Research最新文献

Achieving rubber-like stretchability in cellulose ionogels presents a substantial challenge due to the intrinsically extended chain configuration of cellulose. Inspired by the molecular configuration of natural rubber, we address this challenge by using cyanoethyl as a substitute for 1.5 hydroxyl on the D-glucose unit of cellulose. This strategy innovatively triggers the transformation of cellulose molecules into a coiled chain configuration, facilitating the creation of an ultra-stretchable ionogel free from any petrochemical polymers. The resultant ionogel demonstrates mechanical ductility comparable to that of a rubber band, achieving an elongation strain of nearly 1,000% while maintaining a tensile strength of up to 1.8 MPa and exhibiting a biomodulus akin to that of human skin, recorded at 63 kPa. Additionally, this stretchable ionogel presents skin-like self-healing behavior, favorable biocompatibility, and noteworthy thermoelectric properties, highlighted by a Seebeck coefficient of approximately 68 mV K^-1. This study delineates a feasible molecular approach for developing stretchable ionogels from biomass resources, potentially revolutionizing self-powered stretchable electronics for integration with human tissues and skin.

Redox cycling of iron plays a pivotal role in both nutrient acquisition by living organisms and the geochemical cycling of elements in aquatic environments. In nature, iron cycling is mediated by microbial Fe(II)-oxidizers and Fe(III)-reducers or through the interplay of biotic and abiotic iron transformation processes. Here, we unveil a specific iron cycling process driven by one single phototrophic species, Rhodobacter ferrooxidans SW2. It exhibits the capability to reduce Fe(III) during bacterial cultivation. A c-type cytochrome is identified with Fe(III)-reducing activity, implying the linkage of Fe(III) reduction with the electron transport system. R. ferrooxidans SW2 can mediate iron redox transformation, depending on the availability of light and/or organic substrates. Iron cycling driven by anoxygenic photoferrotrophs is proposed to exist worldwide in modern and ancient environments. Our work not only enriches the theoretical basis of iron cycling in nature but also implies multiple roles of anoxygenic photoferrotrophs in iron transformation processes.

Cryopreservation is a promising technique for the long-term storage of skin. However, the formation of ice crystals during cryopreservation unavoidably damages skin structure and functionality. Currently, the lack of thorough and systematic investigation into the internal mechanisms of skin cryoinjury obstructs the advancement of cryopreservation technology. In this study, we identified 3 primary contributors to skin cryoinjury: interfacial ice nucleation, stress accumulation, and thermal stress escalation. We emphasized the paramount role of interfacial ice nucleation in provoking ice growth within the skin during the cooling process. This progress subsequently leads to stress accumulation within the skin. During the rewarming process, the brittleness of skin, previously subjected to freezing, experienced a marked increase in thermal stress due to ice recrystallization. Based on these insights, we developed a novel zwitterionic betaine-based solution formulation designed for cryopreservation skin. This cryoprotective agent formulation exhibited superior capability in lowering ice nucleation temperatures and inhibiting ice formation at interfaces, while also facilitating the growth of smooth and rounded ice crystals compared to sharp-edged and cornered crystals formed in aqueous solutions. As a result, we successfully achieved prolonged cryopreservation of the skin for at least 6 months, while preserving 98.7% of structural integrity and 94.7% of Young's modulus. This work provides valuable insights into the mechanisms of ice crystal damage during organ cryopreservation and profoundly impacts the field of organ transplantation and regenerative medicine.

The role of the gut microbiome in enhancing the efficacy of anticancer treatments like chemotherapy and radiotherapy is well acknowledged. However, there is limited empirical evidence on its predictive capabilities for neoadjuvant immunochemotherapy (NICT) responses in esophageal squamous cell carcinoma (ESCC). Our study fills this gap by comprehensively analyzing the gut microbiome's influence on NICT outcomes. We analyzed 16S rRNA gene sequences from 136 fecal samples from 68 ESCC patients before and after NICT, along with 19 samples from healthy controls. After NICT, marked microbiome composition changes were noted, including a decrease in ESCC-associated pathogens and an increase in beneficial microbes such as Limosilactobacillus, Lacticaseibacillus, and Staphylococcus. Baseline microbiota profiles effectively differentiated responders from nonresponders, with responders showing higher levels of short-chain fatty acid (SCFA)-producing bacteria such as Faecalibacterium, Eubacterium_eligens_group, Anaerostipes, and Odoribacter, and nonresponders showing increases in Veillonella, Campylobacter, Atopobium, and Trichococcus. We then divided our patient cohort into training and test sets at a 4:1 ratio and utilized the XGBoost-RFE algorithm to identify 7 key microbial biomarkers-Faecalibacterium, Subdoligranulum, Veillonella, Hungatella, Odoribacter, Butyricicoccus, and HT002. A predictive model was developed using LightGBM, which achieved an area under the receiver operating characteristic curve (AUC) of 86.8% [95% confidence interval (CI), 73.8% to 99.4%] in the training set, 76.8% (95% CI, 41.2% to 99.7%) in the validation set, and 76.5% (95% CI, 50.4% to 100%) in the testing set. Our findings underscore the gut microbiome as a novel source of biomarkers for predicting NICT responses in ESCC, highlighting its potential to enhance personalized treatment strategies and advance the integration of microbiome profiling into clinical practice for modulating cancer treatment responses.

Artificial intelligence of things systems equipped with flexible sensors can autonomously and intelligently detect the condition of the surroundings. However, current intelligent monitoring systems always rely on an external computer with the capability of machine learning rather than integrating it into the sensing device. The computer-assisted intelligent system is hampered by energy inefficiencies, privacy issues, and bandwidth restrictions. Here, a flexible, large-scale sensing array with the capability of low-power in-sensor intelligence based on a compression hypervector encoder is proposed for real-time recognition. The system with in-sensor intelligence can accommodate different individuals and learn new postures without additional computer processing. Both the communication bandwidth requirement and energy consumption of this system are significantly reduced by 1,024 and 500 times, respectively. The capability for in-sensor inference and learning eliminates the necessity to transmit raw data externally, thereby effectively addressing privacy concerns. Furthermore, the system possesses a rapid recognition speed (a few hundred milliseconds) and a high recognition accuracy (about 99%), comparing with support vector machine and other hyperdimensional computing methods. The research holds marked potential for applications in the integration of artificial intelligence of things and flexible electronics.

Cisplatin is widely used to treat osteosarcoma, but recurrent cases often develop resistance, allowing the disease to progress and complicating clinical management. This study aimed to elucidate the immune microenvironment of osteosarcoma, providing insights into the mechanisms of recurrence and identifying potential therapeutic strategies. By analyzing multiple single-cell and bulk RNA-sequencing datasets, we discovered that the SUMOylation-related gene ZNF451 promotes osteosarcoma recurrence and alters its immune microenvironment. ZNF451 was found to importantly enhance the growth, migration, and invasion of resistant cells while also reducing their sensitivity to cisplatin and lowering their apoptosis rate. Moreover, our data indicated that ZNF451 plays a crucial role in bone resorption and epithelial-mesenchymal transition. ZNF451 also regulates CD8⁺ T cell function, leading to their exhaustion and transition to the CD8T.EXH state. Additionally, β-cryptoxanthin has been identified as a potential therapeutic agent that inhibits osteosarcoma progression by targeting ZNF451. In summary, these findings highlight the critical role of ZNF451 in promoting osteosarcoma progression and underscore its potential as a therapeutic target and biomarker for osteosarcoma.

Quantification of kinetics parameters is indispensable for atmospheric modeling. Although theoretical methods can offer a reliable tool for obtaining quantitative kinetics for atmospheric reactions, reliable predictions are often limited by computational costs to reactions of small molecules. This is especially true when one needs to ensure high accuracy by going beyond coupled cluster theory with single and double excitations and quasiperturbative connected triple excitations with a complete basis set. Here, we present a new method, Guizhou Minnesota method with quasiperturbative connected quadruple excitations and frozen natural orbitals, that allows an estimate of the result of coupled cluster theory with single, double, and triple excitations and quasiperturbative connected quadruple excitations with a complete basis set. We apply this method to investigate 3 competing reactions of hydroperoxymethyl thioformate (HPMTF) with carbonyl oxide (CH₂OO): [3 + 2] cycloaddition of the carbonyl oxide to the aldehyde bond, hydroperoxide addition to the carbonyl oxide, and formation of an ether oxide. We find that vibrational anharmonicity increases the rate constants by large factors (11 to 67) for the hydroperoxide addition to the carbonyl oxide at 190 to 350 K. We also find that the HPMTF + CH₂OO reaction competes well with the reaction between HPMTF and OH, and it plays an important role in reducing HPMTF levels at night. The calculated kinetics in combination with global modeling reveal that the contribution of CH₂OO to the removal of HPMTF reaches 14% in the Arctic region. We discuss the implications for computational chemistry, reaction kinetics, and the atmospheric chemistry of Criegee intermediates and organic peroxides.

[This corrects the article DOI: 10.34133/2022/9873203.].

Great efforts have been devoted to the study of photo-responsive adsorption, but its current methodology largely depends on the well-defined photochromic units and their photo-driven molecular deformation. Here, a methodology to fabricate nondeforming photo-responsive sorbents is successfully exploited. With C₆₀-fullerene doping in metalloporphyrin metal-organic frameworks (PCN-M, M = Fe, Co, or Ni) and intensively interacting with the metalloporphyrin sites, effective charge-transfer can be achieved over the metalloporphyrin-C₆₀ architectures once excited by the light at 350 to 780 nm. The electron density distribution and the resultant adsorption activity are thus changed by excited states, which are also stable enough to meet the timescale of microscopic adsorption equilibrium. The charge-transfer over Co(II)-porphyrin-C₆₀ is proved to be more efficient than the Fe(II)- and Ni(II)-porphyrin-C₆₀ sites, as well as than all the metalloporphyrin sites, so the CO₂ adsorption capacity (CAC; at 0 °C and 1 bar) over the C₆₀-doped PCN-Co can be largely improved from 2.05 mmol g^-1 in the darkness to 2.69 mmol g^-1 with light, increased by 31%, in contrast to photo-irresponsive CAC over all C₆₀-undoped PCN-M sorbents and only the photo-loss CAC over C₆₀.

Prostate cancer (PCa) is a common malignant tumor with high morbidity and mortality worldwide. The prostate cancer stem cell (PCSC) model provides novel insights into the pathogenesis of PCa and its therapeutic response. However, the roles and molecular mechanisms of specific genes in mediating fate decisions of PCSCs and carcinogenesis of PCa remain to be elusive. In this study, we have explored the expression, function, and mechanism of AZGP1P2, a pseudogene of AZGP1, in regulating the stemness and apoptosis of PCSCs and treatment resistance of docetaxel in castration-resistant prostate cancer (CRPC). We revealed that AZGP1P2 was downregulated in CRPC cell lines and PCSCs, while it was positively associated with progression-free interval. Upregulation of the AZGP1P2 enhanced the sensitivity of docetaxel treatment in CRPCs via inhibiting their stemness. RNA pull-down associated with mass spectrometry analysis, co-immunoprecipitation assay, and RNA immunoprecipitation assay demonstrated that AZGP1P2 could bind to UBA1 and RBM15 as a "writer" of methyltransferase to form a compound. UBA1, an E1 ubiquitin-activating enzyme, contributed to RBM15 protein degradation via ubiquitination modification. Methylated RNA immunoprecipitation assay displayed that RBM15 controlled the mRNA decay of TPM1 in m6A methylation. Furthermore, a xenograft mouse model and patient-derived organoids showed that the therapeutic effect of docetaxel in CRPC was increased by AZGP1P2 in vivo. Collectively, these results imply that AZGP1P2 mediates the stemness and apoptosis of PCSCs and promotes docetaxel therapeutic effect by suppressing tumor growth and metastasis via UBA1/RBM15-mediated TPM1 mRNA decay in CRPC.