with mesogenic units can enable us to manipulate the helical superstructure of liquid crystals, thus achieving a multiple anticounterfeiting technique and a quadridimensional manipulable laser. We also unravel the dual aggregation-induced emission (AIE) behavior of the sterically hindered diarylethene, especially as applied in super-resolution imaging.

Increasing generation of permanent magnet waste has resulted in an urgent need to preserve finite resources. Reforming these wastes as feedstock to produce renewables is an ideal strategy for addressing waste and energy challenges. Herein, our work reports a smart and sustainable strategy to convert iron in magnet wastes into Prussian blue analogues that can serve as cathode materials for sodium-ion batteries. Moreover, a method to control feed rates is proposed to generate high-quality materials with fewer [Fe(CN) 6 ] vacancies at a feed rate of 3 mL min -1 . The recycled Na 1.46 Fe[Fe(CN) 6 ] 0.85 ·□ 0.15 shows low vacancies and excellent cycling stability over 300 cycles (89% capacity retention at 50 mA g -1 ). In operando, evidence indicates that high-quality Prussian blue allows fast sodium-ion mobility and a high degree of reversibility over the course of cycling, although with a three-phase-transition mechanism. This study opens up a future direction for magnet waste created with the expectation of being environmentally reused.

With plenty of charges and rich functional groups, bovine serum albumin (BSA) protein provides effective transport for multiple metallic ions inside blood vessels. Inspired by the unique ionic transport function, we develop a BSA protein coating to stabilize Li anode, regulate Li + transport, and resolve the Li dendrite growth for Li metal batteries (LMBs). The experimental and simulation studies demonstrate that the coating has strong interactions with Li metal, increases the wetting with electrolyte, reduces the electrolyte/Li side reactions, and significantly suppresses the Li dendrite formation. As a result, the BSA coating exhibits excellent stability in the electrolyte and improves the performance of Li|Cu and Li|Li cells as well as the LiFePO 4 |Li batteries. This work reveals that LMBs can benefit from the biological function of BSA, i.e., special transport capability of metallic ions, and lays an important foundation in design of protein-based materials for effectively enhancing the electrochemical performance of energy storage systems.

Exposure to excessive manganese (Mn) is toxic to humans and animals. However, the toxic effects and mechanisms of excessive Mn influencing the vertebrates have been highly overlooked. In the present study, dietary Mn overload significantly increased hepatic lipid and Mn contents, decreased superoxide dismutase 2 (Sod2) activity, increased the Sod2 acetylation level, and induced mitochondrial dysfunction; Mn induced mitochondrial dysfunction through Mtf1/sirtuin 3 (Sirt3)-mediated acetylation of Sod2 at the sites K55 and K70. Meanwhile, mitochondrial oxidative stress was involved in Mn-induced lipotoxicity. Mechanistically, Mn-induced lipotoxicity was via oxidative stress-induced Hsf1 nucleus translocation and its DNA binding capacity to the regions of a peroxisome proliferator-activated receptor g ( pparg ) promoter, which in turn induced the transcription of lipogenic-related target genes. For the first time, our study demonstrated that Mn-induced hepatic lipotoxicity via a mitochondrial oxidative stress-dependent Hsf1/Pparg pathway and Mtf1/ sirt3 -mediated Sod2 acetylation participated in mitochondrial dysfunction. Considering that lipid metabolism and lipotoxicity are widely used as the biomarkers for environmental assessments of pollutants, our study provided innovative and important insights into Mn toxicological and environmental evaluation in aquatic environments.

Due to many special characteristics, zinc oxide nanoparticles (ZnO NPs) are widely used all over the world, leading to their wide distribution in the environment. However, the toxicities and mechanisms of environmental ZnO NP-induced changes of physiological processes and metabolism remain largely unknown. Here, we found that addition of dietary ZnO NPs disturbed hepatic Zn metabolism, increased hepatic Zn and lipid accumulation, downregulated lipolysis, induced oxidative stress, and activated mitophagy; N , N , N ', N '-tetrakis (2-pyridylmethyl) ethylenediamine (TPEN, Zn 2+ ions chelator) alleviated high ZnO NP-induced Zn and lipid accumulation, oxidative stress, and mitophagy. Mechanistically, the suppression of mitochondrial oxidative stress attenuated ZnO NP-activated mitophagy and ZnO NP-induced lipotoxicity. Taken together, our study elucidated that mitochondrial oxidative stress mediated ZnO NP-induced mitophagy and lipotoxicity; ZnO NPs could be dissociated to free Zn 2+ ions, which partially contributed to ZnO NP-induced changes in oxidative stress, mitophagy, and lipid metabolism. Our study provides novel insights into the impacts and mechanism of ZnO NPs as harmful substances inducing lipotoxicity of aquatic organisms, and accordingly, metabolism-relevant parameters will be useful for the risk assessment of nanoparticle materials in the environment.

Incorporating non-aqueous hole-transporting materials (HTMs) to replace the widely used PEDOT:PSS is favorable for improving the stability of tin-lead perovskite solar cells (Sn-Pb PSCs). Herein, hexaazatrinaphthylene (HATNA) is found to be a promising HTM building block for Sn-Pb PSCs. By introducing triphenylamine (TPA) and methoxy-triphenylamine into the HATNA core, molecular energy levels and surface wettability can be well regulated, and a high hole mobility and thermal stability can be maintained. Moreover, a homogeneous Sn-Pb perovskite film with low Sn 4+ contents and vertically orientated grains can be prepared on the substrate TPA-HATNA . Compared with PEDOT:PSS, the optimal TPA-HATNA -based methylammonium-free device enables a 70 mV increase in V OC , delivering a remarkable PCE exceeding 18% (certified 16.4%). Impressively, the TPA-HATNA -based devices without encapsulation retain 90% efficiency after aging for 600 min under maximum-power-point tracking. Our work provides alternative HTMs for boosting the performance of Sn-Pb PSCs.

This study confirmed the participation of a cryptic palmitoyl fatty acyl chain in the biosynthesis of safracin and unraveled a previously ignored peptidase for the removal of the precursor. Furthermore, the post-assembly line tailoring steps are extensively studied in terms of the methyltransferase SacI-catalyzed N-methylation and the FAD-dependent monooxygenase SacJ-catalyzed A-ring oxidation. The timing of these post-NRPS steps is also addressed in this work.

Pancreatic ductal adenocarcinoma (PDAC), as one of the most malignant tumors with dense desmoplastic stroma, forms a specific matrix barrier to hinder effective diagnosis and therapy. To date, a paramount challenge is in the search for intelligent nanotheranostics for such hypopermeable tumors, especially in breaking the PDAC-specific physical barrier. The unpredictable in vivo behaviors of nanotheranostics, that is, real-time tracking where, when, and how they cross the physical barriers and are taken up by tumor cells, are the major bottleneck. Herein, we elaborately design sequence-activated nanotheranostic TCM-U11&Cy@P with dual-channel near-infrared fluorescence outputs for monitoring in vivo behaviors in a sequential fashion. This nanotheranostic with a programmable targeting capability effectively breaks through the PDAC barriers. Ultimately, the released aggregation-induced emission (AIE) particle TCM-U11 directly interacts with PDAC cells and penetrates into the deep tissue. Impressively, this fluorescent nanotheranostic intraoperatively can map human clinical PDAC specimens with high resolution. We believe that this unique sequence-activated fluorescent strategy expands the repertoire of nanotheranostics in the treatment of hypopermeable tumors., Competing Interests: The authors declare no competing financial interest., (© 2022 The Authors. Published by American Chemical Society.)

The performance of single-atom catalysts strongly depends on their particular coordination environments in the near-surface region. Herein, we discover that engineering extra Pt single atoms in the subsurface (Pt subsurf ) can significantly enhance the catalytic efficiency of surface Pt single atoms toward the oxygen reduction reaction (ORR). We experimentally and theoretically investigated the effects of the Pt subsurf single atoms implanted in different positions of the subsurface of Co particles. The local environments and catalytic properties of surface Pt 1 are highly tunable via Pt subsurf doping. Specifically, the obtained Pt 1 @Co/NC catalyst displays a remarkable performance for ORR, achieving mass activity of 4.2 mA μg Pt -1 (28 times higher than that of commercial Pt/C) at 0.9 V versus reversible hydrogen electrode (RHE) in 0.1 M HClO 4 solution with high stability over 30000 cycles.

Decoupling the ion motion and segmental relaxation is significant for developing advanced solid polymer electrolytes with high ionic conductivity and high mechanical properties. Our previous work proposed a decoupled ion transport in a novel protein-based solid electrolyte. Herein, we investigate the detailed ion interaction/transport mechanisms through first-principles density functional theory (DFT) calculations in a vacuum space. Specifically, we study the important roles of charged amino acids from proteins. Our results show that the charged amino acids ( i.e. , Arg and Lys) can strongly lock anions (ClO 4 - ). When locked at a proper position (determined from the molecular structure of amino acids), the anions can provide additional hopping sites and facilitate Li + transport. The findings are supported from our experiments of two protein solid electrolytes, in which the soy protein (with plenty of charged amino acids) electrolyte shows much higher ionic conductivity and lower activation energy in comparison to the zein (lack of charged amino acids) electrolyte.

Developing hard carbon with a high initial Coulombic efficiency (ICE) and very good cycling stability is of great importance for practical sodium-ion batteries (SIBs). Defects and oxygen-containing groups grown along either the carbon edges or the layers, however, are inevitable in hard carbon and can cause a tremendous density of irreversible Na + sites, decreasing the efficiency and therefore causing failure of the battery. Thus, eliminating these unexpected defect structures is significant for enhancing the battery performance. Herein, we develop a strategy of applying a soft-carbon coating onto free-standing hard-carbon electrodes, which greatly hinders the formation of defects and oxygen-containing groups on hard carbon. The electrochemical results show that the soft-carbon-coated, free-standing hard-carbon electrodes can achieve an ultrahigh ICE of 94.1% and long cycling performance (99% capacity retention after 100 cycles at a current density of 20 mA g -1 ), demonstrating their great potential in practical sodium storage systems. The sodium storage mechanism was also investigated by operando Raman spectroscopy. Our sodium storage mechanism extends the "adsorption-intercalation-pore filling-deposition" model. We propose that the pore filling in the plateau area might be divided into two parts: (1) sodium could fill in the pores near the inner wall of the carbon layer; (2) when the sodium in the inner wall pores is close to saturation, the sodium could be further deposited onto the existing sodium.

The changes in the transport behavior of a microswimmer before and after cargo loading are crucial to understanding and control of the motion of a biohybrid microbot. In this work, we show the change in swimming behavior of biflagellated microalgae Chlamydomonas reinhardtii picking up a 4.5 μm polystyrene microbead upon collision. The microswimmer changed from linear forward motion into helical motion upon the attachment of the cargo and swam with a decreased swimming velocity. We revealed the helical motion of the microswimmer upon cargo loading due to suppression of flagella by image analysis of magnified time-lapse images of C. reinhardtii with one microbead attached at the anterior end (between the flagella). Furthered suppression on the flagellum imposed by the loading of the second cargo has led to increased oscillation per displacement traveled and decreased swimming velocity. Moreover, the microswimmer with a microbead attached at the posterior end swam with swimming velocity close to free swimming microalgae and did not exhibit helical swimming behavior. The experimental results and analysis showed that the loading location of the cargo has a great influence over the swimming behavior of the microswimmer. Furthermore, the work balance calculation and mathematical analysis based on Lighthill's model are well consistent with our experimental findings.

Stretchable electronics have demonstrated tremendous potential in wearable healthcare, advanced diagnostics, soft robotics, and persistent human-machine interfaces. Still, their applicability is limited by a reliance on low-throughput, high-cost fabrication methods. Traditional MEMS/NEMS metallization and off-contact direct-printing methods are not suitable at scale. In contrast, screen printing is a high-throughput, mature printing method. The recent development of conductive nanomaterial inks that are intrinsically stretchable provides an exciting opportunity for scalable fabrication of stretchable electronics. The design of screen-printed inks is constrained by strict rheological requirements during printing, substrate-ink attraction, and nanomaterial properties that determine dispersibility and percolation threshold. Here, this review provides a concise overview of these key constraints and a recent attempt to meet them. We begin with a description of the fluid dynamics governing screen printing, deduce from these properties the optimal ink rheological properties, and then describe how nanomaterials, solvents, binders, and rheological agents are combined to produce high-performing inks. Although this review emphasizes conductive interconnections, these methods are highly applicable to sensing, insulating, photovoltaic, and semiconducting materials. Finally, we conclude with a discussion on the future opportunities and challenges in screen-printing stretchable electronics and their broader applicability., Competing Interests: The authors declare no competing financial interest., (© 2021 The Authors. Published by American Chemical Society.)

Integrating nanostructured active materials, antimicrobial components, and rational porous structures is one of the promising approaches for simultaneously boosting removal efficiency, antimicrobial capacity, mechanical property, hydrophobic performance, and air permeability of air filters. However, realizing these performances of an air filter still remains a big challenge. Herein, a multifunctional air filter zNFs-Ag@PT, which is composed of a unique substrate prepared from Ag nanoparticles (AgNPs)-paper towel (PT) microfibers and an upper layer formed from aligned zein nanofibers (zNFs) inspired by a "tug-of-war" repulsion force, is reported. The Ag@PT substrate is fabricated via in situ reduction; and zNFs are prepared by electrospinning a well-prepared zein Pickering emulsion onto a specially designed collector. The innovative collector is a partially conductive design composed of an insulative middle section and two conductive ends. It is demonstrated that the introduction of AgNPs not only endows the zNFs-Ag@PT filter with an effective antimicrobial activity but also provides the substrate with an anisotropic electric field to achieve stretched and aligned zein fibers forming thinner nanofibers than that without AgNPs. As a result, the filtration performances of a zNFs-Ag@PT filter are enhanced. This study initiates an effective way to fabricate bio-based multifunctional air filters with antimicrobial and filtration performances via combining nano- and biotechnology.

Recent advances in flexible materials and wearable electronics offer a noninvasive, high-fidelity recording of biopotentials for portable healthcare, disease diagnosis, and machine interfaces. Current device-manufacturing methods, however, still heavily rely on the conventional cleanroom microfabrication that requires expensive, time-consuming, and complicated processes. Here, we introduce an additive nanomanufacturing technology that explores a contactless direct printing of aerosol nanomaterials and polymers to fabricate stretchable sensors and multilayered wearable electronics. Computational and experimental studies prove the mechanical flexibility and reliability of soft electronics, considering direct mounting to the deformable human skin with a curvilinear surface. The dry, skin-conformal graphene biosensor, without the use of conductive gels and aggressive tapes, offers an enhanced biopotential recording on the skin and multiple uses (over ten times) with consistent measurement of electromyograms. The combination of soft bioelectronics and deep learning algorithm allows classifying six classes of muscle activities with an accuracy of over 97%, which enables wireless, real-time, continuous control of external machines such as a robotic hand and a robotic arm. Collectively, the comprehensive study of nanomaterials, flexible mechanics, system integration, and machine learning shows the potential of the printed bioelectronics for portable, smart, and persistent human-machine interfaces.

Design and fabrication of bimodal structures are essential for successful development of advanced air filters with ultralow airflow resistance. To realize this goal, simplified processing procedures are necessary for meeting the practical needs. Here, a bimodal protein fabric with high-performance air filtration, and effectively lowered airflow resistance is reported. The various functional groups of proteins provide versatile interactions with pollutants. By utilizing a novel and cost-effective "cross-axial" configuration with an optimized condition (75° of contacting angle between solution nozzle and cospinning solvent nozzle), the diffusion in Taylor cone is in situ controlled, which results in the successful production of bimodal protein fabric. The bimodal protein fabric (16.7 g/m 2 areal density) is demonstrated to show excellent filtration performance for removing particulate matter (PM) pollutants and only causes 17.1 Pa air pressure drop. The study of multilayered protein fabric air filters shows a further improvement in filtration performance of removing 97% of PM 0.3 and 99% of PM 2.5 with a low airflow resistance (34.9 Pa). More importantly, the four-layered bimodal protein fabric shows an exceptional long-term performance and maintains a high removal efficiency in the humid environment. This study presents an effective and viable strategy for fabricating bimodal fibrous materials for advanced air filtration.

Sensors that can detect external stimuli and perceive the surrounding areas could offer an ability for soft biomimetic robots to use the sensory feedback for closed-loop control of locomotion. Although various types of biomimetic robots have been developed, few systems have included integrated stretchable sensors and interconnectors with miniaturized electronics. Here, we introduce a soft, stretchable nanocomposite system with built-in wireless electronics with an aim for feedback-loop motion control of a robotic earthworm. The nanostructured strain sensor, based on a carbon nanomaterial and a low-modulus silicone elastomer, allows for seamless integration with the body of the soft robot that can accommodate large strains caused by bending, stretching, and physical interactions with obstacles. A scalable, cost-effective, and screen-printing method manufactures an array of the strain sensors that are conductive and stretchable over 100% with a gauge factor over 38. An array of nanomembrane interconnectors enables a reliable connection between soft sensors and wireless electronics while tolerating the robot's multimodal movements. A set of computational and experimental studies of soft materials, stretchable mechanics, and hybrid packaging provides the key design factors for a reliable, nanocomposite sensor system. The miniaturized wireless circuit, embedded in the robot joint, offers real-time monitoring of strain changes during the motions of a robotic segment. Collectively, the soft sensor system presented in this work shows great potential to be integrated with other flexible, stretchable electronics for applications in soft robotics, wearable devices, and human-machine interfaces.

Remote C-H functionalization at C5 is the most sparingly observed selectivity in the functionalization of indole templates. Herein, we reported that the combination of a AgSbF 6 catalyst and phenyliodine diacetate oxidation enabled the C-H selenylation at the C5 position of indole scaffolds in a selective version, thus leading to the formation of a wide scope of 5-selenylated indole derivatives, which are otherwise difficult to prepare. Mechanistic studies indicated that current transformation follows a radical process, and the tethered C3 pivaloyl group on indole scaffolds plays roles in both blocking the active C3 position and manipulating the electronic affinity of the arenes.

Room-temperature sodium-sulfur (RT-Na/S) batteries hold great promise for sustainable and cost-effective applications. Nevertheless, it remains a great challenge to achieve high capacity and cycling stability due to the low activity of sulfur and the sluggish conversion kinetics between polysulfide intermediates and sodium sulfide. Herein, an electrocatalyzing S cathode is fabricated, which consists of porous core-shell structure and multisulfiphilic sites. The flexible carbon structure effectively buffers volume changes during cycling and provides enclosed spaces to store S 8 with exceptional conductivity. Significantly, the multisulfiphilic sites (ZnS and CoS 2 ) enhance catalysis toward multistep S conversion, which effectively suppresses long-chain polysulfides dissolution and improves the kinetics of short-chain polysulfides. Thus, the obtained S cathodes achieve an enhanced cycling performance (570 mAh g -1 at 0.2 A g -1 over 1000 cycles), decent rate capability (250 mAh g -1 at 1.0 A g -1 over 2000 cycles), and high energy density of 384 Wh kg -1 toward practical applications.

Soft strain sensors that are mechanically flexible or stretchable are of significant interest in the fields of structural health monitoring, human physiology, and human-machine interfaces. However, existing deformable strain sensors still suffer from complex fabrication processes, poor reusability, limited adhesion strength, or structural rigidity. In this work, we introduce a versatile, high-throughput fabrication method of nanostructured, soft material-enabled, miniaturized strain sensors for both structural health monitoring and human physiology detection. Aerosol jet printing of polyimide and silver nanowires enables multifunctional strain sensors with tunable resistance and gauge factor. Experimental study of soft material compositions and multilayered structures of the strain sensor demonstrates the capabilities of strong adhesion and conformal lamination on different surfaces without the use of conventional fixtures and/or tapes. A two-axis, printed strain gauge enables the detection of force-induced strain changes on a curved stem valve for structural health management while offering reusability over 10 times without losing the sensing performance. Direct comparison with a commercial film sensor captures the advantages of the printed soft sensor in enhanced gauge factor and sensitivity. Another type of a stretchable strain sensor in skin-wearable applications demonstrates a highly sensitive monitoring of a subject's motion, pulse, and breathing, validated by comparing it with a clinical-grade system. Overall, the presented comprehensive study of materials, mechanics, printing-based fabrication, and interfacial adhesion shows a great potential of the printed soft strain sensor for applications in continuous structural health monitoring, human health detection, machine-interfacing systems, and environmental condition monitoring.

Developing a rapid sensing platform with effective pesticide degradation capabilities integrated into a single structure and realistic application is an imminent challenge to ensure sustainable agriculture and food safety. Here, we described establishment of a bifunctional nanoscale porphyrinic metal-organic framework (MOF) probe serving as a sensor for detection of trace nitenpyram and as a photocatalyst to facilitate the pesticide degradation. Based on the signal turned "on-off", the strong fluorescence of the probe was quenched by the target, leading to the sensing range from 0.05 to 10.0 μg mL -1 and a detection limit of 0.03 μg mL -1 . Given the versatile design by which the porphyrin photosensitizers were isolated subtly in the MOF to avoid self-quenching, the probe was endowed with sustainable and efficient pesticide photodegradation activity with a degradation rate of ∼95% for nitenpyram. Our work represents powerful all-in-one MOF-derived materials jointly for sensing and degrading pesticide residues in agricultural soils and other pesticide-contaminated environments.

With the purpose to achieve panchromatic absorption for constructing efficient dye-sensitized solar cells (DSSCs), the cosensitization approach of using two dyes with complementary absorption has been developed with great success. However, this approach usually requires time-consuming optimization of a number of parameters for controlling the ratio and distribution of the two coadsorbed dyes on TiO 2 film, which limits the potentials of this strategy. We herein report an alternative approach for developing efficient DSSCs by designing a class of "concerted companion dyes" with two complementary dye components linked covalently. Thus, a newly synthesized organic dye Z2 was linked to a recently reported doubly strapped porphyrin dye XW51 through flexible chains with various lengths to afford XW60 - XW63 . These dyes exhibit excellent absorption and efficiencies in the range of 8.8%-11.7%. Notably, upon coadsorption with chenodeoxycholic acid, XW61 affords an impressive efficiency of 12.4%, a record for iodine electrolyte-based DSSCs, to the best of our knowledge. In addition, these dyes also exhibit the advantages of easy cell fabrication, simple optimization, as well as excellent photostability.

Among the various methods to develop flexible wearable antennas, a serpentine, mesh structure has been a great interest because of its mechanical reliability upon applied strain. However, there is still a significant lack of design guidelines for the open-mesh concept that account for both material and electromagnetic (EM) properties of antennas. In this work, we introduce a comprehensive study of materials, mechanics, fabrication, and system integration for the development of stretchable dipole and patch antennas that have networks of two-dimensional serpentine patterns. A set of computational modeling and experimental validation of open-mesh structures provides the key design guidelines to offer the maximum mechanical stretchability and minimum effective moduli of wearable antennas. Integration of the thin-film antenna traces with various substrates captures the versatility of the deterministic fabrication and material transfer printing methods. The influence of antenna stretching on the EM properties, including return loss, electric and magnetic fields, and far-field radiation patterns, is investigated. EM characterization with mechanical stretching results in different properties of fabricated antennas. The simulation study of specific absorption rates shows a potential for safe applications of dipole and patch stretchable antennas on the human skin.

The fast light-responsive dithienylethenes (DTEs) are one of the most attractive photochromic families because of their excellent thermal irreversibility and fatigue resistance. However, the all-visible-light-activated DTE system still remains challenging because most of them require the harmful high-energy ultraviolet light to trigger their photocyclization reaction. Here, we have for the first time borrowed a specific intramolecular proton transfer (IPT) process and rationally designed a series of all-visible-light-driven DTEs. Incorporating the IPT-functional group to DTE unit gives rise to an extra absorption band with a distinct red shift, which enables the photocyclization of DTEs under stimuli of visible light at 450 nm, as well as ensuring the desirable photoswitching efficiency. The isomerization from OH form to NH form induced by IPT can decrease the energy gap for excitation and photocyclization, thereby affording the all-visible-light-triggered photochromic performance, which can not only work well in a polar solvent system but also show its effectiveness in polymeric gel systems. In this regard, we can provide a general and reliable platform to construct all-visible-light-driven DTEs with excellent reversible photoswitching and broad applicability, especially with avoiding the use of harmful ultraviolet light to induce their photocyclization.

Antarctic krill ( Euphausia superba ) is one of the important bioresources in Antarctic waters, containing many bioactives (e.g., astaxanthin), which have a highly potential value for commercial exploitation. In this study, the effects of processing methods on the content, structural isomers, and composition of astaxanthins (free astaxanthin and astaxanthin esters) were studied. Three drying methods, comprising freeze-drying, microwave drying, and hot-air drying, were used. Free astaxanthin (Ast), astaxanthin monoesters (AM), and astaxanthin diesters (AD) in boiled krill (control) and dried krill were extracted and analyzed using high-resolution mass spectrometry with ultraviolet detection. After the three processes, total astaxanthin loss ranged from 8.6 to 64.9%, and the AM and AD contents ranged from 78.3 to 16.6 and 168.7 to 90.5 μg/g, respectively. Compared to other kinds of astaxanthin esters, astaxanthin esters, which linked to eicosapentaenoic acid and docosahexaenoic acid, as well as the Ast, were more easily degraded, and AM was more susceptible to degradation than AD. All- E -astaxanthin easily transformed to the 13 Z- astaxanthin than to the 9 Z- astaxanthin during the drying process, but the proportions of optical isomers changed due to drying by no more than 5%. The results suggested that freeze-drying, low-power microwave drying (≤1 kW), and low-temperature hot-air drying (≤60 °C) are optimal drying methods for ensuring the quality of krill products., Competing Interests: The authors declare no competing financial interest., (Copyright © 2019 American Chemical Society.)

Sulfur dioxide (SO 2 ) plays significant roles in regulating cell apotosis and inflammation. However, there are complex interactions between small biomolecules in cells, and the identification of these coexisting biomarkers remains a challenge. Herein, we report an AND logic gate based fluorescent probe ( NY-Lyso ), operating by responding to pH differences between organelles in cell and selectively reacting with bisulfite (HSO 3 - ). This approach allows the fluorescence of the probe to remain silent under neutral or alkaline conditions, notably, is activated by costimulation of lower pH and bisulfite. Furthermore, it was confirmed to be biocompatible and could be employed to monitor HSO 3 - in lysosomes of living cells. The proposed method demonstrated more practical and outstanding capabilities in targeted and real-time monitoring, providing an effective optical tool for biomarker sensing.

Molecular detection and manipulation via nanofluidic systems offers new routes for single-molecule analysis to study epigenetic mechanisms and genetic mutation of disease. For detection of single biological molecule, many types of nanomicrofluidic systems have been utilized. Typically, mechanical tethering, fluidic pressure, chemical interactions, or electrical forces allow controllable attraction, enrichment, confinement, and elongation of target molecules. The currently available methods, however, are unable to offer both molecular manipulation and direct and concurrent assessment of target molecules in the system due to the nature of enclosed channels and associated fluidic components. Here, we introduce a wafer-scale nanofluidic system that incorporates an array of accessible open nanochannels and nano-microtrappers to enrich and elongate target molecules (DNA) via the combination of an electric field and hydrodynamic force. The open nanofluidic system allows easy access, direct observation, and manipulation of molecules in the nanochannels. The presence of a stretched single DNA and the efficacy of the nanofluidic system are studied by fluorescence microscopy and atomic force microscopy. Hybrid integration of the nanodevice fabrication with a material transfer printing technique enables to design a highly flexible and transferrable nanofluidic system after molecular concentration.

Although a high-efficiency air filter can be achieved from electrospun nanofabrics, it has been challenging to reduce the pressure drop, increase the filtration capacity, and improve the production rate of the electrospinning process. Here, we report a hierarchically structured all-biomass air filter with high filtration efficiency and low air pressure drop based on applying Pickering emulsions to generate protein-functionalized nanostructures. Specifically, the air filter consists of cellulose nanofibers (CNF)/zein nanoparticles as active fillers prepared from Pickering emulsions and porous structures of microfibers as the frame from wood pulp (WP). The zein-protein-coated nanoparticles, CNF/zein, contribute in multiple ways to improve removal efficiency of the filters. First, the exposed functional groups of zein-protein help to trap air pollutants including toxic gaseous molecules via interaction mechanisms. Second, the nanoparticles with a high surface area promote the capture capability for small particulate pollutants. Meanwhile, the long-micron WP fibers forming a frame with large pores significantly reduce the pressure drop. Via adjusting the component ratios of in the Pickering emulsion, we report an optimized air filter with the high efficiency for capturing both types of pollutants: particulate matter (PM) and chemical gasses such as HCHO and CO, and the extremely low normalized pressure drop, that is, approximately 1/170 of the zein-based nano air filter by electrospinning. This study initiates a cost-effective strategy for forming a hierarchical nano- and microstructure, enabling high efficiency of capturing particulate pollutants of a wide size range and more species. More significantly, this is the first study in which Pickering emulsion is applied as a critical approach with integration of bio- and nano-technology to make high-performance, green air filters.

Cerebral metabolism alterations influence cerebrospinal fluid (CSF) composition and are sensitive to brain injury. In subarachnoid hemorrhage (SAH) patients, Fisher scale, Hunt-Hess scale, and World Federation of Neurological Societies (WFNS) grading scale evaluating SAH severity are inadequate to predict long-term outcome; therefore, in an effort to determine metabolite pattern disparity and discover corresponding biomarkers, we designed an untargeted CSF metabolomic study covering a broad range of metabolites of SAH patients with different severity and outcome. The present study demonstrated the SAH altered the cerebrospinal fluid metabolome involving carbohydrate, lipid, and amino acid metabolism. Pyruvate metabolism was enhanced in SAH patients with Hunt-Hess scale above III, and the CSF pyruvate level was significantly associated with WFNS grading scale above III. There is no significant variation among CSF metabolome in SAH patients with merely different amounts and distribution of bleeding. SAH patients with unfavorable outcome present upregulated CSF amino acids level and enhanced lipid biosynthesis. The present study provides a novel possibility of early identification of patients who might possess unfavorable outcome and further clarification of the underlying pathophysiology.

High-fidelity mapping of amyloid-β (Aβ) plaques is critical for the early detection of Alzheimer's disease. However, in vivo probing of Aβ plaques by commercially available thioflavin derivatives (ThT or ThS) has proven to be extremely limited, as evident by the restriction of enrichment quenching effect, low signal-to-noise ( S/ N) ratio, and poor blood-brain barrier (BBB) penetrability. Herein, we demonstrate a rational design strategy of near-infrared (NIR) aggregation-induced emission (AIE)-active probes for Aβ plaques, through introducing a lipophilic π-conjugated thiophene-bridge for extension to NIR wavelength range with enhancement of BBB penetrability, and tuning the substituted position of the sulfonate group for guaranteeing specific hydrophilicity to maintain the fluorescence- off state before binding to Aβ deposition. Probe QM-FN-SO 3 has settled well the AIE dilemma between the lipophilic requirement for longer emission and aggregation behavior from water to protein fibrillogenesis, thus making a breakthrough in high-fidelity feedback on in vivo detection of Aβ plaques with remarkable binding affinity, and serving as an efficient alternative to the commercial probe ThT or ThS.