Hexagonal boron nitride (h-BN) has lately received great attention in the oxidative dehydrogenation (ODH) reaction of propane to propylene for its extraordinary olefin selectivity in contrast to metal oxides. However, high crystallinity of commercial h-BN and elusive cognition of active sites hindered the enhancement of utilization efficiency. Herein, four kinds of plasmas (N 2 , O 2 , H 2 , Ar) were accordingly employed to regulate the local chemical environment of h-BN. N 2 -treated BN exhibited a remarkable activity, i.e., 26.0 % propane conversion with 89.4 % selectivity toward olefins at 520 8C. Spectroscopy demonstrated that "three-boron center" N-defects in the catalyst played a pivotal role in facilitating the conversion of propane. While the sintering effect of the "BO x " species in O 2 -treated BN, led to the suppressed catalytic performance (12.4 % conversion at 520 8C).
Oxidative dehydrogenation (ODH) of alkane over boron nitride (BN) catalyst exhibits high olefin selectivity as well as a small ecological carbon footprint. Here we report an unusual phenomenon that the in-situ formed olefins under reactions are in turn actively accelerating parent alkane conversion over BN by interacting with hydroperoxyl and alkoxyl radicals and generating reactive species which promote oxidation of alkane and olefin formation, through feeding a mixture of alkane and olefin and DFT calculations. The isotope tracer studies reveal the cleavage of C-C bond in propylene when co-existing with propane, directly evidencing the deep-oxidation of olefins occur in the ODH reaction over BN. Furthermore, enhancing the activation of ethane by the in-situ formed olefins from propane is successfully realized at lower temperature by co-feeding alkane mixture strategy. This work unveils the realistic ODH reaction pathway over BN and provides an insight into efficiently producing olefins.
Boron-containing zeolites have been demonstrated as active catalysts for oxidative dehydrogenation of propane (ODHP) to propene. The challenge is that the origin of the boron active sites remains an unsolved issue. In this study, selfpillared boron-containing MFI zeolite nanosheets with an ultrathin b-axis were synthesized, which exhibited low-temperature activity and stability in the ODHP process. A combination of in situ diffuse reflectance infrared Fourier transform, twodimensional 11 B multiple-quantum MAS NMR, and 11 B{ 1 H} dipolar-heteronuclear multiple-quantum correlation NMR measurements revealed that the MFI zeolite nanosheets with the characteristics of a high specific surface area and abundant Si− OH groups allowed dynamic self-dispersion of highly mobile boron clusters through condensation with surrounding Si−OH groups. The increased number of stable and dispersed oligomeric boron species was responsible for the enhanced catalytic performance and stability in the ODHP process. The catalysts were active at a temperature as low as 390 °C. Upon raising the temperature to 430 °C, a propane conversion of 14.1% could be achieved together with a selectivity of 80.1% toward all olefins.
Hexagonal boron nitride (h‐BN) has lately received great attention in the oxidative dehydrogenation (ODH) reaction of propane to propylene for its extraordinary olefin selectivity in contrast to metal oxides. However, high crystallinity of commercial h‐BN and elusive cognition of active sites hindered the enhancement of utilization efficiency. Herein, four kinds of plasmas (N2, O2, H2, Ar) were accordingly employed to regulate the local chemical environment of h‐BN. N2‐treated BN exhibited a remarkable activity, i.e., 26.0 % propane conversion with 89.4 % selectivity toward olefins at 520 °C. Spectroscopy demonstrated that “three‐boron center” N‐defects in the catalyst played a pivotal role in facilitating the conversion of propane. While the sintering effect of the “BOx” species in O2‐treated BN, led to the suppressed catalytic performance (12.4 % conversion at 520 °C).
Recently, indocyanine green (ICG), as an FDA-approved dye, has been widely used for phototherapy. It is essential to obtain information on the migration and aggregation of ICG in deep tissues. However, existing fluorescence imaging platforms are not able to obtain the structural information of the tissues. Here, we prepared ICG liposomes (ICG-Lips) and built a dual-wavelength photoacoustic computed tomography (PACT) system with piezoelectric ring-array transducer to image the aggregation of ICG-Lips in tumors to guide phototherapy. Visible 780 nm light excited the photoacoustic (PA) effects of the ICG-Lips and near-infrared 1064 nm light provided the imaging of the surrounding tissues. The aggregation of ICG-Lips within the tumor and the surrounding tissues was visualized by PACT in real time. This work indicates that PACT with piezoelectric ring-array transducer has great potential in the real-time monitoring of in vivo drug distribution.
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