期刊
REVIEW OF SCIENTIFIC INSTRUMENTS
卷 82, 期 2, 页码 -出版社
AMER INST PHYSICS
DOI: 10.1063/1.3544020
关键词
-
资金
- National Science Foundation (NSF) [DGE-0504573]
- U.S. Department of Energy (DOE) Office of Basic Energy Sciences, Chemical Sciences Division
- Robert Bosch Foundation
A new ultrahigh vacuum microcalorimeter for measuring heats of adsorption and adsorption-induced surface reactions on complex single crystal-based model surfaces is described. It has been specifically designed to study the interaction of gaseous molecules with well-defined model catalysts consisting of metal nanoparticles supported on single crystal surfaces or epitaxial thin oxide films grown on single crystals. The detection principle is based on the previously described measurement of the temperature rise upon adsorption of gaseous molecules by use of a pyroelectric polymer ribbon, which is brought into mechanical/thermal contact with the back side of the thin single crystal. The instrument includes (i) a preparation chamber providing the required equipment to prepare supported model catalysts involving well-defined nanoparticles on clean single crystal surfaces and to characterize them using surface analysis techniques and in situ reflectivity measurements and (ii) the adsorption/reaction chamber containing a molecular beam, a pyroelectric heat detector, and calibration tools for determining the absolute reactant fluxes and adsorption heats. The molecular beam is produced by a differentially pumped source based on a multichannel array capable of providing variable fluxes of both high and low vapor pressure gaseous molecules in the range of 0.005-1.5 x 10(15) molecules cm(-2) s(-1) and is modulated by means of the computer-controlled chopper with the shortest pulse length of 150 ms. The calorimetric measurements of adsorption and reaction heats can be performed in a broad temperature range from 100 to 300 K. A novel vibrational isolation method for the pyroelectric detector is introduced for the reduction of acoustic noise. The detector shows a pulse-to-pulse standard deviation <= 15 nJ when heat pulses in the range of 190-3600 nJ are applied to the sample surface with a chopped laser. Particularly for CO adsorption on Pt(111), the energy input of 15 nJ (or 120 nJ cm(-2)) corresponds to the detection limit for adsorption of less than 1.5 x 10(12) CO molecules cm(-2) or less than 0.1% of the monolayer coverage (with respect to the 1.5 x 10(15) surface Pt atoms cm(-2)). The absolute accuracy in energy is within similar to 7%-9%. As a test of the new calorimeter, the adsorption heats of CO on Pt(111) at different temperatures were measured and compared to previously obtained calorimetric data at 300 K. (C) 2011 American Institute of Physics. [doi:10.1063/1.3544020]
作者
我是这篇论文的作者
点击您的名字以认领此论文并将其添加到您的个人资料中。
推荐
暂无数据