Real-time detection of 20 amino acids and discrimination of pathologically relevant peptides with functionalized nanopore.

Precise identification and quantification of amino acids is crucial for many biological applications. Here we report a copper(II)-functionalized Mycobacterium smegmatis porin A (MspA) nanopore with the N91H substitution, which enables direct identification of all 20 proteinogenic amino acids when combined with a machine-learning algorithm. The validation accuracy reaches 99.1%, with 30.9% signal recovery. The feasibility of ultrasensitive quantification of amino acids was also demonstrated at the nanomolar range. Furthermore, the capability of this system for real-time analyses of two representative post-translational modifications (PTMs), one unnatural amino acid and ten synthetic peptides using exopeptidases, including clinically relevant peptides associated with Alzheimer's disease and cancer neoantigens, was demonstrated. Notably, our strategy successfully distinguishes peptides with only one amino acid difference from the hydrolysate and provides the possibility to infer the peptide sequence.

Sustainable application of rice-waste for fuels and valuable chemicals-a mini review.

The global annual production of rice is over 750 million tons, and generates a huge amount of biomass waste, such as straw, husk, and bran, making rice waste an ideal feedstock for biomass conversion industries. This review focuses on the current progress in the transformation of rice waste into valuable products, including biochar, (liquid and gaseous) biofuels, valuable chemicals (sugars, furan derivatives, organic acids, and aromatic hydrocarbons), and carbon/silicon-based catalysts and catalyst supports. The challenges and future prospectives are highlighted to guide future studies in rice waste valorization for sustainable production of fuels and chemicals.

Nonvolatile magnetoelectric coupling in two-dimensional van der Waals sandwich heterostructure CuInP2S6/MnCl3/CuInP2S6.

Electrical control of magnetism is of great interest for low-energy-consumption spintronic applications. Due to the recent experimental breakthrough in two-dimensional materials, with the absence of hanging bonds on the surface and strong tolerance for lattice mismatch, heterogeneous integration of different two-dimensional materials provides a new opportunity for coupling between different physical properties. Here, we report the realization of nonvolatile magnetoelectric coupling in vdW sandwich heterostructure CuInP2S6/MnCl3/CuInP2S6. Using first-principles calculations, we reveal that when interfacing with ferroelectric CuInP2S6, the Dirac half-metallic state of monolayer MnCl3 will be destroyed. Moreover, depending on the electrically polarized direction of CuInP2S6, MnCl3 can be a half-metal or a ferromagnetic semiconductor. We unveil that the obtained ferromagnetic semiconductor in MnCl3 can be attributed to the different gain and loss of electrons on the two adjacent Mn atoms due to the sublattice symmetry broken by interlayer coupling. The effects of interfacial magnetoelectric coupling on magnetic anisotropy and ferromagnetic Curie temperature of MnCl3 are also investigated, and a multiferroic memory based on this model is designed. Our work not only provides a promising way to design nonvolatile electrical control of magnetism but also renders monolayer MnCl3 an appealing platform for developing low-dimensional memory devices.

Geochemical characteristics and socioeconomic associations of carbonaceous aerosols in coal-fueled cities with significant seasonal pollution pattern.

Carbonaceous aerosols, comprising organic carbon (OC) and elemental carbon (EC), are critical component of fine particulate matter (PM2.5), with diverse impacts on air quality and human health. This study investigated the concentrations and seasonal patterns of carbonaceous species in PM2.5 during both the heating season (January 2021) and non-heating season (July 2021) in three coal-fueled cities in northern China, as well as the differences in carbonaceous aerosols and their associations with socioeconomic parameters in cities situated on either side of the "Hu Line" in China. The results showed that, owing to intensified coal combustion and unfavorable meteorological conditions, levels of OC, EC, and OC/EC ratios were higher in winter compared to summer. Moreover, the presence of dust (DU) and light pollution (LP) days resulted in elevated OC levels but decreased EC levels. The Char-EC/Soot-EC ratios were highest during LP, followed by CL and DU. A source apportionment analysis demonstrated that coal burning, vehicle exhaust, road dust, and biomass burning were the primary contributors to carbonaceous aerosols, as confirmed by diagnostic ratios, Char-EC/Soot-EC ratios, and PCA analysis. Furthermore, our study found that carbonaceous aerosols concentrations and source apportionment primarily varied with diurnal and seasonal trends and different pollution types. Additionally, at the national scale, population density and urban green space exhibited a positive correlation with OC/EC ratios (p < 0.05), while energy consumption per unit of GDP showed a negative correlation (p < 0.05). The observation that OC/EC ratios were lower in coal-fueled cities than in economy-based cities suggests a more severe pollution scenario. These findings highlight the importance of comprehending of the seasonal variation and chemical characteristics of carbonaceous aerosol for understanding air pollution sources and characteristics, which is essential for both air quality management and human health.

The impact of mulberry leaf extract at three different levels on reducing the glycemic index of white bread.

In this study, the influences of mulberry leaf extract (MLE) addition on the physicochemical properties including the specific volume, texture and sensory features of white bread (WB) were evaluated by the sensory analysis technology. A double-blind, randomised, repeat-measure design was used to study the impact of MLE addition on the postprandial blood glucose response as well as the satiety index of WB. Results showed that the addition of MLE showed no significant effects on the physicochemical properties of WB except for the slight changes of color and bitterness. The addition of MLE significantly reduced the total blood glucose rise after ingestion of WB over 120 minutes, and reduced the GI value of WB in a dose-effect relationship. When the concentration of MLE reached 1.5 g per 100 g available carbohydrate, the GI value of WB could be reduced from 77 to 43. This study provides important information in terms of the appropriateness of MLE when added to more complex real food, the dose-dependent relationship could supply a reference for the application of MLE.

Algorithm of Stability-Analysis-Based Feature Selection for NIR Calibration Transfer.

For conventional near-infrared spectroscopy (NIR) technology, even within the same sample, the NIR spectral signal can vary significantly with variation of spectrometers and the spectral collection environment. In order to improve the applicability and application of NIR prediction models, effective calibration transfer is essential. In this study, a stability-analysis-based feature selection algorithm (SAFS) for NIR calibration transfer is proposed, which is used to extract effective spectral band information with high stability between the master and slave instruments during the calibration transfer process. The stability of the spectrum bands shared between the master and slave instruments is used as the evaluation index, and the genetic algorithm was used to select suitable thresholds to filter out the spectral feature information suitable for calibration transfer. The proposed SAFS algorithm was applied to two near-infrared datasets of corn oil content and larch wood density. Simultaneously, its calibration transfer performances were compared with two classical feature selection methods. The effects of different preprocessing algorithms and calibration transfer algorithms were also assessed. The model with the feature variables selected by the SAFS obtained the best prediction. The SAFS algorithm can simplify the spectral data to be transferred and improve the transfer efficiency, and the universality of the SAFS allows it to be used to optimize calibration transfer in various situations. By combining different preprocessing and classic feature selection methods with this, the sensitivity of the correlation between spectral data and component information are improved significantly, as well as the effect of calibration transfer, which will be deeply developed.

Changes in stoichiometric characteristics of ambient air pollutants pre-to post-COVID-19 in China.

To prevent the Corona Virus Disease 2019 (COVID-19) spreading, Chinese government takes a series of corresponding measures to restrict human mobility, including transportation lock-down and industries suspension, which significantly influenced the ambient air quality and provided vary rare time windows to assess the impacts of anthropological activities on air pollution. In this work, we divided the studied timeframe (2019/12/24-2020/2/24) into four periods and selected 88 cities from 31 representative urban agglomerations. The indicators of PM2.5/PM10 and NO2/SO2 were applied, for the first time, to analyze the changes in stoichiometric characteristics of ambient air pollutants pre-to post-COVID-19 in China. The results indicated that the ratios of NO2/SO2 presented a responding decline, especially in YRD (-5.01), YH (-3.87), and MYR (-3.84), with the sharp reduction of traffic in post-COVID-19 periods (P3-P4: 2.34 ± 0.94 m/m) comparing with pre-COVID-19 periods (P1-P2: 4.49 ± 2.03 m/m). Whereas the ratios of PM2.5/PM10 increased in P1-P3, then decreased in P4 with relatively higher levels (>0.5) in almost all urban agglomerations. Furthermore, NO2 presented a stronger association with PM2.5/PM10 variation than CO; and PM2.5 with NO2/SO2 variation than PM10. In summary, the economic structure, lockdown measures and meteorological conditions could explain the noteworthy variations in different urban agglomerations. These results would be in great help for improving air quality in the post-epidemic periods.

Promoting Aromatic C-H Activation through Reactive Brønsted Acid-Base Pairs on Penta-Coordinated Al-Enriched Amorphous Silica-Alumina.

The surface acidity and local coordination environment of zeolites and amorphous silica-aluminas (ASAs) can promote acid-catalyzed C-H activation in many important hydrocarbon conversion reactions. Acid sites generated by penta-coordinated Al species (AlV) can lead to enhanced acidity and changes in the surface coordination. We evaluated the potential of flame-derived ASAs with enriched AlV for C-H activation using hydrogen/deuterium (H/D) exchange with benzene-d6. With increasing Al content of ASAs, the exchange rate increased, whereas the activation energy (Ea) slightly decreased due to the enhanced Brønsted acidity. The ASAs exhibited significantly higher exchange rates and lower Ea values than the sol-gel-derived ASAs and zeolite H-ZSM-5. The superior activity is attributed to the fact that more oxygen coordinated with AlV species on flame-made ASAs, which can act as acceptors for D+, enhancing the deuterium displacement. These findings could offer a valuable alternative strategy for tailoring high-performance solid acids to promote hydrocarbon conversion reactions.

The shelf-life of chestnut rose beverage packaged in PEN/PET bottles under long term storage: A comparison to packaging in ordinary PET bottles.

The shelf life of chestnut rose beverage is largely dependent on packaging method and storage temperature. In this study, we investigated the effects of packaging beverages in bottles made of either polyethylene terephthalate (PET) or PEN (polyethylene naphthalate)/PET and storage temperature (4, 25, 37, and 55 ℃) on the shelf life of chestnut rose beverage. The physicochemical parameters and enzyme activity of beverages were evaluated, and we found that at 4 °C, the vitamin C, superoxide dismutase, and total polyphenol contents of beverages stored in PEN/PET bottles increased by 9.95 ± 0.49%, 2.86 ± 0.13%, and 3.23 ± 0.09% respectively, compared to beverages in ordinary PET bottles. In addition, other characteristic indicators including total soluble solids, browning index, and color value were also significantly improved. A shelf-life model was established based on the Arrhenius equation, and it will help distributors and consumers to determine the storage time and optimal shelf life of chestnut rose beverage.

Revealing Brønsted Acidic Bridging SiOHAl Groups on Amorphous Silica-Alumina by Ultrahigh Field Solid-State NMR.

Amorphous silica-aluminas (ASAs) are important acidic catalysts and supports for many industrially essential and sustainable processes. The identification of surface acid sites with their local structures on ASAs is of critical importance for tuning their catalytic properties but still remains a great challenge and is under debate. Here, ultrahigh magnetic field (35.2 T) 27Al-{1H} D-HMQC (dipolar-mediated heteronuclear multiple-quantum correlation) two-dimensional NMR experiments demonstrate two types of Brønsted acid sites in ASA catalysts. In addition to the known pseudobridging silanol acid sites, the use of ultrahigh field NMR provides the first direct experimental evidence for the existence of bridging silanol (BS: SiOHAl) acid sites in ASAs, which has been hotly debated in the past few decades. This discovery provides new opportunities for scientists and engineers to develop and apply ASAs in various reaction processes due to the significance of BS in chemical and fuel productions based on its strong Brønsted acidity.

Effect of Hepatitis B Virus Infection on Sperm Quality and Outcomes of Assisted Reproductive Techniques in Infertile Males.

Background: Hepatitis B virus (HBV) infection is one of the health problems and has adverse effects on public health. However, the consequences of male HBV carriers for assisted reproductive techniques (ART) remain unclear. Objective: To examine whether men with HBV would impact sperm quality and the intrauterine insemination (IUI)/ in vitro fertilization (IVF)/ intracytoplasmic sperm injection (ICSI) outcomes. Methods: We retrospectively analyzed data from 681 infertile couples for IUI/IVF/ICSI fresh cycle outcomes. Case group was 176 infertile couples with male HBV infection undergoing embryo transfer in our center (99 for IVF and 77 for ICSI) and 51 infertile couples for IUI. Negative control was 454 non-infected infertility couples, matched for female age, BMI and infertility duration (102 for IUI and 198 for IVF and 154 for ICSI). Results: Sperm viability among infertile men with HBV infection was significantly lower than control group (74.1 ± 13.7 vs. 77.0 ± 12.8, P < 0.01). Sperm motility was significantly decreased in HBV positive men in comparison to the control group (32.5 ± 14.6 vs. 35.5 ± 12.9, P < 0.05). In IVF/ICSI cycles, two groups had similar results in two pronuclear (2PN) fertilization rate, implantation rate, clinical pregnant rate and abortion rate (P > 0.05). There was also no difference in the clinical pregnant rate and abortion rate in IUI cycles (P > 0.05). Conclusion: Men with HBV infection will affect their sperm quality, but not affect the outcomes of ART.

Modular DNA Circuits for Point-of-Care Colorimetric Assay of Infectious Pathogens.

Accurate, specific, and inexpensive detection of multiple infectious pathogens simultaneously is a significant goal for human health and safety. Herein we present a rationally designed modular DNA circuit for point-of-care (POC) detection of a variety of infectious pathogens based on nucleic acid isothermal amplification technology and DNAzyme-mediated colorimetric readout. A modular DNA circuit was constructed with a fixed module and a flexible module and was rationally designed according to genetic targets. On this basis, the platform could detect multiple genetic targets corresponding to infectious pathogens simultaneously. Signal amplification properties of the DNA circuit and the peroxidase-like DNAzyme enable the detection limits to reach the picomolar level. By urea treatment and magnetic separation, the fixed module can be reused at least five times, which makes this assay more economical and environmentally friendly. The detection of genetic infectious pathogens should be accomplished in 2 h with naked-eye observation and may provide an efficient tool for POC analysis of multiple infectious pathogens, especially in resource-poor areas.

Engineering the Distinct Structure Interface of Subnano-alumina Domains on Silica for Acidic Amorphous Silica-Alumina toward Biorefining.

Amorphous silica-aluminas (ASAs) are important solid catalysts and supports for many industrially essential and sustainable processes, such as hydrocarbon transformation and biorefining. However, the wide distribution of acid strength on ASAs often results in undesired side reactions, lowering the product selectivity. Here we developed a strategy for the synthesis of a unique class of ASAs with unvarying strength of Brønsted acid sites (BAS) and Lewis acid sites (LAS) using double-flame-spray pyrolysis. Structural characterization using high-resolution transmission electron microscopy (TEM) and solid-state nuclear magnetic resonance (NMR) spectroscopy showed that the uniform acidity is due to a distinct nanostructure, characterized by a uniform interface of silica-alumina and homogeneously dispersed alumina domains. The BAS population density of as-prepared ASAs is up to 6 times higher than that obtained by classical methods. The BAS/LAS ratio, as well as the population densities of BAS and LAS of these ASAs, could be tuned in a broad range. In cyclohexanol dehydration, the uniform Brønsted acid strength provides a high selectivity to cyclohexene and a nearly linear correlation between acid site densities and cyclohexanol conversion. Moreover, the concerted action of these BAS and LAS leads to an excellent bifunctional Brønsted-Lewis acid catalyst for glucose dehydration, affording a superior 5-hydroxymethylfurfural yield.

Production efficiency and change characteristics of China's apple industry in terms of planting scale.

The global population is rapidly increasing, the arable land area is losing in a large scale, and the water supply capacity is limited. Meanwhile, China is in a critical period of the transformation of apple industrial structure, and the improvement of apple production efficiency is an important way to increase farmers' output and income, moderate-scale operation is the inevitable trend in agricultural modernization. However, few studies have explored the production efficiency of the apple industry from the perspective of planting scale. In China, there are seven major apple-producing provinces: Shaanxi, Shandong, Gansu, Henan, Shanxi, Hebei, and Liaoning. Therefore, based on provincial panel data of the seven main apple-producing areas in China, this study used the Malmquist productivity index and data envelopment analysis to measure the efficiency level of the apple industry. At the same time, the threshold regression model was used to analyze the characteristics of the change in apple planting scale and production efficiency. The results showed that apple production efficiency in different regions of China exhibited regional differences and time series fluctuations. Apple planting scale had a "double" threshold effect, and the impact on apple production efficiency showed a "negative effect-positive effect" trend. Therefore, the suggestion is to appropriately adjust the scale of operation, take measures according to local conditions, promote the upgrading of apple production technology, and realize the integration of apple production and sales by using "Internet +."

Formation and Location of Pt Single Sites Induced by Pentacoordinated Al Species on Amorphous Silica-Alumina.

Alumina and its mixed oxides are popular industrial supports for emerging supported metal catalysts. Pentacoordinated Al (AlV) species are identified as key surface sites for anchoring and stabilizing metal single-site catalysts; however, AlV is rare in conventional amorphous silica-alumina (ASA). Recently, we have developed AlV-enriched ASA, which was applied as a support for the synthesis of Pt single-site catalysts in this work. Each preparation stage and the interaction between Pt and surface Al species were explored by 1H and 27Al solid-state nuclear magnetic resonance spectroscopy, and the formation of the dominant Pt single sites on the surface of AlV-enriched ASA was confirmed by high-angle annular dark-field imaging scanning transmission electron microscopy and energy dispersive spectroscopy line scanning. On the surface of supports without a significant AlV population (Pt/Al2O3 and Pt/SiO2), mainly Pt nanoparticles were formed. This indicates that AlV contributes to the strong metal-support interaction to stabilize the Pt single sites on Pt/ASA, which was characterized by diffuse reflectance infrared Fourier transform spectroscopy combined with CO adsorption, X-ray photoelectron spectroscopy, and electron energy loss spectroscopy. Pt single sites supported on AlV-enriched ASA exhibit excellent chemoselectivity in the hydrogenation of C═O groups, affording 2-3-fold higher yields compared to those of Pt nanoparticles supported on Al2O3 and SiO2.

Highly Efficient NO Abatement over Cu-ZSM-5 with Special Nanosheet Features.

Conventional Cu-ZSM-5 and special Cu-ZSM-5 catalysts with diverse morphologies (nanoparticles, nanosheets, hollow spheres) were synthesized and comparatively investigated for their performances in the selective catalytic reduction (SCR) of NO to N2 with ammonia. Significant differences in SCR behavior were observed, and nanosheet-like Cu-ZSM-5 showed the best SCR performance with the lowest T50 of 130 °C and nearly complete conversion in the temperature range of 200-400 °C. It was found that Cu-ZSM-5 nanosheets [mainly exposed (0 1 0) crystal plane] with abundant mesopores and framework Al species were favorable for the formation of high external surface areas and Al pairs, which influenced the local environment of Cu. This motivated the preferential formation of active copper species and the rapid switch between Cu2+ and Cu+ species during NH3-SCR, thus exhibiting the highest NO conversion. In situ diffused reflectance infrared Fourier transform spectroscopy (DRIFTS) results indicated that the Cu-ZSM-5 nanosheets were dominated by the Eley-Rideal (E-R) mechanism and the labile nitrite species (NH4NO2) were the crucial intermediates during the NH3-SCR process, while the inert nitrates were more prone to generate on Cu-ZSM-5 nanoparticles and conventional one. The combined density functional theory (DFT) calculations revealed that the decomposition energy barrier of nitrosamide species (NH2NO) on the (0 1 0) crystal plane of Cu-ZSM-5 was lower than those on (0 0 1) and (1 0 0) crystal planes. This study provides a strategy for the design of NH3-SCR zeolite catalysts.

Separation, identification, and molecular docking of tyrosinase inhibitory peptides from the hydrolysates of defatted walnut (Juglans regia L.) meal.

Defatted walnut meal protein was hydrolyzed using alcalase to yield tyrosinase inhibitory peptides. After separation by ultrafiltration and Sephadex G-25, the fraction with the highest tyrosinase inhibitory activity was identified using liquid chromatography-tandem mass spectrometry and 606 peptides were obtained. Then, molecular docking was used to screen for tyrosinase inhibitory peptides and to clarify the theoretical interaction mechanism between the peptides and tyrosinase. A peptide with the sequence Phe-Pro-Tyr (FPY, MW: 425.2 Da) was identified and the synthesized peptide inhibited tyrosine monophenolase and diphenolase with IC50 values of 1.11 ± 0.05 and 3.22 ± 0.09 mM, respectively. The inhibition of tyrosinase by FPY was competitive and reversible. Good stability of FPY toward digestion was observed in an in vitro gastrointestinal digestion simulation experiment. These results indicated that FPY can be used as a potential tyrosinase inhibitor in the food, medicine, and cosmetics industries.

Effects of intradialytic resistance exercises on physical performance, nutrient intake and quality of life among haemodialysis people: A systematic review and meta-analysis.

OBJECTIVES: The aim of this systematic reviews was to synthesize the current studies for the effectiveness of intradialytic resistance exercises with usual care on HD people. DESIGN: Meta-analysis of randomized controlled studies. METHODS: A systematic search of seven electronic databases, including PubMed, EMBASE, the Cochrane Library, Web of Science, WanFang, China National Knowledge Infrastructure (CNKI) and SINOMED, was systematically searched up to May 2018. The reference lists of previously reported systematic review were also checked. Pooled analysis was used to determine effection of intradialytic resistance exercises for haemodialysis people. Physical performance, nutrient intake and quality of life were explored, by comparing the association between effect sizes. RESULTS: Fourteen studies of 594 people were included. Compared with control groups, intradialytic resistance exercises significantly improve physical performance included 6-min walk test, sit-to-stand 30 and grip strength. However, no significant improvements were found in nutrient intakes such as dietary protein intake and quality of life.

Effect of whey protein isolate/chitosan/microcrystalline cellulose/PET multilayer bottles on the shelf life of rosebud beverages.

Multilayer bottles consisting of chitosan (CS), microcrystalline cellulose (MCC), whey protein isolate (WPI), and polyethylene terephthalate (PET) were tested as novel materials for packaging and extending shelf life of rosebud beverages. We studied the storage stability at 4 °C, 25 °C, 37 °C, and 55 °C by assessing the physical and biochemical parameters. The results show that multilayer PET bottles had better barrier performance and improved soluble solids content, pH, polyphenol content, color indices, and browning degree in rosebud beverages over the control at all studied temperatures. A shelf life model was established based on the Arrhenius equation, and the number of days when polyphenol contents dropped to <50% of the initial content was defined as the shelf life. Our results highlight the reliability of the prediction model, and we conclude that packaging rosebud beverages in multilayer PET bottles significantly extends the product shelf life, and this benefit was further extended at low temperatures.

Green synthesis of boron and nitrogen co-doped TiO2 with rich B-N motifs as Lewis acid-base couples for the effective artificial CO2 photoreduction under simulated sunlight.

Boron and nitrogen co-doped Titanium dioxide (TiO2) nanosheets (BNT) with high surface area of 136.5 m2 g-1 were synthesized using ammonia borane as the green and triple-functional regent, which avoids the harmful and explosive reducing regents commonly used to create surface defects on TiO2. The decomposition of ammonia borane could incorporate reactive Lewis acid-base (B, N) pairs, together with the as-generated H2 to create mesoporous structure and rich oxygen vacancies in pristine TiO2. The BNTs prepared from various ammonia borane loading are evaluated in photoreduction of carbon dioxide (CO2) with steam under simulated sunlight, achieving about 3.5 times higher carbon monoxide (CO) production than pristine TiO2 under the same conditions. Steady state and transient optical measurements indicated BNT with reduced band gap, rich defect states and elevated conduction band position could enhance the light harvesting efficiency and promote the charge transfer at the catalyst/CO2 interface. Density functional theory simulation and in situ FTIR suggest that the Lewis acid-base (B, N) pairs on BNT may very substantially increase the activation of inert CO2 which facilitates their photoreduction with the hydrogen from the water splitting at the surface defects on TiO2. Finally, a reaction mechanism of Lewis acid-base assisted CO2 photoreduction leading to substantially improved performance is proposed.