Nonlinear dynamics on catalytic surfaces

Imbihl, R.

doi:10.1016/j.cattod.2005.02.045

Cited by 31 publications

(31 citation statements)

References 84 publications

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“…Such sigmoid control is present already on simple crystal surfaces such as platinum crystal catalysts, (85) and similar processes are likely to emerge on composomal surfaces, external as well as internal.…”

Section: Limiting the Bandwidth Of Energy Usedmentioning

confidence: 98%

Compositional complementarity and prebiotic ecology in the origin of life

Hunding¹,

Képès²,

Lancet³

et al. 2006

BioEssays

100

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We hypothesize that life began not with the first self-reproducing molecule or metabolic network, but as a prebiotic ecology of co-evolving populations of macromolecular aggregates (composomes). Each composome species had a particular molecular composition resulting from molecular complementarity among environmentally available prebiotic compounds. Natural selection acted on composomal species that varied in properties and functions such as stability, catalysis, fission, fusion and selective accumulation of molecules from solution. Fission permitted molecular replication based on composition rather than linear structure, while fusion created composomal variability. Catalytic functions provided additional chemical novelty resulting eventually in autocatalytic and mutually catalytic networks within composomal species. Composomal autocatalysis and interdependence allowed the Darwinian co-evolution of content and control (metabolism). The existence of chemical interfaces within complex composomes created linear templates upon which self-reproducing molecules (such as RNA) could be synthesized, permitting the evolution of informational replication by molecular templating. Mathematical and experimental tests are proposed.

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Section: Limiting the Bandwidth Of Energy Usedmentioning

confidence: 98%

Compositional complementarity and prebiotic ecology in the origin of life

Hunding¹,

Képès²,

Lancet³

et al. 2006

BioEssays

100

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“…Such selforganization phenomena are understood in terms of reactiondiffusion processes, which also explains the mesoscopic patterns observed on oriented metal single-crystal surfaces (14,15). However, the nanopatterns observed during a catalytic reaction in a FIM have a spatial scale smaller than typical diffusion lengths.…”

mentioning

confidence: 99%

Nanometric chemical clocks

McEwen

Gaspard

Bocarmé

et al. 2009

Proc. Natl. Acad. Sci. U.S.A.

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Field ion microscopy combined with video techniques and chemical probing reveals the existence of catalytic oscillatory patterns at the nanoscale. This is the case when a rhodium nanosized crystalconditioned as a field emitter tip-is exposed to hydrogen and oxygen. Here, we show that these nonequilibrium oscillatory patterns find their origin in the different catalytic properties of all of the nanofacets that are simultaneously exposed at the tip's surface. These results suggest that the underlying surface anisotropy, rather than a standard reaction-diffusion mechanism, plays a major role in determining the self-organizational behavior of multifaceted nanostructured surfaces. Surprisingly, this nanoreactor, composed of the tip crystal and a constant molecular flow of reactants, is large enough for the emergence of regular oscillations from the molecular fluctuations.field ion microscopy ͉ heterogeneous catalysis ͉ nanopatterns ͉ nonequilibrium oscillations T he Belousov-Zhabotinskii reaction is probably the most famous example of an oscillating chemical reaction in the liquid phase (1, 2). However, studies of oscillations in heterogeneous catalysis begun in the 1970s (3, 4). One decade later, Ertl et al. demonstrated for the first time (5, 6) that oscillatory surface reactions are associated with the occurrence of specific pattern formations ranging from tens to hundreds of micrometers. More recently, oscillations have been discovered on the nanoscale in field electron and field ion microscopes by using video techniques (FEM and FIM, respectively) (7-10). At this length scale of tens of nanometers, self-sustained oscillatory patterns are observed about which little is known. This is certainly the case for the catalytic water production when exposing oxygen and hydrogen to a rhodium field emitter tip (11,12). Our purpose in the present article is to show that this nonequilibrium self-organizational behavior can be understood by taking into account the structural anisotropy of the crystalline tip that results in different catalytic properties on the various nanofacets. Moreover, we demonstrate that the external electric field, as applied in a FIM (of the order of 10 V/nm), promotes surface oxidation thus giving way to a feedback mechanism to explain self-sustained rate oscillations in the H 2 /O 2 /Rh system.The understanding of self-sustained oscillations at the macroscale was pioneered by Prigogine who showed that such phenomena are consistent with thermodynamics as long as the system is open and far from equilibrium (13). Such selforganization phenomena are understood in terms of reactiondiffusion processes, which also explains the mesoscopic patterns observed on oriented metal single-crystal surfaces (14, 15). However, the nanopatterns observed during a catalytic reaction in a FIM have a spatial scale smaller than typical diffusion lengths. Moreover, one may wonder how the molecular fluctuations that manifest themselves in such small systems (16, 17) affect the oscillations. Indeed, their regularity disappears...

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“…Owing to the binding of a gas particle with a vacant adsorption site, the spatial distribution of the charge density of the adsorption site changes. Furthermore, this change depends on different factors connected with the adsorbent and gas particles (see, e.g., [2,6,[19][20][21][22]30]). …”

Section: Statement Of the Problem And General Relationsmentioning

confidence: 99%

“…For example, taking account of lateral interactions between adparticles leads to a hysteresis loop of adsorption isotherms and to different structural changes of the adsorbent surface [5][6][7][8][14][15][16][17][18][19][20][21][22].…”

Section: Introductionmentioning

confidence: 99%

Adsorption-induced surface normal relaxation of a solid adsorbent

Usenko¹

2016

Condens. Matter Phys.

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We investigate adsorption of a gas on the flat surface of a solid deformable adsorbent taking into account thermal fluctuations and analyze in detail the effect of thermal fluctuations on the adsorbent deformation in adsorption. The condition for coexistence of two states of a bistable system of adsorbed particles is derived. We establish the specific properties of the adsorption-induced surface normal relaxation of an adsorbent caused by thermal fluctuations. The mean transition times between two stable states of the bistable system are derived in the parabolic approximation and in the general case.

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Nonlinear dynamics on catalytic surfaces

Cited by 31 publications

References 84 publications

Compositional complementarity and prebiotic ecology in the origin of life

Compositional complementarity and prebiotic ecology in the origin of life

Nanometric chemical clocks

Adsorption-induced surface normal relaxation of a solid adsorbent

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