The reductive cross-coupling of sp3-hybridized carbon centers represents great synthetic values and insurmountable challenges. In this work, we report a nickel-catalyzed deaminative cross-electrophile coupling reaction to construct C(sp)─C(sp3), C(sp2)─C(sp3), and C(sp3)─C(sp3) bonds. A wide range of coupling partners including aryl iodides, bromoalkynes, or alkyl bromides are stitched with alkylpyridinium salts that derived from the corresponding primary amines. The advantages of this methodology are showcased in the two-step synthesis of the key lactonic moiety of (+)-compactin and (+)-mevinolin. The one-pot procedure without isolation of alkylpyridinium tetrafluoroborate salt is also proven to be successful. This cross-coupling strategy of two electrophiles provides a highly valuable vista for the convenient installation of alkyl substituents and late functionalizations of sp3 carbons.
Electrosynthesis has received great attention among researchers in both academia and industry as an ideal technique to promote single electron reduction without the use of expensive catalysts. In this work, we report the electrochemical reduction of Katritzky salts to alkyl radicals by sacrificing the easily accessible metal anode. This catalyst and electrolyte free platform has broad applicability to single electron transfer chemistry, including fluoroalkenylation, alkynylation and thiolation. The deaminative functionalization is facilitated by the rapid molecular diffusion across microfluidic channels, demonstrating the practicality that outpaces the conventional electrochemistry setups.
Owing to the innovative applications of fluorinated compounds in many areas of technology and medicine, methods for the preparation of C-F quaternary fluorine containing compounds are in extremely high demand. Here, we report the discovery of a general procedure for an S 2 reaction catalyzed by Pd/Ding-SKP-type ligands, and that occurs between Colby pro-enolates with MBH carbonates to afford the corresponding products featuring two consecutive stereogenic carbons, including a C-F quaternary stereogenic center. The reactions readily occur at ambient temperatures with high chemical yields and in excellent chemo-, diastereo- and enantioselective manners. This practically attractive stereochemical outcome, coupled with the operational simplicity and structural generality, bodes well for the synthetic application of this process in the preparation of a novel class of biologically relevant fluorine-containing compounds.
This work describes a strategy to utilise uranyl for direct alkynylation and olefination of amides. Uranyl cation (UO22+) has been identified as highly oxidizing agent to abstract hydrogen atoms from...
Spaceborne polarimetric synthetic aperture radar interferometry (PolInSAR) has the potential to deal with large-scale forest height inversion. However, the inversion is influenced by strong temporal decorrelation interference resulting from a large temporal baseline. Additionally, the forest canopy induces phase errors, while the smaller vertical wavenumber (kz) enhances the sensitivity of the inversion to temporal decorrelation, which limits the efficiency in forest height inversion. This research is based on the random volume over ground (RVoG) model and follows the assumptions of the three-stage inversion method, to quantify the impact of repeat-pass spaceborne PolInSAR temporal decorrelation on the relative error of retrieval height, and develop a semi-empirical improved inversion model, using ground data to eliminate the interference of coherence and phase error caused by temporal decorrelation. Forest height inversion for temperate forest in northern China was conducted using repeat-pass spaceborne L-band ALOS2 PALSAR data, and was further verified using ground measurement data. The correction of temporal decorrelation using the improved model provided robust inversion for mixed conifer-broad forest height retrieval as it addressed the over-sensitivity to temporal decorrelation resulting from the inappropriate kz value. The method performed height inversion using interferometric data with temporal baselines ranging from 14 to 70 days and vertical wavenumbers ranging from 0.015 to 0.021 rad/m. The R2 and RMSE reached 0.8126 and 2.3125 m, respectively.
In the analysis of ECG data, it is necessary to first automatically classify the quality of ECG data to facilitate the subsequent processing. PhysioNet/Computing in Cardiology Challenge 2011 and existing researches involve the quality of the entire record of ECG, which fails to maximize utilization of ECG data. In fact, single-lead ECG has been widely used in many fields, such as wearable devices, sleep apnea monitoring, and deriving respiratory rate. However, the present methods for evaluating the data quality by each channel only divide them into two categories: acceptable and unacceptable, which is relatively coarse. This paper proposes a new method for the automatic classification of ECG data quality by channel. This method divides them into four categories: (1) electrode shedding, marked as C3; (2) serious noise interference, under which it is difficult to detect R wave, marked as C2; (3) partial noise interference, under which part of R waves may not be detected correctly, marked as C1; (4) high quality signal, marked as C0. The 2011 competition data was re-marked according to the channel with the help of our designed auxiliary program. This paper defined some features and designed a tree classifier using One-Class Support Vector Machine(OCSVM). The test results of our method show that the detection accuracy of electrode shedding is 93.22%, serious noise interference is 90%, partial noise interference is 89.22%, and high quality signal is 97.19%. It shows that the method has a broad prospect in the automatic preprocessing of ECG data.
SAR data have a longer wavelength and stronger penetrating power compared with traditional optical remote sensing. Therefore, SAR data are more suitable for the estimation of the above-ground biomass (AGB) of forests. This study was aimed at evaluating the sensitivity of L-band full polarization data to AGB. L-band data were improved to estimate the saturation point produced by AGB, and were found to be suitable for estimating a wide range of AGB. This study extracted backscattering coefficients, polarization decomposition variables, and terrain factors. New parameters were constructed from these variables, and their performance in predicting AGB was evaluated. Significant variables found with AGB were added to the multivariate linear model. A statistical analysis showed the presence of multicollinearity between the variables. Therefore, ridge regression, random forest method (RF), and principal component analysis (PCA) were introduced to solve the problem of collinearity. In all the three methods, the saturation of the ridge regression model was low, reaching it at 150 t/ha. Better accuracy was obtained with the RF model. No obvious saturation incident was detected in the model established using the principal component analysis. This could be attributed to the low biomass levels observed in our study area. This model provided accurate results (adjusted r2 = 0.90 rmse = 14.24 t/ha), indicating that L-band data have the potential to estimate AGB. Additionally, suitable variables and models were selected in this study, with the principal component analysis being more helpful in combining various SAR parameters. The achievement of these accurate results could be attributed to the synergy among variables.
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