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用于丙烷氧化脱氢的等离子体调节六方氮化硼的局部环境

Plasma Tuning Local Environment of Hexagonal Boron Nitride for Oxidative Dehydrogenation of Propane.

作者信息

Liu Zhankai, Yan Bing, Meng Shengyan, Liu Rui, Lu Wen-Duo, Sheng Jian, Yi Yanhui, Lu An-Hui

机构信息

State Key Laboratory of Fine Chemicals, Liaoning Key Laboratory for Catalytic Conversion of Carbon Resources, School of Chemical Engineering, Dalian University of Technology, Dalian, 116024, Liaoning, China.

出版信息

Angew Chem Int Ed Engl. 2021 Sep 1;60(36):19691-19695. doi: 10.1002/anie.202106713. Epub 2021 Aug 1.

Abstract

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 , O , H , Ar) were accordingly employed to regulate the local chemical environment of h-BN. N -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 "BO " species in O -treated BN, led to the suppressed catalytic performance (12.4 % conversion at 520 °C).

摘要

六方氮化硼(h-BN)因其在丙烷氧化脱氢(ODH)制丙烯反应中相对于金属氧化物具有非凡的烯烃选择性,近来受到了极大关注。然而,商业h-BN的高结晶度以及对活性位点难以捉摸的认识阻碍了其利用效率的提高。在此,相应地采用了四种等离子体(N、O、H、Ar)来调节h-BN的局部化学环境。经N处理的BN表现出显著的活性,即在520°C下丙烷转化率为26.0%,对烯烃的选择性为89.4%。光谱表明,催化剂中的“三硼中心”N缺陷在促进丙烷转化中起关键作用。而经O处理的BN中“BO”物种的烧结效应导致催化性能受到抑制(520°C下转化率为12.4%)。

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