Facile Dehydrogenation of Ethane on the IrO(110) Surface.
Realizing the efficient and selective conversion of ethane to ethylene is important for improving the utilization of hydrocarbon resources, yet remains a major challenge in catalysis. Herein, ethane dehydrogenation on the IrO(110) surface is investigated using temperature-programmed reaction spectro...
| Publicado en: | Journal of the American Chemical Society Vol. 140; no. 7; pp. 2665 - 2673 |
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| Autores principales: | , , , , |
| Formato: | Artículo |
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American Chemical Society
2/21/2018
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| Acceso en línea: | Ver este registro en EBSCOhost |
| fields | @attributes: recordID: 1 pdfLink: plink: https://search.ebscohost.com/login.aspx?direct=true&db=hlh&AN=128201146&site=ehost-live header: @attributes: shortDbName: hlh uiTerm: 128201146 longDbName: Humanities International Complete uiTag: AN controlInfo: bkinfo: jinfo: jid: 00027863 ACS jtl: Journal of the American Chemical Society issn: 00027863 maglogo: N pubinfo: dt: 2/21/2018 vid: 140 iid: 7 pid: 997 pub: American Chemical Society artinfo: ui: 128201146 10.1021/jacs.7b13599 ppf: 2665 ppct: 8 formats: tig: atl: Facile Dehydrogenation of Ethane on the IrO(110) Surface. aug: au: Yingxue Bian Tao Li Weaver, Jason F. Minkyu Kim Asthagiri, Aravind affil: Department of Chemical Engineering, University of Florida, Gainesville, Florida 32611, United States William G. Lowrie Chemical & Biomolecular Engineering, The Ohio State University, Columbus, Ohio 43210, United States su: Dehydrogenation Ethanes Catalysis Density functional theory Oxidation sug: subj: Dehydrogenation Ethanes Catalysis Density functional theory Oxidation ab: Realizing the efficient and selective conversion of ethane to ethylene is important for improving the utilization of hydrocarbon resources, yet remains a major challenge in catalysis. Herein, ethane dehydrogenation on the IrO(110) surface is investigated using temperature-programmed reaction spectroscopy (TPRS) and density functional theory (DFT) calculations. The results show that ethane forms strongly bound σ-complexes on IrO(110) and that a large fraction of the complexes undergo C-H bond cleavage during TPRS at temperatures below 200 K. Continued heating causes as much as 40% of the dissociated ethane to dehydrogenate and desorb as ethylene near 350 K, with the remainder oxidizing to CO species. Both TPRS and DFT show that ethylene desorption is the rate-controlling step in the conversion of ethane to ethylene on IrO(110) during TPRS. Partial hydrogenation of the IrO(110) surface is found to enhance ethylene production from ethane while suppressing oxidation to CO species. DFT predicts that hydrogenation of reactive oxygen atoms of the IrO(110) surface effectively deactivates these sites as H atom acceptors, and causes ethylene desorption to become favored over further dehydrogenation and oxidation of ethane-derived species. The study reveals that IrO(110) exhibits an exceptional ability to promote ethane dehydrogenation to ethylene near room temperature, and provides molecular-level insights for understanding how surface properties influence selectivity toward ethylene production. pubtype: Academic Journal doctype: Article src: R language: English refInfo: copyright: @attributes: flag: Y dt: @attributes: year: 2018 holdings: @attributes: islocal: N |
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