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Topologicalcrystalline insulators (TCIs) are a new class of topologicalmaterials that possess unique metallic surface states protected bycrystalline mirror symmetry. Their topological surface propertiesare expected to strongly depend on the surface orientation. By combiningdensity functional theory (DFT) calculations and synthesis experiments,we demonstrate the controlled growth of single crystalline nanostructuresof the prototypical TCI SnTe with distinct facets and morphologies.Our calculations suggest that the excess energy of the {111} surfacescan be either higher or lower than that of the {100} surfaces, dependingon the stoichiometry, while the {110} is always higher than the {100}.In our synthesis experiment, we qualitatively controlled the stoichiometryby tailoring the growth temperature and obtained two types of singlecrystalline nanowires: smooth nanowires dominated by {100} facetsat high temperatures and zigzag nanowires composed of both {100} and{111} surfaces at low temperatures. Notably, there is no {110} facetin our nanostructures, strongly supporting the DFT calculations. Ourdevice fabrication and electrical characterizations suggest that bothtypes of nanowires are suitable for transport studies of topologicalsurface states. [ABSTRACT FROM AUTHOR]

Rechargeable aqueous Zn-ion batteries are renowned for their safety, cost-effectiveness, environmental friendliness, and high capacity. However, critical issues, such as restricted electrode kinetics and uncontrolled dendrite growth of Zn anodes, have hindered their practical applications. Here, we propose a gradient solid-like electrolyte (GSLE) to enhance the overall performance of Zn anodes and Zn-ion batteries. It shows a high room-temperature conductivity of 13.3 mS cm -1 with an enhanced Zn 2+ transference number of 0.67. With its negatively charged network, the GSLE establishes a Zn 2+ -rich region at the Zn|electrolyte interface, thereby boosting the interfacial charge transfer and accelerating electrode kinetics. Moreover, the GSLE in situ establishes a ZnSe-containing interphase on the surface of Zn anodes during cycling. Such an interphase effectively guides uniform Zn deposition and inhibits side reactions. As a result, symmetric cells using the GSLE demonstrate stabilized Zn plating/stripping cycling over 1400 h and tolerate a high critical current of 15 mA cm -2 . Furthermore, the assembled vanadium-based full cells deliver a remarkable capacity of 125.4 mAh g -1 at 4 A g -1 and achieve a 90% capacity retention after 1000 cycles.

The emergence of mRNA vaccines has heralded an epoch in disease prevention and treatment. Safe and efficient mRNA delivery systems are highly desired for the widespread application of mRNA therapeutics. Herein, we have designed a facile synthetic pathway for producing ionizable lipids featuring various branched linkers. These lipids have been integrated into lipid nanoparticles (LNPs) to improve the delivery of mRNA vaccines. The influence of linker structure on lipids and LNPs is currently underreported, yet it undeniably exerts a substantial impact on the outcomes. Through systematic screening and formulation optimization, we have identified that LNPs comprising ionizable lipids with a branched β-isobutylglutarate linker (bLNPs) exhibited superior transfection capabilities. In preclinical cancer prevention and treatment models, mRNA vaccines delivered by bLNPs (mRNA-bLNPs) have shown significant efficacy without causing systemic toxicity, highlighting the potential of bLNPs for clinical translation. Our synthetic strategy facilitates the expansion of the LNP library and provides valuable insights into the relationship between linker structures and delivery efficiency, thereby propelling the advancement of LNP technology.

Mesenchymal stem cells (MSCs) have garnered significant attention in biomedical research due to their accessibility and remarkable differentiation potential. However, the lack of efficient and convenient living cell monitoring methods limits their widespread application in tissue engineering and stem cell therapy. Therefore, we present progress in the development of a novel series of fluorescent protein (FP) sensors based on turn-on fluorescent protein biosensors (Turn-on FPBs), termed the LV-cp biosensor system (novel live cell permuted fluorescent protein biosensors). Utilizing phage display technology to screen for affinity peptides specifically targeting MSCs and chondrocytes, the LV-cp were engineered by subcloning these peptides into permuted fluorescent proteins, thereby integrating the fluorescence activation mechanism with the affinity peptides and achieving highly accurate detection and identification of these two cell types using living cells as "fluorescence keys." This system provides a simplified, nontoxic method to replace traditional antibody kits, and strong fluorescence signals can be obtained through various fluorescence detection devices. In addition, the LV-cp biosensors enabled dynamic observation of MSCs differentiation into chondrocytes through changes in the cell fluorescence colors.

The presence of a substantial necrotic core in atherosclerotic plaques markedly heightens the risk of rupture, a consequence of elevated iron levels that exacerbate oxidative stress and lipid peroxidation, thereby sustaining a detrimental cycle of ferroptosis and inflammation. Concurrently targeting both ferroptosis and inflammation is crucial for the effective treatment of vulnerable plaques. In this study, we introduce gallium hexacyanoferrate nanoabsorption catalysts (GaHCF NACs) designed to disrupt this pathological cycle. GaHCF NACs function as highly efficient iron chelators with robust antiferroptosis properties. Through in situ capture of iron within atherosclerotic plaques, these catalysts enhance reactive oxygen species scavenging, initiating an amplified therapeutic response. GaHCF NACs significantly advance plaque regression, stabilization, and vascular functional recovery by inhibiting MAPK13 (p38-δ MAPK) signaling, a key mediator of inflammation and cell death. Importantly, the in situ iron capture process generates a detectable photoacoustic signal, offering a notable diagnostic advantage that allows real-time monitoring of plague status. This multifunctional nanocatalytic platform in situ transforms toxic iron within atherosclerotic plaques into both a therapeutic and diagnostic agent, adapting dynamically to the microenvironment and representing a promising strategy for reducing plaque vulnerability and preventing rupture.

The early diagnosis of Alzheimer's disease (AD) plays a vital role in slowing the progression of AD and improving the quality of human life. However, it is still a challenge in the medical field. Herein, an ultrasensitive fluorescent aptasensor was designed for the detection of special phosphorylated tau181 (P-tau181) by coupling with polyvalent aptamers (PAs) structure, hybridization chain reaction (HCR), and the CRISPR-Cas system. Coupling with the signal amplification strategy, the specific recognition ability of the aptamer, and the high cleavage activity of Cas12a protein, the designed aptasensor showed a wide linear range (0.1-10 6 pg/mL), a low detection limit (0.069 pg/mL), high selectivity, and excellent anti-interference ability for the detection of P-tau181. Moreover, the aptasensor can efficiently analyze P-tau181 in artificial cerebro spinal fluid (aCSF) and serum, proving that it has a promising application in the early diagnosis of AD.

Azobenzene actuators have generated extensive research investment in the field of soft robots, artificial muscles, etc., based on the typical photoresponsive trans - cis isomerization. However, it remains challenging to achieve multiphase actuation at the gas-liquid interface and liquid phase. To solve these problems, this paper demonstrated a simple fabrication method of a Janus azobenzene inverse opal membrane with one side having a polydomain azobenzene inverse opal structure and the other side having a monodomain bulk azobenzene polymer. The introduction of an inverse opal structure increases the interaction area between the liquid and polymer network. The proposed design can freely swim in any direction at the air-liquid interface based on the Marangoni effect or move forward in the liquid phase based on bubble propulsion under UV irradiation. This work is of great significance for the design and fabrication of multiphase photo actuators.

Oral nanomedicines present a preferable avenue for cancer immunotherapy, but their efficacy is limited by gastrointestinal absorption challenges, tumor physiopathologic barriers, and immune evasion mechanisms. Here, we present an approach that combines an oral transcytotic doxorubicin (DOX) nanomedicine with the histone demethylase inhibitor 5-carboxy-8-hydroxyquinoline (IOX1), thereby enabling synergistic chemoimmunotherapy. We demonstrate that IOX1 significantly augments the transcytosis capabilities of DOX-loaded poly(2-( N -oxide- N , N -diethylamino)ethylmethacrylate)-poly(ε-caprolactone) micelles (OPDOX), promoting their transcellular transport across various cellular barriers (villus, endothelial, and tumor cells), thus improving oral adsorption, vascular extravasation, and tumor penetration. Furthermore, IOX1 sensitizes chemotherapy to potentiate DOX-induced immunogenic cell death and downregulates programmed cell death-ligand 1 to disrupt the immune checkpoint mechanism, synergistically boosting robust antitumor immune responses. Consequently, orally administered OPDOX in combination with IOX1 efficiently inhibits CT26 tumor growth, highlighting the significant potential for enhancing the efficacy of oral nanomedicines in cancer chemoimmunotherapy.

It is proven through transmission electron microscope (TEM) analysis that solar sensitizer Cu 2 SnS 3 (CTS) dots prepared via the hot-injection route are nonspherical, polyhedral nanocrystals with the size of ∼11 nm. CTS dots were deposited into a porous TiO 2 layer to form CTS/TiO 2 , an effective type II heterojunction in photoanodes. The electronic and energy band structures of TiO 2 and CTS were studied by the plane-wave ultrasoft pseudopotential method based on density functional theory (DFT) and verified by ultraviolet-visible (UV-vis) spectroscopy. UV-vis and Photoluminescence (PL) spectra show that the CTS/TiO 2 photoanode exhibits wider visible-light absorption as well as lower charge recombination. ZnS quantum dots (QDs) deposited on the CTS/TiO 2 photoanode through the in situ successive ion layer adsorption and reaction (SILAR) method as the passivation layer can inhibit the reverse carrier transfer and increase the photocurrent density by building a potential barrier on the CTS/TiO 2 photoanode and electrolyte interface. When 2-layer ZnS QDs are deposited, the maximum photocurrent density of the photoelectrochemical (PEC) cell composed of a ZnS/CTS/TiO 2 photoanode, a Pt counter electrode, and Na 2 SO 4 solution electrolyte is 8.43 mA/cm 2 and the maximum applied bias photon-to-current efficiency (ABPE) is 7.79%. Under 1 sun (AM 1.5, 100 mW/cm 2 ) with 0.6 V bias, its hydrogen yield reached 125.7 μmol·cm -2 after 4 h with the rate of 31.4 μmol·cm -2 ·h -1 in contrast to the yield of 107.86 μmol·cm -2 with the rate of 21.3 μmol·cm -2 ·h -1 for the CTS/TiO 2 photoanode.

Axl is an important receptor tyrosine protein kinase that plays a key role in the development and progression of various diseases, such as cancer and inflammation. Developing a highly sensitive Axl detection method can help improve accuracy, better address-specific clinical needs, and guide personalized treatment. In this study, a CHA-CRISPR/Cas13 fluorescence probe was established using Axl-specific aptamers as a mediator to displace the polynucleotide chain (TA). Through TA construction, an entropy-driven nucleotide catalytic hairpin assembly system was created to cyclically release RNA that activates clustered regularly interspaced short palindromic repeats (CRISPR)/Cas13 activity, triggering its cleavage activity. The activated CRISPR/Cas13 system cleaves the reporter labeled with BHQ1 and FAM at both ends, leading to the recovery of FAM fluorescence. Based on the optimization design using the free energy (△ G ) and secondary structure software simulation results of the nucleic acid sequence, the fluorescence intensity of the probe is proportional to the concentration of Axl. Results showed a good linear relationship between fluorescence intensity increment and log C Axl ( C Axl in the range of 3.33-667 pM, r = 0.9907). The probe exhibited ultrahigh sensitivity with a detection limit of 0.84 pM. It was successfully applied in the detection of human serum samples, showing a higher Axl level in cervical cancer patients compared to breast cancer patients. The probe was also successfully applied in the imaging of various tumor cells, consistent with serum detection results. In conclusion, this probe represents an effective new method for detecting Axl, demonstrating outstanding specificity and sensitivity. It provides technological support for tumor diagnosis and shows the potential for detecting circulating tumor cells in blood through cell imaging.

Emission trading schemes (ETS) are increasingly becoming a popular policy instrument to balance carbon abatement and economic growth. As a globally unified carbon pricing system has not yet been established, whether regionally operated ETSs cause carbon leakage remains a major concern. Taking China's regional pilot ETSs as a quasi-natural experiment, the study uses the spatial difference-in-differences method to examine how regional ETSs affect carbon emissions in and outside cities of policy implementation. Our analysis finds that China's regional ETS policy contributes to a 6.1% reduction in urban CO 2 emissions and a 6.6% decline in emissions intensity in regulated cities, causing carbon leakages that increase CO 2 emissions in neighboring cities by 1.7% on average. Our finding further suggests that regional ETSs mitigate local CO 2 emissions through outsourcing production, improving energy efficiency and decarbonizing energy structure, whereas the outsourcing of industrial production drives up CO 2 emissions in adjacent cities. Moreover, the performances of regional ETSs vary largely by socioeconomic context and mechanism design. China's regional ETSs reduce CO 2 emissions more effectively in central and industrial cities but with more severe carbon leakage, while rigorous compliance mechanisms and active market trading help deepen carbon abatement and alleviate carbon leakage.

Benzyl alcohol (BA) is a major biomass derivative and can be further converted into deoxybenzoin (DOB) and benzoin (BZ) as high-value products for industrial applications through photocatalytic C-C coupling reaction. The photocatalytic process contains two reaction steps, which are (1) the C-C coupling of BA to hydrobenzoin (HB) intermediates and (2) either dehydration of HB to DOB or dehydrogenation of HB to BZ. We found that generation of DOB or BZ is mainly determined by the activation of C α -H or O-H bonds in HB. In this study, phase junction CdS photocatalysts and Ni/CdS photocatalysts were elaborately designed to precisely control the activation of C α -H or O-H bonds in HB by adjusting the adsorption orientation of HB on the photocatalyst surfaces. After orienting the C α -H groups in HB on the CdS surfaces, the C α -H bond dissociation energy (BDE) at 1.39 eV is lower than the BDE of the O-H bond at 2.69 eV, therefore improving the selectivity of the DOB. Conversely, on Ni/CdS photocatalysts, the O-H groups in HB orient toward the photocatalyst surfaces. The BDE of the O-H bonds is 1.11 eV to form BZ, which is lower than the BDE of the C α -H bonds to the DOB (1.33 eV), thereby enhancing the selectivity of BZ. As a result, CdS photocatalysts can achieve complete conversion of BA to 80.4% of the DOB after 9 h of visible light irradiation, while 0.3% Ni/CdS photocatalysts promote complete conversion of BA to 81.5% of BZ after only 5 h. This work provides a promising strategy in selective conversion of BA to either DOB or BZ through delicate design of photocatalysts., Competing Interests: The authors declare no competing financial interest., (© 2024 The Authors. Published by American Chemical Society.)

Machine learning and data-driven methods have attracted a significant amount of attention for the acceleration of the design of molecules and materials. In this study, a material design protocol based on multimode modeling that combines literature modeling, numerical data collection, textual descriptor design, genetic modeling, experimental validation, first-principles calculation, and theoretical efficiency calculation is proposed, with a case study on designing compatible complex solvent molecules for a halide perovskite film, which is notorious for optoelectronic deactivation under hostile conditions, especially in water. In the multimode modeling design process, the textual descriptors play the central role and store rich literature scientific knowledge, which starts from the construction of a high-dimension literature model based on scientific articles and is realized by a genetic algorithm for materials predictions. The prediction is substantiated by follow-up experiments and first-principles calculations, leading to the successful identification of effective molecular combinations delivering an unprecedented large aqueous photocurrent (increasing by 3 orders of magnitude compared with that of CH 3 NH 3 PbI 3 ) and remarkable aqueous stability (improving from 36% to 89% after immersion in water) under the hostile condition. This study provides a practical route via multimode modeling for accelerating the design of molecule-modified and solution-processed materials in a real scenario.

The activation of cellular ferroptosis is promising in tumor therapy. However, ferroptosis is parallelly inhibited by antiferroptotic substances, including glutathione peroxidase 4 (GPX4), dihydroorotate dehydrogenase (DHODH), and ferroptosis suppressor protein 1 (FSP1). Thus, it is highly desirable, yet challenging, to simultaneously suppress these three antiferroptotic substances for activating ferroptosis. Here, we rationally designed a hollow iron-doped SiO 2 -based nanozyme (FeSHS) loaded with brequinar (BQR) and lificiguat (YC-1), named FeSHS/BQR/YC-1-PEG, for tumor ferroptosis activation. FeSHS were developed through the continuous etching of SiO 2 nanoparticles by iron ions, which exhibit pH/glutathione-responsive biodegradability, along with mimicking the activities of peroxidase, glutathione oxidase, and NAD(P)H oxidase. Specifically, glutathione depletion and NAD(P)H oxidation by FeSHS will suppress the expression of GPX4 and inhibit FSP1 by disrupting the NAD(P)H/FSP1/ubiquinone axis. In addition, the released BQR can suppress the expression of DHODH. Meanwhile, YC-1 is able to increase the cellular polyunsaturated fatty acids (PUFAs) by destroying the HIF-1α/lipid droplet axis. The elevation of levels of iron and PUFAs while simultaneously disrupting the GPX4/DHODH/FSP1 inhibitory pathways by our designed nanoplatform displayed high therapeutic efficacy both in vitro and in vivo . This work elucidates rationally designing smart nanoplatforms for ferroptosis activation and future tumor treatments.

Ultrafine particles (UFPs) dominate the atmospheric particles in number concentration, impacting human health and climate change. However, existing studies primarily rely on mass-based approaches, leading to a restricted understanding of the number-based and chemically resolved health effects of atmospheric UFPs. In this study, we utilized a high-mass-resolution single-particle aerosol mass spectrometer to investigate the online chemical composition and number size distribution of ultrafine, fine, and coarse particles during the summertime in urban Shenzhen, China. Human respiratory deposition dose assessments of particles with varying chemical compositions were further conducted by a respiratory deposition model. The results showed that during our observation, particles containing elemental carbon (EC) were the dominant components in UFPs (0.05-0.1 μm). Compared to fine and coarse particles, UFPs can deposit more deeply into the respiratory tract with a daily dose of ∼2.08 ± 0.67 billion particles. Among the deposited UFPs, EC-cluster particles constituted ∼85.7% in number fraction, accounting for a daily number dose of ∼1.78 billion particles, which poses a greater impact on human health. Simultaneously, we found discrepancies in the chemically resolved particle depositions among number-, surface area-, and mass-based approaches, emphasizing the importance of an appropriate metric for particle health-risk evaluation.

Photocatalysis has high potential in the cleavage of C β -O bond in lignin into high-value aromatic monomers; however, the inefficient C α -H bond activation in lignin and a low hydrogen transfer efficiency on the photocatalyst's surfaces have limited its application in photocatalytic lignin conversion. This study indicates that the cleavage of the C β -O bond can be improved by the generation of the C α radical intermediate through C α -H bond activation, and the formation of desirable aromatic products can be significantly improved by the enhanced hydrogen transfer efficiency from photocatalyst surfaces to aromatic monomeric radicals. We elaborately designed the half-unit-cell MoS 2 /ZnIn 2 S 4 monolayer with a thickness of ∼1.7 nm to promote the hydrogen transfer efficiency on the photocatalyst surfaces. The ultrathin structure can shorten the diffusion distance of charge carriers from the interior to the surfaces and tight interface between MoS 2 and ZnIn 2 S 4 to facilitate the migration of photogenerated electrons from ZnIn 2 S 4 to MoS 2 , therefore improving the selectivity of desirable products. The adsorbed hydroxyl radical (*OH) on the surfaces of MoS 2 /ZnIn 2 S 4 from water oxidation can significantly reduce the bond dissociation energy (BDE) of C α -H bond in PP-ol from 2.38 to 1.87 eV, therefore improving the C α -H bond activation. The isotopic experiments of H 2 O/D 2 O indicate that the efficiency of *OH generation is an important step in C α -H bond activation for PP-ol conversion to aromatic monomers. In summary, PP-ol can completely convert to 86.6% phenol and 82.3% acetophenone after 1 h of visible light irradiation by using 3% MoS 2 /ZnIn 2 S 4 and the assistance of *OH, which shows the highest conversion rate compared to previous works.

mRNA vaccines have been revolutionizing disease prevention and treatment. However, their further application is hindered by inflammatory side effects, primarily caused by delivery systems such as lipid nanoparticles (LNPs). In response to this issue, we prepared cationic lipids (mLPs) derived from mildronate, a small-molecule drug, and subsequently developed the LNP (mLNP-69) comprising a low dose of mLP. Compared with the LNP (sLNP) based on SM-102, a commercially available ionizable lipid, mLNP-69 ensures effective mRNA delivery while significantly reducing local inflammation. In preclinical prophylactic and therapeutic B16-OVA melanoma models, mLNP-69 demonstrated successful mRNA cancer vaccine delivery in vivo, effectively preventing tumor occurrence or impeding tumor progression. The results suggest that the cationic lipids derived from mildronate, which exhibit efficient delivery capabilities and minimal inflammatory side effects, hold great promise for clinical application.

Photocatalytic H 2 O 2 production has attracted much attention as an alternative way to the industrial anthraquinone oxidation process but is limited by the weak interaction between the catalysts and reactants as well as inefficient proton transfer. Herein, we report on a hydrogen-bond-broken strategy in carbon nitride for the enhancement of H 2 O 2 photosynthesis without any sacrificial agent. The H 2 O 2 photosynthesis is promoted by the hydrogen bond formation between the exposed N atoms on hydrogen-bond-broken carbon nitride and H 2 O molecules, which enhances proton-coupled electron transfer and therefore the photocatalytic activity. The exposed N atoms serve as proton buffering sites for the proton transfer from H 2 O molecules to carbon nitride. The H 2 O 2 photosynthesis is also enhanced through the enhanced adsorption and reduction of O 2 gas toward H 2 O 2 on hydrogen-bond-broken carbon nitride because of the formation of nitrogen vacancies (NVs) and cyano groups after the intralayer hydrogen bond breaking on carbon nitride. A high light-to-chemical conversion efficiency (LCCE) value of 3.85% is achieved. O 2 and H 2 O molecules are found to undergo a one-step two-electron reduction pathway by photogenerated hot electrons and a four-electron oxidation process to produce O 2 gas, respectively. Density functional theory (DFT) calculations validate the O 2 adsorption and reaction pathways. This study elucidates the significance of the hydrogen bond formation between the catalyst and reactants, which greatly increases the proton tunneling dynamics.

The development of in situ tumor vaccines offers promising prospects for cancer treatment. Nonetheless, the generation of plenary autologous antigens in vivo and their codelivery to DC cells along with adjuvants remains a significant challenge. Herein, we developed an in situ tumor vaccine using a supramolecular nanoparticle/hydrogel composite (ANP MTO /ALCD) and a deformable nanoadjuvant (PPE R848 ). The ANP MTO /ALCD composite consisted of β-cyclodextrin-decorated alginate (Alg- g -CD) and MTO-encapsulated adamantane-decorated nanoparticles (ANP MTO ) through supramolecular interaction, facilitating the long-term and sustained production of plenary autologous antigens, particularly under a 660 nm laser. Simultaneously, the produced autologous antigens were effectively captured by nanoadjuvant PPE R848 and subsequently transported to lymph nodes and DC cells, benefiting from its optimized size and deformability. This in situ tumor vaccine can trigger a robust antitumor immune response and demonstrate significant therapeutic efficacy in inhibiting tumor growth, suppressing tumor metastasis, and preventing postoperative recurrence, offering a straightforward approach to programming in situ tumor vaccines.

Aerogel-based composites, renowned for their three-dimensional (3D) network architecture, are gaining increasing attention as lightweight electromagnetic (EM) wave absorbers. However, attaining high reflection loss, broad effective absorption bandwidth (EAB), and ultrathin thickness concurrently presents a formidable challenge, owing to the stringent demands for precise structural regulation and incorporation of magnetic/dielectric multicomponents with synergistic loss mechanisms within the 3D networks. In this study, we successfully synthesized a 3D hierarchical porous Fe 3 O 4 /MoS 2 /rGO/Ti 3 C 2 T x MXene (FMGM) composite aerogel via directional freezing and subsequent heat treatment processes. Owing to their ingenious structure and multicomponent design, the FMGM aerogels, featured with abundant heterogeneous interface structure and magnetic/dielectric synergism, show exceptional impedance matching characteristics and diverse EM wave absorption mechanisms. After optimization, the prepared ultralight (6.4 mg cm -3 ) FMGM-2 aerogel exhibits outstanding EM wave absorption performance, achieving a minimal reflection loss of -66.92 dB at a thickness of 3.61 mm and an EAB of 6.08 GHz corresponding to the thickness of 2.3 mm, outperforming most of the previously reported aerogel-based absorbing materials. This research presents an effective strategy for fabricating lightweight, ultrathin, highly efficient, and broad band EM wave absorption materials.

The sluggish kinetics of methanol oxidation reaction (MOR) and poor long-term durability of catalysts are the main restrictions of the large-scale applications of direct methanol fuel cells (DMFCs). Herein, we demonstrated an inspirational ternary Pt 3 Sn 0.5 Mn 0.5 /DMC intermetallic catalyst that reached 4.78 mA cm -2 and 2.39 A mg -1 Pt for methanol oxidation, which were 2.50/2.44 and 5.62/5.31 times that of commercial PtRu/C and Pt/C. After the durability test, Pt 3 Sn 0.5 Mn 0.5 /DMC presented a very low current density attenuation (38.5%), which was significantly lower than those for commercial PtRu/C catalyst (84.2%) and Pt/C (93.1%). Density functional theory (DFT) calculations revealed that the coregulation of Sn and Mn altered the surface electronic structure and endowed Pt 3 Sn 0.5 Mn 0.5 with selective adsorption of Pt for CO and Sn for OH, which optimized the adsorption strength for intermediates and improved the reaction kinetics of MOR. Beyond offering an advanced electrocatalyst, this study provided a new point of view for the rational design of superior methanol oxidation catalysts for DMFC.

Radiation-tolerance and repairable flexible transistors and integrated circuits (ICs) with low power consumption have become hot topics due to their wide applications in outer space, nuclear power plants, and X-ray imaging. Here, we designed and developed novel flexible semiconducting single-walled carbon nanotube (sc-SWCNT) thin-film transistors (TFTs) and ICs. Sc-SWCNT solid-electrolyte-gate dielectric (SEGD) TFTs showcase symmetric ambipolar characteristics with flat-band voltages (V FB ) of ∼0 V, high I ON /I OFF ratios (>10 5 ), and the recorded irradiation resistance (up to 22 Mrad). Moreover, flexible sc-SWCNT ICs, including CMOS-like inverters and NAND and NOR logic gates, have excellent operating characteristics with low power consumption (≤8.4 pW) and excellent irradiation resistance. Significantly, sc-SWCNT SEGD TFTs and ICs after radiation with a total irradiation dose (TID) ≥ 11 Mrad can be repaired after thermal heating at 100 °C. These outstanding characteristics are attributed to the designed device structures and key core materials including SEGD and sc-SWCNT.

Photocatalysis has the potential for lignin valorization to generate functionalized aromatic monomers, but its application has been limited by the slow conversion rate and the low selectivity to desirable aromatic products. In this work, we designed the phase junction CdS with coexposed hexagonal (100) and cubic (220) facets to improve the photogenerated charge carriers' transfer efficiency from (100) facet to (220) facet and the hydrogen transfer efficiency for an enhanced conversion rate of lignin to aromatic monomers. Water is found as a sufficient external hydrogen supplier to increase the yields of aromatic monomers. These innovative designs in the reaction system promoted complete conversion of PP-ol to around 94% of aromatic monomers after 1 h of visible light irradiation, which shows the highest reaction rate and selectivity of target products in comparison with previous works. PP-one is a byproduct from the overoxidation of PP-ol and is usually difficult to be further cleaved to acetophenone and phenol as the desirable aromatic monomers. TEA was first identified in this study as a sacrificial electron donor, a hydrogen source, and a mediator to enhance the cleavage of the C β -O bonds in PP-one. With the assistance of TEA, PP-one can be completely cleaved to desirable aromatic monomer products, and the reaction time is reduced from several hours to 10 min of visible light irradiation.

The development of large-scale integration of optoelectronic neuromorphic devices with ultralow power consumption and broadband responses is essential for high-performance bionics vision systems. In this work, we developed a strategy to construct large-scale (40 × 30) enhancement-mode carbon nanotube optoelectronic synaptic transistors with ultralow power consumption (33.9 aJ per pulse) and broadband responses (from 365 to 620 nm) using low-work function yttrium (Y)-gate electrodes and the mixture of eco-friendly photosensitive Ag 2 S quantum dots (QDs) and ionic liquids (ILs)-cross-linking-poly(4-vinylphenol) (PVP) (ILs-c-PVP) as the dielectric layers. Solution-processable carbon nanotube thin-film transistors (TFTs) showed enhancement-mode characteristics with the wide and controllable threshold voltage window (-1 V∼0 V) owing to use of the low-work-function Y-gate electrodes. It is noted that carbon nanotube optoelectronic synaptic transistors exhibited high on/off ratios (>10 6 ), small hysteresis and low operating voltage (≤2 V), and enhancement mode even under the illumination of ultraviolet (UV, 365 nm), blue (450 nm), and green (550 nm) to red (620 nm) pulse lights when introducing eco-friendly Ag 2 S QDs in dielectric layers, demonstrating that they have the strong fault-tolerant ability for the threshold voltage drifts caused by various manufacturing scenarios. Furthermore, some important bionic functions including a high paired pulse facilitation index (PPF index, up to 290%), learning and memory function with the long duration (200 s), and rapid recovery (2 s). Pavlov's dog experiment (retention time up to 20 min) and visual memory forgetting experiments (the duration of high current for 180 s) are also demonstrated. Significantly, the optoelectronic synaptic transistors can be used to simulate the adaptive process of vision in varying light conditions, and we demonstrated the dynamic transition of light adaptation to dark adaptation based on light-induced conditional behavior. This work undoubtedly provides valuable insights for the future development of artificial vision systems.

Hepatitis B virus (HBV) infection remains a major global health concern, necessitating the development of sensitive and reliable diagnostic methods. In this study, we propose a novel approach to enhance the sensitivity of HBV DNA detection by leveraging a concentration imbalance-driven DNA circuit (CIDDC) as an operational amplifier, coupled with a hybridization-responsive DNA-templated silver nanocluster (DNA-AgNCs) nanoprobe named Q·C6-AgNCs. The CIDDC system effectively converts and amplifies the input HBV DNA into an enriched generic single-stranded DNA output, which subsequently triggers the fluorescence of the DNA-AgNCs reporter upon hybridization, generating a measurable signal for detection. By incorporating the DNA circuit, we not only achieved enhanced sensitivity with a lower detection limit of 0.11 nM but also demonstrated high specificity with single-base mismatch discriminability for HBV DNA detection. Additionally, this mix-and-detect assay format is simple, user-friendly, and isothermal. This innovative strategy holds promise for advancing molecular diagnostics and facilitating the effective management of HBV-related diseases., Competing Interests: The authors declare no competing financial interest., (© 2024 The Authors. Published by American Chemical Society.)

The highly contagious nature and 100% fatality rate contribute to the ongoing and expanding impact of the African swine fever virus (ASFV), causing significant economic losses worldwide. Herein, we developed a cascaded colorimetric detection using the combination of a CRISPR/Cas14a system, G-quadruplex DNAzyme, and microfluidic paper-based analytical device. This CRISPR/Cas14a-G4 biosensor could detect ASFV as low as 5 copies/μL and differentiate the wild-type and mutated ASFV DNA with 2-nt difference. Moreover, this approach was employed to detect ASFV in porcine plasma. A broad linear detection range was observed, and the limit of detection in spiked porcine plasma was calculated to be as low as 42-85 copies/μL. Our results indicate that the developed paper platform exhibits the advantages of high sensitivity, excellent specificity, and low cost, making it promising for clinical applications in the field of DNA disease detection and suitable for popularization in low-resourced areas.

For many years, humans have been relentlessly focused on enhancing battery longevity and boosting energy storage capacities. The performance and durability of a battery depend significantly on the material used for its electrodes. In this context, merging machine learning with density functional theory (DFT) calculations has emerged as a pivotal approach to advancing the exploration of battery crystal structures. We present a new method that combines a graph convolutional neural network (GNN) with a Transformer convolutional layer, which we call Transformer-GNN. To underscore its efficacy, we benchmarked Transformer-GNN against three established statistical machine learning models: Support Vector Machine, Random Forest, and XGBoost. We also developed a standard GNN, which we refer to as Basic-GNN. Additionally, we compared Basic-GNN with Transformer-GNN to highlight the improvements brought about by incorporating the Transformer convolutional layer. The Transformer-GNN model outperforms the other models, achieving the highest R value of 0.82 and the lowest mean squared error of 0.3161. Our findings demonstrate that the Transformer-GNN can profoundly understand battery crystal structures, thus forging the path toward more sophisticated and durable battery systems. Leveraging the GNN model's voltage predictions in tandem with the capacity data sourced from the database, we screened and pinpointed Na(NiO 2 value of 0.82 and the lowest mean squared error of 0.3161. Our findings demonstrate that the Transformer-GNN can profoundly understand battery crystal structures, thus forging the path toward more sophisticated and durable battery systems. Leveraging the GNN model's voltage predictions in tandem with the capacity data sourced from the database, we screened and pinpointed Na(NiO 2 ) 2 as a high-voltage (higher than 5 V), high-capacity sodium cathode material. We conducted DFT calculations on Na(NiO 2 ) 2 and revealed the migration mechanism of the Na ions.

Rice origin authenticity is important for food safety and consumer confidence. The stable isotope composition of rice is believed to be closely related to its water source, which affects its origin characteristics. However, the influence of water availability on the distribution of rice stable isotopes (δ 2 H and δ 18 O) is not clear. In this study, three irrigation waters with different isotopic values were used to investigate isotopic water use effects of Indica and Japonica rice, using pot experiments. Under three different water isotope treatments, the δ 2 H values of Indica polished rice showed significant differences (-65.0 ± 2.3, -60.5 ± 0.8 and -55.8 ± 1.7‰, respectively, p < 0.05) compared to δ 13 C and δ 15 N, as did Japonica polished rice. The values of δ 2 H and δ 18 O of rice became more positive when applying more enriched (in 2 H and 18 O) water, and the enrichment effect was higher in rice than in the corresponding plant tissue. In addition, the δ 2 H and δ 18 O values of Indica rice leaves decreased at the heading stage, increased at the filling stage, and then decreased at the harvest stage. Japonica rice showed a similar trend. δ 2 H changes from stem to leaf were more negative, but δ 18 O changes were more positive, and δ 2 H and δ 18 O values from leaf to rice were more positive for both brown and polished rice. The results from this study will clarify different water isotopic composition effects on rice and provide useful information to improve rice origin authenticity using stable isotope-based methods.

Accurate, ultrasensitive, and point-of-care (POC) diagnosis of the African swine fever virus (ASFV) remains imperative to prevent its spread and limit the losses incurred. Herein, we propose a CRISPR-Cas12a-assisted triplex amplified colorimetric assay for ASFV DNA detection with ultrahigh sensitivity and specificity. The specific recognition of recombinase aided amplification (RAA)-amplified ASFV DNA could activate the Cas12a/crRNA/ASFV DNA complex, leading to the digestion of the linker DNA (bio-L1) on magnetic beads (MBs), thereby preventing its binding of gold nanoparticles (AuNPs) network. After magnetic separation, the release of AuNPs network comprising a substantial quantity of AuNPs could lead to a discernible alteration in color and significantly amplify the plasmonic signal, which could be read by spectrophotometers or smartphones. By combining the RAA, CRISPR/Cas12a-assisted cleavage, and AuNPs network-mediated colorimetric amplification together, the assay could detect as low as 0.1 copies/μL ASFV DNA within 1 h. The assay showed an accuracy of 100% for the detection of ASFV DNA in 16 swine tissue fluid samples, demonstrating its potential for on-site diagnosis of ASFV.

In order to explore the pressure and flame propagation characteristics of gas-coal dust composite explosions, a semiclosed pipeline explosion test platform was built. The shock wave overpressure and explosion flame propagation law of different concentrations of suspended coal dust participating in gas explosions were studied in depth through experiments, and the coal dust motion law was simulated and analyzed based on Fluent software. The experimental results show that the peak pressure of gas-coal dust composite explosion is significantly higher than that of single-phase gas explosion, and the pressure peak increase ratio at the pipeline outlet is the highest; as the suspended coal dust concentration increases, the pressure rise rate at point 3 gradually decreases. Under the condition of 600 g/m 3 coal dust participating in the explosion, the explosion pressure increase speed reduction ratio is 25.65%, the pressure wave secondary peak decreases, and the fluctuation frequency increases. When the explosion flame front passes through the suspended coal dust area, the flame shape changes from 'v' shape to 'finger' shape and propagates forward. The gas-coal dust composite explosion flame propagation speed shows a secondary acceleration phenomenon, after the flame front passes through the coal dust suspension area. As the coal dust concentration increases, the explosion core area moves away from the flame front. The coal dust cloud moves to the right, showing a concave rectangle; the larger the coal dust concentration, the smaller the moving speed. The experimental results and analysis provide an experimental basis for further exploring the mechanism and dynamic mechanism of gas-coal dust coupling explosion., Competing Interests: The authors declare no competing financial interest., (© 2024 The Authors. Published by American Chemical Society.)

In vitro transcription (IVT) of mRNA is a versatile platform for a broad range of biotechnological applications. Its rapid, scalable, and cost-effective production makes it a compelling choice for the development of mRNA-based cancer therapies and vaccines against infectious diseases. The impurities generated during mRNA production can potentially impact the safety and efficacy of mRNA therapeutics, but their structural complexity has not been investigated in detail yet. This study pioneers a comprehensive profiling of IVT mRNA impurities, integrating current technologies with innovative analytical tools. We have developed highly reproducible, efficient, and stability-indicating ion-pair reversed-phase liquid chromatography and capillary gel electrophoresis methods to determine the purity of mRNA from different suppliers. Furthermore, we introduced the applicability of microcapillary electrophoresis for high-throughput (<1.5 min analysis time per sample) mRNA impurity profiling. Our findings revealed that impurities are mainly attributed to mRNA variants with different poly(A) tail lengths due to aborted additions or partial hydrolysis and the presence of double-stranded mRNA (dsRNA) byproducts, particularly the dsRNA 3'-loop back form. We also implemented mass photometry and native mass spectrometry for the characterization of mRNA and its related product impurities. Mass photometry enabled the determination of the number of nucleotides of different mRNAs with high accuracy as well as the detection of their size variants [i.e., aggregates and partial and/or total absence of the poly(A) tail], thus providing valuable information on mRNA identity and integrity. In addition, native mass spectrometry provided insights into mRNA intact mass, heterogeneity, and important sequence features such as poly(A) tail length and distribution. This study highlights the existing bottlenecks and opportunities for improvement in the analytical characterization of IVT mRNA, thus contributing to the refinement and streamlining of mRNA production, paving the way for continued advancements in biotechnological applications.

Developing high-performance electromagnetic interference (EMI) shielding materials that are lightweight and flexible and have excellent mechanical properties is an ideal choice for modern integrated electronic devices and microwave protection. Herein, we report the preparation of core-shell polyaniline (PANI)-based nanofiber membranes for EMI shielding through seed polymerization. Electrospinning a PANI solution leads to homogeneously dispersed PANI on the nanofiber surface, with abundant attachment sites for aniline through electrostatic adsorption and hydrogen bonding interaction, allowing PANI to grow on the nanofiber surfaces. This stable core-shell heterostructure provides more interfaces for reflecting and absorbing microwaves. The PANI/PVDF@PANI membranes achieved a shielding efficiency (SE) of 44.7 dB at a thickness of only 1.2 mm, exhibiting an exceptionally high specific EMI shielding effectiveness (SE/t) of 372.5 dB cm -1 . Furthermore, the composite membrane exhibits outstanding mechanical stability, durability, air permeability, and moisture permeability, also making it suitable for applications such as EM shielding clothing.

Achieving no or low polychlorinated byproduct selectivity is essential for the chlorinated volatile organic compounds (CVOCs) degradation, and the positive roles of water vapor may contribute to this goal. Herein, the oxidation behaviors of chlorobenzene over typical Mn-based catalysts (MnO 2 and acid-modified MnO 2 ) under dry and humid conditions were fully explored. The results showed that the presence of water vapor significantly facilitates the deep mineralization of chlorobenzene and restrains the formation of Cl 2 and dichlorobenzene. This remarkable water vapor-promoting effect was conferred by the MnO 2 substrate, which could suitably synergize with the postconstructed acidic sites, leading to good activity, stability, and desirable product distribution of acid-modified MnO 2 catalysts under humid conditions. A series of experiments including isotope-traced (D 2 O and H 2 18 O) CB-TPO provided complete insights into the direct involvement of water molecules in chlorobenzene oxidation reaction and attributed the root cause of the water vapor-promoting effect to the proton-rich environment and highly reactive water-source oxygen species rather than to the commonly assumed cleaning effect or hydrogen proton transfer processes (generation of active OOH). This work demonstrates the application potential of Mn-based catalysts in CVOCs elimination under practical application conditions (containing water vapor) and provides the guidance for the development of superior industrial catalysts.

The optimal combination of metal ions and ligands for sensing materials was estimated by using a data-driven model developed in this research. This model utilized advanced computational algorithms and a data set of 100,000 literature pieces. The semiconductor metal oxide (SMO) that is most suitable for detecting triethylamine (TEA) with the highest probability was identified by using the Word2vec model, which employed the maximum likelihood method. The loss function of the probability distribution was minimized in this process. Based on the analysis, a novel hierarchical nanostructured tungsten-based coordination with 2,5-dihydroxyterephthalic acid (W-DHTA) was synthesized. This synthesis involved a postsynthetic hydrothermal treatment (psHT) and the self-assembly of tungsten oxide nanorods. The tungsten oxide nanorods had a significant number of oxygen vacancies. Various techniques were used to characterize the synthesized material, and its sensing performance toward volatile organic compound (VOC) gases was evaluated. The results showed that the functionalized tungsten oxide exhibited an exceptionally high sensitivity and selectivity toward TEA gas. Even in a highly disturbed environment, the detection limit for TEA gas was as low as 40 parts per billion (ppb). Furthermore, our findings suggest that the control of oxygen vacancies in sensing materials plays a crucial role in enhancing the sensitivity and selectivity of gas sensors. This approach was supported by the utilization of density functional theory (DFT) computation and machine learning algorithms to assess and analyze the performance of sensor devices, providing a highly efficient and universally applicable research methodology for the development and design of next-generation functional materials.

Molecular networking has emerged as a standard approach for natural product (NP) discovery. However, the current pipeline based on molecular networks tends to prioritize larger clusters comprising multiple nodes. To address this issue, we present the integrated molecular networking workflow for NP dereplication (IMN4NPD). This approach not only expedites the rapid dereplication of extensive clusters within the molecular network but also places specific emphasis on self-looped or pairs of nodes, which are often overlooked by the current methods. By amalgamating the outputs from various computational tools, we efficiently dereplicate compounds falling into specific categories and provide annotations for both large cluster nodes and self-looped or pair of nodes within the molecular network. Furthermore, we have incorporated several fundamentally distinct similarity algorithms, namely, Spec2Vec and MS2DeepScore, for constructing the t-SNE network. Through comparison with modified cosine similarity, we have observed that integrating additional diverse spectral similarity measures, the resulting t-SNE network enhanced the ability to dereplicate NPs. Demonstrating the use case of an ethanol extract of Plumula nelumbinis , we illustrate that an integration of multiple computational solutions with IMN4NPD aids the dereplication, especially self-looped nodes, and in the discovery of novel compounds in NPs.

Development of potential inhibitors to prevent prion protein (PrP) fibrillation is a therapeutic strategy for prion diseases. The prion neuropeptide PrP106-126, a research model of abnormal PrP (PrP Sc ), presents similar physicochemical and biochemical characters to PrP Sc , which is also a target of potential inhibitors against prion deposition. Many flavones have antioxidant, anti-inflammatory, and antibacterial properties, and they are applied in treating prion disorder and other amyloidosis as well. However, the inhibition mechanism of flavones on PrP106-126 fibrillation is still unclear. In the current work, apigenin and nepetin were used to suppress the aggregation of PrP106-126 and to alleviate the peptide-induced cytotoxicity. The results showed that apigenin and nepetin impeded the fibril formation of PrP106-126 and depolymerized the preformed fibrils. They were bound to PrP106-126 predominantly by hydrophobic and hydrogen bonding interactions. In addition, both flavones upregulated cell viability and decreased membrane leakage through reducing peptide oligomerization. The differences in inhibition and cell protection between the two small molecules were presumably attributed to the substitution of hydroxyl and methoxy groups in nepetin, which demonstrated the significant structure-function relationship of flavones with prion neuropeptide and the prospect of flavonoids as drug candidates against prion diseases.

Detecting drug-drug interactions (DDIs) is an essential step in drug development and drug administration. Given the shortcomings of current experimental methods, the machine learning (ML) approach has become a reliable alternative, attracting extensive attention from the academic and industrial fields. With the rapid development of computational science and the growing popularity of cross-disciplinary research, a large number of DDI prediction studies based on ML methods have been published in recent years. To give an insight into the current situation and future direction of DDI prediction research, we systemically review these studies from three aspects: (1) the classic DDI databases, mainly including databases of drugs, side effects, and DDI information; (2) commonly used drug attributes, which focus on chemical, biological, and phenotypic attributes for representing drugs; (3) popular ML approaches, such as shallow learning-based, deep learning-based, recommender system-based, and knowledge graph-based methods for DDI detection. For each section, related studies are described, summarized, and compared, respectively. In the end, we conclude the research status of DDI prediction based on ML methods and point out the existing issues, future challenges, potential opportunities, and subsequent research direction.

Accurate and sensitive detection of single nucleotide polymorphism (SNP) holds significant clinical implications, especially in the field of cancer diagnosis. Leveraging its high accuracy and programmability, the CRISPR system emerges as a promising platform for advancing the identification of SNPs. In this study, we compared two type V CRISPR/Cas systems (Cas12a and Cas14a) for the identification of cancer-related SNP. Their identification performances were evaluated by characterizing their mismatch tolerance to the BRAF gene. We found that the CRISPR/Cas14a system exhibited superior accuracy and robustness over the CRISPR/Cas12a system for SNP detection. Furthermore, blocker displacement amplification (BDA) was combined with the CRISPR/Cas14a system to eliminate the interference of the wild type (WT) and increase the detection accuracy. In this strategy, we were able to detect BRAF V600E as low as 10 3 copies with a sensitivity of 0.1% variant allele frequency. Moreover, the BDA-assisted CRISPR/Cas14a system has been applied to identify the BRAF mutation from human colorectal carcinoma cells, achieving a high sensitivity of 0.5% variant allele frequency, which is comparable to or even superior to those of most commercially available products. This work has broadened the scope of the CRISPR system and provided a promising method for precision medicine.

Effective accumulation and penetration of antibiotics in the biofilm are critical issues for bacterial infection treatment. Red blood cells (RBCs) have been widely utilized to hitchhike nanocarriers for drug delivery. It is vital and challenging to find a nanocarrier with an appropriate affinity toward RBCs and bacteria for selective hitchhiking and release that determines the drug delivery efficiency and specificity. Herein, we report a zwitterionic polymer poly(2-( N -oxide- N , N -diethylamino)ethyl methacrylate) (OPDEA)-based micelle, which can hitchhike on RBCs in blood and preferentially release in the infection site. We found that OPDEA could bind to the RBCs cell membrane via phospholipid-related affinity and transfer to Gram-positive bacteria due to nearly an order of magnitude stronger interaction with the bacteria cell wall. The zwitterionic surface and cell-wall affinity of OPDEA-based micelles also promote their penetration in biofilm. The clarithromycin-loaded OPDEA micelles show efficient drug delivery into the infection site, resulting in excellent therapeutic performance in both peritonitis and pneumonia models by intravenous or spray administration. This simple RBC-selective hitchhiking and releasing antibiotic delivery system provides a promising strategy for the design of antibacterial nanomedicines.

We developed a procedure for selective 2,4-dimethylphenol, DMPh , direct electro-oxidation to 3,3',5,5'-tetramethyl-2,2'-biphenol, TMBh , a C-C coupled product. For that, we used an electrode coated with a product-selective molecularly imprinted polymer (MIP). The procedure is reasonably selective toward TMBh without requiring harmful additives or elevated temperatures. The TMBh product itself was used as a template for imprinting. We followed the template interaction with various functional monomers (FMs) using density functional theory (DFT) simulations to select optimal FM. On this basis, we used a prepolymerization complex of TMBh with carboxyl-containing FM at a 1:2 TMBh- to-FM molar ratio for MIP fabrication. The template-FM interaction was also followed by using different spectroscopic techniques. Then, we prepared the MIP on the electrode surface in the form of a thin film by the potentiodynamic electropolymerization of the chosen complex and extracted the template. Afterward, we characterized the fabricated films by using electrochemistry, FTIR spectroscopy, and AFM, elucidating their composition and morphology. Ultimately, the DMPh electro-oxidation was performed on the MIP film-coated electrode to obtain the desired TMBh product. The electrosynthesis selectivity was much higher at the electrode coated with MIP film in comparison with the reference nonimprinted polymer (NIP) film-coated or bare electrodes, reaching 39% under optimized conditions. MIP film thickness and electrosynthesis parameters significantly affected the electrosynthesis yield and selectivity. At thicker films, the yield was higher at the expense of selectivity, while the electrosynthesis potential increase enhanced the TMBh product yield. Computer simulations of the imprinted cavity interaction with the substrate molecule demonstrated that the MIP cavity promoted direct coupling of the substrate to form the desired TMBh product.

Anticancer nanomedicines have been proven effective in mitigating the side effects of chemotherapeutic drugs. However, challenges remain in augmenting their therapeutic efficacy. Nanomedicines responsive to the pathological abnormalities in the tumor microenvironment (TME) are expected to overcome the biological limitations of conventional nanomedicines, enhance the therapeutic efficacies, and further reduce the side effects. This Review aims to quantitate the various pathological abnormalities in the TME, which may serve as unique endogenous stimuli for the design of stimuli-responsive nanomedicines, and to provide a broad and objective perspective on the current understanding of stimuli-responsive nanomedicines for cancer treatment. We dissect the typical transport process and barriers of cancer drug delivery, highlight the key design principles of stimuli-responsive nanomedicines designed to tackle the series of barriers in the typical drug delivery process, and discuss the "all-into-one" and "one-for-all" strategies for integrating the needed properties for nanomedicines. Ultimately, we provide insight into the challenges and future perspectives toward the clinical translation of stimuli-responsive nanomedicines.

The aim of the present study was to investigate how different polymers affect the dissociation of cocrystals prepared by co-spray-drying active pharmaceutical ingredient (API), coformer, and polymer. Diclofenac acid-l-proline cocrystal (DPCC) was selected in this study as a model cocrystal due to its previously reported poor physical stability in a high-humidity environment. Polymers investigated include polyvinylpyrrolidone (PVP), poly(1-vinylpyrrolidone- co -vinyl acetate) (PVPVA), hydroxypropyl methyl cellulose, hydroxypropylmethylcellulose acetate succinate, ethyl cellulose, and Eudragit L-100. Terahertz Raman spectroscopy (THz Raman) and powder X-ray diffraction (PXRD) were used to monitor the cocrystal dissociation rate in a high-humidity environment. A Raman probe was used in situ to monitor the extent of the dissociation of DPCC and DPCC in crystalline solid dispersions (CSDs) with polymer when exposed to pH 6.8 phosphate buffer and water. The solubility of DPCC and solid dispersions of DPCC in pH 6.8 phosphate buffer and water was also measured. The dissociation of DPCC was water-mediated, and more than 60% of DPCC dissociated in 18 h at 40 °C and 95% RH. Interestingly, the physical stability of the cocrystal was effectively improved by producing CSDs with polymers. The inclusion of just 1 wt % polymer in a CSD with DPCC protected the cocrystal from dissociation over 18 h under the same conditions. Furthermore, the CSD with PVPVA was still partially stable, and the CSD with PVP was stable (undissociated) after 7 days. The superior stability of DPCC in CSDs with PVP and PVPVA was also demonstrated when systems were exposed to water or pH 6.8 phosphate buffer and resulted in higher dynamic solubility of the CSDs compared to DPCC alone. The improvement in physical stability of the cocrystal in CSDs was thought to be due to an efficient mixing between polymer and cocrystal at the molecular level provided by spray drying and in situ gelling of polymer. It is hypothesized that polymer chains could undergo gelling in situ and form a physical barrier, preventing cocrystal interaction with water, which contributes to slowing down the water-mediated dissociation.

As the main anthropogenic source in open seas and coastal areas, ship emissions impact the climate, air quality, and human health. The latest marine fuel regulation with a sulfur content limit of 0.5% went into effect globally on January 1, 2020. Investigations of ship emissions after fuel switching are necessary. In this study, online field measurements at an urban coastal site and modeling simulations were conducted to detect the impact of ship emissions on air quality in the Greater Bay Area (GBA) in China under new fuel regulation. By utilizing a high mass-resolution single particle mass spectrometer, the vanadium(V) signal was critically identified and was taken as a robust indicator for ship-emitted particles (with relative peak area > 0.1). The considerable number fractions of high-V particles (up to 30-40% during ship plumes) indicated that heavy fuel oils via simple desulfurization or blending processes with low-sulfur fuels were extensively used in the GBA to meet the global 0.5% sulfur cap. Our results showed that ship-emitted particulate matter and NO x contributed up to 21.4% and 39.5% to the ambient, respectively, in the summertime, significantly affecting the air quality in the GBA. The sea-land breeze circulation also played an important role in the transport pattern of ship-emitted pollutants in the GBA.

The design and preparation of catalysts with both excellent stability and maximum exposure of catalytic active sites is highly desirable; however, it remains challenging in heterogeneous catalysis. Herein, a entropy-stabilized single-site Mo catalyst via a high-entropy perovskite oxide LaMn 0.2 Fe 0.2 Co 0.2 Ni 0.2 Cu 0.2 O 3 (HEPO) with abundant mesoporous structures was initiated by a sacrificial-template strategy. The presence of electrostatic interaction between graphene oxide and metal precursors effectively inhibits the agglomeration of precursor nanoparticles in a high-temperature calcination process, thereby endowing the atomically dispersed Mo 6+ coordinated with four O atoms on the defective sites of HEPO. The unique structure of single-site Mo atoms' random distribution with an atomic scale greatly enriches the oxygen vacancy and increases surface exposure of the catalytic active sites on the Mo/HEPO-SAC catalyst. As a result, the obtained Mo/HEPO-SAC exhibits robust recycling stability and ultra-high oxidation activity (turnover frequency = 3.28 × 10 -2 ) for the catalytic removal of dibenzothiophene (DBT) with air as the oxidant, which represents the top level and is strikingly higher than the state-of-the-art oxidation desulfurization catalysts reported previously under the same or similar reaction conditions. Therefore, the finding here for the first time expands the application of single-atom Mo-supported HEPO materials into the field of ultra-deep oxidative desulfurization.

Recent experiments report a charge density wave (CDW) in the antiferromagnet FeGe, but the nature of the charge ordering and the associated structural distortion remains elusive. We discuss the structural and electronic properties of FeGe. Our proposed ground state phase accurately captures atomic topographies acquired by scanning tunneling microscopy. We show that the 2 × 2 × 1 CDW likely results from the Fermi surface nesting of hexagonal-prism-shaped kagome states. FeGe is found to exhibit distortions in the positions of the Ge atoms instead of the Fe atoms in the kagome layers. Using in-depth first-principles calculations and analytical modeling, we demonstrate that this unconventional distortion is driven by the intertwining of magnetic exchange coupling and CDW interactions in this kagome material. The movement of Ge atoms from their pristine positions also enhances the magnetic moment of the Fe kagome layers. Our study indicates that magnetic kagome lattices provide a material candidate for exploring the effects of strong electronic correlations on the ground state and their implications for transport, magnetic, and optical responses in materials.

Transcytosis-based active transport of cancer nanomedicine has shown great promise for enhancing its tumor extravasation and infiltration and antitumor activity, but how the key nanoproperties of nanomedicine, particularly particle size, influence the transcytosis remains unknown. Herein, we used a transcytosis-inducing polymer, poly[2-( N -oxide- N , N -diethylamino)ethyl methacrylate] (OPDEA), and fabricated stable OPDEA-based micelles with different sizes (30, 70, and 140 nm in diameter) from its amphiphilic block copolymer, OPDEA- block -polystyrene (OPDEA-PS). The study of the micelle size effects on cell transcytosis, tumor extravasation, and infiltration showed that the smallest micelles (30 nm) had the fastest transcytosis and, thus, the most efficient tumor extravasation and infiltration. So, the 7-ethyl-10-hydroxyl camptothecin (SN38)-conjugated OPDEA micelles of 30 nm had much enhanced antitumor activity compared with the 140 nm micelles. These results are instructive for the design of active cancer nanomedicine.

Appropriate treatments for acute traumas tend to avoid hemorrhages, vascular damage, and infections. However, in the homeostasis-imbalanced wound microenvironment, currently developed therapies could not precisely and controllably deliver biomacromolecular drugs, which are confronted with challenges due to large molecular weight, poor biomembrane permeability, low dosage, rapid degradation, and bioactivity loss. To conquer this, we construct a simple and effective layer-by-layer (LBL) self-assembly transdermal delivery patch, bearing microneedles (MN) coated with recombinant human epidermal growth factor (LBL MN-rhEGF) for a sustained release to wound bed driven by typical electrostatic force. Pyramidal LBL MN-rhEGF patches hold so enough mechanical strength to penetrate the stratum corneum, and generated microchannels allow rhEGF direct delivery in situ. The administrable delivery of biomacromolecular rhEGF through hierarchically coated MN arrays follows the diffusion mechanism of Fick's second law. Numerous efforts further have illustrated that finger-pressing LBL MN-rhEGF patches could not only promote cell proliferation of normal human dermal fibroblasts (NHDF) and human umbilical vein endothelial cells (HUVEC) in vitro but also take significant effects (regenerative epidermis: ∼144 μm; pro-angiogenesis: higher CD31 expression) in accelerating wound healing of mechanically injured rats, compared to the traditional dressing, which relies on passive diffusion. Our proof-of-concept features novel LBL biomacromolecular drug-delivery systems and self-administrated precision medicine modes at the point of care.

Multiplex protein imaging technologies enable deep phenotyping and provide rich spatial information about biological samples. Existing methods have shown great success but also harbored trade-offs between various pros and cons, underscoring the persisting necessity to expand the imaging toolkits. Here we present PACIFIC: photoactive immunofluorescence with iterative cleavage, a new modality of multiplex protein imaging methods. PACIFIC achieves iterative multiplexing by implementing photocleavable fluorophores for antibody labeling with one-step spin-column purification. PACIFIC requires no specialized instrument, no DNA encoding, or chemical treatments. We demonstrate that PACIFIC can resolve cellular heterogeneity in both formalin-fixed paraffin-embedded (FFPE) samples and fixed cells. To further highlight how PACIFIC assists discovery, we integrate PACIFIC with live-cell tracking and identify phosphor-p70S6K as a critical driver that governs U87 cell mobility. Considering the cost, flexibility, and compatibility, we foresee that PACIFIC can confer deep phenotyping capabilities to anyone with access to traditional immunofluorescence platforms., Competing Interests: The authors declare no competing financial interest., (© 2023 The Authors. Published by American Chemical Society.)