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CuWO4 is an n-type oxide semiconductor with a bandgap of 2.2 eV which exhibits great potential for photoelectrochemical (PEC) conversion of solar energy into chemical fuels. However, the photocurrent achieved so far is limited to ∼0.3 mA cm−2 at +1.23 V vs. reversible hydrogen electrode (RHE). Possible limiting factors include slow surface reaction kinetics, poor charge carrier mobility and/or presence of surface defect states. A detailed understanding of the fundamental electronic structure and its correlation with PEC activity is of significant importance for devising strategies for further improvements. In this work, we have synthesized CuWO4 thin films showing a record photocurrent density of 0.50 mA cm−2 at +1.23 V vs. RHE. Importantly, we have used a synergistic combination of photoemission spectroscopy, X-ray absorption spectroscopy and density functional theory (DFT) to unravel the electronic structure of CuWO4. Our results show that the valence band (VB) consists of strongly hybridized states of O 2p6 and Cu 3d9, while the bottom of the conduction band (CB) is primarily composed of unoccupied Cu 3d states. The localized nature of the Cu 3d state leads to the low charge carrier mobility and the localization of the photo-excited electrons to the CB. The combined experimental and theoretical results also indicate that CuWO4 is better described as having a direct but d–d forbidden optical bandgap, leading to a low absorption coefficient for visible light. Furthermore, the implication of the electronic structure on its PEC characteristics and strategies for further improvements by adding Co3O4 as a co-catalyst or surface layer to increase the interfacial band bending to facilitate photo-carriers transport, are discussed. [ABSTRACT FROM AUTHOR]

A highly efficient photoelectrochemical (PEC) strategy was proposed for the determination of ascorbic acid (AA). Cerium-doped tungsten trioxide (Ce-WO 3 ) microrods were synthesized by a hydrothermal method and further characterized through transmission electron microscopy (TEM), X-ray diffraction (XRD), and Raman spectroscopy. Thereafter, they were deposited onto a cleaned fluorine-doped tin oxide (FTO) glass forming the working electrode as the photoactive material. Under strong visible light irradiation, the resulting PEC sensing platform generated the corresponding electron-hole pairs, converting light signals into electrical signals. Ascorbic acid served as a good electron donor to trap holes for improvement of photocurrent responses on Ce-WO 3 /FTO. Besides, the strength of photocurrent signals versus the logarithm of ascorbic acid concentration showed a good linearity over the ascorbic acid concentration range of 100-4000 nM and the limit of detection (LOD) was estimated to be 28.6 nM. Importantly, this PEC sensor had a fast response, high sensitivity, and distinguished selectivity for detecting ascorbic acid. In addition, it also had the features of being simple to fabricate, low production cost, and portable, which made it a promising means of ascorbic acid determination.

Density functional theory (DFT) calculations at the TPSSh-D3(BJ)/def2-TZVP (SMD, water) level of theory were performed to understand the mechanism of redox-neutral depolymerization of four types of lignin-derived aryl ether dimers catalyzed by rhodium-terpyridine ([Rh]) and a binuclear Rh complex ([2Rh]). The cleavage of the C β -O bond in the β-O-4 model compound was initiated by the dehydrogenation of the alcohol moiety into a ketone intermediate, followed by the reductive cleavage of the ether bond, producing phenol and aromatic ketone products. The [Rh]-OH intermediate, generated by the interaction between the Rh-complex and NaOH, facilitated the transformation of the alcohol group to a CO group in the lignin model compound and subsequent H-transfer, selectively forming rhodium-H active species and the ketone intermediate. The [2Rh]-H complex exhibited high reactivity, with energy barriers for a rate-determining C β -O bond breakage of 35.3 kcal mol -1 . In contrast to 1-phenylethan-1-ol and H 2 , lignin itself acted as a good hydrogen source to generate [Rh]-H species. The transformation of β-O-4 model compounds with the γ-OH group occurred via the elimination of the γ-OH group, reduction of the CC bond, and C β -O bond cleavage steps. However, since lignin itself was unable to supply enough hydrogen to form [Rh]-H species, the aromatic products were obtained in low yields, as observed in the experiment.

Background : Many studies have reported the effects of spicy food on human health, but no studies have been conducted on the impact of long-term spicy food consumption on bone mineral density (BMD). This study aimed to investigate the impact of daily consumption of spicy food on BMD in the population aged 50 years and older. Methods : This cross-sectional study was conducted from 2020 to 2022 in Jiangxi Province, China. This study investigated the differences in BMD between non-consumers and daily spicy food consumers in adults aged 50-85 years. A multiple linear regression model was used to investigate the association between spicy food consumption and BMD of the total lumbar spine (LS), femoral neck (FN), and total hip, as well as biochemical markers of bone metabolism (BMBM) levels. Results : The results showed that daily consumption of spicy food was negatively associated with total LS BMD ( β = -0.013, P = 0.015). Subgroup analyses showed this negative association was more pronounced among smokers and drinkers compared to non-smokers ( β : -0.006 vs. -0.042; P for interaction <0.05) and non-drinkers ( β : -0.004 vs. -0.037; P for interaction <0.05). In addition, according to the daily frequency of spicy food consumption, the daily spicy food consumers were categorized into one meal per day, two meals per day, and three meals per day groups. Further analysis revealed that the negative association between spicy food and total LS BMD was progressively stronger as the frequency of daily consumption of spicy food increased ( P for trend <0.05). For BMBM, daily consumption of spicy food was positively associated with serum PINP levels and negatively associated with serum Ca and serum Mg levels. Conclusions : Our study suggested that daily consumption of spicy food was associated with lower LS BMD in middle-aged and older Chinese adults, and this association was more pronounced in the smoking and drinking populations. The adverse effects of spicy food on LS BMD become progressively stronger with increasing frequency of daily consumption of spicy food. In addition, daily consumption of spicy food was associated with higher PINP levels and lower serum Ca and Mg levels.

Optimizing the antibacterial effectiveness of copper ions while reducing environmental and cellular toxicity is essential for public health. A copper chelate, named PAI-Cu, is skillfully created using a specially designed carboxyl copolymer (a combination of acrylic and itaconic acids) with copper ions. PAI-Cu demonstrates a broad-spectrum antibacterial capability both in vitro and in vivo , without causing obvious cytotoxic effects. When compared to free copper ions, PAI-Cu displays markedly enhanced antibacterial potency, being about 35 times more effective against Escherichia coli and 16 times more effective against Staphylococcus aureus . Moreover, Gaussian and ab initio molecular dynamics (AIMD) analyses reveal that Cu+ ions can remain stable in the carboxyl compound's aqueous environment. Thus, the superior antibacterial performance of PAI-Cu largely stems from its modulation of copper ions between mono- and divalent states within the Cu-carboxyl chelates, especially via the carboxyl ligand. This modulation leads to the generation of reactive oxygen species (˙OH), which is pivotal in bacterial eradication. This research offers a cost-effective strategy for amplifying the antibacterial properties of Cu ions, paving new paths for utilizing copper ions in advanced antibacterial applications.

A short and chemoenzymatic synthesis of rotigotine using an IR-36-M5 mutant is reported. Focusing on the residues that directly contact the 2-tetralone moiety, we applied structure-guided semi-rational design to obtain a double-mutant F260W/M147Y, which showed a good isolated yield and S -stereoselectivity >99% toward 2-aminotetralin synthesis. Furthermore, the utility of this biocatalytic protocol was successfully demonstrated in the enantioselective synthesis of rotigotine via enzymatic reductive amination as the key step.

An effective [3 + 2] cycloaddition reaction of difluoromethyl or trifluoromethyl hydrazonoyl bromides with alkylidene pyrazolones was disclosed. This method provides an efficient approach for accessing a variety of highly functionalized fluoroalkyl spiropyrazolones in good yields. This protocol also features some advantages such as easily available and stable substrates, simple operation procedures, and atom and step economy. The formation of ( cis )- and ( trans )-products was discussed.

The metal Al is commonly attached to external circuits as the source and drain in GaN-based field effect transistors, so profound comprehension of the energy transfer between electrons and phonons in Al/GaN is crucial for nanofabrication and thermal management of electronic devices. Time-domain thermoreflectance (TDTR) is an effective technique for measuring the strength of non-equilibrium electron-phonon (e-ph) coupling. The two-temperature model (TTM) is widely employed in conjunction with TDTR methods to determine e-ph coupling factors. However, TTM is a gray method and cannot take into account interactions between electrons and different phonon modes. Therefore, in this work, we use the TDTR technique to analyze the non-equilibrium transport properties of pure Al and the thickness dependence of the e-ph coupling with Al nanofilms, and the coupling strengths of high-energy electrons excited by femtosecond lasers with different modes of phonons are obtained in conjunction with MTM. The results show that the e-ph coupling coefficients of Al nanofilms on GaN substrates are larger than those of pure Al. In conjunction with the TTM, we determined the coupling strength between high-energy electrons excited by femtosecond laser pulses and various phonon modes. Compared to the transverse acoustic branch-1 (TA1) and transverse acoustic branch-2 (TA2) modes, the longitudinal acoustic (LA) phonon mode of Al exhibits a higher e-ph coupling factor. This suggests that the LA mode predominates in the electron relaxation process after ultrafast femtosecond laser excitation. This study provides experimental and theoretical guidance for laser processing and electronic device design.

A photocurrent-polarity-switching photoelectrochemical (PEC) biosensor was developed for the ultrasensitive detection of tobramycin (TOB) through bipedal DNA walker amplification with hemin-induced photocurrent-polarity-switching using a laser-induced zinc oxide/graphene (ZnO/LIG) photoelectrode. Specifically, the ZnO/LIG photoelectrode was synthesized in situ by a laser direct writing (LDW) technique. In the presence of TOB, it reacted with HP1 and HP2 and the DNA walker response was activated to form a stable hemin/G-quadruplex. Furthermore, hemin induced a polarity shift in the photocurrent signal. The developed analytical platform exhibited excellent photoelectron transport performance of ZnO/LIG, the signal amplification effect of the DNA walker strategy, and the photocurrent-polarity-switching ability of hemin. Therefore, it demonstrated satisfying photocurrent responses to the target TOB within the working range of 20 nM-1.0 μM at a low detection limit of 5.43 nM. The PEC platform exhibited good stability, reproducibility, sufficient sensitivity and high selectivity for complex experimental samples. Moreover, the photocurrent-polarity-switching PEC biosensor improved the anti-interference ability and avoided false positives or negatives.

Photo(electro)catalytic chlorine oxidation has emerged as a useful method for chemical transformation and environmental remediation. However, the reaction selectivity usually remains low due to the high activity and non-selectivity characteristics of free chlorine radicals. In this study, we report a photoelectrochemical (PEC) strategy for achieving controlled non-radical chlorine activation on hematite (α-Fe 2 O 3 ) photoanodes. High selectivity (up to 99%) and faradaic efficiency (up to 90%) are achieved for the chlorination of a wide range of aromatic compounds and alkenes by using NaCl as the chlorine source, which is distinct from conventional TiO 2 photoanodes. A comprehensive PEC study verifies a non-radical "Cl + " formation pathway, which is facilitated by the accumulation of surface-trapped holes on α-Fe 2 O 3 surfaces. The new understanding of the non-radical Cl - activation by semiconductor photoelectrochemistry is expected to provide guidance for conducting selective chlorine atom transfer reactions., Competing Interests: There are no conflicts to declare., (This journal is © The Royal Society of Chemistry.)

The merging of traditional microwave absorbing materials with metamaterials holds significant potential for enhancing microwave absorber performance. To unlock this potential, a unified paradigm is urgently required. We have successfully established such a paradigm, focusing on regulating effective electromagnetic parameters and interfacial forms across microscopic, mesoscopic, and macroscopic scales. Building upon this foundation, we introduce an active co-design methodology for jointly optimizing full-scale structures and the concept of "full-scale microwave absorbers" (FSMAs). Under this guidance, performance improvements can be achieved efficiently, leading to crucial breakthroughs. For demonstration, we present a case study designing ultra-thin miniaturized FSMAs capable of ultra-broadband and low-frequency absorption. Simulation results show absorptivity exceeding 90% in the 2-28 GHz range, with absorptivity surpassing 85% and 74% in the 1.5-2 GHz and 1-1.5 GHz ranges, respectively. Additionally, the total thickness and macro period are only 5 mm, roughly equivalent to 0.033 wavelengths of the lowest operating frequency. Most importantly, we have broken the Rozanov limit, with experimental results further validating this design. This work significantly enhances our understanding of microwave absorption and offers a shortcut for pursuing improved performances and breakthroughs.

Pressure is a powerful way to modulate physical properties. Understanding the effect of pressure on the thermal transport properties of thermoelectric materials is of great importance for the efficient design and optimization of thermoelectric performance. In this work, based on first-principles calculations and phonon Boltzmann transport theory, we find that the lattice thermal conductivities of Ag-based chalcopyrites AgXY 2 (X = Al, Ga, and In; Y = S, Se, and Te) are dramatically suppressed by applying pressure. The inherent distorted tetrahedral configuration together with highly delocalized p-orbital electrons promotes the formation of metavalent bonding. The fact of metavalent bonding with a single bonding electron and small electron transfer between neighboring atoms leads to soft low-frequency optical phonons. With the increase of pressure, the softening of acoustic and low-frequency optical phonons induces enhanced anharmonicity and scattering channels. Such strong acoustic-optical phonon coupling results in larger phonon scattering rates and thus lowers the lattice thermal conductivity. These findings not only help unveil the underlying physical mechanisms for the anomalous thermal transport behaviors under high pressure, but also pave the way for the pressure tuning of high-performance Ag-based thermoelectric materials.

Digital microfluidics (DMF) is an innovative technology used for precise manipulation of liquid droplets. This technology has garnered significant attention in both industrial applications and scientific research due to its unique advantages. Among the key components of DMF, the driving electrode plays a role in facilitating droplet generation, transportation, splitting, merging, and mixing. This comprehensive review aims to present an in-depth understanding of the working principle of DMF particularly focusing on the Electrowetting On Dielectric (EWOD) method. Furthermore, it examines the impact of driving electrodes with varying geometries on droplet manipulation. By analyzing and comparing their characteristics, this review offers valuable insights and a fresh perspective on the design and application of driving electrodes in DMF based on the EWOD approach. Lastly, an assessment of the development trend and potential applications of DMF concludes the review, providing an outlook for future prospects in the field., Competing Interests: There are no conflicts to declare., (This journal is © The Royal Society of Chemistry.)

Owing to nano-MoS 2 's excellent anti-friction and anti-wear properties, nano-MoS 2 , which can act as a nano-additive in lubricating oil or solid lubricants, is believed to have great potential in the lubrication of power machinery and moving parts of a spacecraft. The molecular dynamics method was used to construct a rough surface and a multi-level asperity structure to simulate starved lubrication before oil film breakdown, and the lubrication mechanism of MoS 2 as a nano-additive or directly coated on the textured surface could reduce the friction coefficient and wear was explained from the atomic perspective. Simulations showed that the multilayer MoS 2 played a role of load-bearing at light load or low velocity, and slipped into the grooves to repair the surface under heavy load or high velocity. Even if local asperity contact occurs, MoS 2 nanoparticles could accelerate the detachment of the initial asperity contact to prevent large-scale adhesion. The MoS 2 nanoparticles transformed the pure liquid oil film into a liquid-solid composite oil film, which was more suitable for lubrication under heavy load and high velocity because it increased the contact area, protected the friction surface and prevented asperity contact. The proposed lubrication mechanism contributes to understanding the frictional properties of layered nanomaterials under extreme conditions and provides a reference for further application of MoS 2 materials in the field of lubrication.

As a newly emerging class of molecular crystal materials, metal-organic frameworks (MOFs) are extensively used in a variety of fields including catalysis, separation, energy storage, and biosensors, by virtue of their large specific surface area, excellent chemical stability, and adjustable pore size. In particular, several functional materials have been integrated into the MOF structure, which greatly improves the conductivity of MOFs and facilitates the application of MOFs in the field of electrochemical biosensing. Herein, this review highlights the recent applications of MOF composites for photoelectrochemical (PEC) and electrochemiluminescence (ECL) biosensors. This paper first briefly describes the classification and various synthesis methods of MOFs. Then, it comprehensively summarizes different types of MOF-based biosensors in PEC and ECL and their applications. Finally, the challenges and outlook for future work in MOF-based PEC and ECL biosensors are tentatively proposed.

With excellent physical and chemical properties, 2D TMDC materials have been widely used in engineering applications, but they inevitably suffer from the dual effects of strain and device size. As typical 2D TMDCs, HfSe 2 and ZrS 2 are reported to have excellent thermoelectric properties. Thermal transport properties have great significance for exerting the performance of materials, ensuring device lifetime and stable operation, but current research is not detailed enough. Here, first-principles combined with the phonon Boltzmann transport equation are used to study the phonon transport inside monolayer HfSe 2 and ZrS 2 under tensile strain and finite size, and explore the band structure properties. Our research shows that they have similar phonon dispersion curve structures, and the band gap of HfSe 2 increases monotonically with the increase of tensile strain, while the bandgap of ZrS 2 increases and then decreases with the increase of tensile strain. Thermal conductivity has obvious strain dependence: with the increase of tensile strain, the thermal conductivity of HfSe 2 gradually decreases, while that of ZrS 2 increases slightly, and then gradually decreases. Reducing the system size can limit the contribution of phonons with a long mean free path, significantly decreasing thermal conductivity through the controlling effect of tensile strain. The mode contribution of thermal conductivity is systematically investigated, and anharmonic properties including mode and frequency-level scattering rates, group velocity and Grüneisen parameters are used to explain the associated mechanism. Phonon scattering processes and channels in various cases are discussed in detail. Our research provides a detailed understanding of the phonon transport and electronic structural properties of low thermal conductivity monolayers of HfSe 2 and ZrS 2 , and further completes the study of thermal transport of the two materials under strain and size tuning, which will provide a foundation for further popularization and application.

An eco-friendly and efficient electrochemical method for the synthesis of 5-amine-1,2,4-triazole derivatives has been developed by employing hydrazones or in situ generation of hydrazones with cyanamide using KI as the catalyst and electrolyte. This strategy could be smoothly conducted with simple reaction conditions at room temperature without the addition of a chemical oxidant in an undivided cell, and cyanamide has been proven to be of great value in electrosynthesis.

Palbociclib is the world's first CDK4/6 kinase inhibitor to be marketed. However, it is not effective in the treatment of triple negative breast cancer (TNBC) due to the loss of retinoblastoma protein expression. Thus, combinatorial chemotherapy is indispensable for TNBC treatment. Herein, a carrier-free nanomedicine self-assembled from palbociclib dimers and Ce6 for enhanced combined chemo-photodynamic therapy of breast cancer is reported. The dimeric prodrug (Palb-TK-Palb) was synthesized by conjugating two palbociclib molecules to the connecting skeleton containing a ROS-responsive cleavable thioketal bond. The Palb-TK-Palb/Ce6 NP co-delivery nanoplatform was prepared through the self-assembly of Palb-TK-Palb, Ce6 and DSPE-PEG2000. This novel carrier-free formulation as an efficient therapeutic agent showed efficient therapeutic agent loading capacity, high cellular uptake and huge therapeutic performance against breast cancer cells. The results of in vitro antitumor activity and cell apoptosis demonstrated that Palb-TK-Palb/Ce6 NPs presented a better inhibitory effect on the growth of cancer cells due to the palbociclib and Ce6 co-delivery nanomedicine-mediated synergistic chemo-photodynamic therapy. The IC 50 values of Palb-TK-Palb/Ce6 NPs in MDA-MB-231 cells were around 1-2 μM and 2 μM and the Palb-TK-Palb/Ce6 NPs showed an increase in apoptosis up to 91.9%. In general, the carrier-free nanomedicine self-assembled from palbociclib dimers and Ce6 provides options for combinatorial chemo-photodynamic therapy., Competing Interests: There are no conflicts to declare., (This journal is © The Royal Society of Chemistry.)

Herein, we reported a novel photoelectrochemical immunoassay method based on a target-triggered on/off signal of the ultra-structured Bi 2 O 2 S (BOS) photoanode system for the sensitive testing of carcinoembryonic antigens (CEAs) in serum samples. Well-defined three-dimensional sheet-like self-assembled flower-like Bi 2 O 2 S superstructures were obtained using a time-controlled hydrothermal method. Such well-shaped multifaceted surfaces were considered to be good laser cavity mirror surfaces for multifaceted reflection and refraction of excitation light in the material. An elegant enzyme biocatalytic strategy was introduced into the constructed detection model to sensitively detect CEAs. The substrate 4-chloro-1-naphthol (4-CN) was oxidized to 4-chloro-hexadienone (4-CD) under the formation of target-triggered immune complexes against mAb 1 and peroxidase-modified mAb 2 . Subsequently, 4-CD produced by the biocatalytic precipitation reaction was transferred to the photoanodes of Bi 2 O 2 S nanoflowers (BOS NFs) to burst their photoelectric signals, thus achieving the quantification of CEAs. Through optimization of the conditions of the immunization protocol, a good negative photocurrent response to the target CEA was found in the wide range of 0.02-50 ng mL -1 with a detection limit of 11.2 pg mL -1 . Impressively, the reported biocatalytic PEC sensing strategy on superstructures is comparable, or superior, to the gold standard ELISA kit in terms of sensitivity and the target response range. This study presents a target-mediated PEC immunoassay for biocatalytic precipitation based on a self-assembled superstructure of Bi 2 O 2 S, providing a fresh scheme for the analysis of disease-related markers.

Lanthanide-doped inorganic nanocrystals have attracted extensive attention due to their long luminescence lifetime and large Stokes shift. In this work, an immunosensing platform based on CePO 4 :Tb (CPOT) was successfully constructed, which could avoid the autofluorescence interference of complex biological matrices. Specifically, CPOT was synthesized by a solvothermal method, which exhibited H 2 O 2 -responsive luminescence behavior. Taking advantage of this feature, an autofluorescence-free immunosensor with CPOT as the probe and H 2 O 2 as the quencher was developed to detect prostate-specific antigen (PSA). Functionalized liposomes were used to encapsulate glucose oxidase (GOD) and labeled on detection antibodies to improve the sensitivity of the probe. Under the proven optimal experimental conditions, the developed autofluorescence-free immunosensor exhibited a linear luminescence response to the logarithm of PSA concentration (0.005-25 ng mL -1 ) with a limit of detection (LOD) of 3.25 pg mL -1 . The performance shows that the autofluorescence-free immunosensor based on this strategy opens up a new field of vision for clinical PSA detection.

Zintl phase Mg 3 Sb 2 , which has ultra-low thermal conductivity, is a promising anisotropic thermoelectric material. It is worth noting that the prediction and experiment value of lattice thermal conductivity ( κ ) maintain a remarkable difference, troubling the development and application. Thus, we firstly included the four-phonon scattering processes effect and performed the Peierls-Boltzmann transport equation (PBTE) combined with the first-principles lattice dynamics to study the lattice thermal transport in Mg 3 Sb 2 . The results showed that our theoretically predicted κ is consistent with the experimentally measured, breaking through the limitations of the traditional calculation methods. The prominent four-phonon scatterings decreased phonon lifetime, leading to the κ of Mg 3 Sb 2 at 300 K from 2.45 (2.58) W m -1 K -1 to 1.94 (2.19) W m -1 K -1 along the in (cross)-plane directions, respectively, and calculation accuracy increased by 20%. This study successfully explains the lattice thermal transport behind mechanism in Mg 3 Sb 2 and implies guidance to advance the prediction accuracy of thermoelectric materials.

Empagliflozin (Empa, SGLT2 inhibitor) is widely used in clinical situations for the management of diabetes. It has beneficial effects in reducing cardiac dysfunction and heart failure. However, rare studies have reported the potential mechanisms of Empa reaction. Here, we treated db / db diabetic mice with Empa and collected the heart tissue for metabolomics study. We found that db / db mice showed obvious differences in metabolomics profile compared with db / m mice. Many amino acid metabolism pathways and glycerophospholipids and fatty acyl carnitines were significantly enriched in db / db mice. Detailed analysis revealed the alteration of fatty acid oxidation in db / db mice. Interestingly, many metabolites in the fatty acid oxidation pathway, such as myristoleic acid, 12-hydroxydodecanoic acid, (15-carboxypentadecanoyl)carnitine, decanoylcarnitine, and propionylcarnitine, were significantly rescued by Empa treatment. These results suggest that fatty acid oxidation is one of the targets for Empa treatment in the heart of db / db mice. This study provided new possibilities for the development of therapeutic interventions for diabetic cardiomyopathy.

This work reports on the proof-of-concept of a photoelectrochemical (PEC) biosensor with a horseradish peroxidase-single stranded DNA-encoded magnetic bead (MB-ssDNA-HRP) signal probe cleaved by the catalytic hairpin assembly (CHA)-mediated clustered regularly interspaced short palindromic repeats (CRISPR)-Cas12a system for the quantification of microRNA (miR-21) by using yolk-in-shell Au@CdS as a photoactive material.

Molecular tags such as fluorophores are increasingly being replaced with nanoparticles thanks to their superior optical properties, substantial chemical stability, and stability against photobleaching. Herein, we innovatively constructed a new ratiometric fluorescence enzyme-linked immunosorbent assay (RF-ELISA) for the screening of alpha-fetoprotein (AFP) in early hepatocellular carcinoma in vitro diagnostics using carbon dots@SiO 2 @CdTe quantum dots (CDs@SiO 2 @CdTe QDs). Carbon dots with blue fluorescence were initially encapsulated into SiO 2 nanospheres through the typical Stöber method. Thereafter, CdTe QDs with red fluorescence were modified onto the surface of CDs@SiO 2 nanospheres. Dual-emission nanotags with blue and red fluorescent signals were utilized to design a RF-ELISA method for the determination of AFP on the anti-AFP capture antibody-coated microplate using glucose oxidase (GOx)-labeled anti-AFP secondary antibody. After the formation of the sandwiched immunocomplex, GOx catalyzed glucose to generate hydrogen peroxide (H 2 O 2 ), which could quench the red fluorescence of CdTe QDs on the surface of nanotags. Meanwhile, the encapsulated carbon dots in the nanotags could still maintain the initial blue fluorescence intensity. The ratio between red fluorescence intensity and blue-emission intensity could be used for the quantitative monitoring of AFP concentration under optimum conditions. The experimental results indicated that CDs@SiO 2 @CdTe QDs-based RF-ELISA could exhibit a good fluorescence signal with a dynamic linear range of 0.05-60 ng mL -1 at a low detection limit of 8.7 pg mL -1 . Moreover, the fluorescence color of the solution including CDs@SiO 2 @CdTe QDs changed from pink to purple to blue with the increasing AFP level when viewed by the naked eye. Good reproducibility, high specificity, and acceptable stability were achieved for the analysis of target AFP. Importantly, the accuracy of ratiometric fluorescence immunoassay was evaluated to determine human serum samples, giving well-matched results relative to commercially usable human AFP ELISA method.

Sweet tea ( Lithocarpus polystachyus Rehd.), a natural functional food highly rich in dihydrochalcones including trilobatin, phlorizin and phloretin, is reported to possess numerous biological activities especially for treating diabetes. Here, the aim of this systematical review and meta-analysis is to assess the effect of dihydrochalcones in sweet tea (DST) on diabetes and summarize their possible mechanisms. We searched in eight databases including Embase, PubMed, Cochrane, Web of Science, WanFang database, VIP database, China National Knowledge Infrastructure and China Biology Medicine from Jan 2000 to Nov 2021 and ultimately included 21 animal studies in this review. A total of 10 outcome measurements including blood lipid indexes, blood glucose, insulin resistance indicators and oxidative stress biomarkers were extracted for meta-analysis using RevMan 5.4 software. DST significantly decreased the levels of triglyceride (TG), total cholesterol (TC), low-density lipoprotein cholesterol (LDL-c), blood glucose (BG), homeostasis model assessment of insulin resistance (HOMA-IR) and malondialdehyde (MDA), and increased high-density lipoprotein cholesterol (HDL-c), superoxide dismutase (SOD) and glutathione peroxidase (GSH-Px) activity in diabetic animal models. In summary, DST could treat diabetes by regulation of blood glucose/lipid metabolism, oxidative/carbonyl stress, inflammatory response etc .

Nitric oxide (NO) is an exceptional endogenous biological gas that mediates and regulates physiological and pathological processes in the human body. However, its synthesis process is impaired during athero-progression and formation. Hence, a strategy to boost NO production and target endothelial nitric oxide synthase (eNOS) is crucial and intriguing in atherosclerosis (AS) management. Herein, we prepare L-arginine (LA) and lovastatin (LV) co-loaded PLGA nanomedicine to achieve sustainable release for enhancing NO production. The utilization of LA reveals that LA has dual contributions, acting as a NO donor and enhancing the solubility of LV by stabilizing PLGA NPs. PLGA-LA/LV demonstrated its potential to boost NO in vitro and in vivo confirmed using DAF-FM DA, augment eNOS and p-eNOS mRNA and protein levels, and suppress the ki67 proliferation marker in VSMCs; in addition, it lowers the total cholesterol level of blood plasma in C57BL/6 mice. Moreover, PLGA can protect the compound delivered and enhance the bioavailability to reach and get released in the blood circulation after oral administration. Collectively, our results endow a safe and efficient nanomedicine outcome, specifically with potential for AS management.

Osteoarthritis is a significant driver of disability in the elderly with increasing prevalence, and inflammation plays a vital role on its etiology. Licorice is commonly used as a traditional Chinese medicine or food additive, and its prenylated phenolic compounds were recently reported to be able to inhibit osteoarthritis with anti-inflammatory activity. In order to explore more anti-osteoarthritic prenylated phenolic compounds from licorice, we isolated ten compounds (1-10), with three new ones (1-3), from the ethyl acetate extract of Glycyrrhiza uralensis . Compound 2 (glycyuralin R) was a racemic 3-phenoxy-chromanone, and we achieved its chiral separation for the first time. Compounds 1, 2, 7 and 8 showed significant NO inhibitory ability in IL-1β-stimulated mouse primary chondrocytes, and we further confirmed the anti-inflammatory activity of 1 (glycyuralin Q) by evaluating its effect on osteoarthritis-related iNOS, COX-2, TNF-α, IL-6, MMP3, MMP13 and NF-κB based on various experimental methods. These results clarified the potential of several prenylated phenolic compounds, especially 1 in licorice, as the lead compounds for osteoarthritis.

C-reactive proteins (CRPs; an acute-phase protein) in patients with initial acute cerebral infarction neurological rehabilitation prediction have a significant correlation. In this work, a simple and sensitive anodic-stripping voltammetric (ASV) immunosensing system was innovatively designed for the quantitative screening of target CRPs using biomimetic-mineralized bifunctional antibody-Cu 3 (PO 4 ) 2 nanoflowers as molecular tags. In this system, a monoclonal anti-CRP antibody-anchored microtiter plate was utilized to specifically capture target CRPs from the sample. For detection, a sandwiched immunoreaction mode was employed with the antibody-Cu 3 (PO 4 ) 2 nanoflowers in the presence of analytes. Subsequent ASV measurement of copper ions (Cu 2+ ) released under acidic conditions from the bifunctional nanoflowers was conducted at an in situ prepared mercury film electrode. The introduction of hybrid nanoflowers greatly increased the loading amount of copper ions on the molecular tag, thereby amplifying the detectable signal of electrochemical immunoassay. Meanwhile, factors influencing the analytical properties of the electrochemical immunoassay were investigated in detail. By combining the high-efficiency nanohybrids with signal amplification, the dynamic concentration range of electrochemical immunoassay spanned from 0.01 ng mL -1 to 100 ng mL -1 toward the target CRP. The limit of detection was calculated to be 0.0079 ng mL -1 at 3 S blank criterion. Intra- and interassay imprecisions (relative standard deviations: RSDs) were less than or equal to 6.72%. Good anti-interference ability, long-term storage stability, and acceptable accuracy for the evaluation of human serum specimens were observed during a series of procedures to determine the target protein. In addition, the bifunctional nanoflower-based immunosensing system offers promise for the simple, cost-effective analysis of disease-related proteins.

Renal transplantation is the most effective treatment for end-stage renal disease, but the long-term prognosis of organs after transplantation is not ideal. In recent years, the importance of gut microbes and metabolites in the study of disease mechanisms has gradually received attention. However, the coordination between gut microbes and the metabolism of renal transplant patients needs further study. We integrated 16s sequencing and metabolomics data to describe the changes in the serum and fecal metabolites of renal transplant patients. Our data revealed that the gut microbial diversity decreased and the relative abundance of many bacteria, such as Enterococcus and Streptococcus , significantly changed after transplantation. In addition, a large number of amino acids and peptides in serum and feces significantly changed, suggesting an abnormal amino acid metabolism after transplantation. Spearman's correlation analysis revealed the changes in the co-metabolism pattern between gut microbes and the host metabolism after transplantation. Furthermore, Enterococcus was found to be correlated with renal functions and metabolites reflecting renal damage. This study provides potential gut microbes and metabolites impacting renal health, which helps in understanding the renal damage in patients with kidney transplantation.

Thermoelectric materials with excellent performance can efficiently and directly convert waste heat into electrical energy. In today's era, finding thermoelectric materials with excellent performance and adjusting the thermoelectric parameters are essential for the sustainable development of energy in the context of the energy crisis and global warming. Through first-principles calculations, we notice that two-dimensional (2D) orthogonal ScX 2 (X = C and N) compounds show great potential in the field of thermoelectricity. Different from most materials containing C or N atoms, which are generally accompanied by high lattice thermal conductivity (TC), the 2D o -ScX 2 exhibited a rather low and anisotropic lattice TC. The κ 3L (the lattice thermal conductivity including the effect of three-phonon scattering and isotope scattering) of o -ScC 2 along the X and Y directions are 2.79 W m -1 K -1 and 1.55 W m -1 K -1 , and those of o -ScN 2 are 1.57 W m -1 K -1 and 0.56 W m -1 K -1 . By calculating the fourth-order interatomic force constants (IFCs), we obtain the κ 3+4L with the additional four-phonon scattering effect. Our results clearly show that four-phonon scattering plays an important role in the TC of the two materials, the κ 3+4L of o -ScC 2 is only half of its κ 3L. Furthermore, it can be noticed that the low lattice TCs of o -ScX 2 (X = C and N) are the result of many factors, e.g. , heavy atom doping, the strong anharmonicity caused by the vibration of Sc atoms in the out-of-plane direction and C(N) atoms in the in-plane direction, important four-phonon scattering and strongly polarized covalent bonds between X atoms and Sc atoms. Moreover, it is interesting to find that the thermal transport properties of o -ScX 2 are led by a different phonon mechanism, e.g. , the different TCs of o -ScC 2 and o -ScN 2 are determined by the anharmonic characteristic, and the harmonic characteristic plays a more important role in the anisotropy of o -ScX 2 (X = C and N). In general, our research can be expected to provide important guidance for the application of o -ScX 2 (X = C and N) in the thermoelectric field.

A simple thermal aptasensing platform was devised for the sensitive detection of organophosphate pesticides (using malathion as a model target) based on the efficient self-heating reaction of a warming pad with a switchable target responsive enzyme-encapsulated three-dimensional (3D) DNA hydrogel using a portable thermometer as a signal readout in this work. The existence of the target malathion would open the catalase-3D network and lots of catalase was released from the hydrogel, which could efficiently convert H 2 O 2 to an O 2 molecule. The product O 2 is the critical condition for the self-heating of the warming pad. Thereafter, the temperature was enhanced with the increasing amount of O 2 . The strategy displays outstanding specificity, reproducibility and stability. Moreover, this method can be easily extended to monitor other molecules using different aptamer sequences in practical applications.

This work reports a photoelectrochemical (PEC) biosensing platform for the sensitive and specific screening of thrombin by using graphene oxide-coated copper-doped zinc oxide quantum dots (Cu 0.3 Zn 0.7 O-GO QDs) as the photoactive materials and glucose oxidase-encapsulated DNA nanoflowers (GOx-DFs) for signal amplification. Interestingly, the coated graphene oxide nanosheets on the surface of the Cu 0.3 Zn 0.7 O QDs could cause the charge to transfer rapidly and ameliorate the photocorrosion. The doped copper into the quantum dots could enhance the absorption of visible light by tuning the band gap of ZnO QDs, therefore increasing the photocurrent under visible irradiation. Upon addition of target thrombin, a sandwiched reaction was carried out between thrombin aptamer and GOx-DFs, accompanying the formation of nanocomposites with the magnetic microparticles (MMPs)/thrombin/GOx-DFs. Followed by magnetic separation, the carried GOx oxidized glucose to H 2 O 2 , thus resulting in the increasing photocurrent of the Cu 0.3 Zn 0.7 O-GO QD-modified electrode. Under optimum conditions, the developed PEC biosensing platform exhibited good analytical performance with a linear range of 50-10 000 fM thrombin and a limit of detection of 29 fM. Impressively, our strategy offers a new horizon in developing bridge-connected graphene-coated nanomaterials and novel signal amplification strategy for the development of PEC biosensors.

Diabetic nephropathy (DN) is a microvascular complication that is becoming a worldwide public health concern. The aim of this study was to assess the effects of dietary soy isoflavone intervention on renal function and metabolic syndrome markers in DN patients. Seven databases including Medline, the Cochrane Central Register of Controlled Trials, Science Direct, Web of Science, Embase, China National Knowledge Infrastructure, and WanFang were searched for controlled trials that assessed the effects of soy isoflavone treatment in DN patients. Finally, a total of 141 patients from 7 randomized controlled trials were included. The meta-analysis showed that dietary soy isoflavones significantly decreased 24-hour urine protein, C-reactive protein (CRP), blood urea nitrogen (BUN), total cholesterol (TC), triglycerides (TG), low-density lipoprotein cholesterol (LDL-C), and fasting blood glucose (FBG) in DN patients. The standard mean difference was -2.58 (95% CI: -3.94, -1.22; P = 0.0002) for 24-hour urine protein, -0.67 (95% CI: -0.94, -0.41; P < 0.00001) for BUN, -6.16 (95% CI: -9.02, -3.31; P < 0.0001) for CRP, -0.58 (95% CI: -0.83, -0.33; P < 0.00001) for TC, -0.41 (95% CI: -0.66, -0.16; P < 0.00001) for TG, -0.68 (95% CI: -0.94, -0.42; P < 0.00001) for LDL-C, and -0.39 (95% CI: -0.68, -0.10; P = 0.008) for FBG. Therefore, soy isoflavones may ameliorate DN by significantly decreasing 24-hour urine protein, BUN, CRP, TC, TG, LDL-C, and FBG.

This study reports a photoelectrochemical biosensor for dopamine-loaded liposome-encoded magnetic beads cleaved by clustered regularly interspaced short palindromic repeats (CRISPR)/Cas 12a system for the quantification of human papilloma virus (HPV)-related DNA using neodymium-doped BiOBr nanosheets (Nd-BiOBr) as a photoactive matrix. Magnetic beads and dopamine-loaded liposomes are covalently attached to the both ends of ssDNA to construct dumbbell-shaped dopamine-loaded liposome-encoded magnetic bead (DLL-MB) probes. When the guide RNA binds to the target HPV-16, the ssDNA will be cleaved by Cas12a, thereby degrading the double dumbbell probes. After magnetic separation, the dissolved DLLs are treated with Triton X-100 to release the dopamine (as an electron donor), which was then detected by an amplified photocurrent using the Nd-BiOBr-based photoelectrode.

Prostate-specific antigen (PSA), a glycoprotein that is most likely to cause prostate cancer, has attracted widespread attention in recent years due to its increasing threat to people's lives and health. Herein, we developed a new signal-amplified photoelectrochemical (PEC) immunosensing method for quantitative monitoring of the target PSA based on the ion-exchange reaction for the in situ formation of ZnO/CdS/Ag 2 S nanohybrids triggered by the as-released silver ions (Ag + ) from silver nanolabels. Initially, the introduction of a target PSA caused the formation of a sandwich immunocomplex in an anti-PSA capture antibody (cAb)-coated microplate with the help of a silver nanoparticle-labeled detection antibody (AgNPs-dAb). Thereafter, the introduced AgNPs were dissolved with acid to release numerous silver ions. In this regard, an ion-exchange reaction occurred between the silver ions and ZnO/CdS nanorods on the photosensitive electrode, thus producing ZnO/CdS/Ag 2 S nanohybrids to generate a relatively strong photocurrent. Under optimal conditions, the ion-exchange reaction-based PEC immunoassay exhibited a good linear range of 0.05-50 ng mL -1 and allowed the detection of the target PSA at a concentration as low as 0.018 ng mL -1 . In addition, the PEC immunoassay displayed satisfactory repeatability, high specificity, and acceptable method accuracy. Importantly, the ion-exchange reaction-based PEC immunoassay provides a new perspective for the detection of other disease-related biomarkers by controlling the corresponding antibodies.

The quantitative prediction of nonadiabatic transitions between different electronic states is important to understand ultrafast processes in photochemistry. A variety of mixed quantum-classical molecular dynamics methods such as surface hopping and Ehrenfest mean-field have been developed. However, how to choose an appropriate one from a wide diversity of dynamics algorithms to study a realistic photochemical process is still unclear. In this work, we implemented 30 combinations of different mixed quantum-classical dynamics methods, including 24 surface hopping models with 8 decoherence corrections and 3 momentum rescaling strategies as well as 6 mean-field models. Then we performed numerical investigations by simulating the photoisomerization of cis-azobenzene combined with on-the-fly electronic structure calculations. Predictions of the S1 lifetime and the quantum yield of the photoproduct using different models are distinct. Surface hopping is more robust than mean-field in our test system. Moreover, the choice of momentum rescaling methods in surface hopping brings more significant changes than decoherence corrections, while a large discrepancy between simulation results with different mean-field algorithms has been observed.

With the ability to alter the inherent interatomic electrostatic interactions, modulating external electric field strength is a promising approach to tune the phonon transport behavior and enhance the thermoelectric performance of two-dimensional (2D) materials. Here, by applying an electric field (Ez = 0.1 V Å-1), it is predicted that an ultralow value of the lattice thermal conductivity (0.016 W m-1 K-1) at 300 K of 2D indium selenide (InSe) is nearly three orders of magnitude lower than that under an electric field of 0 V Å-1 (27.49 W m-1 K-1). Meanwhile, we calculated the variations in the electrical conductivities, electronic thermal conductivities, Seebeck coefficients, and figure of merit (ZT) of 2D InSe along with the carrier (hole and electron doping) concentrations under some representative electric fields. Owing to the smaller total thermal conductivity along the armchair and zigzag directions, p-type doped 2D InSe at Ez = 0.1 V Å-1 exhibits a larger ZT value (∼1.6) compared to the ZT value (∼0.1) without an electric field at room temperature. The peak ZT value (∼0.53) of the n-type 2D InSe at Ez = 0.1 V Å-1 is much higher than that without an electric field (∼0.02) at the same temperature. Our results pave the way for applying an external electric field to modulate the phonon transport properties and greatly promote the thermoelectric performance of some specific 2D semiconductor materials without altering their crystal structure.

Flexible electric-double-layer (EDL) thin film transistors (TFTs) based on a vertical InGaZnO 4 (IGZO) channel are fabricated at room temperature. Such TFTs show a low operation voltage of 1.0 V due to the large specific gate capacitance of 3.8 μF cm -2 related to electric-double-layer formation. The threshold voltage, drain current on/off ratio and subthreshold swing are estimated to be -0.1 V, 1.2 × 10 6 and 80 mV per decade, respectively. The combination of low voltage, high current on-to-off ratio and room temperature processing make the flexible vertical-IGZO-channel TFTs very promising for low-power portable flexible electronics applications., Competing Interests: There are no conflicts to declare., (This journal is © The Royal Society of Chemistry.)

In the present work, the quantum trajectory mean-field approach, which is able to overcome the overcoherence problem, was generalized to simulate internal conversion and intersystem crossing processes simultaneously. The photoinduced ring-opening and subsequent rearrangement reactions of isolated 2(5H)-thiophenone were studied based on geometry optimizations on critical structures and nonadiabatic dynamics simulations using this method. Upon 267 nm irradiation, the molecule is initially populated in the 1ππ* state. After a sudden rupture of one C-S bond within 100 fs in this state, the lowest two singlet excited states and the lowest two triplet excited states become quasi-degenerated, and then the intersystem crossing processes between singlet and triplet states accompanied by rearrangement reactions can be observed several times. Compared with our previous nonadiabatic simulations in the absence of intersystem crossing (ChemPhotoChem, 2019, 3, 897-906), some new nonadiabatic relaxation pathways involving triplet states and different ring-opening products were identified. The present work provides new mechanistic insights into the photoinduced ring-opening of thio-substituted heterocyclic molecules and reveals the importance of nonadiabatic dynamics simulation that is able to deal with multiple electronic states with different spin multiplicities.

Herein a rapid and sensitive fluorometric bioanalysis platform for mercury(ii) (Hg2+) detection was innovatively developed using ultrathin two-dimensional MXenes (Ti3C2) as fluorescence quencher and Hg2+-induced exonuclease III (Exo III)-assisted target recycling strategy for efficient signal amplification. Initially, fluorophore-labeled single-stranded DNA (FAM-labeled probe) can be easily adsorbed onto the surface of ultrathin Ti3C2 nanosheets by hydrogen bonding and metal chelating interaction, and the fluorescence signal emitted by the FAM-labeled probe is quenched strongly owing to the fluorescence resonance energy transfer between the FAM and ultrathin Ti3C2 nanosheets. Upon sensing the target Hg2+, the protruding DNA fragment at the 3' end of hairpin will hybridize with primer (hairpin-Hg2+-primer), and then further digested by Exo III to produce a probe (nicker). The released target Hg2+ and primer continue to participate in the next recycling, resulting in more hairpin probes becoming nickers. The combination of a large number of nickers and FAM-probe resulted in a significant increase in the fluorescence signal of the system, which was attributed to the fact that the double helix DNA was more rigid and separated from the surface of the ultrathin Ti3C2 nanosheets. The obvious fluorescence signal change of the Ti3C2-based Exo III-assisted target recycling can be accurately monitored by fluorescence spectrometry, which is also proportional to the concentration of Hg2+. Under optimum operating conditions, the peak intensity (520 nm wavelength) of fluorescence increased with increasing Hg2+ within a wide dynamic working range from 0.05 nM to 50 nM (R2 = 0.9913) with a limit of detection down to 42.5 pM. The proposed strategy uses ultrathin MXenes as a platform for binding nucleic acids, which contributes to its potential in nucleic acid hybridization-based biosensing and/or nucleic acid signal amplification bio-applications.

Colorectal cancer (CRC) is the third most common cancer around the world. Recent findings suggest that cancer stem cells (CSCs) play a pivotal role in the resistance to current therapeutic modalities, including surgery and chemotherapy. Photodynamic therapy (PDT) is a promising non-invasive therapeutic strategy for advanced metastatic CRC. Traditional photosensitizers such as pyropheophorbide-a (Pyro) lack tumor selectivity, causing unwanted treatment-related toxicity to the surrounding normal tissue. In order to enhance the targeting properties of Pyro, we synthesize a novel photosensitizer, CD133-Pyro, via the conjugation of Pyro to a peptide domain targeting CD133, which is highly expressed on CRC CSCs and correlated with poor prognosis of CRC patients. We demonstrate that CD133-Pyro possesses the targeted delivery capacity both in CRC CSCs derived from HT29 and SW620 cell lines and in a xenograft mouse model of tumor growth. CD133-Pyro PDT can promote the production of reactive oxygen species (ROS), suppress the stemness properties, and induce autophagic cell death in CRC CSCs. Furthermore, CD133-Pyro PDT has a potent inhibitory effect on CRC CSC-derived xenograft tumors in nude mice. These findings may offer a useful and important strategy for the treatment of CRC through targeting CSCs.

Through the first-principles density functional theory and the phonon Boltzmann transport equation, we investigated the phonon transport characteristics inside 1T-TiSe2. The calculation results of the lattice thermal conductivity (κl) show that the κl of TiSe2 is extremely low (1.28 W (m K)-1, 300 K) and decreases with the shrinkage of the sample size. Moreover, the results also prove the isotropic nature of thermal transport. By decomposing the contribution of the thermal conductivity according to the frequency, the κl of the single-layer TiSe2 is primarily attributed to the acoustic phonons and a small portion of optical phonons, with the frequency range of 0-4.5 THz. The calculation of the scattering rate further illustrates the competition of different scattering modes in this frequency range to verify the change in thermal conductivity of different sample sizes. The high scattering rate and low group velocity lead to the low thermal conductivity of the optical phonon mode in TiSe2. In addition, reducing the size of the system can significantly limit the thermal conductivity by eliminating the contribution of long mean free path phonons. When the characteristic length of the single-layer TiSe2 is about 14.92 nm, κl reduces to half. Our results also show that TiSe2 has an extremely high Grüneisen parameter (about 2.62). Further decomposition of the three-phonon scattering phase space and scattering rate demonstrates that in the range 0-4.5 THz, the absorption process is the main conversion form of phonons. We conclude that, due to the high Grüneisen parameter, the high anharmonicity in TiSe2 leads to the extremely low κl. This study provides κl related to the temperature, frequency, and MFP, and deeply discusses the phonon transport in TiSe2, which has great significance to further adjust the thermal conductivity to develop highly efficient thermoelectric materials and promote the application of devices based on TiSe2.

Green tea polyphenol epigallocatechin-3-gallate (EGCG) may help prevent metabolic syndrome and nonalcoholic fatty liver disease (NAFLD). However, the underlying mechanisms of its protective effects are complicated and remain unclear. With the gut-liver axis theory as a foundation, the present study investigated the effects of EGCG on intestinal mucosal immunity in male C57BL/6 mice fed a high-fat Western diet or the diet supplemented with 0.4% dietary EGCG (w/w) for 14 weeks. Dietary EGCG supplementation effectively prevented changes-including excessive accumulation of visceral and hepatic fat, abnormal liver function, and elevated concentrations of serum and liver inflammatory cytokines-known to be caused by high-fat diets. In addition, serum lipopolysaccharide concentrations decreased by 94.3%. RNA sequencing data of differentially expressed genes in ileal samples among three groups indicated that most of the pathways in the Kyoto Encyclopedia of Genes and Genomes in the first 20 enrichment levels were related to immunity and inflammatory reactions. Real-time reverse transcription quantitative polymerase chain reaction was used to determine alterations in expression levels of key genes related to intestinal immune function and inflammatory responses from ileal and colonic samples. Changes in secretory immunoglobulin A in the small intestine, serum, and feces further demonstrated improved intestinal mucosal immunity in the EGCG-treated mice. In conclusion, dietary EGCG effectively prevented the development of NAFLD and significantly improved intestinal mucosal immunity in mice with obesity induced by a high-fat diet. However, whether improved intestinal immune function is the key mechanism underlying the health benefits of dietary EGCG warrants further research.

A highly compressible and all-solid-state polydimethylsiloxane (PDMS) sponge-based flexible capacitance sensor modified with polypyrrole (PPy) was designed as the signal readout for the sensitive immunoassay of prostate-specific antigen (PSA). This system mainly consisted of a compressible capacitance sensor, immunoreaction protocol and gas delivery channel. The capacitance sensor was connected to a single microplate by a syringe, whereas the immunoreaction was carried out in the microplate. The conjugated catalase with the detection antibody via biotin-streptavidin interaction could trigger gas generation to cause a pressure change, thus resulting in the increase in the capacitance of the PPy-PDMS sponge observed with an LCR-6100 digital bridge capacitance meter. By coupling with the capacitance sensor, the capacitance change could be monitored in real time to achieve portable detection of PSA. Under the optimal conditions, the compressible supercapacitor PPy-PDMS sponge showed great electrochemical performance and remained stable under compressive strains. The capacitance increased with increasing target PSA concentration within a dynamic working range of 0.1-50 ng mL-1 at a detection limit of 57 pg mL-1. Moreover, acceptable reproducibility, precision and high specificity were obtained from PSA analysis, and were in good accordance with the commercial PSA ELISA kit.

With the development of modern society, we have witnessed a significant increase of people who join in sport exercises, which also brings significantly increasing exercise-induced muscle injuries, resulting in reduction and even cessation of participation in sports and physical activities. Although severely injured muscles can hardly realize full functional restoration, skeletal muscles subjected to minor muscle injuries ( e.g. , tears, lacerations, and contusions) hold remarkable regeneration capacity to be healed without therapeutic interventions. However, delayed diagnosis or inappropriate prognosis will cause exacerbation of the injuries. Therefore, timely diagnosis and prognosis of muscle injuries is important to the recovery of injured muscles. Here, in this review, we discuss the definition and classification of exercise-induced muscle injuries, and then analyze their underlying mechanism. Subsequently, we provide detailed introductions to both conventional and emerging techniques for evaluation of exercise-induced muscle injuries with focus on emerging portable and wearable devices for point-of-care testing (POCT). Finally, we point out existing challenges and prospects in this field. We envision that an integrated system that combines physiological and biochemical analyses is anticipated to be realized in the future for assessing muscle injuries., Competing Interests: There are no conflicts to declare., (This journal is © The Royal Society of Chemistry.)

Methods based on enzyme labels or nano labels have been developed for immunoassays, but most of them have low sensitivity and are unsuitable for low-abundance protein diagnostics and biosecurity. Herein, an innovative quartz crystal microbalance (QCM) immunosensing method was designed for high-efficiency detection of carcinoembryonic antigen (CEA) from serum samples with colorectal cancer patients by using horseradish peroxidase (HRP) nanoparticles as the enhancer, accompanying enzymatic biocatalytic precipitation (EBCP) toward 4-chloro-1-naphthol (4-CN) on an anti-CEA capture antibody-conjugated QCM probe. Initially, HRP nanospheres were synthesized on the basis of the reverse micelle method with the assistance of glutaraldehyde cross-linking, and then covalently conjugated onto polyclonal anti-CEA detection antibodies. The QCM immunosensing probe was prepared by immobilizing monoclonal anti-CEA capture antibodies on an l-cysteine-modified gold substrate. In the presence of target CEA, a sandwich-type immunoreaction was carried out between capture antibody and detection antibody, thereby resulting in the attachment of HRP nanospheres on the gold probe. Upon addition of 4-CN in the QCM cell, the carried HRP nanospheres catalyzed the 4-CN oxidation to produce an insoluble precipitate on the gold electrode, thus causing a change in the frequency. Relative to the conventional HRP-labeled strategy and direct antigen-antibody reaction, improved analytical features were obtained with HRP nanospheres. With the HRP nanosphere labeling method, the factors influencing the performance of the immunoassay were also studied. The covalent conjugation of antibodies with HRP nanospheres and the gold substrate achieved a good repeatability and intermediate precision down to 10.7%. Under optimum conditions, the frequency variation of the QCM immunoassay was proportional to the target CEA concentration within a dynamic linear range of 0.01-100 ng mL-1 with a detection limit (LOD) of 7.8 pg mL-1. In addition, the developed QCM immunoassay showed high specificity and long-term storage stability, and could be used for the analysis of human serum samples with consistent results in comparison with those obtained from the commercial enzyme-linked immunosorbent assay (ELISA) method.

Understanding the mechanism of a catalytic reaction is of fundamental importance not only scientifically but also technologically to the design of high-performance catalysts. In this work, the mechanisms of 1-phenyl-1-propyne and cis-β-methylstyrene hydrogenations catalyzed by Cu55 and ligand-coated Cu55 are explored in detail by means of density functional theory (DFT). The calculated results indicate that the semihydrogenation selectivity of the catalyst can be effectively controlled by employing a suitable ligand. That is, the PCy3 and PPh3 ligands used to coat Cu55 can largely raise the energy barrier of the rate-determining step for cis-β-methylstyrene hydrogenation. By the study of energy decomposition analysis (EDA) and charge density difference, it can be found that the deformation energies of the substrate fragments play a crucial role in the energy barriers of the rate-determining steps. The large hindrance effect of the ligands is beneficial for improving the semihydrogenation selectivity of the catalysts. This study provides significant information for future catalyst design and on the physical origin of the phosphine ligand-coated nanoparticle catalysis for semihydrogenation.

Methods based on prussian blue nanoparticles (PBNPs) have been reported for photothermal immunoassays in analytical nanoscience fields but most suffer from low sensitivity and are not beneficial for routine use. Herein, we design an in situ amplified near-infrared (NIR) photothermal immunoassay for the quantitative screening of neuron-specific enolase (NSE) on a portable thermometer using PBNP-encapsulated nanoliposomes as photosensitive materials. Biotinylated liposomes loaded with numerous prussian blue nanoparticles were synthesized through a typical reverse-phase evaporation method. The photothermal immunoassay was carried out in an anti-NSE capture antibody-coated microplate using the biotinylated anti-NSE secondary antibody. With the sandwiched immunoreaction and the biotin-avidin linkage, the subsequent photothermal measurement of PBNPs released from the liposomes with buffered surfactant including Tween 20 was conducted on a digital thermometer under near-infrared 808 nm laser irradiation, accompanied by the convertion of NIR-light wavelength to heat. Under the optimum conditions, the photothermal immunoassay displayed a wide dynamic concentration range of 0.1-100 ng mL-1 with a low detection limit for NSE of 0.053 ng mL-1. Good reproducibility (RSD ≤ 2.78% for intra-assay; RSD ≤ 4.39% for inter-assay), high selectivity against other biomarkers, and a long-term stability (≥94.9% of the initial signal during six-month storage) were acquired in the photothermal immunoassay. Impressively, the analysis of 7 human serum specimens for target NES via the photothermal immunoassay also gave well-matched results with the referenced human NSE enzyme-linked immunosorbent assay.