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Oxidative Dehydrogenation on Nanocarbon: Revealing the Catalytic Mechanism using Model Catalysts
Guo, Xiaoling; Qi, Wei; Liu, Wei; Yan, Pengqiang; Li, Fan; Liang, Changhai; Su, Dangsheng; Qi, W; Su, DS (reprint author), Chinese Acad Sci, Shenyang Natl Lab Mat Sci, Inst Met Res, Shenyang 110016, Peoples R China.
2017-02-01
发表期刊ACS CATALYSIS
ISSN2155-5435
卷号7期号:2页码:1424-1427
摘要Model catalysts offer a direct method to determine the active-site structures and mechanisms on nanocarbon catalysts. In this report, we show that the ketonic carbonyl groups are the catalytic center of the nanocarbon-catalyzed alkane oxidative dehydrogenation (ODH) reaction, and we reveal the catalytic mechanism using conjugated polymeric model catalysts containing only ketonic carbonyl groups. An in situ infrared (IR) analysis provides spectroscopic evidence of the "working" configurations of the active sites in association with the redox cycle of the ketonic carbonyl-hydroxyl pairs. Carbonyl reduction (H abstraction from hydrocarbon) is shown to be a kinetically relevant step. An O-18 isotope tracer experiment further shows that the activation and exchange of molecular oxygen at the surface active sites are fast processes under common reaction conditions.; Model catalysts offer a direct method to determine the active-site structures and mechanisms on nanocarbon catalysts. In this report, we show that the ketonic carbonyl groups are the catalytic center of the nanocarbon-catalyzed alkane oxidative dehydrogenation (ODH) reaction, and we reveal the catalytic mechanism using conjugated polymeric model catalysts containing only ketonic carbonyl groups. An in situ infrared (IR) analysis provides spectroscopic evidence of the "working" configurations of the active sites in association with the redox cycle of the ketonic carbonyl-hydroxyl pairs. Carbonyl reduction (H abstraction from hydrocarbon) is shown to be a kinetically relevant step. An O-18 isotope tracer experiment further shows that the activation and exchange of molecular oxygen at the surface active sites are fast processes under common reaction conditions.
部门归属[guo, xiaoling ; liang, changhai] dalian univ technol, sch chem engn, lab adv mat & catalyt engn, dalian 116023, peoples r china ; [guo, xiaoling ; qi, wei ; liu, wei ; yan, pengqiang ; li, fan ; su, dangsheng] chinese acad sci, shenyang natl lab mat sci, inst met res, shenyang 110016, peoples r china
关键词Heterogeneous Catalysis Carbon Catalysis Alkane Oxidative Dehydrogenation Model Catalysts Kinetics
学科领域Chemistry, Physical
资助者NSFC [21573256, 91645114, 2161101164, 21303226, 51521091]; Joint Research Program of Natural Science Foundation of Liaoning Province-Shenyang National Laboratory for Materials Science [2015021010]; Youth Innovation Promotion Association, CAS
收录类别SCI
语种英语
文献类型期刊论文
条目标识符http://ir.imr.ac.cn/handle/321006/78320
专题中国科学院金属研究所
通讯作者Qi, W; Su, DS (reprint author), Chinese Acad Sci, Shenyang Natl Lab Mat Sci, Inst Met Res, Shenyang 110016, Peoples R China.
推荐引用方式
GB/T 7714
Guo, Xiaoling,Qi, Wei,Liu, Wei,et al. Oxidative Dehydrogenation on Nanocarbon: Revealing the Catalytic Mechanism using Model Catalysts[J]. ACS CATALYSIS,2017,7(2):1424-1427.
APA Guo, Xiaoling.,Qi, Wei.,Liu, Wei.,Yan, Pengqiang.,Li, Fan.,...&Su, DS .(2017).Oxidative Dehydrogenation on Nanocarbon: Revealing the Catalytic Mechanism using Model Catalysts.ACS CATALYSIS,7(2),1424-1427.
MLA Guo, Xiaoling,et al."Oxidative Dehydrogenation on Nanocarbon: Revealing the Catalytic Mechanism using Model Catalysts".ACS CATALYSIS 7.2(2017):1424-1427.
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