Chemical Insights into the Design and Development of Face Centered Cubic Ruthenium Catalysts for Fischer Tropsch Synthesis
文献类型：期刊论文
| 作者 | Li, Wei-Xue2,5; Li, Wei-Zhen1; Liu, Jin-Xun2,5; Gu, Jun1; Zhou, Wu3,4; Yao, Si-Yu1; Si, Rui6; Guo, Yu1; Su, Hai-Yan5; Yan, Chun-Hua1 |
| 刊名 | JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
 |
| 出版日期 | 2017-02-15 |
| 卷号 | 139期号:6页码:2267-2276 |
| ISSN号 | 0002-7863 |
| DOI | 10.1021/jacs.6b10375 |
| 文献子类 | Article |
| 英文摘要 | 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 mol(CO).mol(Ru)(-1).h(-1) 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. |
| WOS关键词 | SHAPE-CONTROLLED SYNTHESIS ; MINIMUM ENERGY PATHS ; ELASTIC BAND METHOD ; CO HYDROGENATION ; SILVER NANOPARTICLES ; NICKEL-CATALYSTS ; SADDLE-POINTS ; LOWER OLEFINS ; COBALT ; PHASE |
| WOS研究方向 | Chemistry |
| 语种 | 英语 |
| WOS记录号 | WOS:000394482200028 |
| 出版者 | AMER CHEMICAL SOC |
| 源URL | [http://cas-ir.dicp.ac.cn/handle/321008/169396]  |
| 专题 | 大连化学物理研究所_中国科学院大连化学物理研究所 |
| 通讯作者 | Li, Wei-Xue; Zhang, Ya-Wen; Ma, Ding |
| 作者单位 | 1.Peking Univ, Coll Chem & Mol Engn, BNLMS, Beijing 100871, Peoples R China 2.Univ Sci & Technol China, Hefei Natl Lab Phys Sci Microscale, CAS Ctr Excellence Nanosci, Dept Chem Phys,Coll Chem & Mat Sci,iChEM, Hefei 230026, Peoples R China 3.Univ Chinese Acad Sci, CAS Key Lab Vacuum Sci, Sch Phys Sci, Beijing 100049, Peoples R China 4.Oak Ridge Natl Lab, Mat Sci & Technol Div, Oak Ridge, TN 37831 USA 5.Chinese Acad Sci, Dalian Inst Chem Phys, State Key Lab Mol React Dynam, State Key Lab Catalysis, Dalian 116023, Peoples R China 6.Chinese Acad Sci, Shanghai Inst Appl Phys, Shanghai Synchrotron Radiat Facil, Shanghai 201204, Peoples R China |
| 推荐引用方式 GB/T 7714 | Li, Wei-Xue,Li, Wei-Zhen,Liu, Jin-Xun,et al. Chemical Insights into the Design and Development of Face Centered Cubic Ruthenium Catalysts for Fischer Tropsch Synthesis[J]. JOURNAL OF THE AMERICAN CHEMICAL SOCIETY,2017,139(6):2267-2276. |
| APA | Li, Wei-Xue.,Li, Wei-Zhen.,Liu, Jin-Xun.,Gu, Jun.,Zhou, Wu.,...&Ma, Ding.(2017).Chemical Insights into the Design and Development of Face Centered Cubic Ruthenium Catalysts for Fischer Tropsch Synthesis.JOURNAL OF THE AMERICAN CHEMICAL SOCIETY,139(6),2267-2276. |
| MLA | Li, Wei-Xue,et al."Chemical Insights into the Design and Development of Face Centered Cubic Ruthenium Catalysts for Fischer Tropsch Synthesis".JOURNAL OF THE AMERICAN CHEMICAL SOCIETY 139.6(2017):2267-2276. |
入库方式： OAI收割
来源：大连化学物理研究所
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