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Macrophages make up a heterogeneous population of immune cells that exhibit diverse phenotypes and functions in health and disease. Although macrophage epigenomic and transcriptomic profiles have been reported, the proteomes of distinct macrophage populations under various pathological conditions remain largely elusive. Here, we employed a label-free proteomic approach to characterize the diversity of the hepatic macrophage pool in an experimental model of CCl4-induced liver fibrosis. We found a decrease in the proportion of liver resident embryo-derived KCs (EmKCs), and a drastic increase in the proportion of monocyte-derived KCs (MoKCs) and CLEC2–Macs. Proteomic profiling revealed that MoKCs largely resembled EmKCs, whereas CLEC2–Macs exhibited greater proteomic alternations compared with EmKCs, suggesting two distinct destinations for monocyte differentiation during liver fibrosis. Furthermore, CLEC2–Macs were characterized by increased expression of proteins associated with inflammatory response, antigen processing and presentation processes, which may be involved in the pathogenesis of liver fibrosis. Collectively, our study provides insights into the considerable heterogeneity within the hepatic macrophage pool during liver fibrosis.

Rapid quantitative testing of illegal drugs is urgently needed for precisely cracking down on drug crimes. Herein, an optimized paper-based surface-enhanced Raman spectroscopy (SERS) platform with patterned printing of plasmonic nanoparticles was constructed for the on-site quick testing of illegal drugs in urine. The filter paper was first coated with a layer of positive-charged chitosan, so as to reduce its roughness by filling the holes of the cellulose matrix and enhance the adhesion of negative-charged silver ink. Subsequently, hydrophobic modification was performed based on the binary silylation reaction, which could obviously improve the sensitivity of the paper-based SERS substrate by concentrating the amount of analyte. Meanwhile, SERS-active silver ink was fabricated and further printed on the surface of the above modified paper with custom-designed pattern (3 × 6). The performance of this SERS platform was assessed by using crystal violet (CV) as a model tag, and the obtained results proved it possesses excellent sensitivity and reproducibility, in which the relative standard deviation (RSD) dropped remarkably. More importantly, as a proof of concept, rapid detection of standard methylamphetamine (MAMP), one of the most widely abused drugs, was achieved with a limit of detection (LOD) of 1.43 ppb using a portable Raman spectrometer. And it also had a good capability in human urine sample detection, with a correlation index (R2) up to 0.9927. This optimized paper-based SERS platform was easily manufactured, cheap, and portable, providing a new strategy for the on-site detection of illicit drugs.

Herein, we present a copper-catalyzed method for oxidative α-double bond formation in α-amino ketone compounds using DTBP as the oxidant. This process, involving homocoupling of α-amino radicals and arylamine release, efficiently produces a series of enaminone skeletons. The strategy has a broad substrate scope and functional group tolerance. In particular, arylamines bearing electron-rich substituents exhibit a pronounced reactivity. This approach facilitates the synthesis of diverse enaminones, enabling the efficient construction of nitrogen-containing heterocycles.

Skyrmion Hall effect (SkHE) remains an obstacle for the application of magnetic skyrmions. While methods have been established to cancel or compensate SkHE in artificial antiferromagnets and ferrimagnets, eliminating intrinsic SkHE in ferromagnets is still a big challenge. Here, we propose a strategy to eliminate SkHE by intercalating nonmagnetic elements into van der Waals bilayer ferromagnets featuring in-plane ferromagnetism. The in-plane magnetism, along with a delicate balance among exchange interactions, Dzyaloshinskii–Moriya interactions (DMI), and magnetocrystalline anisotropy, creates interlayer bimerons/quadmerons, whose polarity can be controlled by DMI. Opposite DMI in the upper and lower layers results in opposite polarity and topological charge number Q-locking of topological spin texture, therefore, eliminating the SkHE. By intercalating Sr (Ba) in bilayer VSe2, we identify ten topological magnetic structures with zero topological charge number. Furthermore, we present a phase diagram illustrating diverse magnetic configurations achievable within the bimagnetic atomic layer, offering valuable guidance for future investigations.

In this paper, the output tracking control problem for fractional-order (FO) systems with inaccessible state is investigated, and a new fractional-order model reference adaptive control (FOMRAC) method is proposed. The designed FO adaptive update law is able to adjust the controller parameters online in real time according to the system output information. Compared with the classical output feedback FOMRAC method, the proposed FOMRAC strategy only needs the online updating of a scalar function, which significantly reduces the complexity of the controller design and the online computational burden, and can achieve better control effect. Furthermore, the scheme ensures the boundedness of the closed-loop signals and that the mean value of the squared norm of the output error converges to zero. Finally, simulation results are carried out to verify the effectiveness of the established approach.

Realizating of a low work function (WF) and room-temperature stability in electrides is highly desired for various applications, such as electron emitters, catalysts, and ion batteries. Herein, a criterion based on the electron localization function (ELF) and projected density of states (PDOS) in the vacancy of the oxide electride [Ca24Al28O64]4+(4e–) (C12A7) was adopted to screen out 13 electrides in single-metal oxides. By creating oxygen vacancies in nonelectride oxides, we find out 9 of them showed vacancy-induced anionic electrons. Considering the thermodynamic stability, two electrides with ordered vacancies, Nb3O3and Ce4O3, stand out and show vacancy-induced zero-dimensional anionic electrons. Both exhibit low WFs, namely 3.1 and 2.3 eV for Nb3O3and Ce4O3, respectively. In the case of Nb3O3, the ELF at oxygen vacancies decreases first and then increases during the decrease in the total number of electrons in self-consistent calculations due to Nb’s multivalent state. Meanwhile, Ce4O3displays promise for ammonia synthesis due to its low hydrogen diffusion barrier and low activation energy. Further calculations revealed that CeO with disordered vacancies at low concentrations also exhibits electride-like properties, suggesting its potential as a substitute for Ce4O3.

This paper uses the 2010 and 2020 Population Census micro-data to analyze relevant characteristics and trends over the decade. The analysis includes the following aspects: population size of rural children left-behind, their age structure and sex composition, regional distribution, living arrangements, and educational development. The findings show that the population size of rural children left-behind remained large, and the likelihood of children being left-behind was closely related to age, with no significant difference by sex. An increasing proportion of rural children left-behind were cared for by grandparents as more mothers migrated between 2010 and 2020. Rural children left-behind no longer had an advantage in educational opportunities compared with average rural children. Over-age attendance was more prevalent among rural children left-behind than all rural children. Continuous attention should be paid to the issue of rural children left-behind and efforts should be made to address its root causes.

P3-layered transition oxide cathodes have garnered considerable attention owing to their high initial capacity, rapid Na+kinetics, and less energy consumption during the synthesis process. Despite these merits, their practical application is hindered by the substantial capacity degradation resulting from unfavorable structural transformations, Mn dissolution and migration. In this study, we systematically investigated the failure mechanisms of P3 cathodes, encompassing Mn dissolution, migration, and the irreversible P3–O3′ phase transition, culminating in severe structural collapse. To address these challenges, we proposed an interfacial spinel local interlocking strategy utilizing P3/spinel intergrowth oxide as a proof-of-concept material. As a result, P3/spinel intergrowth oxide cathodes demonstrated enhanced cycling performance. The effectiveness of suppressing Mn migration and maintaining local structure of interfacial spinel local interlocking strategy was validated through depth-etching X-ray photoelectron spectroscopy, X-ray absorption spectroscopy, and in situ synchrotron-based X-ray diffraction. This interfacial spinel local interlocking engineering strategy presents a promising avenue for the development of advanced cathode materials for sodium-ion batteries.

A wide range of N-CF3imidoyl chlorides were synthesized for the first time via the N-trifluoromethylation of nitriles in DCM by using AlCl3-activated PhICF3Cl as the CF3source. The reactions of them with N-/O-/S-nucleophiles, as well as with 1,3-dipoles, were carried out to efficiently deliver N-CF3amidines/imidates/thioimidates and N-CF3azoles, demonstrating that they are a class of scalable NCF3-containing synthons in the synthesis of N-CF3compounds.

High-temperature rechargeable batteries are essential for energy storage in elevated-temperature situations. Due to the resource abundance of potassium, high-temperature K-ion batteries are drawing increasing research interest. However, raising the working temperature would aggravate the chemical and mechanical instability of the KIB anode, resulting in very fast capacity fading, especially when high capacity is pursued. Here, we demonstrated that a porous conductive metal–organic framework (MOF), which is constructed by N-rich aromatic molecules and CuO4units via π–d conjugation, could provide multiple accessible redox-active sites and promised robust structure stability for efficient potassium storage at high temperatures. Even working at 60 °C, this MOF anode could deliver high initial capacity (455 mAh g–1), impressive rate, and extraordinary cyclability (96.7% capacity retention for 1600 cycles), which is much better than those of reported high-temperature KIB anodes. The mechanistic study revealed that C═N groups and CuO4units contributed abundant redox-active sites; the synergistic effect of π–d conjugated character and reticular porous architecture facilitated the K+/e–transport and ensured an insoluble electrode with small volume deformation, thus achieving stable high-capacity potassium storage.

Background Non-alcoholic fatty liver disease (NAFLD) is severely affecting the quality of people’s life. Rhapontigenin (RA) is a stilbene compound isolated from RhubarbL., which has been reported to have an effect on cholesterol diet-induced hyperlipidemia in rats. This study aims to explore the pharmacodynamics and the mechanism of RA obtained from Rheum franzenbachiiMunt. against NAFLD. RA was extracted from the roots of the RheumL. (Polygonaceae) plant Rheum franzenbachiiMunt.Materials and Methods RA was extracted by Sephadex-gel column and identified by high-performance liquid chromatography (HPLC)-UV and HR-ESI-MS. The pharmacodynamic indexes of L-02 cells and mice treated with RA were determined by histological staining and ELISA, while the expression of autophagy-related proteins was analyzed by Western blot.Results The results in vivoshowed that the liver structure of RA-treatment mice was normal, and the organ coefficient was significantly decreased. It also showed that RA could significantly reduce the expression of reactive oxygen species (ROS) in the liver as well as inhibit oxidative stress and inflammatory response. Interestingly, the autophagy inhibitor 3-methyladenine (3-MA) could reverse the effect of RA on NAFLD, which further confirmed that RA plays an anti-NAFLD role through activating lipophagy.Conclusion It suggested that RA has an effect on NAFLD by down-regulating the expression of Acyl-CoA oxidase 1 (ACOX1), p-mTOR, and p-Unc-51-like kinase 1 (ULK1), then inhibiting Acetyl-CoA (A-CoA) production, and up-regulating the expression of autophagy protein 5 (Atg5) to promote the lipophagy of lipocytes.

Chiral inorganic nanoparticles (NPs) possess enantiospecific properties that have broad potential applications. However, the mechanisms underlying the formation of chiral NPs, especially in the initial stage, have remained elusive at the atomic level. Here, we investigate the nucleation and growth processes of 85 Au atoms (Au85) in the presence of chiral (l-/d-cysteine, Cys) and achiral (propyltrimethylammounium chloride, PTAC) surface ligands by using atomistic molecular dynamics simulations. Subsequent circular dichroism (CD) spectral calculations demonstrate that Au85-l-Cys and Au85-d-Cys clusters are chiral enantiomers. The finding highlights the role of chiral surface ligands in inducing the enantioselective growth of chiral clusters. Further simulation shows that the Au85-PTAC cluster, in which the capping ligands are achiral, also exhibits CD signals. The calculation results indicate that the chirality in Au clusters originates from the geometrical distortions, and chiral surface ligands are optional for the formation of chiral clusters. This work provides insight into the fundamental processes governing the formation of chiral NPs.

Tumor-associated macrophages (TAMs) are key regulators in tumor progression, but the precise role of bone marrow-derived monocytes (Mons) as TAM precursors and their dynamic phenotypes regulated by the tumor microenvironment (TME) remain unclear. Here, we developed an optimized microproteomics workflow to analyze low-cell-number mouse myeloid cells. We sorted TAMs and their corresponding Mons (1 × 105per sample) from individual melanoma mouse models at both the early and late stages. We established the protein expression profiles for these cells by mass spectrometry. Subsequently, we analyzed the dynamics phenotypes of TAMs and identified a characteristic protein expression profile characterized by upregulated cholesterol metabolism and downregulated immune responses during tumor progression. Moreover, we found the downregulation of both STAT5 and PYCARD expression not only in late-stage TAMs but also in late-stage Mons, indicating a loss of the ability to induce inflammatory responses prior to Mons infiltration into TME. Taken together, our study provides valuable insights into the progression-dependent transitions between TAMs and their precursor cells, as well as the cross-organ communications of tumor and bone marrow.

Studying molecular recognition in aqueous environments is crucial for understanding biological processes. Herein, we present a series of N-doped endo-functionalized anthracene-based cavities by introducing inward-directed pyridine units. The subtle modifications can significantly affect the binding properties of these receptors, which is similar to the mutations in biological systems. Combining theoretical calculations and molecular recognition experiments demonstrated that these “mutations” have an impact on the hydrophobicity and charge distribution of the hosts, consequently significantly influencing molecular recognition. This is crucial for understanding the intricate mechanisms of molecular-level interactions in biological receptors.

Two-dimensional conductive metal-organic frameworks (2D c-MOFs) with high flexibility in structure design and functionalization have inspired numerous research interests as promising multifunctional materials due to their porous structure, high conductivity, and rich redox active sites. This review offers a concise overview of 2D c-MOF syntheses and their applications in rechargeable batteries. The electron transport mechanism of 2D c-MOFs will be briefly introduced first. Then we discuss the designs and syntheses of 2D c-MOFs, emphasizing the conjugate structure for high conductivity and the redox activity for efficient energy storage. The electrochemical behaviors of the 2D c-MOFs in different rechargeable battery systems are summarized with attention to their structure-performance correlations and storage mechanism. Particular attention is paid to the significant applied potential of 2D c-MOFs in the Na-ion batteries (NIBs) and K-ion batteries (KIBs), which are more sustainable battery chemistries but are plagued by the dissatisfactory battery performances due to the large size of the Na+and K+. The challenges and opportunities regarding their efficient synthesis and rechargeable battery applications are also discussed. We expect this review will spark new endeavors to promote the further development of 2D c-MOFs for advanced rechargeable batteries.

P2-type layered oxide, Na2/3Ni1/3Mn2/3O2, has drawn particular interest as a promising cathode material for sodium-ion batteries (SIBs) due to its fast sodium-ion transport channels with low migration potential. However, some catastrophic flaws, such as air instability, complicated multiphase evolution, and irreversible anionic redox, limit its electrochemical performance and hinder its application. Here, an air-stable single-crystal P2-type Na2/3Ni1/3Mn1/3Ti1/3O2is proposed based on the multifunctional structural modulation of Ti substitution that could alleviate the issues for practical SIBs. As a result, the cathode with high energy density shows excellent air stability and highly reversible phase transitions (P2-OP4), and delivers faster kinetics and stable anion redox chemistry. Meanwhile, a thorough investigation of the relationship between structure, function, and properties is demonstrated, emphasizing formation processes, electrochemical behavior, structural evolution, and air stability. Overall, this study provides the direction of multifunctional structural modulation for the development of high-performance sodium-based layered cathode materials for practical applications.

The hybrid anode formed by hard carbon with more disordered mesoporous structure and lithophilic groups and deposition lithium keeps the reversibility of lithium metal and the uniform deposition of lithium, which shows excellent fast charging performance.

To efficiently and conveniently realize the topology design with many degrees of freedom (DoFs), this work proposes an inverse topological design method (ITDM) based on machine learning for frequency-selective-surface (FSS) structures from a novel perspective. In the proposed ITDM, the input is a set of desired $\vert \text{S}11\vert $ curves, and the output is the predicted FSS structure presented as an image to directly reveal the distribution of binary pixels in the modeling domain. To obtain the training dataset, an efficient training dataset construction strategy is proposed based on several classical FSS structures. The advantage of this approach is that the training samples can be guaranteed with high-quality; thus, the convergence of the model is faster. Two numerical examples of single-layer and double-layer FSS structures involving large numbers of binary variables (900 and 1800, respectively) are employed to validate the effectiveness of the proposed ITDM. Meanwhile, the fabricated topological structures are also measured to verify the performance of a designed FSS obtained from ITDM.

Hepatocellular carcinoma (HCC), particularly when accompanied by microvascular invasion (MVI), has a markedly high risk of recurrence after liver resection. Adjuvant immunotherapy is considered a promising avenue. This multicenter, open-label, randomized, controlled, phase 2 trial was conducted at six hospitals in China to assess the efficacy and safety of adjuvant sintilimab, a programmed cell death protein 1 inhibitor, in these patients. Eligible patients with HCC with MVI were randomized (1:1) into the sintilimab or active surveillance group. The sintilimab group received intravenous injections every 3 weeks for a total of eight cycles. The primary endpoint was recurrence-free survival (RFS) in the intention-to-treat population. Key secondary endpoints included overall survival (OS) and safety. From September 1, 2020, to April 23, 2022, a total of 198 eligible patients were randomly allocated to receive adjuvant sintilimab (n= 99) or undergo active surveillance (n= 99). After a median follow-up of 23.3 months, the trial met the prespecified endpoints. Sintilimab significantly prolonged RFS compared to active surveillance (median RFS, 27.7 versus 15.5 months; hazard ratio 0.534, 95% confidence interval 0.360–0.792; P= 0.002). Further follow-up is needed to confirm the difference in OS. In the sintilimab group, 12.4% of patients experienced grade 3 or 4 treatment-related adverse events, the most common of which were elevated alanine aminotransferase levels (5.2%) and anemia (4.1%). These findings support the potential of immune checkpoint inhibitors as effective adjuvant therapy for these high-risk patients. Chinese Clinical Trial Registry identifier: ChiCTR2000037655.

Manganese-based layered oxides are prospective cathode materials for sodium-ion batteries (SIBs) due to their low cost and high theoretical capacities. The biphasic intergrowth structure of layered cathode materials is essential for improving the sodium storage performance, which is attributed to the synergistic effect between the two phases. However, the in-depth formation mechanism of biphasic intergrowth materials remains unclear. Herein, the layered/tunnel intergrowth Na0.6MnO2(LT-NaMO) as a model material was successfully prepared, and their formation processes and electrochemical performance were systematically investigated. In situ high-temperature X-ray diffraction displays the detailed evolution process and excellent thermal stability of the layered/tunnel intergrowth structure. Furthermore, severe structural strain and large lattice volume changes are significantly mitigated by the interlocking effect between the phase interfaces, which further enhances the structural stability of the cathode materials during the charging/discharging process. Consequently, the LT-NaMO cathode displays fast Na+transport kinetics with a remarkable capacity retention of ∼70.5% over 300 cycles at 5C, and its assembled full cell with hard carbon also exhibits high energy density. These findings highlight the superior electrochemical performance of intergrowth materials due to interlocking effects between layered and tunnel structures and also provide unique insights into the construction of intergrowth cathode materials for SIBs.