Chemical Insights into the Design and Development of Face Centered Cubic Ruthenium Catalysts for Fischer Tropsch Synthesis
Li, WZ; Liu, JX; Gu, J; Zhou, W; Yao, SY; Si, R; Guo, Y; Su, HY; Yan, CH; Li, WX; Zhang, YW; Ma, D
2017
发表期刊JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
ISSN0002-7863
卷号139期号:6页码:2267-2276
文章类型期刊论文
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.
DOI10.1021/jacs.6b10375
收录类别SCI
语种英语
WOS记录号WOS:000394482200028
引用统计
被引频次:23[WOS]   [WOS记录]     [WOS相关记录]
文献类型期刊论文
条目标识符http://ir.sinap.ac.cn/handle/331007/27271
专题中科院上海应用物理研究所2011-2018年
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Li, WZ,Liu, JX,Gu, J,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, WZ.,Liu, JX.,Gu, J.,Zhou, W.,Yao, SY.,...&Ma, D.(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, WZ,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.
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