Such a large ZFS energy yields a very strong single-ion magnetic anisotropy of easy-plane type resembling that of rare-earth ions. Its microscopic origin is the unusual linear coordination of the Co(I) ions in Li2(Li1-xCox)N with two nitrogen ligands. Our calculations also evidence a strong 3d-4s hybridization of the electronic shells resulting in significant electron spin density at the 59Co nuclei, which may be responsible for the experimentally observed extraordinary large hyperfine structure of the ESR signals. Altogether, our experimental spectroscopic and computational results enable comprehensive insights into the remarkable properties of the Li2[Li1-x(TM)x]N magnets on the microscopic level.Soluble oligomers formed by amyloidogenic intrinsically disordered proteins are some of the most cytotoxic species linked to neurodegeneration. Due to the transient and heterogeneous nature of such oligomeric intermediates, the underlying self-association events often remain elusive. NMR relaxation measurements sensitive to zero-frequency spectral densities (J(0)), such as the 15N – R2 rates, are ideally suited to map sites of self-association at atomic resolution without the need of exogenous labels. Such experiments exploit the dynamic exchange between NMR visible monomers and slowly tumbling oligomers. However,15N – R2 rates are also sensitive to intrinsic monomer dynamics, and it is often difficult to discern these contributions from those arising from exchange with oligomers. Another challenge pertains to defining a hierarchy of self-association. Here, using the archetypical amyloidogenic protein alpha synuclein (αS), we show that the temperature-dependence of 15N – R2 effectively identifies self-association sites with reduced bias from internal dynamics. The key signature of the residues involved in self-association is a nonlinear temperature-dependence of 15N – R2 with a positive ΔR2/ΔT slope. These two hallmarks are systematically probed through a thermal R2 correlation matrix, from which the network of residues involved in self-association as well as the hierarchy of αS self-association sites is extracted through agglomerative clustering. We find that aggregation is initiated by residues within the NAC region that is solvent inaccessible in αS fibrils and eventually extends to the N-terminal segment harboring familial PD mutations. These hierarchical self-association maps help dissect the essential drivers of oligomerization and reveal how amyloid inhibitors affect oligomer formation.The remediation of organohalides from water is a challenging process in environment protection and water treatment. Herein, we report a molecular copper(I) complex with two triazole units, CuT2, in a heterogeneous aqueous system that is capable of dechlorinating dichloromethane (CH2Cl2) to afford hydrocarbons (methane, ethane, and ethylene). The catalytic performance is evaluated in water and presented high Faradaic efficiency (average 70% CH4) across a range of potentials (-1.1 to -1.6 V vs Ag/AgCl) and high activity (maximum -25.1 mA/cm2 at -1.6 V vs Ag/AgCl) with a turnover number of 2.0 × 107. The CuT2 catalyst also showed excellent stability for 14 h of constant exposure to CH2Cl2 and 10 h of CH2Cl2 exposure cycling. The control compound, a copper-free triazole unit (T1), was also investigated under the same condition and showed inferior catalytic activity, indicating the importance of the copper center. Plausible catalytic mechanisms are proposed for the formation of C1 and C2 products via radical intermediates. Computational studies provided additional insight into the reaction mechanism and the selectivity toward the CH4 formation. The findings in this study demonstrate that complex CuT2 is an efficient and stable catalyst for the dehalogenation of CH2Cl2 and could potentially be used for the exploration of the removal of halogenated species from aqueous systems.Secondary organic aerosol (SOA) plays a critical role in sustained haze pollution in megacities. Traditional observation of atmospheric aerosols usually analyzes the ambient organic aerosol (OA) but neglects the SOA formation potential (SOAFP) of precursors remaining in ambient air. Knowledge on SOAFP is still limited, especially in megacities suffering from frequent haze. In this study, the SOAFP of ambient air in urban Beijing was characterized at different pollution levels based on a two-year field observation using an oxidation flow reactor (OFR) system. Both OA and SOAFP increased as a function of ambient pollution level, in which increasing concentrations of precursor volatile organic compounds (VOCs) and decreasing atmospheric oxidation capacity were found to be the two main influencing factors. To address the role of the atmospheric oxidation capacity in SOAFP, a relative OA enhancement ratio (EROA = 1 + SOAFP/OA) and the elemental composition of the OA were investigated in this study. The results indicated that the atmospheric oxidation capacity was weakened and resulted in higher SOAFP on more polluted days. The relationship found between SOAFP and the atmospheric oxidation capacity could be helpful in understanding changes in SOA pollution with improving air quality in the megacities of developing countries.Understanding and controlling the dynamics of active Brownian objects far from equilibrium are fundamentally important for emerging technologies such as artificial micro/nanomotors for drug deliveries and noninvasive microsurgery. However, direct observation and control of unidirectional propulsion of individual nanoscale objects are technically challenging due to the required spatiotemporal resolution. Here, we report in situ visualization and manipulation of unidirectional superfast ballistic dynamics of a single-photon-activated gold nanoparticle (NP) along the liquid-gas interface by four-dimensional electron microscopy (4D EM) at nanometer and nanosecond scales. We observed that, upon repetitive femtosecond laser excitation, the NP at the liquid-gas interface exhibits a continuously superfast unidirectional translation with a linear dependence of its root mean squared velocity (νrms) on either the laser fluence or repetition rate. Under a single femtosecond pulse excitation, the NP exhibits a superfast ballistic translation at the nanosecond time scale. Combined experiment and physical modeling reveals that the superfast unidirectional, ballistic translation is driven by unidirectional random impulsive forces arising from the nanobubbles (NBs) induced by enhanced laser heating as a result of plasmonic excitation, which is controllable by tuning the laser characteristics. This directional plasmonic NB-propulsion mechanism sheds light on the design of light-controllable artificially intelligent micro/nanomotor systems.Nanoporous anodic alumina optical microcavities (NAA-μQVs) with spectrally tunable resonance band and surface chemistry are used as model light-confining photonic crystal (PC) platforms to elucidate the combined effect of spectral light confinement features and surface chemistry on optical sensitivity. These model nanoporous PCs show well-resolved, spectrally tunable resonance bands (RBs), the central wavelength of which is engineered from ∼400 to 800 nm by the period of the input anodization profile. The optical sensitivity of the as-produced (hydrophilic) and dichlorodimethylsilane-functionalized (hydrophobic) NAA-μQVs is studied by monitoring dynamic spectral shifts of their RB upon infiltration with organic- and aqueous-based analytical solutions of equally varying refractive index, from 1.333 to 1.345 RIU. Our findings demonstrate that hydrophilic NAA-μQVs show ∼81 and 35% superior sensitivity to their hydrophobic counterparts for organic- and aqueous-based analytical solutions, respectively. Interestingly, the sensitivity of hydrophilic NAA-μQVs per unit of spectral shift is more than 3-fold higher in organic than in aqueous matrices upon equal change of refractive index, with values of 0.347 ± 0.002 and 0.109 ± 0.001 (nm RIU-1) nm-1, respectively. Conversely, hydrophobic NAA-μQVs are found to be slightly more sensitive toward changes of refractive index in aqueous medium, with sensitivities of 0.072 ± 0.002 and 0.066 ± 0.006 (nm RIU-1) nm-1 in water- and organic-based analytical solutions, respectively. Our advances provide insights into critical factors determining optical sensitivity in light-confining nanoporous PC structures, with implications across optical sensing applications, and other photonic technologies.Surfactants, mimics of contamination, play an important role in nanobubble nucleation, stability, and growth at the electrode surface. Herein, we utilize single-molecule fluorescence microscopy as a sensitive imaging tool to monitor nanobubble dynamics in the presence of a surfactant. Our results show that the presence of anionic and nonionic surfactants increase the rate of nanobubble nucleation at all potentials in a voltage scan. The fluorescence and electrochemical responses indicate the successful lowering of the critical gas concentration needed for nanobubble nucleation across all voltages. Furthermore, we demonstrate that the accumulation of surfactants at the gas-liquid interface changes the interaction of fluorophores with the nanobubble surface. Specifically, differences in fluorophore intensity and residence lifetime at the nanobubble surface suggest that the labeling of nanobubbles is affected by the nature of the nanobubble (size, shape, etc.) and the structure of the gas-liquid interface (surfactant charge, hydrophobicity, etc.).Bacterial infections are a major threat to human health, exacerbated by increasing antibiotic resistance. These infections can result in tremendous morbidity and mortality, emphasizing the need to identify and treat pathogenic bacteria quickly and effectively. Recent developments in detection methods have focused on electrochemical, optical, and mass-based biosensors. Advances in these systems include implementing multifunctional materials, microfluidic sampling, and portable data-processing to improve sensitivity, specificity, and ease of operation. Concurrently, advances in antibacterial treatment have largely focused on targeted and responsive delivery for both antibiotics and antibiotic alternatives. Antibiotic alternatives described here include repurposed drugs, antimicrobial peptides and polymers, nucleic acids, small molecules, living systems, and bacteriophages. Finally, closed-loop therapies are combining advances in the fields of both detection and treatment. This review provides a comprehensive summary of the current trends in detection and treatment systems for bacterial infections.Antimicrobial resistance to existing antibiotics represents one of the greatest threats to human health and is growing at an alarming rate. To further complicate treatment of bacterial infections, many chronic infections are the result of bacterial biofilms that are tolerant to treatment with antibiotics because of the presence of metabolically dormant persister cell populations. Together these threats are creating an increasing burden on the healthcare system, and a „preantibiotic” age is on the horizon if significant action is not taken by the scientific and medical communities. While the golden era of antibiotic discovery (1940s-1960s) produced most of the antibiotic classes in clinical use today, followed by several decades of limited development, there has been a resurgence in antibiotic drug discovery in recent years fueled by the academic and biotech sectors. Historically, great success has been achieved by developing next-generation variants of existing classes of antibiotics, but there remains a direion for increased efforts by the scientific community to leverage synthetic chemistry and chemical microbiology toward novel antibiotics that can combat the growing crisis of MDR and tolerant bacterial infections.Guaiacyl acetone (GA) is a phenolic carbonyl emitted in significant quantities by wood combustion that undergoes rapid aqueous-phase oxidation to produce aqueous secondary organic aerosol (aqSOA). We investigate the photosensitized oxidation of GA by an organic triplet excited state (3C*) and the formation and aging of the resulting aqSOA in wood smoke-influenced fog/cloud water. The chemical transformations of the aqSOA were characterized in situ using a high-resolution time-of-flight aerosol mass spectrometer. Additionally, aqSOA samples collected over different time periods were analyzed using high-performance liquid chromatography coupled with a photodiode array detector and a high-resolution Orbitrap mass spectrometer (HPLC-PDA-HRMS) to provide details on the molecular composition and optical properties of brown carbon (BrC) chromophores. Our results show efficient formation of aqSOA from GA, with an average mass yield around 80%. The composition and BrC properties of the aqSOA changed significantly over the course of reaction. Three generations of aqSOA products were identified via positive matrix factorization analysis of the aerosol mass spectrometry data. Oligomerization and functionalization dominated the production of the first-generation aqSOA, whereas fragmentation and ring-opening reactions controlled the formation of more oxidized second- and third-generation products. Significant formation of BrC was observed in the early stages of the photoreaction, while organic acids were produced throughout the experiment. High-molecular weight molecules (m/z > 180) with high aromaticity were identified via HPLC-PDA-HRMS and were found to account for a majority of the UV-vis absorption of the aqSOA.The discovery of complete ammonia oxidation (comammox) has altered our understanding of nitrification, which is the rate-limiting process in the global nitrogen cycle. However, understanding the ecological role of comammox or its contribution to nitrification in both natural and artificial ecosystems is still in its infancy. Here, we investigated the community distribution and function of comammox bacteria in riparian ecosystems and analyzed interactions between comammox and other nitrogen cycling microorganisms. The comammox bacterial abundance and rate were higher in summer than in winter and higher in nonrhizosphere soils than in the rhizosphere. Fringe soils in the riparian zone comprise a comammox hotspot, where the abundance (2.58 × 108 copies g-1) and rate (0.86 mg N kg-1 d-1) of comammox were not only higher than at other sampling sites but also higher than those of other ammonia oxidation processes. The comammox rate correlated significantly positively with relative abundance of the comammox species Candidatus Nitrospira nitrificans but not with that of the species Candidatus Nitrospira nitrosa. Analysis of comammox interaction with other ammonia-oxidizing processes revealed ammonia-oxidizing archaea to dominate interface soils, comammox to dominate in fringe soils, and anaerobic ammonium oxidation (anammox) to dominate in interface sediments of the riparian zone. These results indicate that comammox may constitute an important and currently underestimated process of microbial nitrification in riparian zone ecosystems.Superhydrophobic, flexible, and ultrahigh-performance electromagnetic interference (EMI) shielding papers are of paramount importance to safety and long-term service under external mechanical deformations or other harsh service environments because they fulfill the growing demand for multipurpose materials. Herein, we fabricated multifunctional papers by incorporating sputter-deposited nickel nanoparticles (NiNPs) and a fluorine-containing coating onto cellulose filter papers coated with silver nanowires (AgNWs). AgNW networks with sputter-deposited NiNPs provide outstanding magnetic properties, electrical conductivity, and EMI shielding performance. At an AgNW content of 0.109 vol % and a NiNP content of 0.013 mg/cm2, the resultant papers exhibit a superior EMI shielding effectiveness (SE) of 88.4 dB. Additionally, the fluorine-containing coating endows the resultant papers with a high contact angle of 149.7°. Remarkably, the obtained papers still maintain a high EMI SE even after 1500 bending cycles or immersion in water, salt, or strong alkaline solutions for 2 h, indicating their outstanding mechanical robustness and chemical durability. This work opens a new window for designing and implementing ultrahigh-performance EMI shielding materials.No one can have missed the growing global environmental problems with plastics ending up as microplastics in food, water, and soil, and the associated effects on nature, wildlife, and humans. A hitherto not specifically investigated source of microplastics is polymer blends. A 1 g polymer blend can contain millions to billions of micrometer-sized species of the dispersed phase and therefore aging-induced fragmentation of the polymer blends can lead to the release of an enormous amount of microplastics. Especially if the stability of the dispersed material is higher than that of the surrounding matrix, the risk of microplastic migration is notable, for instance, if the matrix material is biodegradable and the dispersed material is not. The release can also be much faster if the matrix polymer is biodegradable. The purpose of writing this feature article is to arise public and academic attention to the large microplastic risk from polymer blends during their development, production, use, and waste handling.Diabetic cardiac autonomic neuropathy (DCAN) is a complication that affects more than 60% of diabetic patients. There is evidence for the involvement of P2X4 receptor in DCAN. This study showed that the expression of the long noncoding RNA (lncRNA) UC.360+ was increased in the stellate ganglion (SG) of type 2 diabetes mellitus (DM) rats, and in situ hybridization revealed a clear presence of UC.360+ in SG neurons. The potential roles of UC.360+ in DCAN and its relationship with P2X4 receptor in SG were further explored via application of the short hairpin RNA (shRNA) against lncRNA UC.360+ in DM rats. The abnormal cardiac sympathetic changes in diabetic rats were improved after treatment with lncRNA UC.360+ shRNA. In the SG of these shRNA-treated DM rats, the upregulation of P2X4, tumor necrosis factor-α (TNF-α), interleukin 1β (IL-1β), and phosphorylated ERK1/2 was inhibited. Thus, lncRNA UC.360+ shRNA treatment may improve DCAN mediated by the P2X4 receptor in SG.The coronavirus disease-2019 (COVID-19) pandemic, caused by the pathogen severe acute respiratory syndrome coronavirus 2 (SARS-CoV-2), started in China during late 2019 and swiftly spread worldwide. Since COVID-19 emergence, many therapeutic regimens have been relentlessly explored, and although two vaccines have just received emergency use authorization by different governmental agencies, antiviral therapeutics based neutralizing antibodies and small-drug inhibitors can still be vital viable options to prevent and treat SARS-CoV-2 infections. The viral spike glycoprotein (S-protein) is the key molecular player that promotes human host cellular invasion via recognition of and binding to the angiotensin-converting enzyme 2 gene (ACE2). In this work, we report the results obtained by mutating in silico the 18 ACE2 residues and the 14 S-protein receptor binding domain (S-RBDCoV-2) residues that contribute to the receptor/viral protein binding interface. Specifically, each wild-type protein-protein interface residue was replaced by a hydrophobic (isoleucine), polar (serine and threonine), charged (aspartic acid/glutamic acid and lysine/arginine), and bulky (tryptophan) residue, respectively, in order to study the different effects exerted by nature, shape, and dimensions of the mutant amino acids on the structure and strength of the resulting binding interface. The computational results were next validated a posteriori against the corresponding experimental data, yielding an overall agreement of 92%. Interestingly, a non-negligible number of mis-sense variations were predicted to enhance ACE2/S-RBDCoV-2 binding, including the variants Q24T, T27D/K/W, D30E, H34S7T/K, E35D, Q42K, L79I/W, R357K, and R393K on ACE2 and L455D/W, F456K/W, Q493K, N501T, and Y505W on S-RBDCoV-2, respectively.Lung-secreted IgG and IgM antibodies are valuable biomarkers for monitoring the local immune response against respiratory infections. These biomarkers are found in lower airway secretions that need to be liquefied prior to analysis. Traditional methods for sample liquefaction rely on reducing disulfide bonds, which may damage the structure of the biomarkers and hamper their immunodetection. Here, we propose an alternative enzymatic method that uses O2 bubbles generated by endogenous catalase enzymes in order to liquefy respiratory samples. The proposed method is more efficient for liquefying medium- and high-viscosity samples and does not fragment the antibodies. This prevents damage to antigen recognition domains and recognition sites for secondary antibodies that can decrease the signal of immunodetection techniques. The suitability of the enzymatic method for detecting antibodies in respiratory samples is demonstrated by detecting anti-SARS-CoV-2 IgG and IgM to viral N-protein with gold standard ELISA in bronchial aspirate specimens from a multicenter cohort of 44 COVID-19 patients. The enzymatic detection sharply increases the sensitivity toward IgG and IgM detection compared to the traditional approach based on liquefying samples with dithiothreitol. This improved performance could reveal new mechanisms of the early local immune response against respiratory infections that may have gone unnoticed with current sample treatment methods.Stem cell derived small extracellular vesicles (sEVs) have been proved to promote neurological recovery after stroke. Recent studies demonstrate a phenomenal tissue repair ability in embryonic stem cell derived sEVs (ESC-sEVs). However, whether ESC-sEVs could protect against ischemic stroke remains unknown. Immune responses play an essential role in the pathogenesis of ischemic stroke, and modulating post-stroke immune responses ameliorates ischemia-induced brain damage. In this study, we aim to determine the therapeutic function of ESC-sEVs, specifically focusing on their role in immunomodulation after ischemic stroke. ESC-sEVs are intravenously administered after transient middle cerebral artery occlusion. ESC-sEVs significantly decrease leukocyte infiltration, inflammatory cytokine expression, neuronal death, and infarct volume and alleviate long-term neurological deficits and tissue loss after ischemic stroke. Interestingly, ESC-sEVs induce a marked increase in regulatory T cells (Tregs) after stroke. Further, ESC-sEV-afforded immunomodulatory function and neuroprotection against stroke are dependent on Tregs, as the depletion of Tregs almost completely abrogates the protective effects. Mechanistically, proteomic analysis reveals the enrichment of TGF-β, Smad2, and Smad4 proteins in ESC-sEVs, which could be delivered to activate the TGF-β/Smad pathway in CD4+ T cells and therefore induce Treg expansion. ESC-sEVs modulate neuroinflammation and protect against ischemic stroke through the expansion of Tregs, a process that is partially dependent on the activation of the TGF-β/Smad signaling pathway by the transfer of TGF-β, Smad2, and Smad4. The results suggest ESC-sEVs might be a candidate for immune modulation.Small Molecule Enhancement SpectroscopY (SMolESY) was employed to develop a unique and fully automated computational solution for the assignment and integration of 1H nuclear magnetic resonance (NMR) signals from metabolites in challenging matrices containing macromolecules (herein blood products). Sensitive and reliable quantitation is provided by instant signal deconvolution and straightforward integration bolstered by spectral resolution enhancement and macromolecular signal suppression. The approach is highly efficient, requiring only standard one-dimensional 1H NMR spectra and avoiding the need for sample preprocessing, complex deconvolution, and spectral baseline fitting. The performance of the algorithm, developed using >4000 NMR serum and plasma spectra, was evaluated using an additional >8800 spectra, yielding an assignment accuracy greater than 99.5% for all 22 metabolites targeted. Further validation of its quantitation capabilities illustrated a reliable performance among challenging phenotypes. The simplicity and complete automation of the approach support the application of NMR-based metabolite panel measurements in clinical and population screening applications.Doping-induced solubility control (DISC) patterning is a recently developed technique that uses the change in polymer solubility upon doping, along with an optical dedoping process, to achieve high-resolution optical patterning. DISC patterning can produce features smaller than predicted by the diffraction limit; however, no mechanism has been proposed to explain such high resolution. Here, we use diffraction to spatially modulate the light intensity and determine the dissolution rate, revealing a superlinear dependence on light intensity. This rate law is independent of wavelength, indicating that patterning resolution is not dominated by an optical dedoping reaction, as was previously proposed. Instead we show here that the optical patterning mechanism is primarily controlled by the thermal profile generated by the laser. To quantify this effect, the thermal profile and dissolution rate are modeled using a finite-element model and compared against patterned line cross sections as a function of wavelength, laser intensity, and dwell time. Our model reveals that although the laser-generated thermal profile is broadened considerably beyond the profile of the laser, the highly temperature dependent dissolution rate results in selective dissolution near the peak of the thermal profile. Therefore, the key factor in achieving super-resolution patterning is a strongly temperature dependent dissolution rate, a common feature of many polymers. In addition to suggesting several routes to improved resolution, our model also demonstrates that doping is not required for optical patterning of conjugated polymers, as was previously believed. Instead, we demonstrate that superlinear resolution optical patterning should be attainable in any conjugated polymer simply by tuning the solvent quality during patterning, thus extending the applicability of our method to a wide class of materials. We demonstrate the generality of photothermal patterning by writing sub-400 nm features into undoped PffBT4T-2OD.Solar light-driven fuel production from carbon dioxide using organic photocatalysts is a promising technique for sustainable energy sources. Band gap engineering in sustainable organic photocatalysts for improving efficiency and fulfilling the requirements is highly anticipated. Here, we present a new strategy to engineer the band gap in covalent organic framework (COF) photocatalysts by varying the push-pull electronic effect. To implement this strategy, we have designed and synthesized four different COFs using a tripodal amine 4,4′,4″-(1,3,5-triazine-2,4,6-triyl)tris(([1,1′-biphenyl]-4-amine)) [Ttba] with 1,3,5-triformylbenzene (COF-1), 2,4,6-triformylphloroglucinol (COF-2), 2,4,6-triformylphenol (COF-3), and 2,4,6-triformylresorcinol (COF-4). On varying the number of hydroxyl units in the aldehyde precursor, the resulting COFs allow the fine-tuning of their band gap and band edge positions and result in different morphologies with varying surface areas. The enhanced optical properties of COF-3 and COF-4 with very suitable band gaps of 2.02 and 1.95 eV, respectively, enable them to demonstrate a high-efficiency photobiocatalytic system for NADH photoregeneration and enhanced visible light-driven formic acid production at a rate of 226.3 μmol g-1 in 90 min. The triazine core enables efficient charge separation, while the hydroxyl groups induce an electronic push-pull effect, regulating their photocatalytic efficiency. The results demonstrated the morphology-guided enhanced surface area and dual keto-enol tautomerism-induced push-pull effect in asymmetrical charge distribution as key features in the fine-tuning of the photocatalysts.Two-dimensional transition-metal compounds (2DTMCs) are promising materials for electrochemical applications, but 2DTMCs with metallicity and active basal planes are rare. In this work, we proposed a simple and effective strategy to extract 2DTMCs from non-van der Waals bulk materials and established a material library of 79 2DTMCs, which we named as anti-MXenes since they are composed of one M atomic layer sandwiched by two X atomic layers. By means of density functional theory computations, 24 anti-MXenes were confirmed to be thermodynamically, dynamically, mechanically, and thermally stable. The metallicity and active basal plane endow these anti-MXenes with potential as excellent electrode materials, for example, as electrocatalysts for hydrogen evolution reactions (HER). Among the noble-metal free anti-MXenes with favorable H-binding, CuS can boost HER at the whole range of H coverages, while CoSi, FeB, CoB, and CoP show promise for HER at some specific H coverages. The active sites are the tetra-coordinating nonmetal atoms at the basal planes, thus rendering a very high density of active sites for these materials. CoB is also a promising anode material for lithium-ion batteries, showing low Li diffusion energy barriers, a very high capacity, and a suitable open circuit voltage. This work promotes the „computational exfoliation” of 2D materials from non-van der Waals bulks and exemplifies the applications of anti-MXenes in various electrochemical processes.We present a collagen-mimetic protein of bacterial origin based upon a modified subdomain of the collagen-like Sc12 protein from Streptococcus pyogenes, as an alternative collagen-like biomaterial platform that is highly soluble, forms stable, homogeneous, fluid-like solutions at elevated concentrations, and that can be efficiently fabricated into hydrogel materials over a broad range of pH conditions. This extended bacterial collagen-like (eBCL) protein is expressed in a bacterial host and purified as a trimeric assembly exhibiting a triple helical secondary structure in its collagen-like subdomain that is stable near physiological solution conditions (neutral pH and 37 °C), as well as over a broad range of pH conditions. We also show how this sequence can be modified to include biofunctional attributes, in particular, the Arg-Gly-Asp (RGD) sequence to elicit integrin-specific cell binding, without loss of structural function. Furthermore, through the use of EDC-NHS chemistry, we demonstrate that members of this eBCL protein system can be covalently cross-linked to fabricate transparent hydrogels with high protein concentrations (at least to 20% w/w). These hydrogels are shown to possess material properties and resistance to enzymatic degradation that are comparable or superior to a type I collagen control. Moreover, such hydrogels containing the constructs with the RGD integrin-binding sequence are shown to promote the adhesion, spreading, and proliferation of C2C12 and 3T3 cells in vitro. Due to its enhanced solubility, structural stability, fluidity at elevated concentrations, ease of modification, and facility of cross-linking, this eBCL collagen-mimetic system has potential for numerous biomedical material applications, where the ease of processing and fabrication and the facility to tailor the sequence for specific biological functionality are desired.The development of smart size-tunable drug delivery nanoplatform enables the solving of the paradox of inconsistent size-dependence of high tumor accumulation and deep penetration during its delivery process, thus achieving superior cancer treatment efficacy. Herein, we report a size-shrinkable nanomicelle complex system with an initial size of 101 nm enabling effective retention around the tumor periphery and could destruct to ultrasmall nanomicelles triggered by a near-infrared (NIR) laser to realize the deep tumor penetration. The nanomicelle system is consisted of an upper critical solution temperature (UCST)-type block copolymer poly(acrylamide-acrylonitrile)-polyethylene glycol-lipoic acid (p(AAm-co-AN)-g-PEG-LA) encapsulating gold nanorods. Upon the irradiation of the NIR laser at the tumor site, gold nanorods could convert the light energy to heat energy, realizing the photothermal ablation of superficial tumor tissue. Concurrently, the large micelles split into a cascade of ultrasmall micelles (∼7 nm), which could easily penetrate into the deep site of the tumor and achieve the in situ „on-demand” release of the loaded drug to exert superior combined photothermal-chemotherapy of cancer. By the precise manipulation of laser, the micelle complex system realized the hierarchical killing from the superficial-to-deep tumor and achieved almost complete tumor growth inhibition on the established xenograft liver tumor mice model.One of the biggest bottlenecks in modern drug discovery efforts is in tackling the undruggable proteome. Currently, over 85% of the proteome is still considered undruggable because most proteins lack well-defined binding pockets that can be functionally targeted with small molecules. Tackling the undruggable proteome necessitates innovative approaches for ligand discovery against undruggable proteins as well as the development of new therapeutic modalities to functionally manipulate proteins of interest. Chemoproteomic platforms, in particular activity-based protein profiling (ABPP), have arisen to tackle the undruggable proteome by using reactivity-based chemical probes and advanced quantitative mass spectrometry-based proteomic approaches to enable the discovery of „ligandable hotspots” or proteome-wide sites that can be targeted with small-molecule ligands. These sites can subsequently be pharmacologically targeted with covalent ligands to rapidly discover functional or nonfunctional binders against therapf next-generation small-molecule induced-proximity-based therapeutic modalities that go beyond degradation. Exciting days lie ahead in this field as chemical biology becomes an increasingly major driver in drug discovery, and chemoproteomic approaches are sure to be a mainstay in developing next-generation therapeutics.There has been a growing interest in the development of efficient flexible organic solar cells (OSCs) due to their unique capacity to provide energy sources for flexible electronics. To this end, it is required to design a compatible interlayer with low processing temperature and high electronic quality. In this work, we present that the electronic quality of the ZnO interlayer fabricated from a low-temperature (130 °C) sol-gel method can be significantly improved by doping an organic small molecule, TPT-S. The doped TPT-S, on the one hand, passivates uncoordinated Zn-related defects by forming N-Zn bonds. On the other hand, photoinduced charge transfer from TPT-S to ZnO is confirmed, which further fills up electron-deficient trap states. This renders ZnO improved electron transport capability and reduced charge recombination. By illuminating devices with square light pulses of varying intensities, we also reveal that an unfavorable charge trapping/detrapping process observed in low-temperature-processed devices is significantly inhibited after TPT-S doping. OSCs based on PBDB-T-2FIT-4F with ZnOTPT-S being the cathode interlayer yield efficiencies of 12.62 and 11.33% on rigid and flexible substrates, respectively. These observations convey the practicality of such hybrid ZnO in high-performance flexible devices.To improve automobile safety, identifying driver fatigue is considerably crucial because it is one of the main causes of traffic accidents. In this research, smart systems based on a triboelectric nanogenerator are designed, which can provide driver status monitoring and fatigue warning in real time. The smart system consists of a self-powered steering-wheel angle sensor (SSAS) and a signal processing unit. The SSAS, which comprises a stator, a rotor, and a sleeve, is mounted on the steering rod, and the electrodes are designed with a phase difference to improve the resolution of the sensor. The turning angle of the steering wheel operated by the driver is recorded by the SSAS; meanwhile, the number of rotations, the average angle, and other parameters in the driver’s recorded data are analyzed by the signal processing unit from which a warning threshold for each parameter is determined. The system assesses the status of the driver in real-time by comparing these parameters and threshold values, and experimental results demonstrate that driver status is accurately judged. This work has important potential applications in the fields of traffic safety and intelligent driving.Development of smart switchable surfaces to solve the inevitable bacteria attachment and colonization has attracted much attention; however, it proves very challenging to achieve on-demand regeneration for noncontaminated surfaces. We herein report a smart, host-guest interaction-mediated photo/temperature dual-controlled antibacterial surface, topologically combining stimuli-responsive polymers with nanobactericide. From the point of view of long-chain polymer design, the peculiar hydration layer generated by hydrophilic poly(2-hydroxyethyl methacrylate) (polyHEMA) segments severs the route of initial bacterial attachment and subsequent proliferation, while the synergistic effect on chain conformation transformation poly(N-isopropylacrylamide) (polyNIPAM) and guest complex dissociation azobenzene/cyclodextrin (Azo/CD) complex greatly promotes the on-demand bacterial release in response to the switch of temperature and UV light. Therefore, the resulting surface exhibits triple successive antimicrobial functions simultaneously (i) resists ∼84.9% of initial bacterial attachment, (ii) kills ∼93.2% of inevitable bacteria attack, and (iii) releases over 94.9% of killed bacteria even after three cycles. The detailed results not only present a potential and promising strategy to develop renewable antibacterial surfaces with successive antimicrobial functions but also contribute a new antimicrobial platform to biomedical or surgical applications.The self-assembly of block copolymers in a confined space has been proven to be a facile and robust strategy for fabricating assembled structures with various potential applications. Herein, we employed a new pH-responsive polymer self-assembly method to regulate ion transport inside artificial nanochannels. The track-etched asymmetric nanochannels were functionalized with PS22k-b-P4VP17k/hPS4k blend polymers, and the ionic conductance and rectification properties of the proposed system were investigated. The pH-actuated changes in the surface charge and wettability resulted in the selective pH-gated ionic transport behavior. The designed system showed a good switching property to the pH stimulus and could recover during the repetitive experiments. The gating ability of the polymer-nanochannel system increased with increasing the weight of the homopolymer, and the proposed platform demonstrated robust stability and reusability. Numerical and the dissipative particle dynamics simulations were implemented to emulate the pH-dependent self-assembling behavior of diblock copolymers in a confined space, which were consistent with the experimental observations. As an example of the self-assembly of polymers in nanoconfinements, this work provides a facile and robust strategy for the regulation of ion transport in synthetic nanochannels. Meanwhile, this work can be further extended to design artificial smart nanogates for various applications such as mass delivery and energy harvesting.The high electrical conductivity of 1T’-WTe2 deserves particular attention and may show a high potential for hydrogen evolution reaction (HER) catalysis. However, the actual activity certainly does not match expectations, and the inferior HER activity is actually still ambiguous at the atomic level. Unraveling the underlying HER behaviors of 1T’-WTe2 will give rise to a new family of HER catalysts. Our structural analysis reveals that the inferior activity could result from insufficient charge density around the Te site and blocked adsorption channel at the W site, which cause too weak hydrogen adsorption. Herein, we fabricated a single WTe2 sheet-based electrocatalytic microdevice for directly extracting enhanced HER activity of doped electronegative F atoms. The overpotential at -10 mA cm-2 reduced to 0.27 V after F doping compared to 0.45 V for the original state. In situ electrochemical measurement and electrical tests on a single sheet indicate that doped F can regulate surface charge and hydrogen adsorption behavior. Furthermore, the theory simulation uncovers that the smaller atomic radius of F contributes to an empty coordination environment; meanwhile, strong electronegativity induces hydrogen adsorption. Thus, the ΔGH* at W sites around the doped F is as low as 0.18 eV. Synergistically modulating the charge properties and opening steric hindrance provides a new pathway to rationally construct electrocatalysts and beyond.The local lipid microenvironment of transmembrane receptors is an essential factor in G protein coupled receptor (GPCR) signaling. However, tools are currently missing for studying endogenously expressed GPCRs in primary cells and tissues. Here, we introduce fluorescent environment-sensitive GPCR ligands for probing the microenvironment of the receptor in living cells using fluorescence microscopy under no-wash conditions. We designed and synthesized antagonist ligands of the oxytocin receptor (OTR) by conjugating a high-affinity nonpeptidic OTR ligand PF-3274167 to the environment-sensitive fluorescent dye Nile Red. The length of the polar PEG spacer between the pharmacophore and the fluorophore was adjusted to lower the nonspecific interactions of the probe while preserving a strong fluorogenic response. We demonstrated that the new probes embed into the lipid bilayer in the vicinity of the receptor and convey information about the local polarity and the lipid order via the wavelength-shifting emission of the Nile Red fluorophore.ConspectusVibrational wavepacket motions on potential energy surfaces are one of the critical factors that determine the reaction dynamics of photoinduced reactions. The motions of vibrational wavepackets are often discussed in the interpretation of observables measured with various time-resolved vibrational or electronic spectroscopies but mostly in terms of the frequencies of wavepacket motions, which are approximated by normal modes, rather than the actual positions of the wavepacket. Although the time-dependent positions (that is, the trajectory) of wavepackets are hypothesized or drawn in imagined or calculated potential energy surfaces, it is not trivial to experimentally determine the trajectory of wavepackets, especially in multidimensional nuclear coordinates for a polyatomic molecule. Recently, we performed a femtosecond X-ray liquidography (solution scattering) experiment on a gold trimer complex (GTC), [Au(CN)2-]3, in water at X-ray free-electron lasers (XFELs) and elucidated the time-dependent poquently, the other covalent bond is formed for the longer Au-Au pair within 360 fs. The resultant trimer complex has a symmetric and linear geometry, implying the occurrence of bent-to-linear transformation concomitant with the formation of two equivalent covalent bonds, and exhibits vibrations that can be unambiguously assigned to specific normal modes based on the wavepacket trajectory, even without the vibrational frequencies provided by quantum calculation.Introducing oxygen vacancy (Vo) has been considered as an effective and significant method to accelerate the sluggish electrocatalytic nitrogen reduction reaction (NRR). In this work, a series of bimetallic zeolitic imidazolate frameworks based on ZIF-67 and ZIF-8 with varied ratios of Co/Zn have been applied as precursors to prepare Vo-rich Zn-doped Co3O4 nanopolyhedrons (Zn-Co3O4) by a low-temperature oxidation strategy. Zn-Co3O4 presents an ammonia yield of 22.71 μg h-1 mgcat.-1 with a high faradaic efficiency of 11.9% for NRR under ambient conditions. The remarkable catalytic performances are believed to result from the plentiful Vo as the Lewis acid sites and electron-rich Co sites to promote the adsorption and dissociation of N2 molecules. Remarkably, Zn-Co3O4 also demonstrates a high electrochemical stability. This work presents a guiding method for developing a stable and efficient electrocatalyst for the NRR.A novel transparent conductive conductor composed of a silver nanowire (AgNW) network and MoOx on a flexible polyethylene terephthalate (PET) substrate, with contemporaneously improved adhesion and reduced resistivity, is prepared using the full-solution process without high-temperature annealing. Under the optimized conditions, a MoOx/AgNW/MoOx multilayer is achieved, which shows much superior optoelectronic performance to that obtained from ITO with a high optical transmittance of 89.2% and a low sheet resistance of ∼12.5 Ω/sq. Unlike pure AgNW films, the sheet resistance is little changed after the tape and ultrasonication tests, illustrating a very strong adhesion to the PET substrate after the encapsulation of MoOx. Moreover, the multilayer film exhibits excellent stability to resist mechanical bending and acid damage. In addition, the successful implementation of the flexible transparent heater demonstrates the practical application value of the electrode.After sufficient doses are manufactured and logistical barriers are reduced, convincing an overwhelming majority of people to receive a COVID-19 vaccination may be the next major challenge during this pandemic. A group of experts recently proposed strategies that have compelling rationales and are well grounded in behavioral science. However, their approaches may sometimes be unacceptable, impractical, and/or unsuccessful. Therefore, other strategies will be greatly needed to address vaccine hesitancy. The present commentary offers 8 additional promising approaches forming a framework known as PANDEMIC. This acronym stands for the following strategies presumptive language, asking for advice, norms on an anonymous level, description of favorable attributes, emphasizing clinicians’ own experiences, mandated choice, images, and communication of risk. Each of the strategies is discussed in turn. Many of the proposed strategies have empirical support for achieving desired outcomes in other domains. However, the PANDEMIC framework is untested in regard to increasing the uptake of COVID-19 vaccinations. Therefore, the strategies should be carefully evaluated before they are widely disseminated through public health announcements, email distribution lists, electronic health record messages, and other outlets.

Corticosteroid injections are proven to be effective in the management of carpal tunnel syndrome (CTS); however, the optimal injection site still remains unclear.

To compare the efficacy of perineural vs. peritendinous target sites for corticosteroid injection in CTS.

A Randomized, Single-Blind, Controlled Trial.

Outpatients, tertiary care center.

Forty-six patients were equally randomized into two intervention groups as Group A (18 F and 5 M, mean age;50.0 ± 15.9 years, mean symptom duration;5.9 ± 3.3 months) and Group B (19 F, 4 M patients, mean age;54.3 ± 15.0 years, mean symptom duration;5.9 ± 4.7 months).

Methylprednisolone acetate (40 mg) and 1 mL of 1% trimecaine hydrochloride was injected next to the median nerve (Group A) or among flexor tendons away from the nerve (Group B) under ultrasound (US) guidance. The visual analogue scale was used as the primary outcome measure, and the symptom severity scale and functional status scale of the Boston Carpal Tunnel Questionnaire were used as the inous injections without compromising the treatment efficacy and safety. Herewith, US guidance is, for sure, necessary for performing safe and accurate injections.

Motor impairments in children with cerebral palsy significantly reduce their ability to learn and adapt bimanual actions into their life roles. The current evidence on bimanual coordination performance in children with hemiplegic cerebral palsy were mostly drawn from kinematic studies. Whether these kinematic findings on bimanual motor performance can be observed when performing daily life activities in a natural environment is not clear. Further, there is no evidence what and how the verbal prompting influences bilateral motor performance. We intend to explore its role on bimanual motor performance as well.

This study aimed to investigate the bimanual motor performance in everyday life activities of children with hemiplegic cerebral palsy and the role of verbal prompts in facilitating affected hand use.

Observational study.

Local medical center and community.

Twenty-five children with hemiplegic cerebral palsy and 25 age-matched typically developing children.

The Observation-based Test of Capacitovements.

Chronic musculoskeletal pain (CMP), Generalized Joint Hypermobility (GJH) and pain-related fear have influence on physical functioning in adolescents.

To evaluate differences in physical functioning between adolescents with CMP, GJH or the combination of both, and in addition evaluate the potential contribution of pain-related fear.

Observational, cross-sectional design.

The adolescents with CMP were recruited by a physician in rehabilitation medicine and measured in the university outpatient rehabilitation clinic (Adelante/Maastricht University Medical Center+, the Netherlands). The adolescents without CMP were recruited in the Southern area of the Netherlands and measured in the university outpatient rehabilitation clinic (Adelante/Maastricht University Medical Center+, the Netherlands).

Four subgroups of adolescents were included; 21 adolescents with CMP without GJH, 9 adolescents with CMP and GJH, 51 adolescents without CMP without GJH, and 11 adolescents without CMP with GJH.

Outcome measures No differences were found in physical functioning and pain-related fear between hypermobile adolescents with CMP compared to nonhypermobile adolescents with CMP. Future rehabilitation treatment in hypermobile adolescents with CMP should also focus on psychological components, such as pain-related fear.

No differences were found in physical functioning and pain-related fear between hypermobile adolescents with CMP compared to nonhypermobile adolescents with CMP. Future rehabilitation treatment in hypermobile adolescents with CMP should also focus on psychological components, such as pain-related fear.