Alkanes are an abundant and valuable resource for transformation into value-added fine chemicals.However, selective functionalization of specific C(sp 3 )-H bonds in alkanes is a significant challenge, particularly for alkyl-alkyl bond formation, due to the small differences in reactivity between the various C(sp 3 )-H bonds in alkanes and their intrinsic inertness. Herein, we report a silver-catalyzed site-selective C(sp 3 )-H benzylation of simple alkanes using N-triftosylhydrazones as a convenient carbene precursor, which enables the synthesis of diverse array of alkylated aromatics. The reaction proceeds under mild conditions to afford high-value-added alkylarenes in generally high yields, with exquisite site selectivity and good functional group compatibility. A one-pot two-step protocol starting from aldehydes was also realized, thereby constituting a formal reductive alkylation of aryl aldehydes by alkanes. Experimental investigations and DFT calculations reveal that the role of the Tp Br3 Ag catalyst is threefold: it modulates the carbene reactivity, inhibits carbene dimerization, and avoids over-insertion of the product. All three aspects are crucial for the success of this first site-selective intermolecular insertion of donor carbenoids into C(sp 3 )-H bonds of simple alkanes. Methods Supporting InformationDetailed information about the experimental procedures as well as analytical data is provided in the Supplementary Information.
Revegetation has been the primary management approach for solving the problems caused by severe soil erosion in the Loess Plateau. The objectives of this work were to explore the successional trajectory of the different types of restoration and discuss their potential effectiveness for the control of soil erosion. The presence and coverage of plants in 40 permanent plots were investigated during two periods (2003-2006 and 2013). The naturally and artificially revegetated communities studied in the two surveys were classified using two-way indicator species analysis, and their relationships were analyzed using detrended correspondence analysis. Under natural revegetation, the communities succeed in the following order: annual plants → perennial plants → short rhizome tufts and subshrubs. Under artificial revegetation, succession was interrupted by artificial planting, and a Gramineae herb layer persisted through the years with few changes in species composition. Additionally, species richness, diversity, and evenness increased, while ecological dominance decreased during succession in both revegetation types. Succession rate was rapid at the initial stage and then slowed down gradually. Succession followed different trajectories under natural and artificial revegetation, and based on the potential effects of the two approaches on soil erosion and soil desiccation, we suggest that natural revegetation is preferable over artificial revegetation. Figure 7. Changes in relative species cover between the first and second surveys in different natural revegetation communities. This figure is available in colour online at wileyonlinelibrary.com/journal/ldr 926 M. KOU ET AL.
The insertion of carbenes into the α-C–H bonds of ethers represents one of the most powerful approaches to access polysubstituted α-branched ethers. However, intermolecular carbene insertions remain challenging, since current approaches are generally limited to the use of toxic and potentially explosive α-diazocarbonyl compounds. We now report a silver-catalyzed α-C–H benzylation of ethers using bench-stable N-triftosylhydrazones as safe and convenient carbene precursors. This approach is well suited for both inter- and intramolecular insertions to deliver medicinally relevant homobenzylic ethers and 5–8-membered oxacycles in good yields. The synthetic utility of this strategy is demonstrated by its easy scalability, broad scope with valuable functional groups, high regioselectivity, and late-stage functionalization of complex oxygen-containing molecules. The relative reactivities of different types of silver carbenes and C−H bonds were also investigated by experments and DFT calculations.
Gully erosion is a serious environmental problem worldwide, causing soil loss, land degradation, silting up of reservoirs and even catastrophic flooding. Mapping gully features from remote sensing imagery is crucial for assisting in understanding gully erosion mechanisms, predicting its development processes and assessing its environmental and socio-economic effects over large areas, especially under the increasing global climate extremes and intensive human activities. However, the potential of using increasingly available high-resolution remote sensing imagery to detect and delineate gullies has been less evaluated. Hence, 130 gullies occurred along a transect were selected from a typical watershed in the hilly and gully region of the Chinese Loess Plateau, and visually interpreted from a Pleiades-1B satellite image (panchromatic-sharpened image at 0.5 m resolution fused with 2.0 m multi-spectral bands). The interpreted gullies were compared with their measured data obtained in the field using a differential global positioning system (GPS). Results showed that gullies could generally be accurately interpreted from the image, with an average relative error of gully area and gully perimeter being 11.1% and 8.9%, respectively, and 74.2% and 82.3% of the relative errors for gully area and gully perimeter were within 15%. But involving field measurements of gullies in present imagery-based gully studies is still recommended. To judge whether gullies were mapped accurately further, a standard adopting one-pixel tolerance along the mapped gully edges was proposed and proved to be practical. Correlation analysis indicated that larger gullies could be interpreted more accurately but increasing gully shape complexity would decrease interpreting accuracy. Overall lower vegetation coverage in winter due to the withering and falling of vegetation rarely affected gully interpreting. Furthermore, gully detectability on remote sensing imagery in this region was lower than the other places of the world, due to the overall broken topography in the Loess Plateau, thus images with higher resolution than normally perceived are needed when mapping erosion features here. Taking these influencing factors (gully dimension and shape complexity, vegetation coverage, topography) into account will be favorable to select appropriate imagery and gullies (as study objects) in future imagery-based gully studies. Finally, two linear regression models were built to correct gully area (Aip, m2) and gully perimeter (Pip, m) visually extracted, by connecting them with the measured area (Ams, m2) and perimeter (Pms, m). The correction models were Ams=1.021Aip+0.139 and Pms=0.949Pip+ 0.722, respectively. These models could be helpful for improving the accuracy of interpreting results, and further accurately estimating gully development and developing more effective automated gully extraction methods on the Loess Plateau of China.
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