Auto-accelerated dehydrogenation of alkane assisted by in-situ formed olefins over boron nitride under aerobic conditions

被引:19
作者
Liu, Zhankai [1 ]
Liu, Ziyi [1 ]
Fan, Jie [1 ]
Lu, Wen-Duo [1 ]
Wu, Fan [1 ]
Gao, Bin [1 ]
Sheng, Jian [1 ]
Qiu, Bin [1 ]
Wang, Dongqi [1 ]
Lu, An-Hui [1 ]
机构
[1] Dalian Univ Technol, Sch Chem Engn, State Key Lab Fine Chem, Liaoning Key Lab Catalyt Convers Carbon Resources, Dalian 116024, Liaoning, Peoples R China
基金
中国国家自然科学基金;
关键词
SELECTIVE OXIDATIVE DEHYDROGENATION; GAS-PHASE REACTION; LIGHT ALKANES; PROPANE DEHYDROGENATION; CATALYSTS; PROPYLENE; OXIDE;
D O I
10.1038/s41467-022-35776-3
中图分类号
O [数理科学和化学]; P [天文学、地球科学]; Q [生物科学]; N [自然科学总论];
学科分类号
07 ; 0710 ; 09 ;
摘要
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. Oxidative dehydrogenation of alkanes over boron nitride catalysts provides a new opportunity for efficient olefin production. Here, the authors discover in situ formed olefins can promote parent alkane conversion, and achieve activation of ethane by propane-derived olefins at a lower temperature.
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收藏
页数:9
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