166 research outputs found

    Direct structural identification of carbenium ions and investigation of host-guest interaction in the methanol to olefins reaction obtained by multinuclear NMR correlations

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    Probing and determining the intermediates formed during catalytic reactions in heterogeneous catalysis are strong challenges. Using C-13 labelling and two dimensional C-13-C-13 through-bond NMR correlations, we directly reveal the structures of a range of carbenium ion species formed during the conversion of methanol to olefins on acidic H-ZSM-5 zeolite by mapping the carbon-carbon bond connectivities. Additionally, we use C-13-Al-27 and Si-29-C-13 through-space NMR experiments to probe the interactions between the confined carbon species (including carbenium ions) and the framework of the zeolite, which quantitatively provide an estimate for the carbon-aluminium and carbon-silicon distances, respectively

    Individual tree-based forest species diversity estimation by classification and clustering methods using UAV data

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    Monitoring forest species diversity is essential for biodiversity conservation and ecological management. Currently, unmanned aerial vehicle (UAV) remote sensing technology has been increasingly used in biodiversity monitoring due to its flexibility and low cost. In this study, we compared two methods for estimating forest species diversity indices, namely the spectral angle mapper (SAM) classification approach based on the established species-spectral library, and the self-adaptive Fuzzy C-Means (FCM) clustering algorithm by selected biochemical and structural features. We conducted this study in two complex subtropical forest areas, Mazongling (MZL) and Gonggashan (GGS) National Nature Forest Reserves using UAV-borne hyperspectral and LiDAR data. The results showed that the classification method performed better with higher values of R2 than the clustering algorithm for predicting both species richness (0.62 > 0.46 for MZL and 0.55 > 0.46 for GGS) and Shannon-Wiener index (0.64 > 0.58 for MZL, 0.52 > 0.47 for GGS). However, the Simpson index estimated by the classification method correlated less with the field measurements than the clustering algorithm (R2 = 0.44 and 0.83 for MZL and R2 = 0.44 and 0.62 for GGS). Our study demonstrated that the classification method could provide more accurate monitoring of forest diversity indices but requires spectral information of all dominant tree species at individual canopy scale. By comparison, the clustering method might introduce uncertainties due to the amounts of biochemical and structural inputs derived from the hyperspectral and LiDAR data, but it could acquire forest diversity patterns rapidly without distinguishing the specific tree species. Our findings underlined the advantages of UAV remote sensing for monitoring the species diversity in complex forest ecosystems and discussed the applicability of classification and clustering methods for estimating different individual tree-based species diversity indices

    Correction of UAV LiDAR-derived grassland canopy height based on scan angle

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    Grassland canopy height is a crucial trait for indicating functional diversity or monitoring species diversity. Compared with traditional field sampling, light detection and ranging (LiDAR) provides new technology for mapping the regional grassland canopy height in a time-saving and cost-effective way. However, the grassland canopy height based on unmanned aerial vehicle (UAV) LiDAR is usually underestimated with height information loss due to the complex structure of grassland and the relatively small size of individual plants. We developed canopy height correction methods based on scan angle to improve the accuracy of height estimation by compensating the loss of grassland height. Our method established the relationships between scan angle and two height loss indicators (height loss and height loss ratio) using the ground-measured canopy height of sample plots with 1×1m and LiDAR-derived heigh. We found that the height loss ratio considering the plant own height had a better performance (R2 = 0.71). We further compared the relationships between scan angle and height loss ratio according to holistic (25–65cm) and segmented (25–40cm, 40–50cm and 50–65cm) height ranges, and applied to correct the estimated grassland canopy height, respectively. Our results showed that the accuracy of grassland height estimation based on UAV LiDAR was significantly improved with R2 from 0.23 to 0.68 for holistic correction and from 0.23 to 0.82 for segmented correction. We highlight the importance of considering the effects of scan angle in LiDAR data preprocessing for estimating grassland canopy height with high accuracy, which also help for monitoring height-related grassland structural and functional parameters by remote sensing

    Fast detection and structural identification of carbocations on zeolites by dynamic nuclear polarization enhanced solid-state NMR

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    Acidic zeolites are porous aluminosilicates used in a wide range of industrial processes such as adsorption and catalysis. The formation of carbocation intermediates plays a key role in reactivity, selectivity and deactivation in heterogeneous catalytic processes. However, the observation and determination of carbocations remain a significant challenge in heterogeneous catalysis due to the lack of selective techniques of sufficient sensitivity to detect their low concentrations. Here, we combine 13C isotopic enrichment and efficient dynamic nuclear polarization magic angle spinning nuclear magnetic resonance spectroscopy to detect carbocations in zeolites. We use two dimensional 13C–13C through-bond correlations to establish their structures and 29Si–13C through-space experiments to quantitatively probe the interaction between multiple surface sites of the zeolites and the confined hydrocarbon pool species. We show that a range of various membered ring carbocations are intermediates in the methanol to hydrocarbons reaction catalysed by different microstructural β-zeolites and highlight that different reaction routes for the formation of both targeted hydrocarbon products and coke exist. These species have strong van der Waals interaction with the zeolite framework demonstrating that their accumulation in the channels of the zeolites leads to deactivation. These results enable understanding of deactivation pathways and open up opportunities for the design of catalysts with improved performances
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