Catalysis on microcomposite surfaces

Abstract Photoemission electron microscopy (PEEM) has revealed a rich variety of spatiotemporal patterns, ranging from reaction fronts and spiral waves to standing waves and chemical turbulence, during the catalytic oxidation of CO as well as the reduction of NO on various Pt single crystal surfaces. More recent experiments have focused on the spatiotemporal dynamics of these catalytic reactions on microstructured and microcomposite reacting domains, constructed using microelectronics fabrication techniques. Representative domain scales for these surfaces are in the micrometer range, comparable to the typical wave-lengths of concentration patterns on the clean catalytic surface. In this work we present computational and experimental studies of the effect of microcomposite surface geometry and properties on catalytic reaction dynamics. Controlled surface heterogeneities can gradually suppress certain types of reaction patterns; they can also act as “pacemakers” for the catalytic surface. The composite surface will, under some conditions, appear as a uniform “effective medium” with behavior different than that observed on each of its individual components; this can also be accompanied by significant changes in the overall reaction rate.

[1]  A. Winfree,et al.  Electrical turbulence in three-dimensional heart muscle. , 1994, Science.

[2]  Dan Luss,et al.  Traveling temperature fronts on catalytic ribbons , 1993 .

[3]  A. Winfree Varieties of spiral wave behavior: An experimentalist's approach to the theory of excitable media. , 1991, Chaos.

[4]  Kenneth Showalter,et al.  Chemical waves in inhomogeneous excitable media , 1991 .

[5]  Ertl,et al.  Modification of spatiotemporal pattern formation in an excitable medium by continuous variation of its intrinsic parameters: CO oxidation on Pt(110). , 1994, Physical review. B, Condensed matter.

[6]  Barkley,et al.  Linear stability analysis of rotating spiral waves in excitable media. , 1992, Physical review letters.

[7]  Markus Bär,et al.  Spiral waves in a surface reaction: Model calculations , 1994 .

[8]  Hsueh-Chia Chang,et al.  Low-dimensional spatio-temporal thermal dynamics on nonuniform catalytic surfaces , 1993 .

[9]  G. Ertl,et al.  Spatiotemporal concentration patterns associated with the catalytic oxidation of CO and Au covered Pt(110) surfaces , 1995 .

[10]  H. Meinhardt Pattern formation in biology: a comparison of models and experiments , 1992 .

[11]  M. Kordesch,et al.  A UHV-compatible photoelectron emission microscope for applications in surface science , 1991 .

[12]  Scheffler,et al.  Local Chemical Reactivity of a Metal Alloy Surface. , 1995, Physical review letters.

[13]  H. Saltsburg,et al.  Linear Metal Nanostructures and Size Effects of Supported Metal Catalysts , 1992, Science.

[14]  M. Cross,et al.  Pattern formation outside of equilibrium , 1993 .

[15]  Graham,et al.  Catalysis on microstructured surfaces: Pattern formation during CO oxidation in complex Pt domains. , 1995, Physical review. E, Statistical physics, plasmas, fluids, and related interdisciplinary topics.

[16]  Dan Luss,et al.  Temperature pulse dynamics on a catalytic ring , 1993 .

[17]  K Asakura,et al.  Effects of Boundaries on Pattern Formation: Catalytic Oxidation of CO on Platinum , 1994, Science.

[18]  Gerhard Ertl,et al.  Oscillatory Kinetics in Heterogeneous Catalysis , 1995 .

[19]  Mark A. Kramer,et al.  Algorithm 658: ODESSA–an ordinary differential equation solver with explicit simultaneous sensitivity analysis , 1988, TOMS.

[20]  Jack Xin,et al.  Existence and nonexistence of traveling waves and reaction-diffusion front propagation in periodic media , 1993 .

[21]  D. Barkley A model for fast computer simulation of waves in excitable media , 1991 .

[22]  M. Bär,et al.  Dispersion relation and spiral rotation in an excitable surface reaction , 1992 .

[23]  Epstein,et al.  Refraction and reflection of chemical waves. , 1993, Physical review letters.