Chemical Insights into the Design and Development of Face-Centered Cubic Ruthenium Catalysts for Fischer-Tropsch Synthesis.
Ruthenium is a promising low-temperature catalyst for Fischer-Tropsch synthesis (FTS). However, its scarcity and modest specific activity limit its widespread industrialization. We demonstrate here a strategy for tuning the crystal phase of catalysts to expose denser and active sites for a higher ma...
| Publicado en: | Journal of the American Chemical Society Vol. 139; no. 6; pp. 2267 - 2277 |
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| Autores principales: | , , , , , , , , , , , |
| Formato: | Artículo |
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American Chemical Society
2/15/2017
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| Materias: | |
| 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=121320761&site=ehost-live header: @attributes: shortDbName: hlh uiTerm: 121320761 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: 2/15/2017 vid: 139 iid: 6 pid: 997 pub: American Chemical Society artinfo: ui: 121320761 10.1021/jacs.6b10375 ppf: 2267 ppct: 10 formats: tig: atl: Chemical Insights into the Design and Development of Face-Centered Cubic Ruthenium Catalysts for Fischer-Tropsch Synthesis. aug: au: Wei-Zhen Li Jin-Xun Liu Jun Gu Wu Zhou Si-Yu Yao Rui Si Yu Guo Hai-Yan Su Chun-Hua Yan Wei-Xue Li Ya-Wen Zhang Ding Ma affil: Beijing National Laboratory for Molecular Sciences (BNLMS), College of Chemistry and Molecular Engineering, Peking University, Beijing 100871, China Department of Chemical Physics, College of Chemistry and Materials Science, iChEM, CAS Center for Excellence in Nanoscience, Hefei National Laboratory for Physical Sciences at the Microscale, University of Science and Technology of China, Hefei 230026, China State Key Laboratory of Catalysis, State Key Laboratory of Molecular Reaction Dynamics, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian 116023, China School of Physical Sciences, CAS Key Laboratory of Vacuum Sciences, University of Chinese Academy of Sciences, Beijing 100049, China Materials Science and Technology Division, Oak Ridge National Laboratory, Oak Ridge, Tennessee 37831, United States Shanghai Synchrotron Radiation Facility, Shanghai Institute of Applied Physics, Chinese Academy of Sciences, Shanghai 201204, China su: Ruthenium catalysts Face centered cubic structure Fischer-Tropsch process Density functional theory Dissociation (Chemistry) sug: subj: Ruthenium catalysts Face centered cubic structure Fischer-Tropsch process Density functional theory Dissociation (Chemistry) ab: Ruthenium is a promising low-temperature catalyst for Fischer-Tropsch synthesis (FTS). However, its scarcity and modest specific activity limit its widespread industrialization. We demonstrate here a strategy for tuning the crystal phase of catalysts to expose denser and active sites for a higher mass-specific activity. Density functional theory calculations show that upon CO dissociation there are a number of open facets with modest barrier available on the face-centered cubic (fcc) Ru but only a few step edges with a lower barrier on conventional hexagonal-closest packed (hcp) Ru. Guided by theoretical calculations, water-dispersible fcc Ru catalysts containing abundant open facets were synthesized and showed an unprecedented mass-specific activity in the aqueous-phase FTS, 37.8 molmolh at 433 K. The mass-specific activity of the fcc Ru catalysts with an average size of 6.8 nm is about three times larger than the previous best hcp catalyst with a smaller size of 1.9 nm and a higher specific surface area. The origin of the higher mass-specific activity of the fcc Ru catalysts is identified experimentally from the 2 orders of magnitude higher density of the active sites, despite its slightly higher apparent barrier. Experimental results are in excellent agreement with prediction of theory. The great influence of the crystal phases on site distribution and their intrinsic activities revealed here provides a rationale design of catalysts for higher mass-specific activity without decrease of the particle size. pubtype: Academic Journal doctype: Article src: R language: English refInfo: copyright: @attributes: flag: Y dt: @attributes: year: 2017 holdings: @attributes: islocal: N |
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