The effects of global coupling through the gas phase in oscillatory surface chemical reactions are investigated using a model which represents the complex Ginzburg–Landau equation with an additional integral term. Depending on the parameters of the model, global coupling is found to have either a synchronizing or desynchronizing effect. Respectively, the breakdown of global coupling requires the presence of strong supercritical inhomogeneities or spontaneously occurs in a uniform system.
Using the model of the complex Ginzburg–Landau equation with global coupling, the influence of long-range interactions on the turbulent state of oscillatory reaction–diffusion systems is investigated. Experimental realizations of such a system are, e.g., oscillatory reactions on single crystal surfaces where some of the phenomena we simulate have been observed experimentally. We find that strong global coupling suppresses turbulence by transforming it into a pattern of standing waves or into uniform oscillations. Weaker global coupling gives rise to an intermittent turbulent state which retains partial synchrony.
Previous investigations have demonstrated that the formation of chemical waves in the NO+H2 reaction on Rh(110) involves a cyclic transformation of the surface structure via various N,O-induced reconstructions, i.e., starting form the c(2×6)-O a cycle is initiated comprising the formation of a (2×3)/(3×1)-N and a mixed c(2×4)-2O,N structure. The stability and reactivity of these structures has been investigated in titration experiments as well as under stationary reaction conditions employing LEED, work function, rate measurements, and thermal desorption spectroscopy. It was shown that the c(2×6)-O and c(2×4)-2O,N structures exhibit a low reactivity whereas the (2×1)/(2×1)-N displays only a small to moderate decrease in catalytic activity (≈20%–30%) compared to the clean surface. On the basis of these results, an excitation mechanism for pulses in the NO+H2 reaction on Rh(110) was constructed consisting of the sequence c(2×6)-O, (2×1)/(3×1)-N c(2×4)-2O,N, c(2×6)-O.
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