Search

Properties of layered superconductors can vary drastically when thinned down from bulk to monolayer owing to the reduced dimensionality and weakened interlayer coupling. In transition metal dichalcogenides (TMDs), the inherent symmetry breaking effect in atomically thin crystals prompts novel states of matter such as Ising superconductivity with an extraordinary in-plane upper critical field. Here, we demonstrate that two-dimensional (2D) superconductivity resembling those in atomic layers but with more fascinating behaviors can be realized in the bulk crystals of two new TMD-based superconductors Ba 0.75 ClTaS 2 and Ba 0.75 ClTaSe 2 with superconducting transition temperatures 2.75 and 1.75 K, respectively. They comprise an alternating stack of H-type TMD layers and Ba-Cl layers. In both materials, intrinsic 2D superconductivity develops below a Berezinskii-Kosterlitz-Thouless transition. The upper critical field along the ab plane ( H c 2 | | a b ) exceeds the Pauli limit ( μ 0 H p ); in particular, Ba 0.75 ClTaSe 2 exhibits an extremely high μ 0 H c 2 | | a b ≈ 14 μ 0 H p and a colossal superconducting anisotropy ( H c 2 | | a b / H c 2 ⊥ a b ) of ∼150. Moreover, the temperature-field phase diagram of Ba 0.75 ClTaSe 2 under an in-plane magnetic field contains a large phase regime of vortex dissipation, which can be ascribed to the Josephson vortex motion, signifying an unprecedentedly strong fluctuation effect in TMD-based superconductors. Our results provide a new path toward the establishment of 2D superconductivity and novel exotic quantum phases in bulk crystals of TMD-based superconductors.

High-sensitivity fluorescent probes provide a powerful tool for understanding life processes and functioning mechanisms. Therefore, the development of a universal strategy to optimize probes holds substantial importance. Herein, we developed a novel strategy for common probe upgrades: rather than simply pursuing a higher fluorescence intensity of the probe itself, we tried to promote the detection sensitivity by enhancing the probe-substrate interactions. Fortified with polyionic polymers, self-assembled probes could be endowed with enhanced attractions to the substrate. In this work, we took the AChE-AuNCs detection system as a typical and important example to verify this concept of the "enrichment-enhanced detection" strategy (EED strategy). Two probes, AuNCs@GC and AuNCs@CMCS, with similar composing polymers (chitosan derivatives), microstructures, fluorescence profiles, and distinct charges were delicately designed and thoroughly studied. CMCS with an abundance of negatively charged carboxy groups plays an important role in the enrichment of thiocholine through electrostatic interactions. Thus, despite having similar composing components, structures, and almost identical fluorescence profiles, the negatively charged composite shows superior sensitivity (15.2-fold enhancement) and response time (2-fold faster) compared to the AuNCs@GC, thereby validating the feasibility of the EED strategy. Overall, our work validates the EED strategy and applies it to the accurate detection of AChE activity. We believe that this strategy offers substantial insights for the generalization and enhancement of advanced nanoprobes.

The restructuring of dilute alloys under gas environments has shown a great impact on their catalytic performance due to intriguing structural sensitivity, but the structural dynamics and underlying mechanism remains elusive. Herein, we directly resolved the distinct dynamic behaviors of PdFe 0.08 dilute alloys under CO or O 2 environment by multidimensional imaging. The stronger binding of gaseous CO with Fe atoms stimulates Fe segregation out of the PdFe 0.08 , resulting in 3D growth of Fe islands, whereas the dissociative adsorption of O 2 results in 2D layer-by-layer growth of segregated FeO as encapsulation overlayers that bind strongly with the Pd surface underneath. Such varied structures remarkably tune the catalytic activity for CO oxidation, showing a considerably high activity for a CO-treated sample. Our results reveal the competitive mechanism between adsorbate-metal and metal-metal interaction for gas-induced surface segregation, which should be highly considered for the rational design of dilute alloys with dynamically tuned structure and reactivity.

The retinoic acid receptor-related orphan receptor γt (RORγt) is a key regulator of Th17 cells, associated with autoimmune diseases, making it a significant drug target. Herein, we designed and synthesized 1-(phenylsulfonyl)-1,2,3,4-tetrahydroquinoline derivatives, improving upon GSK2981278 to enhance bioavailability. Of which, D4 exhibited superior bioavailability (F = 48.1 and 32.9% in mice and rats, respectively) compared to GSK2981278 (F = 6.2 and 4.1%, respectively), and effectively treated psoriasis in mice at lower doses. Moreover, for the first time, we report the efficacies of a RORγt inverse agonist in mouse models of rheumatoid arthritis. ( R )-D4 , the eutomer of D4 , matched or exceeded GSK2981278's therapeutic effects at lower doses, with no adverse effects observed after 2 weeks of administration. These results position ( R )-D4 as a promising and orally bioavailable candidate for Th17-mediated autoimmune disease treatment.

Perovskite light-emitting diodes (PeLEDs) have attracted significant interest in next-generation intelligent displays. Vacuum deposition is a promising method for integrating PeLEDs into intelligent displays due to its high manufacturability and easy pixelation, as proven in industrial organic light-emitting diode production. However, achieving spatially confined grains with optimized crystal remains challenging in vacuum-deposited perovskite. Here, a trisource coevaporation strategy is proposed to introduce MABr to form the MA x Cs 1- x PbBr 3 structure with carriers' spatial confinement and defect suppression as well. This approach enables PeLEDs to contain excellent external quantum efficiency (EQE), which is nearly 10-fold as the untreated device. Based on this, we realize the first reported vacuum-deposited transparent PeLEDs with double-sided emission and an amazing maximum EQE of 7.6% by replacing Al with an optimized Ag:Mg electrode. These transparent PeLEDs are integrated into a bifunctional intelligent display device with both accurate heart rate detection and imaging display, which exhibit bright patterned emission and accurate heart rate detection.

Room-temperature sodium-sulfur (RT Na-S) batteries with high energy density and low cost are considered promising next-generation electrochemical energy storage systems. However, their practical feasibility is seriously impeded by the shuttle effect of sodium polysulfide (NaPSs) resulting from the sluggish reaction kinetics. Introducing a suitable catalyst to accelerate conversion of NaPSs is the most used strategy to inhibit the shuttle effect. Traditional catalytic approaches often want to avoid the irreversible phase transition of the catalyst at a deep discharge. On the contrary, here, we leverage the intrinsic structural tunability of the MoS 2 catalyst in the opposite direction and innovatively propose a voltage modulation strategy for in situ generation of trace Mo single atoms (Mo SAC ) during the first charge-discharge process, leading to the formation of highly active catalytic phases (MoS 2 /Mo SAC ) through the self-reconstruction. Theoretical calculations reveal that the incorporation of Mo SAC modulates the electronic structure of the Mo d-band center, which not only effectively promotes the d-p orbital hybridization but also accelerates the catalytic intermediate desorption by the bonding transition, the dynamic single-atom synergistic catalytic mechanism enhances the adsorption response between the metal active site and NaPSs, which significantly improves the sulfur redox reaction (SRR), and the initial capacity of the MoS 2 /Mo SAC /CF@S cell at 0.2 A g -1 is increased by 46.58% compared to that of the MoS 2 /CF@S cell. The discovery of the MoS 2 /Mo SAC /CF catalyst provides new insights into adjusting the structure and function of transition metal disulfide catalysts at the atomic scale, offering hope for the development of high-specific-energy RT Na-S batteries.

The neighborhood effect averaging problem (NEAP) is a fundamental statistical phenomenon in mobility-dependent environmental exposures. It suggests that individual environmental exposures tend toward the average exposure in the study area when considering human mobility. However, the universality of the NEAP across various environmental exposures and the mechanisms underlying its occurrence remain unclear. Here, using a large human mobility data set of more than 27 000 individuals in the Chicago Metropolitan Area, we provide robust evidence of the existence of the NEAP in a range of individual environmental exposures, including green spaces, air pollution, healthy food environments, transit accessibility, and crime rates. We also unveil the social and spatial disparities in the NEAP's influence on individual environmental exposure estimates. To further reveal the mechanisms behind the NEAP, we perform multiscenario analyses based on environmental variation and human mobility simulations. The results reveal that the NEAP is a statistical phenomenon of regression to the mean (RTM) under the constraints of spatial autocorrelation in environmental data. Increasing travel distances and out-of-home durations can intensify and promote the NEAP's impact, particularly for highly dynamic environmental factors like air pollution. These findings illuminate the complex interplay between human mobility and environmental factors, guiding more effective public health interventions.

Photodynamic therapy (PDT) has gained widespread acceptance as a clinical cancer treatment modality and has been attracting intensive attention on developing novel PDT strategies. However, the hypoxic environment in tumors is considered as a significant challenge for efficient type II PDT, based on the inference of the highly oxygen-concentration-related 1 O 2 generation. Contrary to this conventional understanding, our research demonstrates oxygen concentration independence in the photosensitized generation of 1 O 2 , as evidenced through steady-state and transient spectroscopy for chlorin e6 and methylene blue from normoxic to hypoxic conditions. We propose an oxygen-concentration-independent kinetic model, suggesting that efficient 1 O 2 generation can take place as long as the triplet-state lifetime ratio of the photosensitizer (τ h /τ n ) is in a similar range to pO 2 n /pO 2 h . Our findings provide insights into PDT mechanisms and indicate that the oxygen concentration reduction concerns may not be critical for effective PDT in hypoxic tumor environments.

Aiming at the time and space limitation of gas control in the first mining face of newly built outburst mine, this study takes Longfeng Coal Mine in Guizhou as the engineering background and puts forward a concept of far- and near-field gas collaborative joint control based on "orientation + general drilling". The correlation between effective extraction radius and extraction time of No. 9 coal seam is determined by establishing the mathematical model of gas migration in which stress field, diffusion field, and seepage field are coupled. Combined with the mining and deployment planning of the first mining face, the three-level strengthened regional gas management scheme of "directional middle, cross-layer, and cross-layer supplement" was designed, the spacing of drilling holes was optimized, and the spatiotemporal collaborative joint management system of gas advanced large areas was constructed. Practice has proven that the three-level gas extraction cooperative and joint management mode adopted in the 1903 first mining face effectively realized the spatiospatial matching of gas extraction and mining progress at all levels, realized the gas extraction standard and safe mining in advance, and provided an effective technical solution for the gas treatment of the first mining face in the newly built outburst mine., Competing Interests: The authors declare no competing financial interest., (© 2024 The Authors. Published by American Chemical Society.)

Aqueous zinc ion batteries are excellent energy storage devices with high safety and low cost. However, the corrosion reaction and zinc dendrite formation occurring on the surface of zinc anodes are hindering their further development. To solve the problems, zirconium acetate (ZA) was used as an electrolyte additive in the ZnSO 4 electrolyte. Attributing to the higher electro-positivity of Zr 4+ than Zn 2+ , these high valence metal cations preferentially adsorb onto the surface of metallic zinc, shielding parasitic reactions between zinc and electrolyte, reshaping the electric field distribution, and directing preferential homogeneous deposition of Zn-ions on the Zn (002) crystal plane. Furthermore, the adsorption of Zr 4+ on the Zn metal after electrochemical cycles can enhance the energy barrier of zinc atom diffusion, resulting in high resistance of corrosion and manipulation of the Zn 2+ nucleation configuration. Attributing to these properties, the Zn//Zn symmetric cell with an electrolyte additive of ZA was able to cycle for 400 h under an extremely high current density of 40 mA cm -2 with an area capacity of 2 mAh cm -2 . Meanwhile, the MnO 2 //Zn coin cell still had 81.7 mAh g -1 (85% retention of capacity) after 850 cycles under a current density of 1 A g -1 .

Time reversal symmetry breaking in superconductors, resulting from external magnetic fields or spontaneous magnetization, often leads to unconventional superconducting properties. In this way, an intrinsic phenomenon called the Fulde-Ferrell-Larkin-Ovchinnikov (FFLO) state may be realized by the Zeeman effect. Here, we construct the FFLO state in an artificial CrOCl/NbSe 2 van der Waals (vdW) heterostructure by utilizing the superconducting proximity effect of NbSe 2 flakes. The proximity-induced superconductivity demonstrates a considerably weak gap of about 0.12 meV, and the in-plane upper critical field reveals the behavior of the FFLO state. First-principles calculations uncover the origin of the proximitized superconductivity, which indicates the importance of Cr vacancies or line defects in CrOCl. Moreover, the FFLO state could be induced by the inherent large spin splitting in CrOCl. Our findings not only provide a practical scheme for constructing the FFLO state but also inspire the discovery of an exotic FFLO state in other two-dimensional vdW heterostructures.

This study conducts a systematic investigation into the catalytic mechanism of norcoclaurine synthase (NCS), a key enzyme in the biosynthesis of tetrahydroisoquinolines (THIQs) with therapeutic applications. By integration of LiGaMD and DFT calculations, the reaction pathway of NCS is mapped, providing detailed insights into its catalytic activity and selectivity. Our findings underscore the critical role of E103 in substrate capture and reveal the hitherto unappreciated influence of nonpolar residues M183 and L76 on tunnel dynamics. A prominent discovery is the identification of a high-energy barrier (44.2 kcal/mol) associated with the aromatic electrophilic attack, which pinpoints the rate-limiting step. Moreover, we disclose the existence of dual transition states leading to different products with the energetically favored six-membered ring formation consistent with experimental evidence. These mechanistic revelations not only refine our understanding of NCS but also advocate for a renewed emphasis on enzyme tunnel engineering for optimizing THIQs biosynthesis. The research sets the stage for translating these findings into practical enzyme modifications. Our results highlight the potential of NCS as a biocatalyst to overcome the limitations of current synthetic methodologies, such as low yields and environmental impacts, and provide a theoretical contribution to the efficient, eco-friendly production of THIQs-based pharmaceuticals.

Enhancing the antimicrobial activity of high-efficiency particulate air (HEPA) filters while maintaining filtration efficiency and pressure drop is currently an urgent issue for preventing the spread of pathogenic microorganisms. Herein, inspired by vines which can enwind fences to fix as well as decorate them, a flexible antimicrobial chitin nanofiber (ChNF@CuO x ) was fabricated and loaded onto the rigid glass fiber (GF) skeleton of a HEPA filter. Through the physical interaction, ChNF@CuO x was spontaneously enwound on GF, and ChNF@CuO x itself interweaved to form a new nanonetwork between the GF skeleton. The obtained antimicrobial air filter (ChNF@CuO x /GF) with a unique nanonetwork increased the filtration efficiency of the HEPA filter. Meanwhile, it possessed excellent inactivation ability against Staphylococcus aureus , Escherichia coli , and Candida albicans due to the urchin-like in situ grown CuO x on the ChNF. In particular, the oxygen vacancies generated unexpectedly in CuO x enabled it to produce reactive oxygen species. After eight cycles of antimicrobial assays, the antimicrobial rates of bacteria were higher than 99.5%, and those of fungi were greater than 98.3%. The successful synthesis of antimicrobial fibers and the construction of multidimensional nanoscale structures through a simple postprocessing method provide a new design mentality for antimicrobial functionalization for HEPA filters.

Diabetic wounds are prone to recurrent infections, often leading to delayed healing. To address this challenge, we developed a chitin-copper sulfide (CuS@CH) composite sponge, which combines bacterial trapping with near-infrared (NIR) activated phototherapy for treating infected diabetic wounds. CuS nanoparticles were synthesized and incorporated in situ within the sponge using a chitin assisted biomineralization strategy. The positively charged chitin surface effectively adhered bacteria, while NIR irradiation of CuS generated reactive oxygen species (ROS) heat and Cu 2+ to rapidly damage the trapped bacteria. This synergistic effect resulted in an exceptional antibacterial performance against E. coli (∼99.9%) and S. aureus (∼99.3%). The bactericidal mechanism involved NIR-induced glutathione oxidation, membrane lipid peroxidation, and increased membrane permeability. In diabetic mouse models, the CuS@CH sponge accelerated the wound healing of S. aureus infected wounds by facilitating collagen deposition and reducing inflammation. Furthermore, the sponge demonstrated good biocompatibility. This dual-functional platform integrating bacterial capture and NIR-triggered phototherapy shows promise as an antibacterial wound dressing to promote healing of infected diabetic wound.

Foodborne illnesses caused by Salmonella bacteria pose a significant threat to public health. It is still challenging to detect them effectively. Herein, biotemplated Janus disk-shaped magnetic microrobots (BJDMs) based on diatomite are developed for the highly efficient detection of Salmonella in milk. The BJDMs were loaded with aptamer, which can be magnetically actuated in the swarm to capture Salmonella in a linear range of 5.8 × 10 2 to 5.8 × 10 5 CFU/mL in 30 min, with a detection limit as low as 58 CFU/mL. In addition, the silica surface of BJDMs exhibited a large specific surface area to adsorb DNA from captured Salmonella, and the specificity was also confirmed via tests of a mixture of diverse foodborne bacteria. These diatomite-based microrobots hold the advantages of mass production and low cost and could also be extended toward the detection of other types of bacterial toxins via loading different probes. Therefore, this work offers a reliable strategy to construct robust platforms for rapid biological detection in practical applications of food safety.

Electronic-grade isopropyl alcohol is widely utilized in the cleaning of semiconductors and microelectronic components. Removing ions like Pb 2+ is crucial since the presence of impurities may cause degradation of electronics, increased failure rates, and short circuits. Membrane materials offer a number of advantages in the field of adsorption separation; however, the lack of adsorption sites results in limited adsorption capacity. In the current work, guanidino-grafted NH 2 -MIL-101(Fe) was incorporated into polyvinylidene fluoride (PVDF) to prepare MOF/PVDF mixed matrix membranes (NM/PVDF) for the removal of Pb 2+ from isopropanol. Benefiting from the larger specific surface area and more lone electron pairs in the guanidine group, the Pb 2+ adsorption capacity of the as-prepared NM/PVDF membrane was 29.4458 mg/g, which was higher than that of the NH 2 -MIL-101(Fe)/PVDF membrane (20.9306 mg/g) and the pure PVDF membrane (6.7324 mg/g). The NM/PVDF membrane was able to reduce the concentration of Pb 2+ from 500 to 86.73 ppb. This work highlights the potential of guanidine-grafted Fe-based MOFs/PVDF membranes as adsorbents for acquisition of electronic-grade solvents.

The FLT3-ITD (internal tandem duplication) mutant has been a promising target for acute myeloid leukemia (AML) drug discovery but is now facing the challenge of resistance due to point mutations. Herein, we have discovered a type II FLT3 inhibitor, SILA-123 . This inhibitor has shown highly potent inhibitory effects against FLT3-WT (IC 50 = 2.1 nM) and FLT3-ITD (IC 50 = 1.0 nM), tumor cells with the FLT3-ITD mutant such as MOLM-13 (IC 50 = 0.98 nM) and MV4-11 (IC 50 = 0.19 nM), as well as BaF3 cells associated with the FLT3-ITD mutant and point mutations like BaF3-FLT3-ITD-G697R (IC 50 = 3.0 nM). Moreover, SILA-123 exhibited promising kinome selectivity against 310 kinases (S score (10) = 0.06). In in vivo studies, SILA-123 significantly suppressed the tumor growth in MV4-11 (50 mg/kg/d, TGI = 87.3%) and BaF3-FLT3-ITD-G697R (50 mg/kg/d, TGI = 60.0%) cell-inoculated allograft models. Our data suggested that SILA-123 might be a promising drug candidate for FLT3-ITD-positive AML.

Ship emissions are a significant source of air pollution, and the primary policy to control is fuel oil quality improvement. However, the impact of this policy on particle size distribution and composition characteristics remains unclear. Measurements were conducted on nine different vessels (ocean-going vessels, coastal cargo ships, and inland cargo ships) to determine the impact of fuel upgrading ( S < 0.1% m/m marine gas oil (MGO) vs S < 0.5% m/m heavy fuel oil (HFO)) on elemental carbon (EC) and polycyclic aromatic hydrocarbons (PAHs) emitted by ships. (1) Fuel improvement significantly reduced EC and PAH emission, by 31 ± 25 and 45 ± 38%, respectively. However, particle size distributions showed a trend toward finer particles, with the peak size decreasing from D P = 0.38-0.60 μm (HFO) to D P = 0.15-0.25 μm (MGO), and the emission factor of D P < 100 nm increased. (2) Changes in emission characteristics led to an increase in the toxicity of ultrafine particulate matter. (3) Ship types and engine conditions affected the EC and PAH particle size distributions. Inland ships have a more concentrated particle size distribution. Higher loads result in higher emissions. (4) The composition and engine conditions of fuel oils jointly affected pollutant formation mechanisms. MGO and HFO exhibited opposite EC emissions when emitting the same level of PAHs.

Circulating tumor cells (CTCs) are recognized as promising targets for liquid biopsy, which play an important role in early diagnosis and efficacy monitoring of cancer. However, due to the extreme scarcity of CTCs and partial size overlap between CTCs and white blood cells (WBCs), the separation and detection of CTCs from blood remain a big challenge. To address this issue, we fabricated a microfluidic chip by integrating a passive contraction-expansion array (CEA) inertial sorting zone and an active magnetophoresis zone with the trapezoidal groove and online coupled it with inductively coupled plasma mass spectrometry (ICP-MS) for rapid separation and precise detection of MCF-7 cells (as a model CTC) in blood samples. In the integrated microfluidic chip, most of the small-sized WBCs can be rapidly removed in the circular CEA inertial sorter, while the rest of the magnetically labeled WBCs can be further captured in the trapezoidal groove under the magnetic field. As a result, the rapid separation of MCF-7 cells from blood samples was achieved with an average recovery of 91.6% at a sample flow rate of 200 μL min -1 . The developed online integrated inertial-magnetophoresis microfluidic chip-ICP-MS system has been applied for the detection of CTCs in real clinical blood samples with a fast analysis speed (5 min per 1 mL blood). CTCs were detected in all 24 blood samples from patients with different types of cancer, exhibiting excellent application potential in clinical diagnosis.

Transition metal sulfides (TMSs) show the potential to be competitive candidates as next-generation anode materials for Li-ion batteries (LIBs) due to their high theoretical specific capacity. However, sluggish ionic/electronic transportation and huge volume change upon lithiation/delithiation remain major challenges in developing practical TMS anodes. We rationally combine structural design and interface engineering to fabricate a tubular-like nanocomposite with embedded crystalline Cu 9 S5 nanoparticles and amorphous MoS x in a carbon matrix (C/Cu 9 S 5 -MoS x NTs). On the one hand, the hybrid integrated the advantages of 1D hollow nanostructures and carbonaceous materials, whose high surface-to-volume ratios, inner void, flexibility, and high electronic conductivity not only enhance ion/electron transfer kinetics but also effectively buffer the volume changes of metal sulfides during charge/discharge. On the other hand, the formation of crystalline-amorphous heterostructures between Cu 9 S 5 and MoS x could further boost charge transfer due to an induced built-in electric field at the interface and the presence of a long-range disorder phase. In addition, amorphous MoS x offers an extra elastic buffer layer to release the fracture risk of Cu 9 S 5 crystalline nanoparticles during repetitive electrochemical reactions. Benefiting from the above synergistic effect, the C/Cu 9 S 5 -MoS x electrode as an LIB anode in an ether-based electrolyte achieves a high-rate capability (445 mAh g -1 at 6 A g -1 ) and superior ultralong-term cycling stability, which delivers an initial discharge capacity of 561 mAh g -1 at 2 A g -1 and its retention capacity after 3600 cycles (376 mAh g -1 ) remains higher than that of commercial graphite (372 mAh g -1 ).

Ternary content-addressable memory (TCAM) is promising for data-intensive artificial intelligence applications due to its large-scale parallel in-memory computing capabilities. However, it is still challenging to build a reliable TCAM cell from a single circuit component. Here, we demonstrate a single transistor TCAM based on a floating-gate two-dimensional (2D) ambipolar MoTe 2 field-effect transistor with graphene contacts. Our bottom graphene contacts scheme enables gate modulation of the contact Schottky barrier heights, facilitating carrier injection for both electrons and holes. The 2D nature of our channel and contact materials provides device scaling potentials beyond silicon. By integration with a floating-gate stack, a highly reliable nonvolatile memory is achieved. Our TCAM cell exhibits a resistance ratio larger than 1000 and symmetrical complementary states, allowing the implementation of large-scale TCAM arrays. Finally, we show through circuit simulations that in-memory Hamming distance computation is readily achievable based on our TCAM with array sizes up to 128 cells.

Bacterial infections have been a serious threat to mankind throughout history. Natural antimicrobial peptides (AMPs) and their membrane disruption mechanism have generated immense interest in the design and development of synthetic mimetics that could overcome the intrinsic drawbacks of AMPs, such as their susceptibility to proteolytic degradation and low bioavailability. Herein, by exploiting the self-assembly and pore-forming capabilities of sequence-defined peptoids, we discovered a family of low-molecular weight peptoid antibiotics that exhibit excellent broad-spectrum activity and high selectivity toward a panel of clinically significant Gram-positive and Gram-negative bacterial strains, including vancomycin-resistant Enterococcus faecalis (VREF), methicillin-resistant Staphylococcus aureus (MRSA), methicillin-resistant Staphylococcus epidermidis (MRSE), Escherichia coli , Pseudomonas aeruginosa , and Klebsiella pneumoniae . Tuning the peptoid side chain chemistry and structure enabled us to tune the efficacy of antimicrobial activity. Mechanistic studies using transmission electron microscopy (TEM), bacterial membrane depolarization and lysis, and time-kill kinetics assays along with molecular dynamics simulations reveal that these peptoids kill both Gram-positive and Gram-negative bacteria through a membrane disruption mechanism. These robust and biocompatible peptoid-based antibiotics can provide a valuable tool for combating emerging drug resistance.

Contact engineering on monolayer layer (ML) semiconducting transition metal dichalcogenides (TMDs) is considered the most challenging problem toward using these materials as a transistor channel in future advanced technology nodes. The typically observed strong Fermi-level pinning induced in part by the reaction of the source/drain contact metal and the ML TMD frequently results in a large Schottky barrier height, which limits the electrical performance of ML TMD field-effect transistors (FETs). However, at a microscopic level, little is known about how interface defects or reaction sites impact the electrical performance of ML TMD FETs. In this work, we have performed statistically meaningful electrical measurements on at least 120 FETs combined with careful surface analysis to unveil contact resistance dependence on interface chemistry. In particular, we achieved a low contact resistance for ML MoS 2 FETs with ultrahigh-vacuum (UHV, 3 × 10 -11 mbar) deposited Ni contacts, ∼500 Ω·μm, which is 5 times lower than the contact resistance achieved when deposited under high-vacuum (HV, 3 × 10 -6 mbar) conditions. These electrical results strongly correlate with our surface analysis observations. X-ray photoelectron spectroscopy (XPS) revealed significant bonding species between Ni and MoS 2 under UHV conditions compared to that under HV. We also studied the Bi/MoS 2 interface under UHV and HV deposition conditions. Different from the case of Ni, we do not observe a difference in contact resistance or interface chemistry between contacts deposited under UHV and HV. Finally, this article also explores the thermal stability and reliability of the two contact metals employed here.

Toxic heavy metals are widely present in typical scenarios, such as mines and electroplating wastewater, presenting significant risks to biological and environmental safety. Membrane processes encounter a challenge in effectively intercepting heavy metals due to their small hydration radius. This research showcases the high efficiency of micelle-enhanced nanofiltration (MENF) in removing heavy metals. At the critical micelle concentration, sodium dodecyl sulfate demonstrated a high removal of Cu 2+ , Ni 2+ , Zn 2+ , and Cd 2+ while maintaining substantial potential for complexation of heavy metals. The formation of micelles and the bonding of heavy metals with surfactants bolstered the resistance of heavy metal ions to transmembrane transport. The presence of heavy metals in ionic form in wastewater facilitated their complexation with surfactants or micelles. Notably, the valence state and concentration of interfering ions in the environment could slightly influence the removal of heavy metals by MENF. Additionally, MENF displayed remarkable antifouling properties. The loose gel layer created by surfactant molecules and the micelle enhanced the membrane permeability and reduced the scaling tendency of heavy metals. This study contributes to an improved understanding of the mechanisms involved in heavy metal rejection by using MENF.

Copper-doped Bi 2 Se 3 (Cu x Bi 2 Se 3 ) is of considerable interest for tailoring its electronic properties and inducing exotic charge correlations while retaining the unique Dirac surface states. However, the copper dopants in Cu x Bi 2 Se 3 display complex electronic behaviors and may function as either electron donors or acceptors depending on their concentration and atomic sites within the Bi 2 Se 3 crystal lattice. Thus, a precise understanding and control of the doping concentration and sites is of both fundamental and practical significance. Herein, we report a solution-based one-pot synthesis of Cu x Bi 2 Se 3 nanoplates with systematically tunable Cu doping concentrations and doping sites. Our studies reveal a gradual evolution from intercalative sites to substitutional sites with increasing Cu concentrations. The Cu atoms at intercalative sites function as electron donors while those at the substitutional sites function as electron acceptors, producing distinct effects on the electronic properties of the resulting materials. We further show that Cu 0.18 Bi 2 Se 3 exhibits superconducting behavior, which is not present in Bi 2 Se 3 , highlighting the essential role of Cu doping in tailoring exotic quantum properties. This study establishes an efficient methodology for precise synthesis of Cu x Bi 2 Se 3 with tailored doping concentrations, doping sites, and electronic properties., Competing Interests: The authors declare no competing financial interest., (© 2024 The Authors. Co-published by University of Science and Technology of China and American Chemical Society.)

Self-powered wearable electronic products have rapidly advanced in the fields of sensing and health monitoring, presenting greater challenges for triboelectric materials. The limited surface polarity and structural defects in wood fibers restrict their potential as substitutes for petroleum-based materials. This study used bagasse fiber as the raw material and explored various methods, including functionalizing cellulose nanofibrils (CNFs) with polydopamine (PDA), in situ embedding of silver particles, filtration, and freeze-drying. These methods aimed to enhance the triboelectric output, antibacterial properties, and filtration properties of lignocellulosic materials. The Ag/PDA/CNF-based triboelectric nanogenerator (TENG) demonstrated an open-circuit voltage of 211 V and a short-circuit current of 18.1 μA. An aerogel prepared by freeze-drying the Ag/PDA/CNF material, combined with a polyvinylidene fluoride nanofiber structure fabricated by electrospinning, constitutes the TENG unit. A self-powered respiratory detection mask was created using this combination, achieving a filtration efficiency of 94.23% for 0.3 μm particles and an antibacterial rate exceeding 99%. In addition, it effectively responded to respiratory frequency signals of slow breathing, normal breathing, and shortness of breath, with the output electrical signal correlating with the respiratory frequency. This study considerably contributes to advancing wood fiber-based triboelectric materials as alternatives to petroleum-derived materials in self-powered wearable electronic products for medical applications., Competing Interests: The authors declare no competing financial interest., (© 2024 The Authors. Published by American Chemical Society.)

Steviol glycosides (SGs) are a natural sweetener widely used in the food and beverage industry, but the low solubility and stability of SG aqueous solutions greatly limit their application performance, especially in liquid formulations. In this work, we explore the solubility behavior of rebaudioside A (Reb A) in water, a major component of SGs, with the aim of clarifying the underlying mechanisms of the solubility and stability constraints of SGs, as well as the impact on their multifunctional properties. We demonstrate for the first time that Reb A exhibits hierarchical self-assembly in solutions, forming spherical micelles first when the concentration exceeds its critical micelle concentration (5.071 mg/mL), which then further assemble into large rod-like aggregates. The formation of such large Reb A aggregates is mainly dominated by hydrogen bonding and short-range Coulomb interaction energy, thus leading to the low solubility and precipitation of Reb A solutions. Surprisingly, aggregated Reb A structures display significantly improved organoleptic properties, revealing that self-aggregation can be developed as a simple, efficient, and green strategy for improving the taste profile of SGs. Additionally, the self-aggregation of Reb A at high concentrations impairs active encapsulation and also affects its interfacial and emulsifying properties.

There has been widespread concern about the health hazards of per- and polyfluoroalkyl substances (PFAS), which may be the risk factor for hyperuricemia with evidence still insufficient in the general population in China. Here, we conducted a nationwide study involving 9,580 adults aged 18 years or older from 2017 to 2018, measured serum concentrations of uric acid and PFAS (PFOA, PFOS, 6:2 Cl-PFESA, PFNA, PFHxS) in participants, to assess the associations of individual PFAS with hyperuricemia, and estimated a joint effect of PFAS mixtures. We found positive associations of higher serum PFAS with elevated odds of hyperuricemia in Chinese adults, with the greatest contribution from PFOA (69.37%). The nonmonotonic dose-response (NMDR) relationships were observed for 6:2 Cl-PFESA and PFHxS with hyperuricemia. Participants with less marine fish consumption, overweight, and obesity may be the sensitive groups to the effects of PFAS on hyperuricemia. We highlight the potential health hazards of legacy long-chain PFAS (PFOA) once again because of the higher weights of joint effects. This study also provides more evidence about the NMDR relationships in PFAS with hyperuricemia and emphasizes a theoretical basis for public health planning to reduce the health hazards of PFAS in sensitive groups.

Two-dimensional (2D) semiconducting materials with anisotropic physical properties have induced lively interest due to their application in the field of polarizing devices. Herein, we have designed a family of penta-PtXY (X = Se, Te; Y = S, Te; X ≠ Y) monolayers and predicted the electronic and optical properties based on the first-principles calculation. The results suggest that the penta-PtXY (X = Se, Te; Y = S, Te; X ≠ Y) monolayers are indirect-gap semiconductors with a medium bandgap of 2.29-2.66 eV. The penta-PtXY (X = Se, Te; Y = S, Te; X ≠ Y) monolayers own a remarkable mechanical anisotropy with a high Young's modulus anisotropic ratio (3.0). In addition, the penta-PtXY (X = Se, Te; Y = S, Te; X ≠ Y) monolayers exhibit a high anisotropy ratio of hole/electron mobility in the x and y directions (1.16-3.54). The results calculated by the G 0 W 0 +BSE method indicate that the single-layers also bear a salient optical anisotropy ratio (1.56-2.11). The integration of the anisotropic electronic, optical, and mechanical properties entitles penta-PtXY (X = Se, Te; Y = S, Te; X ≠ Y) monolayers as potential candidates in multifunctional polarized nanodevices., Competing Interests: The authors declare no competing financial interest., (© 2024 The Authors. Published by American Chemical Society.)

The slow redox kinetics of lithium-sulfur batteries severely limit their application, and sulfur utilization can be effectively enhanced by designing different cathode sulfur host materials. Herein, we report the hollow porous nanofiber LaNi 0.6 Co 0.4 O 3 as a bidirectional host material for lithium-sulfur batteries. After Co is substituted into LaNiO 3 , oxygen vacancies are generated to enhance the material conductivity and enrich the active sites of the material, and the electrochemical reaction rate can be further accelerated by the synergistic catalytic ability of Ni and Co elements in the B-site of the active site of LaNi 0.6 Co 0.4 O 3 . As illustrated by the kinetic test results, LaNi 0.6 Co 0.4 O 3 effectively accelerated the interconversion of lithium polysulfides, and the nucleation of Li 2 S and the dissolution rate of Li 2 S were significantly enhanced, indicating that LaNi 0.6 Co 0.4 O 3 accelerated the redox kinetics of the lithium-sulfur battery during the charging and discharging process. In the electrochemical performance test, the initial discharge specific capacity of S/LaNi 0.6 Co 0.4 O 3 was 1140.4 mAh g -1 at 0.1 C, and it was able to release a discharge specific capacity of 584.2 mAh g -1 at a rate of 5 C. It also showed excellent cycling ability in the long cycle test, with a single-cycle capacity degradation rate of only 0.08%. Even under the harsh conditions of high loaded sulfur and low electrolyte dosage, S/LaNi 0.6 Co 0.4 O 3 still delivers excellent specific capacity and excellent cycling capability. Therefore, this study provides an idea for the future development of bidirectional high-activity electrocatalysts for lithium-sulfur batteries.

Organic matter (OM) and clay minerals are important components in shale, which are intimately associated with each other in the form of organoclay complexes. The diverse mineral-OM associations result in varying OM occurrences, which possess distinct hydrocarbon generation potential and ultimately affect the accumulation of shale oil. Therefore, the investigation of the heterogeneity of organoclay complexes is crucial to gaining a comprehensive understanding of the varying exploration potential of shale oil resources. In the present study, shale samples from three intervals in Dongying Depression were collected to investigate the mineralogical and organic characteristics of the organoclay complexes, aiming to explore their impact on the yield and composition of shale oil. Results showed that the smectite gradually converted into illite, which was accompanied by the release of OM from clay mineral interlayers and the desorption of chemically adsorbed OM. The yield and composition of shale oil cannot solely be explained by the OM content and types in the shale. Instead, they are intricately linked to the evolution of minerals and OM occurrence. From the perspective of the heterogeneity of organoclay complexes, despite the abundant OM content in shallower intervals (Es3x), the shale oil formation remains limited due to the low degree of mineral evolution and the stabilization of the adsorbed OM by clay minerals. Consequently, this leads to a higher proportion of resin, which is not conducive to the mobility of shale oil. In contrast, despite the OM content varying slightly in the deeper interval (Es4s), the elevated smectite illitization degree promotes the desorption of OM and its conversion into hydrocarbons. This results in a substantial increase in shale oil formation and a higher proportion of saturates, greatly enhancing the mobility of shale oil. These findings are profoundly significant for understanding shale oil generation and accumulation., Competing Interests: The authors declare no competing financial interest., (© 2024 The Authors. Published by American Chemical Society.)

Simultaneous circular dichroism and wavefront manipulation have gained considerable attention in various applications, such as chiroptical spectroscopy, chiral imaging, sorting and detection of enantiomers, and quantum optics, which can improve the miniaturization and integration of the optical system. Typically, structures with n-fold rotational symmetry ( n ≥ 3) are used to improve circular dichroism, as they induce stronger interactions between the electric and magnetic fields. However, manipulating the wavefront with these structures remains challenging because they are commonly considered isotropic and lack a geometric phase response in linear optics. Here, we propose and experimentally demonstrate an approach to achieve simultaneous circular dichroism (with a maximum value of ∼0.62) and wavefront manipulation using a plasmonic metasurface made up of C3 Archimedes spiral nanostructures. The circular dichroism arises from the magnetic dipole-dipole resonance and strong interactions between adjacent meta-atoms. As a proof of concept, two metadevices are fabricated and characterized in the near-infrared regime. This configuration possesses the potential for future applications in photodetection, chiroptical spectroscopy, and the customization of linear and nonlinear optical responses.

Sodium-ion batteries (SIBs) have significant potential for applications in portable electric vehicles and intermittent renewable energy storage due to their relatively low cost. Currently, hard carbon (HC) materials are considered commercially viable anode materials for SIBs due to their advantages, including larger capacity, low cost, low operating voltage, and inimitable microstructure. Among these materials, renewable biomass-derived hard carbon anodes are commonly used in SIBs. However, the reports about biomass hard carbon from basic research to industrial applications are very rare. In this paper, we focus on the research progress of biomass-derived hard carbon materials from the following perspectives: (1) sodium storage mechanisms in hard carbon; (2) optimization strategies for hard carbon materials encompassing design, synthesis, heteroatom doping, material compounding, electrolyte modulation, and presodiation; (3) classification of different biomass-derived hard carbon materials based on precursor source, a comparison of their properties, and a discussion on the effects of different biomass sources on hard carbon material properties; (4) challenges and strategies for practical of biomass-derived hard carbon anode in SIBs; and (5) an overview of the current industrialization of biomass-derived hard carbon anodes. Finally, we present the challenges, strategies, and prospects for the future development of biomass-derived hard carbon materials.

Flexible sensors are of great interest due to their potential applications in human physiological signal monitoring, wearable devices, and healthcare. However, sensor devices employed for cardiovascular testing are normally bulky and expensive, which hamper wearability and point-of-care use. Herein, we report a simple method for preparing multifunctional flexible sensors using hydrazine hydrate (N 2 H 4 ·H 2 O) as the reducing agent, graphene as the active material, and polyethylene (PE) tape as the encapsulation material. The flexible sensor produced with this method has a low detection limit of 100 mg, a fast response and recovery time of 40 and 20 ms, and shows no performance degradation even after up to 30,000 motion cycles. The sensors we have developed are capable of monitoring the pulse with relative accuracy, which presents an opportunity to replace bulky devices and normalize cardiovascular testing in the future. In order to further broaden the application field, the sensor is installed as a sensor array to recognize objects of different weights and shapes, showing that the sensor has excellent application potential in wearable artificial intelligence.

Herein, we disclosed a highly efficient pathway toward 3-selenylated chromone derivatives via electrocatalytic cascade selenylation/cyclization/deamination of 2-hydroxyaryl enaminones with diselenides. This method showed mild conditions, easy operation, wide substrate scope, and good functional group tolerance. Furthermore, this electrosynthesis strategy was amendable to scale-up the reaction. Additionally, the preliminary experiments revealed that this reaction probably proceeded via a cation pathway instead of a radical pathway.

Developing inexpensive, efficient, and stable catalysts is crucial for reducing the cost of electrolytic hydrogen production. Recently, polyoxometalates (POMs) have gained attention and widespread use due to their excellent electrocatalytic properties. This study designed and synthesized three composite materials, NF/PMo n W 12- n , by using phosphomolybdic-tungstic heteropolyacids as precursors to grow in situ on nickel foam via the hydrothermal process and subsequent calcination. Then, their catalytic performances are systematically investigated. This work demonstrates that the NF/PMo n W 12- n catalysts generate more low valent oxides under the synergistic effect of Mo and W, further enhancing activity for hydrogen evolution reaction (HER). Among these electrocatalysts, NF/PMo 6 W 6 exhibits the perfect HER performance, η 10 is only 74 mV. It also shows great stability during long-term electrolysis. The current study introduces a fresh approach for producing electrocatalysts that are both cost-effective and highly efficient.

We were attracted to the therapeutic potential of inhibiting Casitas B-lineage lymphoma proto-oncogene-b (Cbl-b), a RING E3 ligase that plays a critical role in regulating the activation of T cells. However, given that only protein-protein interactions were involved, it was unclear whether inhibition by a small molecule would be a viable approach. After screening an ∼6 billion member DNA-encoded library (DEL) using activated Cbl-b, we identified compound 1 as a hit for which the cis -isomer ( 2 ) was confirmed by biochemical and surface plasmon resonance (SPR) assays. Our hit optimization effort was greatly accelerated when we obtained a cocrystal structure of 2 with Cbl-b, which demonstrated induced binding at the substrate binding site, namely, the Src homology-2 (SH2) domain. This was quite noteworthy given that there are few reports of small molecule inhibitors that bind to SH2 domains and block protein-protein interactions. Structure- and property-guided optimization led to compound 27 , which demonstrated measurable cell activity, albeit only at high concentrations., Competing Interests: The authors declare no competing financial interest., (© 2024 American Chemical Society.)

Promising targeted therapy options to overcome drug resistance and side effects caused by platinum(II) drugs for treatment in hepatocellular carcinoma are urgently needed. Herein, six novel multifunctional platinum(IV) complexes through linking platinum(II) agents and glycyrrhetinic acid (GA) were designed and synthesized. Among them, complex 20 showed superior antitumor activity against tested cancer cells including cisplatin resistance cells than cisplatin and simultaneously displayed good liver-targeting ability. Moreover, complex 20 can significantly cause DNA damage and mitochondrial dysfunction, promote reactive oxygen species generation, activate endoplasmic reticulum stress, and eventually induce apoptosis. Additionally, complex 20 can effectively inhibit cell migration and invasion and trigger autophagy and ferroptosis in HepG-2 cells. More importantly, complex 20 demonstrated stronger tumor inhibition ability than cisplatin or the combo of cisplatin/GA with almost no systemic toxicity in HepG-2 or A549 xenograft models. Collectively, complex 20 could be developed as a potential anti-HCC agent for cancer treatment.

Magnetic micro/nanorobots are promising platforms for targeted drug delivery, and their construction with soft and flexible features has received extensive attention for practical applications. Despite significant efforts in this field, facile fabrication of magnetic microrobots with flexible structures and versatility in targeted therapy remains a big challenge. Herein, we proposed a novel universal strategy to fabricate a biohybrid flexible sperm-like microrobot (BFSM) based on a Chlorella ( Ch .) cell and artificial flagella, which showed great potential for targeted chemo-photothermal therapy for the first time. In this approach, microspherical Ch. cells were utilized to construct the microrobotic heads, which were intracellularly deposited with core-shell Pd@Au, extracellularly magnetized with Fe 3 O 4 , and further loaded with anticancer drug. The magnetic heads with excellent photothermal and chemotherapeutic capability were further assembled with flexible polypyrrole nanowires via biotin-streptavidin bonding to construct the BFSMs. Based on the exquisite head-to-tail structures, the BFSMs could be effectively propelled under precessing magnetic fields and move back and forth without a U-turn. Moreover, in vitro chemo-photothermal tests were conducted to verify their performance of targeted drug delivery toward localized HeLa cells. Due to this superior versatility and facile fabrication, the BFSMs demonstrated great potential for targeted anticancer therapy.

Recovery and separation of anthropogenic emissions of electronic specialty gases (F-gases, such as CF 4 and SF 6 ) from the semiconductor sector are of critical importance. In this work, the hierarchical porous UiO-66-Br 2 @PS/DVB-packed column was constructed by a high internal phase emulsions strategy. UiO-66-Br 2 @PS/DVB exhibits a superior selectivity of CF 4 /N 2 (2.67) and SF 6 /N 2 (3.34) predicted by the IAST due to the diffusion limitation in the micropore and the gas-framework affinity. Especially, UiO-66-Br 2 @PS/DVB showed significant CF 4 and SF 6 retention and enabled the successful separation of CF 4 /N 2 and SF 6 /N 2 with a resolution of 2.37 and 8.89, respectively, when used as a packed column in gas chromatography. Compared with the Porapak Q column, the HETP of the UiO-66-Br 2 @PS/DVB-packed column decreased and showed good reproducibility. This research not only offers a convenient method for fabricating a hierarchical porous MOF-packed column but also showcases the prospective utilization of MOFs for the separation of the F-gas/N 2 mixture.

Although cisplatin has been widely used for clinical purposes, its application is limited due to its obvious side effects. To mitigate the defects of cisplatin, here, six "multitarget prodrugs" were synthesized by linking cisplatin and NF-κB inhibitors. Notably, complex 9 demonstrated a 63-fold enhancement in the activity against A549/CDDP cells with lower toxicity toward normal LO2 cells compared to cisplatin. Additionally, complex 9 could effectively cause DNA damage, induce mitochondrial dysfunction, generate reactive oxygen species, and induce cell apoptosis through the mitochondrial pathway and ER stress. Remarkably, complex 9 effectively inhibited the NF-κB/MAPK signaling pathway and disrupted the PI3K/AKT signaling transduction. Importantly, complex 9 showed superior in vivo antitumor efficiency compared to cisplatin or the combination of cisplatin/ 4 , without obvious systemic toxicity in A549 or A549/CDDP xenograft models. Our results demonstrated that the dual-acting mechanism endowed the complexes with high efficiency and low toxicity, which may represent an efficient strategy for cancer therapy.

Removal of hetero ions from the hydrogen peroxide solution is a crucial step in purifying electronic-grade H 2 O 2 . Conventional adsorption materials are challenged to meet the need for the simultaneous adsorption of both anions and cations in solvents. UiO-66 (Zr) modified by acetic acid and amino group for simultaneous adsorption of phosphate and Pb 2+ in H 2 O 2 purification was fabricated in this work. The as-prepared defective UiO-66-NH 2 (Zr) demonstrated a significant increase in specific surface area and porosity, along with more exposed sites for phosphate and Pb 2+ adsorption. The adsorption capacity of De-UiO-66-NH 2 for phosphate and Pb 2+ in H 2 O 2 solution was 52.28 mg g -1 and 35.4 mg g -1 , which is 1.19 times and 1.88 times that of unmodified UiO-66 (Zr), respectively. The trace simultaneous adsorption with both 100 ppb phosphate and Pb 2+ showed removal rates of 94.0% and 88.7%, respectively, confirming the practicality of MOF materials in the purification of electronic chemicals. This work highlights the potential of Zr-based MOFs as anionic and cationic simultaneous adsorbents for highly efficient purification of electronic-grade solvents.

Synthetic biology is creating genetically engineered organisms at an increasing rate for many potentially valuable applications, but this potential comes with the risk of misuse or accidental release. To begin to address this issue, we have developed a system called GUARDIAN that can automatically detect signatures of engineering in DNA sequencing data, and we have conducted a blinded test of this system using a curated Test and Evaluation (T&E) data set. GUARDIAN uses an ensemble approach based on the guiding principle that no single approach is likely to be able to detect engineering with perfect accuracy. Critically, ensembling enables GUARDIAN to detect sequence inserts in 13 target organisms with a high degree of specificity that requires no subject matter expert (SME) review.

Graphene oxide (GO) exhibits a strong adsorption capacity for the removal of heavy metal ions from liquids, making it a topic of increasing interest among researchers. However, a significant challenge persists in the preparation of graphene oxide-based adsorbents that possess both high structural stability and excellent adsorption capacity. In this paper, a green and environmentally friendly ternary composite aerogel based on graphene was successfully synthesized. The adsorption capacity of graphene oxide was enhanced through diethylenetriaminepentaacetic acid modification, while the incorporation of composite carboxymethyl cellulose improved the structural stability of the composite aerogel in liquid. The composite aerogel demonstrates robust interactions between its components and features a multiscale porous structure. Adsorption tests conducted with Pb(II) revealed that the GO/DTPA/CMC (GDC) composite aerogel exhibits a favorable adsorption capacity. The study of adsorption kinetics and isotherms indicated that the adsorption process follows the quasi-secondary adsorption model and Freundlich adsorption model, suggesting a chemical multilayer adsorption mechanism, and the maximum adsorption capacity for Pb(II) ions was 521.917 mg/g based on the quasi-quadratic kinetic model fitting. X-ray photoelectron spectroscopy (XPS) and scanning electron microscopy (SEM) analyses, performed before and after adsorption, confirmed that the adsorption of Pb(II) primarily occurs through chelation, complexation, proton exchange, and electrostatic interactions between ions and active sites such as hydroxyl and carboxyl groups. This study presents an innovative strategy for simultaneously enhancing the adsorption properties of graphene oxide-based composite aerogels and ensuring solution stability.

Cytochrome P450 1B1 (CYP1B1) contributes to the metabolic inactivation of chemotherapeutics when overexpressed in tumor cells. Selective inhibition of CYP1B1 holds promise for reversing drug resistance. In our pursuit of potent CYP1B1 inhibitors, we designed and synthesized a series of 2-phenylquinazolin-4-amines. A substantial proportion of these newly developed inhibitors demonstrated inhibitory activity against CYP1B1, accompanied by improved water solubility. Remarkably, compound 14b exhibited exceptional inhibitory efficacy and selectivity toward CYP1B1. Molecular docking studies suggested that the expansion of the π-system through aromatization, the introduction of an amine group, and iodine atom augmented the binding affinity. Furthermore, inhibitors 14a , 14b , and 14e demonstrated the ability to significantly reduce the resistance in A549 cells to paclitaxel, while also inhibiting the migration and invasion of these cells. Finally, radioiodine labeling experiments shed light on the metabolic pathway of compound 5l in mice, highlighting the potential of 125 I- 5l as a radioactive probe for future research endeavors.

Over the past decades, the role of rearranged during transfection (RET) alterations in tumorigenesis has been firmly established. RET kinase inhibition is an essential therapeutic target in patients with RET-altered cancers. In clinical practice, initial efficacy can be achieved in patients through the utilization of multikinase inhibitors (MKIs) with RET inhibitory activity. However, the effectiveness of these MKIs is impeded by the adverse events associated with off-target effects. Recently, many RET-selective inhibitors, characterized by heightened specificity and potency, have been developed, representing a substantial breakthrough in the field of RET precision oncology. This Perspective focuses on the contemporary understanding of RET mutations, recent advancements in next-generation RET inhibitors, and the challenges associated with resistance to RET inhibitors. It provides valuable insights for the development of next-generation MKIs and selective RET inhibitors.

In view of the application prospects in biomedicine of ( E )-1-(4-(diethyla-mino)-2-hydroxybenzylidene)-4,4-dimethylthiosemicarbazide (DAHTS), the behavior of excited-state dynamics and photophysical properties were studied using the density functional theory/time-dependent density functional theory method. A series of studies indicated that the intramolecular hydrogen-bond (IHB) intensity of DAHTS was enhanced after photoexcitation. This was conducive to promoting the excited-state intramolecular proton-transfer (ESIPT) process. Combining the analysis of the IHB and hole-electron, it revealed that the molecule underwent both the ESIPT process and the twisted charge-transfer (TICT) process. Relying on exploration of the potential energy surface, it was proposed that the different competitive mechanisms between the ESIPT and TICT processes were regulated by solvent polarity. In acetonitrile (ACN) solvent, the ESIPT process occurred first, and the TICT process occurred later. In contrast, in the CYH solvent, the molecule first underwent the TICT process and then the ESIPT process. Furthermore, we raised the possibility that the TICT behavior was the cause of weak fluorescence emission for the DAHTS in CYH and ACN solvents. By the dimer correlation analysis, the corresponding components of triple fluorescence emission were clearly assigned, corresponding to the monomer, dimer, and ESIPT isomer in turn. Our work precisely elucidated the photophysical mechanism of DAHTS and the attribution of the triple fluorescence emission components, which provided valuable guidance for the development and regulation of bioactive fluorescence probes with multiband and multicolor emission characteristics.

Natural copper oxygenases provide fundamental principles for catalytic oxidation with kinetically inert molecular oxygen, but it remains a marked challenge to mimic both their structure and function in an entity. Inspired by the Cu A enzymatic sites, herein we report two new photoactive binuclear copper-iodine- and bisbenzimidazole-comodified coordination polymers to reproduce the natural oxo-functionalization repertoire in a unique photocatalytic pathway. Under light irradiation, the Cu-halide coordination polymers effectively reduce NHP esters and complete oxygen reduction activation via photoinduced electron transfer for the aerobic oxidative coupling of hydroquinone with terminal alkynes, affording hydroxyl-functionalized ketones with high efficiency and selectivity. This supramolecular approach to developing bioinspired artificial oxygenases that merge transition metal- and photocatalysis supplies a new way to fabricate distinctive photocatalysts with desirable catalytic performances and controllable precise active sites.