Chemical Insights into the Design and Development of Face Centered Cubic   Ruthenium Catalysts for Fischer Tropsch Synthesis

doi:10.1021/jacs.6b10375

CORC > 北京大学 > 化学与分子工程学院

	Chemical Insights into the Design and Development of Face Centered Cubic Ruthenium Catalysts for Fischer Tropsch Synthesis
	Li, Wei-Zhen ; Liu, Jin-Xun ; Gu, Jun ; Zhou, Wu ; Yao, Si-Yu ; Si, Rui ; Guo, Yu ; Su, Hai-Yan ; Yan, Chun-Hua ; Li, Wei-Xue ; Zhang, Ya-Wen ; Ma, Ding
刊名	JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
	2017
关键词	SHAPE-CONTROLLED SYNTHESIS MINIMUM ENERGY PATHS ELASTIC BAND METHOD CO HYDROGENATION SILVER NANOPARTICLES NICKEL-CATALYSTS SADDLE-POINTS LOWER OLEFINS COBALT PHASE
DOI	10.1021/jacs.6b10375
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.; National Natural Science Foundation of China [21225315, 91645202, 21473003, 21273224, 21573005, 21621061, 21271011]; Chinese Academy of Sciences; National Key Research and Development Program of China [2013CB834603, 2013CB933100, 2016YFB0701100]; Strategic Priority Research Program of the Chinese Academy of Sciences [XDA090301001, XDB17010200]; Beijing Natural Science Foundation [2162019]; SCI(E); ARTICLE; 6; 2267-2276; 139
语种	英语
内容类型	期刊论文
源URL	[http://ir.pku.edu.cn/handle/20.500.11897/475126]
专题	化学与分子工程学院
推荐引用方式 GB/T 7714	Li, Wei-Zhen,Liu, Jin-Xun,Gu, Jun,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.
APA	Li, Wei-Zhen.,Liu, Jin-Xun.,Gu, Jun.,Zhou, Wu.,Yao, Si-Yu.,...&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.
MLA	Li, Wei-Zhen,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 (2017).