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•A highly curved and ultrathin P-doped PdMo bimetallene is engineered.•The catalyst has superior performance in electrooxidation of various alcohols.•The activity for ORR surpasses ...that of commercial Pt/C catalyst.•DFT reveals that P doping enhances both OH adsorption and CO desorption.
The commercialization of direct alcohol fuel cells (DAFCs) relies on the development of high performance electrocatalysts for both the alcohol oxidation reaction and the oxygen reduction reaction (ORR). In this study, a novel phosphorus-doped palladium-molybdenum (P-PdMo) bimetallene with a partially amorphous structure is demonstrated. The ultrathin and curved morphology of the nanosheets, combined with electronic regulation by phosphorus atoms, facilitates OH adsorption and CO desorption. Consequently, the catalyst exhibits significantly enhanced activity and durability in the electrooxidation of alcohols, including methanol, ethanol, ethylene glycol, and glycerol. Particularly toward ethanol oxidation, the P-PdMo bimetallene displays exceptional mass and specific activities up to 4.95 A mg-1Pd and 8.28 mA cm−2, respectively. Furthermore, the P-PdMo bimetallene demonstrates outstanding ORR performance, with an onset potential of 1.0 V and a half-wave potential of 0.88 V. Overall, this study opens new avenues in metallene electrocatalysts and advancing toward the practical implementation of DAFCs.
The carrier lifetime is one of the key parameters for perovskite solar cells (PSCs). However, it is still a great challenge to achieve long carrier lifetimes in perovskite films that are comparable ...with perovskite crystals owning to the large trap density resulting from the unavoidable defects in grain boundaries and surfaces. Here, by regulating the electronic structure with the developed 2‐thiopheneformamidinium bromide (ThFABr) combined with the unique film structure of 2D perovskite layer caped 2D/3D polycrystalline perovskite film, an ultralong carrier lifetime exceeding 20 µs and carrier diffusion lengths longer than 6.5 µm are achieved. These excellent properties enable the ThFA‐based devices to yield a champion efficiency of 24.69% with a minimum VOC loss of 0.33 V. The unencapsulated device retains ≈95% of its initial efficiency after 1180 h by max power point (MPP) tracking under continuous light illumination. This work provides important implications for structured 2D/(2D/3D) perovskite films combined with unique FA‐based spacers to achieve ultralong carrier lifetime for high‐performance PSCs and other optoelectronic applications.
By regulating the electronic structure with ThFABr, an ultralong carrier lifetime exceeding 20 µs and carrier diffusion lengths longer than 6.5 µm is achieved in 2D/3D polycrystalline perovskite films. These excellent properties enable the ThFA‐based devices yielding a champion efficiency of 24.69% and a high VOC of 1.21 V, coupled with significantly improved operational stability.
Researches on indoleamine-2,3-dioxygenase-1 (IDO1), a neoplastic pathogenesis-related protein, have provided a new angle of view to regulate malignancy-related immunosuppression. However, the ...therapeutic efficacy of IDO1 inhibitors is subject to key limitations as both cancer and dendritic cells tend to be trapped in the IDO1-mediated immune dysfunction, which poses challenges to the inhibitory potency of drug regimens in multiple targets. Here, we report on the fabrication technique of a biomimetic nanocarrier that is endowed with the whole array of cancer cell membrane proteins for encapsulating the most used IDO1 probe indoximod (IND). By fully utilizing the homologous adhesion proteins and antigenic motifs on cytomembrane, these nanoparticulate particles are capable of infiltrating tumors and actively accumulating in cancer and dendritic cells, as well as hitching a ride on dendritic cells to tumor-draining lymph nodes. Ultimately, by increasing the distribution of drugs in both tumor cells and dendritic cells in tumor-draining lymph nodes, these formulations greatly enhance the efficacy of IND without the aid of chemotherapeutic drugs, achieving substantial control of tumor growth. Overall, this leverage of bionanotechnology maximizes the therapeutic potential of IND and can provide a theoretical reference for the clinical application of IDO1 inhibitors.
Global greenhouse gas (GHG) emissions from food loss and waste (FLW) are not well characterized from cradle to grave. Here GHG emissions due to FLW in supply chain and waste management systems are ...quantified, followed by an assessment of the GHG emission reductions that could be achieved by policy and technological interventions. Global FLW emitted 9.3 Gt of CO
equivalent from the supply chain and waste management systems in 2017, which accounted for about half of the global annual GHG emissions from the whole food system. The sources of FLW emissions are widely distributed across nine post-farming stages and vary according to country, region and food category. Income level, technology availability and prevailing dietary pattern also affect the country and regional FLW emissions. Halving FLW generation, halving meat consumption and enhancing FLW management technologies are the strategies we assess for FLW emission reductions. The region-specific and food-category-specific outcomes and the trade-off in emission reductions between supply chain and waste management are elucidated. These insights may help decision makers localize and optimize intervention strategies for sustainable FLW management.
Research question: More than 100 variants have been identified in the TUBB8 gene, which account for approximately 30% of infertile women with oocyte maturation defects. But what is the correlation ...between the highly phenotypic diversity and genetic variability? Are there other variants in TUBB8 related to female infertility?
Design: TUBB8 resequencing was performed in 80 female subjects who were experiencing infertility and were seeking treatment with assisted reproductive technologies (ART), or had ever experienced ART failure due to oocyte maturation defects. All variants were evaluated with pedigree analysis, population frequency, in-silico analysis and molecular modelling. The effects of the variants on oocytes/arrested embryos were assessed by morphological observations, immunostaining, embryo biopsies and chromosome euploidy analysis.
Results: Nine missense variants and two frameshift variants from an additional 15 families were identified, including four novel variants and seven previously reported recurrent variants. These TUBB8 variants were related to highly variable phenotypes, including abnormalities in oocyte maturation or morphology, fertilization failure, embryonic development abnormalities and implantation failure. Also further clarified were the incomplete penetrance of heterozygous p.E108K, the likely benign significance of heterozygous p.A313V and the clinical effect of a novel variant of p.R380C.
Conclusions: This study significantly expands the variant spectrum of the TUBB8 gene and, together with the available findings on TUBB8 variants and female infertility, will potentially facilitate the genetic counselling of infertile women in future.
Foods and water can be contaminated with antibiotics in China, which may affect children's health, but evidence on antibiotic exposure with precocious puberty (PP) is limited. This study explored the ...association of antibiotic exposure with PP in a school-based setting. A cross-sectional study with multistage stratified cluster random sampling was conducted in Zhongshan City, Guangdong Province and Qufu City, Shandong Province in China from October 11 to December 5, 2019. A first-morning urine sample was collected to detect antibiotic exposure. We detected 33 of 45 types of antibiotics from eight categories in 928 primary school children aged 6–12 years using HPLS-MS/MS. Detection rate of antibiotics was stratified by sex, study site, and BMI. The Tanner stages were assessed by professional pediatricians from local hospitals. PP is defined as the onset of secondary characters before 8-year-old or menarche before 10-year-old for girls and before 9-year-old for boys. Multivariable logistic regression was performed to examine the association between antibiotic exposure and PP after adjusting potential confounders. The overall detection rate of antibiotics was 93.0% in 928 children. We found the detection rate of tetracyclines and fluoroquinolones in children with PP was significantly higher than that of children with normal puberty (41.4% vs 29.9%, 56.8% vs 50.6%, respectively, all p < 0.05). Both fluoroquinolones (odds ratio (OR): 1.835, 95% confidence interval (CI): 1.066–3.158) and tetracyclines (OR: 2.120, 95% CI: 1.175–3.825) were associated with increased OR of PP after adjusting sex, age, BMI, study site, and family income. Specifically, compared to the values less than the limits of detection, low concentration of ofloxacin from fluoroquinolones (OR: 2.056, 95% CI: 1.091–3.875) and high concentration of chlortetracycline (OR: 3.027, 95% CI: 1.126–8.140) and tetracycline from tetracyclines (OR: 2.756, 95% CI: 1.167–6.506) were associated with increased OR of PP. Exposure to antibiotics, especially fluoroquinolones and tetracyclines was positively associated with precocious puberty.
•First study on antibiotics exposure in precocious puberty by HPLC-MS/MS.•928 primary school children aged 6–12 years were included.•45 types of antibiotics were measured using HPLC-MS/MS.•Antibiotic level was major contributor to overall variance in risk estimate.
•A high-precision ML-based SST retrieval framework is proposed for offshore waters.•The selection of features should be strictly optimized during model construction.•Adding time-related features and ...initial temperature improves the model accuracy.•RF outperforms the traditional physical model and DNN in SST retrieval accuracies.•The proposed framework based on RF proved to be portable for independent samples.
High-precision sea surface temperature (SST) data is essential for monitoring and management of offshore environment. SST retrievals from thermal infrared remote sensing have the advantages in time frequency and space coverage over measurements from ships and buoys. However, traditional SST retrieval models are not fully applicable for offshore waters where seawater conditions change a lot, due to simple functional forms and empirical fitting of model parameters. Machine learning (ML) is introduced because it doesn’t need to define specific model rules or unknown parameters, which is more intelligent to deal with complex retrieval problems in a data-driven way. But the applicability of ML has not been investigated in the North Yellow Sea of China, and the selection of driving features for model construction has not been fully discussed. Here, we designed a high-precision SST retrieval framework based on random forest (RF) with optimal feature combination using MODIS data and in-situ SST measurements during 2013–2020 in the northern part of the North Yellow Sea. The performances of different feature combinations were assessed based on model testing accuracies and the RF output feature importance. Compared with previous ML-based SST retrieval studies, we added two time-related features (i.e., day of the year and month) and one feature as initial temperature (i.e., SST retrieval from split-window algorithm), which reduced the testing error by around 15 % and 11 %, respectively. The retrieval results were validated with in-situ measurements, showing that the RF model achieved better accuracies (R2 = 0.987, SD = 0.842 °C, MAE = 0.675 °C, RMSE = 0.841 °C) than the improved split-window algorithm (named as ISW) and deep neural network. Compared with ISW, the spatial distribution of RF retrieval map exhibited similar variation across four seasons, mainly differed in the coastal areas or at the formation of temperature fronts. Note that the constructed RF model was still reliable when applied to the independent samples in 2021. This study contributes to improve the accuracy of offshore SST retrieval under different seawater conditions and provides references for SST monitoring.
We report the exfoliation of two‐dimensional polyoxometalate‐encapsulating MOF (POM−Co‐MOF) into atomically thick nanosheets for highly efficient desulfurization application. Two‐dimensional ...layer‐structured MOF Co2(H2O)4(BTX)3PMo12O40 (BTX=1,4‐Bis(1,2,4‐triazol‐1‐ylmethyl)benzene) is featured with Keggin‐type POM wrapped in MOF skeleton via coordinating to cobalt with terminal oxygen. Wet ball‐milling and sonication assisted top‐down exfoliation in acetonitrile successfully delaminates POM‐MOF into nanosheets, which creates more accessible active sites and efficiently decreases the restriction of mass transfer during the reaction, and thus enhances the desulfurization efficiency. In comparison with bulk POM‐MOF, delaminated nanosheets exhibit a 14‐fold higher desulfurization efficiency via monitoring dibenzothiophene oxidation process (TON value of ca. 400) using H2O2 as oxidant. Meanwhile, POM−Co‐MOF nanosheets also show superior desulfurization performance in model oil system.
Get skinny with ultrasheets: Inaccessible active sites and limited mass transfer restrict the catalytic performance of bulk MOF. We report the exfoliation of 2D POM−Co‐MOF into ultrathin nanosheets via a top‐down delamination strategy. Compared with the pristine MOF, the delaminated nanosheets possess more accessible active sites and much less restriction of mass transfer, which give rise to the superior catalytic performance on oxidative desulfurization reaction.
Sulfur-containing substances in sewers frequently incur unpleasant odors, corrosion-related economic loss, and potential human health concerns. These observations are principally attributed to ...microbial reactions, particularly the involvement of sulfate-reducing bacteria (SRB) in sulfur reduction process. As a multivalent element, sulfur engages in complex bioreactions in both aerobic and anaerobic environments. Organic sulfides are also present in sewage, and these compounds possess the potential to undergo transformation and volatilization. In this paper, a comprehensive review was conducted on the present status regarding sulfur transformation, transportation, and remediation in sewers, including both inorganic and organic sulfur components. The review extensively addressed reactions occurring in the liquid and gas phase, as well as examined detection methods for various types of sulfur compounds and factors affecting sulfur transformation. Current remediation measures based on corresponding mechanisms were presented. Additionally, the impacts of measures implemented in sewers on the subsequent wastewater treatment plants were also discussed, aiming to attain better management of the entire wastewater system. Finally, challenges and prospects related to the issue of sulfur-containing substances in sewers were proposed to facilitate improved management and development of the urban water system.
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•Transformation and emission of inorganic and organic sulfur components in sewers is reviewed.•Various strategies for mitigating sulfur-containing pollutants are critically discussed.•The measures imposed in sewers to control sulfur-containing pollutants inevitably impact WWTPs.•Current knowledge gaps and perspectives for the control and management of sulfur-containing substances are highlighted.
Peptides are a particular molecule class with inherent attributes of some small-molecule drugs and macromolecular biologics, thereby inspiring continuous searches for peptides with therapeutic and/or ...agrochemical potentials. However, the success rate is decreasing, presumably because many interesting but less-abundant peptides are so scarce or labile that they are likely ‘overlooked’ during the characterization effort. Here, we present the biochemical characterization and druggability improvement of an unprecedented minor fungal RiPP (ribosomally synthesized and post-translationally modified peptide), named acalitide, by taking the relevant advantages of metabolomics approach and disulfide-bridged substructure which is more frequently imprinted in the marketed peptide drug molecules. Acalitide is biosynthetically unique in the macrotricyclization via two disulfide bridges and a protease (AcaB)-catalyzed lactamization of AcaA, an unprecedented precursor peptide. Such a biosynthetic logic was successfully re-edited for its sample supply renewal to facilitate the identification of the in vitro and in vivo antiparkinsonian efficacy of acalitide which was further confirmed safe and rendered brain-targetable by the liposome encapsulation strategy. Taken together, the work updates the mining strategy and biosynthetic complexity of RiPPs to unravel an antiparkinsonian drug candidate valuable for combating Parkinson's disease that is globally prevailing in an alarming manner.
Acalitide is an anti-parkinsonian minor fungal RiPP with its macrotricyclic molecular framework sculpted by the unique biosynthetic pathway which is re-edited for its sample supply renewal. Display omitted
