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Ionic thermoelectric materials can generate extraordinarily high thermal voltage under small temperature differences due to their orders of magnitude larger Seebeck coefficient than that of electronic materials. Together with their low-cost, environmentally friendly compositions and solution processability, electrolytes have brought renewed prosperity in thermoelectric fields. Despite the rapid growing number of good-performance materials, yet to be implemented in devices, the main challenge is the understanding of the mechanism of the large Seebeck coefficient in practical electrolytes. Here, we show that the ion/polymer interaction in PEG based electrolytes does not only affect the mobility of the ions, but also has a great impact on the Seebeck coefficient. By delicately varying the types of solvent and the concentration of the solute, we could tune the molar conductivity of the electrolytes and correlate with the Seebeck coefficient. The linear relation between the Seebeck coefficient and the logarithm of the molar conductivity is in agreement with the recently reported thermoelectric ratchet effect in ions with hopping dynamics. This could lead to new design rules for ionic thermoelectrics. [ABSTRACT FROM AUTHOR]

The advantages of large output thermovoltage and sustainable constituent materials have generated a rapid growth in research about ionic thermoelectrics. Recently, giant values of ionic Seebeck coefficients up to 10–26 mV K−1 have been reported. However, the fundamental understanding of the ionic thermoelectric effect is still rudimentary and there is a lack of a well-established measurement standard. In this work, we systematically studied the ionic thermoelectric properties of gel electrolytes made of hydroxyethyl cellulose and an ionic liquid. We discovered that the absorbed water from the atmosphere into the cellulose/ionic liquid gel dramatically increases the apparent ionic Seebeck coefficient from 3 to 12.5 mV K−1. We identified the contribution of a hydrovoltaic voltage generated from water concentration difference as the main reason for the enhanced apparent ionic Seebeck coefficient, which depends on the kinetics of water absorption and desorption on the cold and hot side of the device. Finally, we demonstrated that it is possible to harvest electricity and charge a supercapacitor with intermittent temperature gradients by using this combination of ionic Seebeck voltage and hydrovoltaic voltage. [ABSTRACT FROM AUTHOR]

Finding new luminescent materials is always a meaningful goal in the field of photoelectricity studies. Herein, a new diphosphate compound Ba2LiGa(P2O7)2 (BLGP) was prepared using a high-temperature flux method. It displays an anionic chain structure of [LiGa(P2O7)2]∞, constructed from P2O7, LiO5 and GaO6 polyhedra. The Ba2+ ions are distributed in the voids between the [LiGa(P2O7)2]∞ chains, bonding them and maintaining charge balance. To test its potential as a luminescent host, Eu3+ doped phosphors BLGP:xEu3+ (x = 0.05, 0.10, 0.15, 0.20, 0.25 and 0.30) were synthesized and studied in detail. Upon 394 nm light irradiation, BLGP:xEu3+ showed bright orange emission with a dominant peak at 595 nm due to the 5D0 → 7F1 transition of Eu3+. The optimal doping amount of Eu3+ is 0.20, and the internal quantum efficiency of the phosphor B1.8LGP:0.2Eu3+ was determined to be 67%. The temperature quenching behavior of B1.8LGP:0.2Eu3+ was studied, suggesting that the photoluminescence (PL) intensity decreased to about 50% at 450 K due to thermal quenching. All these features show that this compound is a good luminescent host material for Eu3+ activators. [ABSTRACT FROM AUTHOR]

The self-assembled fabrication of large-area opal photonic crystals (PCs) that are free of cracks has remained a challenge which greatly limits the practicality of such a structure in optical and electronic applications. We report a new route in this paper for fabricating centimeter scale crack-free opal PC films in which the latex spheres are bound together through coordination bonds. The elimination of cracks in the PCs is attributed to the formation of metal ion–polymer latex spheres coordination complexes which is confirmed by shifts of the binding energy of the metal ion after the reaction. The coordination bonds enhance the interactions between the polymer latex spheres, which can neutralize the adhesion stress caused by the substrate and tension stress caused by the shrinkage of the latex spheres during the evaporation of solvent. The as-prepared PC films show a uniform diffraction color and excellent reflection properties, which proves that the formation of coordination bonds does not weaken the contrasts of the refractive index or the optical quality of the PCs. This facile fabrication of large area, crack-free opal PCs will offer significant insight into the preparation and applications of PCs in optical devices. [ABSTRACT FROM AUTHOR]

We study how the electronic structure of a single bilayer Bi on a single quintuple layer Bi2Se3 (Bi2Te3) changes with interface polarization, strain and H adsorption using first-principles calculations. We find that for strained systems the Dirac cone state does not show in the band gap. Coupled with strain and H adsorption, the six spin-polarized Dirac cones in the band gap are created by the interfacing two gapped films. The internal electrical field can result in variations in the work function relative to Bi and Bi2Se3 surfaces. Our findings confirm that the interface polarization, strain and atomic adsorption are the effective means to manipulate electronic structures and topological states on non-metallic surfaces, which could be helpful for realizing atomically thin spintronic devices. [ABSTRACT FROM AUTHOR]

We conducted electrochemical experiments on 5083 aluminum alloy with different microstructures and measured the samples before and after corrosion by SEM and EBSD. At the same time, density functional theory was used to calculate the chloride ion adsorption behavior of the Mg 2 Al 3 phase, which explained the corrosion mechanism on a multi-scale. The results indicated that edge and heart specimens with varying grain sizes exhibited different trends post heat treatment. Specifically, increasing temperature led to larger grain sizes in the heart region, while smaller grain sizes were observed at the edge. Furthermore, the quantity of the second phase was higher after heat treatment at 550 °C compared to 520 °C. The grain size affects the densification of the passivation film and the potential difference between the second phase and the substrate, leading to variations in corrosivity. Density functional theory calculation demonstrates that the Mg 2 Al 3 (001)MgAl and (001)Al surfaces exhibit higher susceptibility to Cl - adsorption, showing the lowest adsorption energies of Cl - at the Mg-top of (001)MgAl and Al-top sites of (001)Al. A stronger bond between Cl - and Mg atoms leads to intergranular corrosion in different directions.

Luminous materials with a rapid lifetime response have garnered significant interest in sensing technology. In this work, the transition element Mn doped phosphor Sr 2 TiO 4 :Mn 4+ was synthesized by a traditional high temperature solid phase method. The emission peak of Sr 2 TiO 4 :0.009Mn 4+ aligns closely with the absorption peak of phytochrome P fr . The temperature-dependent photoluminescence (PL) spectra and lifetime of Sr 2 TiO 4 :0.009Mn 4+ were examined within the temperature range of 273-323 K. The temperature sensing characteristics based on the lifetime were analyzed, and the maximum relative sensitivity was 14.93% K -1 at 309 K. The high sensitivity of the Sr 2 TiO 4 :0.009Mn 4+ phosphor makes it a promising material for temperature sensing applications.

The aggregation of Aβ monomers into oligomers with β-sheet structures is an important cause of Alzheimer's disease (AD), while the Aβ 42 peptide is more toxic and prone to aggregate. It is of great significance to study the inhibition mechanism of Aβ 42 monomer aggregation and find excellent inhibitors for the treatment of AD. Research in recent years has focused on small molecule compounds and nanoparticles, but they all have certain limitations. As a new type of porous material, a porous organic cage (POC) has potential application feasibility in the biomedical field due to its unique physicochemical properties. In this work, molecular dynamics simulations were used for the first time to explore the interaction and conformational transformation of the Aβ 42 peptide in CC3 crystals with different morphologies (planar and spherical). The results show that the adsorption of the Aβ 42 peptide on different CC3 crystals is mainly achieved through strong van der Waals forces. During the simulations, the Aβ 42 peptide undergoes various degrees of structural changes. Compared to that in water, this binding induces more irregular structures, such as turns and 3-helices, and inhibits the production of β-sheets, while enhancing the overall backbone rigidity of the Aβ 42 peptide. The transformation analysis of peptide conformation is further complemented by free energy landscape and cluster analysis. These findings provide a strong basis for CC3 crystals as novel inhibitors to inhibit the toxicity and aggregation of the Aβ 42 peptide.

Chemotherapy-induced immunologic cell death is haunted by the non-specific distribution of chemotherapeutic drugs and insignificant immune activation effects, which render efforts to inhibit the distant metastasis of tumors frustrated. Given the pivotal role that lymph nodes play in tumor metastasis, it is of vital importance whether the drug delivery to tumor-draining lymph nodes (TDLNs) succeeds. In the current study, we developed a doxorubicin-albumin complex (DOX-HSA) solution with the specific ability to simultaneously target the primary tumor and the TDLNs. DOX-HSA could effectively activate and amplify the immunogenic cell death (ICD) effect in both the tumor tissues and the TDLNs, resulting in increased release of damage-associated molecular patterns (DAMPs), which further promoted phagocytosis and maturation of dendritic cells (DCs), stimulated activation of CD8 + T cells, and then significantly enhanced the therapeutic effects of doxorubicin on orthotopic 4T1 tumor-bearing model mice. Therefore, the DOX-HSA solution demonstrated a more prominent ability to control cancer cells and curb metastasis, as well as improved security by reducing cardiotoxicity and myelosuppression toxicity of doxorubicin itself. This DOX-HSA strengthened the synergistic anti-tumor effects based on the ICD effect in combination with traditional chemotherapy, thus providing promising prospects for clinical application.

Five/six-membered benzolactams are significant blocks in both organic and medicinal chemistry. Achieving 5/6-membered benzolactams from the same starting compound under varying reaction conditions presents a significant challenge. Herein, palladium-catalyzed free amine-oriented regioselective C-H activations/carbonylations mediated by hexacarbonylmolybdenum, leading to diverse sizes of benzolactams, respectively, have been developed. Six-membered dihydroisoquinolinones can be obtained selectively in acetic acid using benzoquinone as an oxidant. While unfavorable five-membered isoindolinones were formed in the presence of Cu(II) as an oxidant and dihydrooxazole ligands in 1,2-dichlorobenzene. The substituents on the phenyl ring also had a great influence on the regioselectivity of the reaction. In addition, an asymmetric version of the reaction has also been attempted preliminarily.

Delayed fluorescence (DF) is a unique emitting phenomenon of great interest for important applications in organic optoelectronics. In general, DF requires well-separated frontier orbitals, inherently corresponding to charge transfer (CT)-type emitters. However, facilitating intrinsic DF for local excited (LE)-type conjugated emitters remains very challenging. Aiming to overcome this obstacle, we demonstrate a new molecular design strategy with a DF-inactive B,N-multiple resonance (MR) emitter as a model system. Without the necessity of doping with heavy atoms, we synthesized a co-facial dimer in which an excimer-like state (S exc ) was expected to facilitate efficient reverse intersystem crossing (RISC, T 1 → S exc ) and intrinsic DF. Benefiting from greatly enhanced SOC and reduced Δ E ST , the proof-of-concept emitter Np-2CzB exhibited k RISC up to 6.5 × 10 5 s -1 and intrinsic DF with >35% contribution ( Φ DF / Φ F ) in dilute solution. Further investigation indicated that S exc state formation relies on an optimized co-facial distance ( d = ∼4.7 Å), strong inter-chromophore interaction ( J coul > 450 cm -1 ) and a rigid structure ( Γ S 1 →S 0 < 350 cm -1 ). Although our strategy was demonstrated with a B,N-MR emitter, it can be applicable to many LE-type conjugated emitters without intrinsic DF. By triggering potential DF emission, many classic emitters might play a more important role in optoelectronics., Competing Interests: The authors declare no competing financial interest., (This journal is © The Royal Society of Chemistry.)

The Mallory reaction, which involves the photocyclization of stilbenes/diarylethenes and their analogues into polycyclic aromatics, is of significant synthetic importance. However, its application to tertiary benzanilides has not been explored to date. Besides, most of the reported Mallory reactions require ultraviolet irradiation. In this study, we show the first Mallory reaction of tertiary benzanilides promoted by visible light via iminium intermediates formed in situ from tertiary benzanilide, Tf 2 O (triflic anhydride) and pyridine. UV/vis absorption spectroscopy combined with density functional theory (DFT) calculations revealed that the formation of the iminium intermediate decreased the HOMO-LUMO energy gap, thereby enhancing visible light absorption. This study provides a rapid and practical approach for the preparation of the phenanthridinone skeleton and provides a new idea for the design of new visible light photoswitches., Competing Interests: The authors declare no conflict of interest., (This journal is © The Royal Society of Chemistry.)

The steric effect is one of the most widely used concepts for chemical understanding in publications and textbooks, yet a well-accepted formulation of this effect is still elusive. Experimentally, this concept was quantified by the acid-catalyzed hydrolysis of esters, yielding the so-called Taft steric parameter. Theoretically, we recently proposed a density-based scheme to quantify the effect from density functional theory. In this work, we directly compare these two schemes, one from theory and the other from experiment. To this end, we first establish the ester hydrolysis mechanism with multiple water molecules explicitly considered and then apply the energetic span model to represent the hydrolysis barrier height between the two schemes. Our results show that the barrier height of the reaction series is strongly correlated with both Taft steric parameters from experiment and steric quantification from theory. We also obtained strong correlations with steric potential, steric force, and steric charge from our theoretical scheme. Strong correlations with a few information-theoretic quantities are additionally unveiled. To the best of our knowledge, this is the first time in the literature that such a direct comparison between theoretical and experimental results is made. These results also suggest that our proposed two-water three-step mechanism for ester hydrolysis is effective, and our theoretical quantification of the steric effect is valid, robust, and experimentally comparable. In our view, this work should have satisfactorily addressed the issue of how the steric effect can be formulated and quantified, and thus it lays the groundwork for future applications.

In this work, a green, efficient and catalyst-free synthesis of a series of structurally novel ( E )-diethyl 2-styrylquinoline-3,4-dicarboxylates via a direct olefination reaction between diethyl 2-methylquinoline-3,4-dicarboxylate and various aromatic aldehydes was successfully accomplished by employing eco-friendly 1,3-dimethylurea/l-(+)-tartaric acid (DMU/LTA) as an inexpensive, non-toxic and reusable reaction medium. This methodology has the attractive advantages of mild reaction conditions, simple experimental operation, and the absence of any dangerous catalysts or unsafe volatile organic solvents, with satisfactory to good yields. Subsequently, a primary in vitro evaluation for their anti-proliferative activity against human cancer cell lines A549, HT29 and T24 revealed that the compound with the 3,4,5-trimethoxystyryl moiety exhibited potent anti-tumor activity with IC 50 values of 2.38, 4.52 and 9.86 μmol L -1 , respectively, thereby being equipotent or even better than the reference cisplatin., Competing Interests: The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (This journal is © The Royal Society of Chemistry.)

We show the synthesis and conformational studies of a series of 7,7-disubstituted-dibenzo[ b , d ]oxepin-6(7 H )-ones that feature biaryl-bridged seven-membered lactones with a quaternary carbon center, in which the larger substituents prefer the axial positions. Further studies on the crystal structures and DFT calculations revealed that the high selectivity observed is attributed to the volume of substituents., Competing Interests: There are no conflicts to declare., (This journal is © The Royal Society of Chemistry.)

PKMYT1, a member of the WEE family, plays a crucial role in the cell cycle by specifically phosphorylating CDK1-CyclinB at Tyr15 and Thr14. Recent investigations have revealed that the amplification of CCNE1 and the inhibition of PKMYT1 kinase collectively result in synthetic lethality, further indicating that PKMYT1 is promising as an effective target for tumor therapy. Existing PKMYT1 inhibitors are mostly derivatives of RP-6306 or pan-inhibitors, limiting their further development. Herein, we conducted virtual screening of a natural product library, and in vitro enzyme experiments demonstrated that EGCG, GCG, and luteolin exhibited potent inhibitory activities with IC 50 values of 0.137 μM, 0.159 μM, and 1.5 μM, respectively. Subsequently, analysis of the hit compounds and RP-6306, using different molecular simulation methods, revealed that stable hydrogen bonds with Asp251 and Glu157 in the DFG region were vital for binding to PKMYT1, more so than hydrogen bonds in the hinge and loop regions., Competing Interests: There are no conflicts to declare., (This journal is © The Royal Society of Chemistry.)

Photo-responsive luminescent materials capable of responding to light stimuli are crucial in the realm of sophisticated encryption, anti-counterfeiting, and optical data storage. Yet, the development of such materials that also feature self-healing capabilities, swift reaction times, light weight, fatigue resistance, dynamic display abilities, and enhanced security measures is exceedingly rare and presents considerable challenges. Herein, a novel family of self-healing and photo-stimuli-responsive photoluminescent polymers are reported, which is achieved by interlinking terpyridine- and spiropyran-functionalized polymers through N-Ln coordination bonds and hydrogen bonding among the polymer chains. The resulting polymers exhibit good processability, superior tensile strength, fast self-healing ability, and photo-stimuli-responsive performance. The photo-stimuli-responsive properties include unique color shifts (colorless and purple) and light-controlled time-dependent fluorescence modulation (green-, red-, and yellow-emission), which stem from fine-tuning the isomerization of spiropyran and leveraging the fluorescence resonance energy transfer (FRET) from Ln-Tpy donors to spiropyran acceptors, respectively. Besides, these polymers have been successfully applied in dynamic multi-level information encryption applications. We are convinced that these smart materials, crafted through our innovative approach, hold vast potential for applications in information storage, cutting-edge anti-counterfeiting encryption, UV-sensing, and light-writing technologies, marking a novel strategy in the design of photosensitive luminescent smart materials., Competing Interests: There are no conflicts to declare., (This journal is © The Royal Society of Chemistry.)

Objectives : Osteoarthritis (OA) stands as the prevailing progressive musculoskeletal disease, serving as the primary cause of chronic pain and activity limitations among adults over 40. Flavan-3-ols, common polyphenolic compounds, are believed to harbor anti-inflammatory and anti-aging properties. This study explores the relationship between flavan-3-ol intake and osteoarthritis risk in individuals over the age of 40 in the US. Methods : This study included 7452 participants over the age of 40 from three cycles (2007-2008, 2009-2010, and 2017-2018) of the National Health and Nutrition Examination Survey. Information on OA history was obtained via home surveys. Information on flavan-3-ol monomers intake was obtained using a survey from the Food and Nutrient Database for Dietary Studies. We used a logistic regression model and restricted cubic spline to analyze the relationships between flavan-3-ol monomers and OA. Stratified analyses were also conducted in this study. Results : There were 1056 participants with OA and 6396 without OA. Compared to the first tertile (T1) group, the adjusted odds ratio with a 95% confidence interval (CI) of logistic regression model 2 for the flavan-3-ol T2 group was 1.296 (0.979-1.715) ( p = 0.068), the OR for (-)-epigallocatechin was 1.292 (1.025-1.629) ( p = 0.032), and the OR for (-)-epicatechin 3-gallate was 1.348 (1.013, 1.793) ( p = 0.042). A dose-response curve indicated a non-linear association ( p for non-linearity <0.05) between OA and total flavan-3-ol monomers (nadir point: 483.29 mg, 95% CI: 0.61-0.90). No interaction effects were found in the subgroup analysis. Conclusions : In individuals over 40 in the US, the average daily dietary intake of flavan-3-ol monomers manifests a J-shaped relationship with OA risk.

Soyasaponins, recognized for their anti-inflammatory and antioxidant effects, have not yet been fully explored for their role in combating enterotoxigenic Escherichia coli (ETEC) infections. Recent findings identified them in small-molecule metabolites of Bacillus , suggesting their broader biological relevance. This research screened 88 strains of B. halotolerans , identifying the strain BH M20221856 as significantly inhibitory against ETEC growth in vitro . It also reduced cellular damage and inflammatory response in IPEC-J2 cells. The antimicrobial activity of BH M20221856 was attributed to its small-molecule metabolites rather than secretory proteins. A total of 69 small molecules were identified from the metabolites of BH M20221856 using liquid chromatography mass spectrometry/mass spectrometry (LC-MS/MS). Among these, soyasaponin I (SoSa I) represented the largest multiple change in the enrichment analysis of differential metabolites and exhibited potent anti-ETEC effects in vivo . It significantly reduced the bacterial load of E. coli in mouse intestines, decreased serum endotoxin, D-lactic acid, and oxidative stress levels and alleviated intestinal pathological damage and inflammation. SoSa I enhanced immune regulation by mediating the p105-Tpl2-ERK signaling pathway. Further evaluations using transepithelial electrical resistance (TEER) and cell permeability assays showed that SoSa I alleviated ETEC-induced damage to epithelial barrier function. These results suggest that BH M20221856 and SoSa I may serve as preventative biologics against ETEC infections, providing new insights for developing strategies to prevent and control this disease.

A programmably engineered stochastic RNA nanowalker powered by duplex-specific nuclease (DSN) is developed. By utilizing poly-adenine-based spherical nucleic acids (polyA-SNA) to accurately regulate the densities of DNA tracks, the nanowalker showcases its capability to identify miRNA-21, miRNA-486, and miRNA-155 with quick kinetics and attomolar sensitivity, positioning it as a promising option for cancer clinical surveillance.

In the growing body of scientific literature, the structure and information of drugs are usually represented in two-dimensional vector graphics. Drug compound structures in vector graphics form are difficult to recognize and utilize by computers. Although the current OCSR paradigm has shown good performance, most existing work treats it as a single isolated whole. This paper proposes a multi-stage cognitive neural network model that predicts molecular vector graphics more finely. Based on cognitive methods, we construct a model for fine-grained perceptual representation of molecular images from bottom to top, and in stages, the primary representation of atoms and bonds is potential discrete label sequence (atom type, bond type, functional group, etc. ). The second stage represents the molecular graph according to the label sequence, and the final stage evolves in an extensible manner from the molecular graph to a machine-readable sequence. Experimental results show that MMSSC-Net outperforms current advanced methods on multiple public datasets. It achieved an accuracy rate of 75-94% on cognitive recognition at different resolutions. MMSSC-Net uses a sequence cognitive method to make it more reliable in interpretability and transferability, and provides new ideas for drug information discovery and exploring the unknown chemical space., Competing Interests: There are no conflicts to declare., (This journal is © The Royal Society of Chemistry.)

Exosome-like nanoparticles (ELNs) are novel naturally occurring plant ultrastructures and contain unique bioactive components. However, the potential applications and biological functions of plant ELNs, especially in the context of health promotion and disease prevention, remain largely unexplored. This study aimed to explore the biological activities and functional mechanisms of Actinidia arguta -derived exosome-like nanoparticles (AAELNs). We reported the development of AAELNs, which possess particle sizes of 157.8 nm and a negative surface charge of -23.07 mV, uptaking by RAW264.7 cells, and reduction of oxidative stress by decreasing the activity of GSH-Px and T-SOD and increasing the content of MDA. Through the use of high-throughput sequencing technology, 12 known miRNA families and 23 additional miRNAs were identified in AAELNs, GO and KEGG term enrichment analysis revealed the potential of AAELNs-miRNAs in modulating neural-relevant behaviors. Additionally, LC-MS/MS analysis detected a total of 32 major lipid classes, 430 lipid subclasses, and 1345 proteins in AAELNs. Furthermore, in vivo fluorescence disappearance and in vitro fermentation experiments demonstrated that AAELNs were able to enter the colon and improve the microbial structure. These findings suggest that AAELNs could serve as nanoshuttles in food, potentially offering health-enhancing properties.

Carbon-based catalysts catalyze methane decomposition to produce hydrogen is a very attractive technical route. Carbon black in carbon-based catalysts has the advantages of high catalytic activity, good stability and better tolerance to toxic impurities such as sulphur in the feedstock, which has become a hot topic of research for many scientists. In this work, the effect of heat treatment on the structural and surface properties of carbon blacks and their catalytic performance in hydrogen production from methane decomposition was investigated. A commercial carbon blacks N110 was selected to heat treatment with nitrogen or carbon dioxide atmosphere at 850 °C, respectively. The Raman spectrums indicated that the graphitization degree of modified carbon under two atmospheres were promoted with the treatment time increasing. BET results revealed that the specific surface area of the carbon black treated under carbon dioxide increased, while the specific surface area was unchanged for that of the carbon black treated under nitrogen. The catalytic test of the two modified carbon blacks for methane decomposition exhibited the almost same activity, which meant that the graphitization degree of carbon black is the key factor for methane decomposition rather than the specific surface area. It was suggested that highly graphitized carbon black could be used as the potential catalysts for hydrogen production from methane decomposition., Competing Interests: The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (This journal is © The Royal Society of Chemistry.)

Herein, we report that prism[6]arenes (PrS[6]R) can form charge-transfer (CT) inclusion complexes with tropylium tetrakis[3,5-bis(trifluoromethyl)-phenyl]borate (G) in chloroform solution with an obvious CT band at 560 nm. Moreover, the CT complex PrS[6]Et⊃G showed Cl - /Ag + responsiveness which can be easily monitored by the naked eye.

Amorphous, α, β, and γ-phase yttrium disilicate Y 2 Si 2 O 7 pellets were synthesized by spark plasma sintering, and their chemical durability and degradation mechanisms were investigated via semi-dynamic leaching test in pH = 3 nitric acid at 90 °C. All crystalline phases displayed relatively congruent dissolution with a slight preferential release of Y. The amorphous sample showed clear incongruent dissolution with preferential release of Y, leading to a surface reorganization reaction and the formation of a SiO 2 passivation layer 20-25 μm thick on the surface of the sample. This passivation layer led to a continuous decrease in the elemental release rates of the amorphous sample. The γ-phase sample displayed the lowest short-term and long-term leaching rates of Y and Si, followed by the β, α, and then amorphous sample. The crystalline samples showed increasing release rates over time indicating a dissolution-controlled reaction mechanism. Post-leaching microstructural characterization of the β and γ samples revealed variations in the corrosion levels of the surface grains, indicating a dependence on grain orientation., Competing Interests: The authors declare that they have no conflict of interest., (This journal is © The Royal Society of Chemistry.)

Flexible strain sensors have drawn a lot of interest in various applications including human mobility tracking, rehabilitation/personalized health monitoring, and human-machine interaction, but suffer from interference of electromagnetic (EM). To overcome the EM interference, flexible force sensors without sensitive electronic elements have been developed, with drawbacks of bulky modules that hinders their applications in remote measurement with power-free environment. Therefore, it is highly desirable to fabricate a compact wireless flexible force sensor but it is still a challenge. Here, we demonstrate a fluorescent flexible force sensor based on aggregation-induced emission (AIE) doped liquid crystal elastomer (LCE) experimentally. The proposed force sensor film can be used to measure force through the variation of fluorescent intensity induced by the extension or contraction of LCE film, which leads to reduce or increase of the aggregation degree of AIE molecules within. This compact wireless force sensor features lightweight, low-cost, high flexibility, passivity and anti-EM interference, which also enables the naked eye observation. The proposed sensor provides inspiration and a platform for a new concept of non-contact detection, showing application potential in human-friendly interactive electronics and remote-control integration platform.

It has been reported that the length of branched alkyl side chains on fused-ring electron acceptors confers different impacts on properties versus solubility of BJH blends. However, because this impact on a non-fused acceptor backbone has rarely been studied, we examined the impact of molecular optimization from alkyl chain tuning based on non-fused thiazolothiazole small-molecule acceptors. The length of the side chain on the thiophene bridge was modified from 2-butyloctyl to 2-ethylhexyl, which corresponds to small molecules TTz3(C4C6) and TTz3(C2C4), respectively. Compared with the reported TTz3(C6C8) with long alkyl side chains, TTz3(C4C6) and TTz3(C2C4) exhibited stronger molecular aggregation, higher absorption coefficients, and greater redshifted UV absorption. Unexpectedly, after the alkyl chain was slightly shortened in this type of acceptor system, devices were successfully fabricated, but it was necessary to reduce the blending concentration at low rotation speeds due to the sharp decrease in the solubility of corresponding acceptor materials. Thus, the obtained unfavorable thickness and morphology of the active layer caused a decrease in J sc and FF. As a consequence, TTz3(C4C6)- and TTz3(C2C4)-based devices showed an unsatisfactory power conversion efficiency of 6.02% and 2.71%, respectively, when donors were paired with the wide bandgap donor J71, which is inferior to that of TTz3(C6C8)-based devices (8.76%). These results indicate that it is challenging to determine the limit of the adjustable range of side chains to modify non-fused thiazolothiazole small-molecule acceptors for high-performance non-fullerene solar cells., Competing Interests: The authors declare no conflicts of interest., (This journal is © The Royal Society of Chemistry.)

Environmentally friendly and highly efficient blue luminescent materials are an unremitting pursuit in the optoelectronic field. Herein, we assembled a new 0D lead-free metal halide of (F-PPA)ZnBr4, which exhibits narrow blue light emission with a remarkable PLQY of 50.15%, high stability and high detection sensitivity toward UV light. These results indicate the potential for the application of low-dimensional zinc-based halides in multiple optoelectronic devices.

Inspired by thermally sensitive ion channels in human skin, a polarized membrane composed of a ferroelectric polymer fiber matrix is used to double the heat-induced potential in ionic thermoelectric devices. The comparison of the thermal potentials between different directions of polarization and temperature gradient indicates the importance of cation-dipole interactions for the enhancement.

In recent years, remarkable advancements have been achieved in the field of halide perovskite solar cells (PSCs). However, the commercialization of PSCs has been impeded by challenges such as Pb leakage and the instability of hybrid organic-inorganic perovskites (HOIPs). Hence, the future lies in the development of environmentally friendly inorganic lead-free halide perovskites (LFHPs) based on elements like Sn, Ge, Bi, Sb, and Cu, which show great promise for photovoltaic applications. However, LFHP photovoltaic cells still face challenges such as low efficiency, poor film quality, and stability in comparison to HOIPs. These limitations significantly hinder their further development. To address these issues, element doping strategies, including cationic and anionic doping, as well as the use of additives, are frequently employed. These strategies aim to improve film quality, passivate defects, reduce the band gap, and enhance device performance and stability. In this paper, we aim to provide a comprehensive review of the recent research progress in doping strategies for LFHPs.

Owing to their theranostic properties, cerium oxide (CeO 2 ) nanoparticles have attracted considerable attention for their key applications in nanomedicine. In this study, ultrasmall CeO 2 nanoparticles (particle diameter = 1-3 nm) as X-ray contrast agents with an antioxidant effect were investigated for the first time. The nanoparticles were coated with hydrophilic and biocompatible poly(acrylic acid) (PAA) and poly(acrylic acid- co -maleic acid) (PAAMA) to ensure satisfactory colloidal stability in aqueous media and low cellular toxicity. The synthesized nanoparticles were characterized using high-resolution transmission electron microscopy, X-ray diffraction, Fourier transform-infrared spectroscopy, thermogravimetric analysis, dynamic light scattering, cell viability assay, photoluminescence spectroscopy, and X-ray computed tomography (CT). Their potential as X-ray contrast agents was demonstrated by measuring phantom images and in vivo CT images in mice injected intravenously and intraperitoneally. The X-ray attenuation of these nanoparticles was greater than that of the commercial X-ray contrast agent Ultravist and those of larger CeO 2 nanoparticles reported previously. In addition, they exhibited an antioxidant effect for the removal of hydrogen peroxide. The results confirmed that the PAA- and PAAMA-coated ultrasmall CeO 2 nanoparticles demonstrate potential as highly sensitive radioprotective or theranostic X-ray contrast agents., Competing Interests: There are no conflicts to declare., (This journal is © The Royal Society of Chemistry.)

A general strategy to program self-resettable and dissipative toehold-mediated strand displacement reactions was proposed, using DNA strands as the fuel and lambda exonuclease as the fuel-consuming unit. This non-equilibrium system is reversible and temporally controllable. Furthermore, it can be well integrated into a DNA network to temporally control its cascade reaction or dynamic behaviour.

Injectable self-healing hydrogels are being widely used in drug delivery, tissue engineering, and other fields. Because of their excellent biocompatibility and biodegradability, polypeptides are an ideal candidate for preparing injectable self-healing hydrogels. In this study, a polypeptide-based hydrogel with dual response to hydrogen peroxide and light was obtained by copolymerizing 4-arm PEG-amine, N -( p -nitrophenoxycarbonyl)-l-methionine, and N -( p -nitrophenoxycarbonyl)-γ- o -nitrobenzyl-l-glutamate. The hydrogel exhibits injectable self-healing behavior due to the hydrophobic interactions among peptide blocks, which also act as the reservoir of hydrophobic drug molecules. In the presence of hydrogen peroxide or under light irradiation, the thioether bond in methionine was oxidized to sulfoxide, whereas the o -nitro benzyl ester bond was broken to form glutamic acid. As a result, the corresponding hydrophobic blocks of polypeptide become hydrophilic, accelerating the release of drug molecules loaded in the polypeptide hydrophobic blocks. Using this technique, the controlled release of hydrophobic drug molecules was achieved. Our efforts could provide a new strategy for the preparation of self-healing hydrogels based on polypeptides with a dual response to hydrogen peroxide and light. In this view, the practical application of polypeptides in drug delivery, tissue engineering, and other fields, could be expanded and advanced., Competing Interests: There are no conflicts to declare., (This journal is © The Royal Society of Chemistry.)

Invasive fungal infections, with high morbidity and mortality, have become one of the most serious threats to human health. There are a few kinds of clinical antifungal drugs but large amounts of them are used, so there is an urgent need for a new structural type of antifungal drug. In this study, we carried out three rounds of structural optimisation and modification of the compound YW-01, which was obtained from the preliminary screening of the group, by using the strategy of scaffold hopping. A series of novel phenylpyrimidine CYP51 inhibitors were designed and synthesised. In vitro antifungal testing showed that target compound C6 exhibited good efficacy against seven common clinically susceptible strains, which was significantly superior to the clinical first-line drug fluconazole. Subsequently in vitro tests on metabolic stability and cytotoxicity revealed that C6 was safe and stable for hepatic microsomal function. Finally, C6 warranted further exploration as a possible novel structural type of CYP51 inhibitor., Competing Interests: The authors declare that there are no conflicts of interests., (This journal is © The Royal Society of Chemistry.)

Nanodiamonds (ND) are chemically inert and stable owing to their sp 3 covalent bonding structure, but their surface sp 2 graphitic carbons can be easily homogenized with diverse functional groups via oxidation, reduction, hydrogenation, amination, and halogenation. Further surface conjugation of NDs with hydrophilic ligands can boost their colloidal stability and functionality. In addition, NDs are non-toxic as they are made of carbons. They exhibit stable fluorescence without photobleaching. They also possess paramagnetic and ferromagnetic properties, making them suitable for use as a new type of fluorescence imaging (FI) and magnetic resonance imaging (MRI) probe. In this review, we focused on recently developed ND production methods, surface homogenization and functionalization methods, biocompatibilities, and biomedical imaging applications as FI and MRI probes. Finally, we discussed future perspectives., Competing Interests: There are no conflicts to declare., (This journal is © The Royal Society of Chemistry.)

Background : Chronic inflammation contributes to the occurrence and progression of many diseases. Most previous clinical studies have explored the effect of high-dose CoQ10 supplements on inflammation. Food is another important source of CoQ10, but the relationship between the intake of CoQ10 from dietary sources and inflammation was unknown. We aimed to explore the dose-response association between the intake of dietary-derived CoQ10 and inflammation-related biomarkers. Methods : Seven thousand nine hundred and fifty-three Chinese adults from the China Health and Nutrition Survey (CHNS) were the subjects of this cross-sectional investigation. Dietary CoQ10 intake was assessed using dietary information from three days. High-sensitivity C-reactive protein (hsCRP) and white blood cell count (WBC) were assessed using fasting venous blood. Results : In an adjusted linear regression model, CoQ10 consumption from dietary sources was inversely associated with hsCRP, with effect sizes in each group: Q2 ( β = -0.85 mg L -1 , 95% CI: -1.43 to -0.28 mg L -1 , P = 0.004), Q3 ( β = -0.70 mg L -1 , 95% CI: -1.28 to -0.12 mg L -1 , P = 0.017), and Q4 ( β = -0.79 mg L -1 , 95% CI: -1.39 to -0.19 mg L -1 , P = 0.010). Moreover, restricted cubic splines (RCS) revealed a non-linear L-shaped association between dietary-derived CoQ10 consumption and hsCRP ( P nonlinear < 0.001). According to subgroup analyses, these relationships were more significant in males, or >45 years old ( P trend < 0.05). Nevertheless, no significant relationship was found between dietary-derived CoQ10 intake and WBC. Conclusions : These findings suggested a significant negative association between dietary-derived CoQ10 and hsCRP levels.

Background : Hypertension is closely associated with excessive sodium intake, and low-sodium salt has been shown to lower blood pressure. However, whether low-sodium salt interacts with genetic variation related to salt sensitivity of blood pressure is unclear. Methods : A total of 259 hypertensive patients who completed the previous 3 years of a low-sodium salt vs. normal salt intervention were included in our study. Genetic risk scores (GRSs) of systolic blood pressure (SBP) and diastolic blood pressure (DBP) were respectively built for each participant. A general linear regression model and a generalized mixed model were applied to identify the interaction effects between low-sodium salt intervention and ENaC genetic variation on SBP/DBP changes and trajectories over 3 years. Findings : during the 3-year intervention, both SBP and DBP levels showed a significant decline in the low-sodium salt intervention group than those in the normal salt intervention group over 3 years ( P salt intervention group = 0.001 for SBP and P salt intervention group = 0.006 for DBP). Furthermore, a gene-diet interaction was found for the SBP change trajectory over 3 years ( P SBP-GRS×salt intervention group = 0.011); specifically, significant SBP reductions were found between salt intervention groups in the high SBP-GRS group (-18.77 vs. -9.58 mmHg, P salt intervention group = 0.001), but not in the low SBP-GRS group (-15.71 vs. -14.62 mmHg, P salt intervention group = 0.791). No interaction effect between low-sodium salt intervention and genetic variation of ENaC was found for changes in DBP. Conclusions : Higher ENaC genetic variation is associated with a greater reduction in SBP in response to a low-sodium salt intervention. Hypertensive patients with higher ENaC genetic variation may experience a greater benefit in SBP reductions by consuming low-sodium salt. ( Trial registration : chiCTR-TRC-09000538, https://www.chictr.org.cn).

Developing new and understanding multicomponent reactions (MCRs) is an appealing but challenging task. Herein, Rh(iii)-catalyzed multicomponent double C-H annulations of cyclic diimines (or diketones and acetone), alkynes, and ammonium acetate to assemble functionalized 1,1'-biisoquinolines and C-bridged 1,1'-bisisoquinolines with controllable 14 N/ 15 N editing in one shot has been developed. Through a combination of isotopic-labeling ( 2 H, 18 O, and 15 N) experiments, crystallography, and time-dependent ESI-MS, the reaction process was studied in detail. Ammonium acetate accounts for two rounds of Hofmann elimination and iminization, thus leading to an unprecedented imine dance, cyclic imine → N -alkenyl imine → NH imine. The N -alkenyl imine can immediately guide a C-H annulation (N-retention channel), and some of it is converted into NH-imine to trigger another annulation (N-exchange channel). The channels and 15 N ratios can be regulated by the reaction mode and acidity. Moreover, the resulting 1,1'-biisoquinolines are a privileged ligand scaffold which is exemplified herein by a hydrazine-iodine exchange reaction to form drug-like benzo[ c ]cinnolines., Competing Interests: The authors declare no competing financial interest., (This journal is © The Royal Society of Chemistry.)

A novel metal-organic framework (MOF) Zn-PBC (H 2 PBC = pyridine-3,5-bis(phenyl-4-carboxylic acid)) was designed and synthesized via a solvothermal reaction with the H 2 PBC ligand, and produced a strong fluorescence. The material exhibited good stability and an ideal luminescent property in water. In addition, it was found that Zn-PBC displayed a different fluorescent response to different types of amino acids, and the mechanism was investigated. This research might give insight to the interaction between MOFs and amino acids, which would provide a strategy to fabricate MOF-based sensors for biomolecules in future.

Recently, mechanical biosensors have attracted more attention on single molecule detection due to its high accuracy, low cost, and convenience. However, the sensitivity of the mechanical biosensors restricted their clinical application. Herein, a mechanical biosensor based on membrane-mediated magneto-stress-electric coupled sensitization (MSEC-MMB) was developed to enhance performance. Through introducing Fe 3 O 4 nanoparticles (MNPs) to traditional stress-electric biosensors and applying a magnetic field, a magneto-stress-electric coupled biosensing system was constructed. The sensitivity of the MSEC-MMB was improved via enhancing the deformation of the mechanical membrane, which was demonstrated by detecting HSA. The optimal limit of detection (LOD) was 24 pg mL -1 under a magnetic field of 50 mT. The LOD was significantly 1 order of magnitude lower than that without the magnetic field. Besides, the MSEC-MMB showed a high specificity, selectivity, and stability. The clinical proteinuria samples were accurately detected, suggesting a good practicability of the MSEC-MMB. All these results proved the high sensitivity and practicality of the MSEC-MMB and provide a platform for early nephropathy diagnosis.

Our recent study [M. Li et al.Phys. Chem. Chem. Phys ., 2023, 25 , 2595-2605] unveiled that the impact of an external electric field on molecular acidity and aromaticity for benzoic acid is directional, which can be understood using changes in frontier orbitals and partial charges. However, it is unclear if the effect will disappear when substituting groups are present and whether new patterns of changes will show up. In this work, as a continuation of our efforts to appreciate the impact of external electric fields on physiochemical properties, we find that the directionality effect is still in place for substituted benzoic acid derivatives and that there exists the additivity effect with respect to the number of substituent groups, regardless of the direction of the applied field and the type of substituting groups. We confirm the findings using electron-donating and electron-accepting groups with the electric field applied either parallelly or perpendicularly to the carboxyl group along the benzene ring. The directionality and additivity effects uncovered from this work should enrich the body of our knowledge about the impact of external electric fields on physiochemical properties and could be applicable to other systems and properties as well.

Self-assembled peptide-based hydrogels have shown great potential in bio-related applications due to their porous structure, strong mechanical stability, high biocompatibility, and easy functionalization. Herein, the structure and characteristics of hydrogels and the mechanism of action of several regular secondary structures during gelation are investigated. The factors influencing the formation of peptide hydrogels, especially the pH responsiveness and salt ion induction are analyzed and summarized. Finally, the biomedical applications of peptide hydrogels, such as bone tissue engineering, cell culture, antigen presentation, antibacterial materials, and drug delivery are reviewed.