155 research outputs found

    Donor–Acceptor Fluorophores for Energy-Transfer-Mediated Photocatalysis

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    Triplet–triplet energy transfer (EnT) is a fundamental activation pathway in photocatalysis. In this work, we report the mechanistic origins of the triplet excited state of carbazole-cyanobenzene donor–acceptor (D–A) fluorophores in EnT-based photocatalytic reactions and demonstrate the key factors that control the accessibility of the 3LE (locally excited triplet state) and 3CT (charge-transfer triplet state) via a combined photochemical and transient absorption spectroscopic study. We found that the energy order between 1CT (charge transfer singlet state) and 3LE dictates the accessibility of 3LE/3CT for EnT, which can be effectively engineered by varying solvent polarity and D–A character to depopulate 3LE and facilitate EnT from the chemically more tunable 3CT state for photosensitization. Following the above design principle, a new D–A fluorophore with strong D–A character and weak redox potential is identified, which exhibits high efficiency for Ni(II)-catalyzed cross-coupling of carboxylic acids and aryl halides with a wide substrate scope and high selectivity. Our results not only provide key fundamental insight on the EnT mechanism of D–A fluorophores but also establish its wide utility in EnT-mediated photocatalytic reactions

    Digital Closed-Loop Driving Technique Using the PFD-Based CORDIC Algorithm for a Biaxial Resonant Microaccelerometer

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    A digital closed-loop driving technique is presented in this paper that uses the PFD- (phase frequency detector-) based CORDIC (coordinate rotation digital computer) algorithm for a biaxial resonant microaccelerometer. A conventional digital closed-loop self-oscillation system based on the CORDIC algorithm is implemented and simulated using Simulink software to verify the system performance. The system performance simulations reveal that the incompatibility between the sampling frequency and effective bits of AD and DA convertors limits further performance improvements. Therefore, digital, closed-loop self-oscillation using the PFD-based CORDIC algorithm is designed to further optimize the system performance. The system experimental results illustrate that the optimized system using the PFD-based CORDIC improves the bias stability of the resonant microaccelerometer by more than 5.320 times compared to the conventional system. This demonstrates that the optimized digital closed-loop driving technique using the PFD-based CORDIC for the biaxial resonant microaccelerometer is effective

    A multi-scale mapping approach based on a deep learning CNN model for reconstructing high-resolution urban DEMs

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    The scarcity of high-resolution urban digital elevation model (DEM) datasets, particularly in certain developing countries, has posed a challenge for many water-related applications such as flood risk management. A solution to address this is to develop effective approaches to reconstruct high-resolution DEMs from their low-resolution equivalents that are more widely available. However, the current high-resolution DEM reconstruction approaches mainly focus on natural topography. Few attempts have been made for urban topography, which is typically an integration of complex artificial and natural features. This study proposed a novel multi-scale mapping approach based on convolutional neural network (CNN) to deal with the complex features of urban topography and to reconstruct high-resolution urban DEMs. The proposed multi-scale CNN model was firstly trained using urban DEMs that contained topographic features at different resolutions, and then used to reconstruct the urban DEM at a specified (high) resolution from a low-resolution equivalent. A two-level accuracy assessment approach was also designed to evaluate the performance of the proposed urban DEM reconstruction method, in terms of numerical accuracy and morphological accuracy. The proposed DEM reconstruction approach was applied to a 121 km2 urbanized area in London, United Kingdom. Compared with other commonly used methods, the current CNN-based approach produced superior results, providing a cost-effective innovative method to acquire high-resolution DEMs in other data-scarce regions

    Selective Excited-State Dynamics in a Unique Set of Rationally Designed Ni Porphyrins

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    In this work, we report the design and photophysical properties of a unique class of Ni porphyrins, in which the tert-butyl benzene substituents at the meso positions of the macrocycle were tethered by ethers with alkyl linkers. This not only results in the permanently locked ruf distortion of the macrocycle but also enables the engineering of the degree of distortion through varying the length of alkyl linkers, which addressed the complication of uncertainty in the specific structural distortions that has long plagued the porphyrin photophysical community. Using advanced time-resolved optical and X-ray absorption spectroscopy, we observed tunability in the excited-state relaxation pathway depending on the degree of distortion and characterized the associated transient intermediate structure. These findings provide a new avenue to afford accessibility to a wide range of excited-state properties in nonplanar porphyrins

    Assessing the Carbon Emission Driven by the Consumption of Carbohydrate-Rich Foods: The Case of China

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    peer-reviewedBackground: Carbohydrate-rich (CR) foods are essential parts of the Chinese diet. However, CR foods are often given less attention than animal-based foods. The objectives of this study were to analyze the carbon emissions caused by CR foods and to generate sustainable diets with low climate impact and adequate nutrients. Methods: Twelve common CR food consumption records from 4857 individuals were analyzed using K-means clustering algorithms. Furthermore, linear programming was used to generate optimized diets. Results: Total carbon emissions by CR foods was 683.38g CO2eq per day per capita, accounting for an annual total of 341.9Mt CO2eq. All individuals were ultimately divided into eight clusters, and none of the popular clusters were low carbon or nutrient sufficient. Optimized diets could reduce about 40% of carbon emissions compared to the average current diet. However, significant structural differences exist between the current diet and optimized diets. Conclusions: To reduce carbon emissions from the food chain, CR foods should be a research focus. Current Chinese diets need a big change to achieve positive environmental and health goals. The reduction of rice and wheat-based foods and an increase of bean foods were the focus of structural dietary change in CR food consumption.Natural Science Foundation of Guangdong Provinc

    Higher Dietary Se Intake Is Associated With the Risk of New-Onset Fracture: A National Longitudinal Study for 20 Years

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    Background: The association between dietary selenium (Se) intake and osteoporosis-related fractures remains inconsistent. We aimed to examine the dose relationship between Se intake and incident fracture among Chinese adults. Methods: The dietary data were retrieved from the China Health and Nutrition Survey conducted between 1991 and 2011, and 17,150 participants aged above 20 were included. A 3-day, 24-h recall of food intake was performed to assess cumulative average dietary Se intake. The fracture was based on self-report in each survey between 1997 and 2011. The association between Se intake and fracture was tested by Cox regression, and the non-linear association was examined by restricted cubic splines (RCS). Results: There were 976 fracture cases during a mean of 10.2 years follow-up. In a fully adjusted Cox model, across the quartiles of Se intake, the hazard ratios (HRs) for fracture were 1.07 (95% CI .86–1.33), 1 (reference), 1.25 (95% CI 1.02–1.53), and 1.33 (95% CI 1.07–1.65). RCS showed a parabolic association (P non-linear = 0.037) between Se and fracture for men as well as a U-shape dose-response (P non-linear = 0.04) between Se and fracture for subjects living in highly urbanized areas. Conclusion: In conclusion, there is a non-linear association between selenium intake and fracture, with higher intake associated with increased risk. The shape of the association varies by gender and urbanization level

    Frequent alterations in cytoskeleton remodelling genes in primary and metastatic lung adenocarcinomas

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    The landscape of genetic alterations in lung adenocarcinoma derived from Asian patients is largely uncharacterized. Here we present an integrated genomic and transcriptomic analysis of 335 primary lung adenocarcinomas and 35 corresponding lymph node metastases from Chinese patients. Altogether 13 significantly mutated genes are identified, including the most commonly mutated gene TP53 and novel mutation targets such as RHPN2, GLI3 and MRC2. TP53 mutations are furthermore significantly enriched in tumours from patients harbouring metastases. Genes regulating cytoskeleton remodelling processes are also frequently altered, especially in metastatic samples, of which the high expression level of IQGAP3 is identified as a marker for poor prognosis. Our study represents the first large-scale sequencing effort on lung adenocarcinoma in Asian patients and provides a comprehensive mutational landscape for both primary and metastatic tumours. This may thus form a basis for personalized medical care and shed light on the molecular pathogenesis of metastatic lung adenocarcinoma
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