Is the methanation reaction over Ru single crystals structure dependent?

نویسندگان

  • Søren B Vendelbo
  • Martin Johansson
  • Jane H Nielsen
  • Ib Chorkendorff
چکیده

The influence of monoatomic steps and defects on the methanation reaction over ruthenium has been investigated. The experiments are performed on a Ru(0 1 54) ruthenium single crystal, which contains one monoatomic step atom for each 27 terrace atoms. The methanation activity is measured at one bar of hydrogen and CO in a high pressure cell, which enables simultaneous measurements of the local reactivity of the well defined single crystal surface and the global reactivity of the entire crystal and its auxiliary support. By adding sulfur we observe that the measured activity from the well defined stepped front-side of the crystal is poisoned faster than the entire crystal containing more defects. We also observe that additional sputtering of the well-defined front-side increases the reactivity measured on the surface. Based on this, we conclude that the methanation reaction takes place on undercoordinated sites, such as steps and kinks, and that the methanation reaction is extremely structure dependent. Simulations of the flow, temperature, and product distributions in the high pressure cell are furthermore presented as supplementary information.

برای دانلود متن کامل این مقاله و بیش از 32 میلیون مقاله دیگر ابتدا ثبت نام کنید

ثبت نام

اگر عضو سایت هستید لطفا وارد حساب کاربری خود شوید

منابع مشابه

Chapter III : Catalytic Activation of CO Over Single Crystals

The catalytic activation of CO single crystal surfaces is reviewed. Examples are provided which demonstrate the relevance of single crystal studies for modeling the behavior of high surface area supported catalysts. The coupling of an apparatus for the measurement of reaction kinetics at elevated pressures with an ultrahigh vacuum system for surface analysis allows detailed study of structure s...

متن کامل

Surface Science Letters Catalytic Methanation over Single Crystal Nickel and Ruthenium: Reaction Kinetics on Different Crystal Planes and the Correlation of Surface Carbide Concentration with Reaction Rate

The kinetics of the reaction of H, and CO over single crystals of nickel ((100) and (111)) and ruthenium ((110) and (001)) have been studied as a function of pressure and Hz/CO ratio. A striking correlation has been observed between the measured surface carbide concentration and the rate of methane production while varying the Ha/CO ratio and the total pressure. This correlation is shown to be ...

متن کامل

Surface Science Letters Measurement of Active Carbon on Ruthenium (110): Relevance to Catalytic Methanation

The detection, by Auger electron spectroscopy (AES), of fractional monolayers of carbon on Ru is difficult because of the interference between the Ru (273 eV) and C (272 eV) transitions [I ,2]. In attempting to deal with this problem, two methods of analysis have been used. In the first, the ratio of the 273 eV signal (p-p height) to the 231 eV Ru signal is monitored [3,4]. Because the 231 eV s...

متن کامل

A comparative study on the kinetics of carbon dioxide methanation over bimetallic and monometallic catalysts

In this paper, Ni/Al and La-Ni/Al catalysts were prepared with a co-impregnation method and employed in carbon dioxide methanation reaction. The catalytic results showed that the catalyst with (10wt.%) of lanthanum and (20wt.%) nickel had the highest activity at low temperatures in CO2 methanation and the La-Ni/Al catalysts changed the reaction path by lowering its activation energy and consequ...

متن کامل

ذخیره در منابع من


  با ذخیره ی این منبع در منابع من، دسترسی به آن را برای استفاده های بعدی آسان تر کنید

برای دانلود متن کامل این مقاله و بیش از 32 میلیون مقاله دیگر ابتدا ثبت نام کنید

ثبت نام

اگر عضو سایت هستید لطفا وارد حساب کاربری خود شوید

عنوان ژورنال:
  • Physical chemistry chemical physics : PCCP

دوره 13 10  شماره 

صفحات  -

تاریخ انتشار 2011