From: "Mit Microsoft Internet Explorer 7 gespeichert" Subject: Wiley InterScience :: Article :: HTML Full Text Date: Sat, 13 Sep 2008 15:32:42 +0200 MIME-Version: 1.0 Content-Type: multipart/related; type="multipart/alternative"; boundary="----=_NextPart_000_0043_01C915B5.F66DBAA0" X-MimeOLE: Produced By Microsoft MimeOLE V6.0.6000.16669 This is a multi-part message in MIME format. ------=_NextPart_000_0043_01C915B5.F66DBAA0 Content-Type: application/octet-stream Content-Transfer-Encoding: quoted-printable Content-Location: http://1.2.3.4/bmi-int-js/bmi.js var bmi_ie;var bmi_ns;var bmi_imageObjSelected;var = bmi_toolTip=3D"Shift+R improves the quality of this image. CTRL+F5 = reloads the whole page.";var bmi_ns_tooltip=3D"Shift+Reload reloads the = whole page.";var bmi_toolTipSeperator=3D" ... 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    3D"Jump

    Angewandte = Chemie=20 International Edition
    ISSN: 1521-3773=20 (Online)
    ISSN: 1433-7851 (Print)

    Volume 47, Issue 19, 2008.
    Pages: = 3524-3535
    • Top of page
    • Abstract
    • 1. Introduction
    • 2. The Surface Science Approach to Heterogeneous = Catalysis:=20 Ammonia Synthesis
    • 3. Self-Organisation and Complexity: Oxidation of = Carbon=20 Monoxide
    • 4. Conclusions
    • References
    List of Images
    Abstract Only

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    3D"About

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    Angewandte Chemie International Edition
    Volume 47, Issue 19, 2008. Pages: 3524-3535

    Copyright © 2008 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim

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    '); } =0A= function display_fig003(size) { var i =3D new Array(); i[0] =3D = 'nfig003'; i[1] =3D 'mfig003'; var hwnd =3D newfigwin(); dochead(hwnd, = ''); copyright(hwnd); otherlinks(hwnd, 'fig003', size); imagelink(hwnd, = i[size]); gcaption_fig003(hwnd); caption_fig003(hwnd); doctail(hwnd); = hwnd.document.close(); hwnd.focus(); } =0A= function caption_fig004(hwnd) { hwnd.document.write('Figure 4. Surface topography and chemical composition of an industrial ammonia = synthesis catalyst.[10]
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    '); } =0A= function display_fig004(size) { var i =3D new Array(); i[0] =3D = 'nfig004'; i[1] =3D 'mfig004'; var hwnd =3D newfigwin(); dochead(hwnd, = ''); copyright(hwnd); otherlinks(hwnd, 'fig004', size); imagelink(hwnd, = i[size]); gcaption_fig004(hwnd); caption_fig004(hwnd); doctail(hwnd); = hwnd.document.close(); hwnd.focus(); } =0A= function caption_fig005(hwnd) { hwnd.document.write('Figure 5. a) Illustration of the process of dissociative chemisorption of a = diatomic molecule; b) one-dimensional Lennard-Jones diagram; = c) two-dimensional representation of equipotential lines as = function of the distance x of the molecule from the surface and = the separation y between the two atoms.
    '); } =0A= function gcaption_fig005(hwnd) { hwnd.document.write('WILEY-VCH

    '); } =0A= function display_fig005(size) { var i =3D new Array(); i[0] =3D = 'nfig005'; i[1] =3D 'mfig005'; var hwnd =3D newfigwin(); dochead(hwnd, = ''); copyright(hwnd); otherlinks(hwnd, 'fig005', size); imagelink(hwnd, = i[size]); gcaption_fig005(hwnd); caption_fig005(hwnd); doctail(hwnd); = hwnd.document.close(); hwnd.focus(); } =0A= function caption_fig006(hwnd) { hwnd.document.write('Figure 6. STM image from a Pt(111) surface (5.3=D75.5 mm) after exposure to = a small concentration of O2 molecules at 165 K.[15]
    '); } =0A= function gcaption_fig006(hwnd) { hwnd.document.write('WILEY-VCH

    '); } =0A= function display_fig006(size) { var i =3D new Array(); i[0] =3D = 'nfig006'; i[1] =3D 'mfig006'; var hwnd =3D newfigwin(); dochead(hwnd, = ''); copyright(hwnd); otherlinks(hwnd, 'fig006', size); imagelink(hwnd, = i[size]); gcaption_fig006(hwnd); caption_fig006(hwnd); doctail(hwnd); = hwnd.document.close(); hwnd.focus(); } =0A= function caption_fig007(hwnd) { hwnd.document.write('Figure 7. STM snapshots from O atoms adsorbed on a Ru(001) surface at = 300 K:[18] a) at very small coverage; b) at higher coverage. A short = movie showing the motion of the O atoms in real time is presented = in the Supporting Information.
    '); } =0A= function gcaption_fig007(hwnd) { hwnd.document.write('WILEY-VCH

    '); } =0A= function display_fig007(size) { var i =3D new Array(); i[0] =3D = 'nfig007'; i[1] =3D 'mfig007'; var hwnd =3D newfigwin(); dochead(hwnd, = ''); copyright(hwnd); otherlinks(hwnd, 'fig007', size); imagelink(hwnd, = i[size]); gcaption_fig007(hwnd); caption_fig007(hwnd); doctail(hwnd); = hwnd.document.close(); hwnd.focus(); } =0A= function caption_fig008(hwnd) { hwnd.document.write('Figure 8. The structure of N atoms chemisorbed on a Fe(100) surface:[21] a) top = view; b) side view. The distances are given in Å = (1 Å=3D10 nm).
    '); } =0A= function gcaption_fig008(hwnd) { hwnd.document.write('WILEY-VCH

    '); } =0A= function display_fig008(size) { var i =3D new Array(); i[0] =3D = 'nfig008'; i[1] =3D 'mfig008'; var hwnd =3D newfigwin(); dochead(hwnd, = ''); copyright(hwnd); otherlinks(hwnd, 'fig008', size); imagelink(hwnd, = i[size]); gcaption_fig008(hwnd); caption_fig008(hwnd); doctail(hwnd); = hwnd.document.close(); hwnd.focus(); } =0A= function caption_fig009(hwnd) { hwnd.document.write('Figure 9. The variation of the relative coverage N atoms (y) = chemisorbed at 693 K at various Fe single-crystal surfaces with = exposure to gaseous N2[22] (1 L=3D1.33=D710-6 mbar s is about the exposure that would suffice to form a = complete monolayer if each incident molecule is adsorbed).
    '); } =0A= function gcaption_fig009(hwnd) { hwnd.document.write('WILEY-VCH

    '); } =0A= function display_fig009(size) { var i =3D new Array(); i[0] =3D = 'nfig009'; i[1] =3D 'mfig009'; var hwnd =3D newfigwin(); dochead(hwnd, = ''); copyright(hwnd); otherlinks(hwnd, 'fig009', size); imagelink(hwnd, = i[size]); gcaption_fig009(hwnd); caption_fig009(hwnd); doctail(hwnd); = hwnd.document.close(); hwnd.focus(); } =0A= function caption_fig010(hwnd) { hwnd.document.write('Figure 10. Mechanism and potential energy diagram of ammonia synthesis on iron.[26] The energies = are given in kJ mol-1.
    '); } =0A= function gcaption_fig010(hwnd) { hwnd.document.write('WILEY-VCH

    '); } =0A= function display_fig010(size) { var i =3D new Array(); i[0] =3D = 'nfig010'; i[1] =3D 'mfig010'; var hwnd =3D newfigwin(); dochead(hwnd, = ''); copyright(hwnd); otherlinks(hwnd, 'fig010', size); imagelink(hwnd, = i[size]); gcaption_fig010(hwnd); caption_fig010(hwnd); doctail(hwnd); = hwnd.document.close(); hwnd.focus(); } =0A= function caption_fig011(hwnd) { hwnd.document.write('Figure 11. Microkinetics of catalytic ammonia synthesis: Comparison of the yield = calculated on the basis of the mechanism presented in Figure 10 (y axis) with experimental data from industrial plants (x axis).[27]
    '); } =0A= function gcaption_fig011(hwnd) { hwnd.document.write('WILEY-VCH

    '); } =0A= function display_fig011(size) { var i =3D new Array(); i[0] =3D = 'nfig011'; i[1] =3D 'mfig011'; var hwnd =3D newfigwin(); dochead(hwnd, = ''); copyright(hwnd); otherlinks(hwnd, 'fig011', size); imagelink(hwnd, = i[size]); gcaption_fig011(hwnd); caption_fig011(hwnd); doctail(hwnd); = hwnd.document.close(); hwnd.focus(); } =0A= function caption_fig012(hwnd) { hwnd.document.write('Figure 12. Cartoon illustrating a car exhaust catalyst and the mechanism of CO = oxidation.
    '); } =0A= function gcaption_fig012(hwnd) { hwnd.document.write('WILEY-VCH

    '); } =0A= function display_fig012(size) { var i =3D new Array(); i[0] =3D = 'nfig012'; i[1] =3D 'mfig012'; var hwnd =3D newfigwin(); dochead(hwnd, = ''); copyright(hwnd); otherlinks(hwnd, 'fig012', size); imagelink(hwnd, = i[size]); gcaption_fig012(hwnd); caption_fig012(hwnd); doctail(hwnd); = hwnd.document.close(); hwnd.focus(); } =0A= function caption_fig013(hwnd) { hwnd.document.write('Figure 13. Structures of CO (a), O (b), and O+CO (c) chemisorbed on a Rh(111) = surface.[29] = Distances are given in Å.
    '); } =0A= function gcaption_fig013(hwnd) { hwnd.document.write('WILEY-VCH

    '); } =0A= function display_fig013(size) { var i =3D new Array(); i[0] =3D = 'nfig013'; i[1] =3D 'mfig013'; var hwnd =3D newfigwin(); dochead(hwnd, = ''); copyright(hwnd); otherlinks(hwnd, 'fig013', size); imagelink(hwnd, = i[size]); gcaption_fig013(hwnd); caption_fig013(hwnd); doctail(hwnd); = hwnd.document.close(); hwnd.focus(); } =0A= function caption_fig014(hwnd) { hwnd.document.write('Figure 14. Mechanism and energy diagram for the catalytic oxidation of CO on = Pt.
    '); } =0A= function gcaption_fig014(hwnd) { hwnd.document.write('WILEY-VCH

    '); } =0A= function display_fig014(size) { var i =3D new Array(); i[0] =3D = 'nfig014'; i[1] =3D 'mfig014'; var hwnd =3D newfigwin(); dochead(hwnd, = ''); copyright(hwnd); otherlinks(hwnd, 'fig014', size); imagelink(hwnd, = i[size]); gcaption_fig014(hwnd); caption_fig014(hwnd); doctail(hwnd); = hwnd.document.close(); hwnd.focus(); } =0A= function caption_fig015(hwnd) { hwnd.document.write('Figure 15. Onset of temporal oscillations of the rate of CO2 = formation on a Pt(110) surface.[34] T=3D470 K; pCO=3D3=D710-5 mbar.
    '); } =0A= function gcaption_fig015(hwnd) { hwnd.document.write('WILEY-VCH

    '); } =0A= function display_fig015(size) { var i =3D new Array(); i[0] =3D = 'nfig015'; i[1] =3D 'mfig015'; var hwnd =3D newfigwin(); dochead(hwnd, = ''); copyright(hwnd); otherlinks(hwnd, 'fig015', size); imagelink(hwnd, = i[size]); gcaption_fig015(hwnd); caption_fig015(hwnd); doctail(hwnd); = hwnd.document.close(); hwnd.focus(); } =0A= function caption_fig016(hwnd) { hwnd.document.write('Figure 16. Variation of the number of furs n (in thousands) from hares = and lynxes delivered to Hudson's Bay Company with time.[37]
    '); } =0A= function gcaption_fig016(hwnd) { hwnd.document.write('WILEY-VCH

    '); } =0A= function display_fig016(size) { var i =3D new Array(); i[0] =3D = 'nfig016'; i[1] =3D 'mfig016'; var hwnd =3D newfigwin(); dochead(hwnd, = ''); copyright(hwnd); otherlinks(hwnd, 'fig016', size); imagelink(hwnd, = i[size]); gcaption_fig016(hwnd); caption_fig016(hwnd); doctail(hwnd); = hwnd.document.close(); hwnd.focus(); } =0A= function caption_fig017(hwnd) { hwnd.document.write('Figure 17. The Lotka-Volterra model describing the observation in Figure 16.
    '); } =0A= function gcaption_fig017(hwnd) { hwnd.document.write('WILEY-VCH

    '); } =0A= function display_fig017(size) { var i =3D new Array(); i[0] =3D = 'nfig017'; i[1] =3D 'mfig017'; var hwnd =3D newfigwin(); dochead(hwnd, = ''); copyright(hwnd); otherlinks(hwnd, 'fig017', size); imagelink(hwnd, = i[size]); gcaption_fig017(hwnd); caption_fig017(hwnd); doctail(hwnd); = hwnd.document.close(); hwnd.focus(); } =0A= function caption_fig018(hwnd) { hwnd.document.write('Figure 18. Structures of the Pt(110) surface:[39] a) the 1=D72 structure of the clean = surface; b) the 1=D71 structure representing termination of = the bulk structure.
    '); } =0A= function gcaption_fig018(hwnd) { hwnd.document.write('WILEY-VCH

    '); } =0A= function display_fig018(size) { var i =3D new Array(); i[0] =3D = 'nfig018'; i[1] =3D 'mfig018'; var hwnd =3D newfigwin(); dochead(hwnd, = ''); copyright(hwnd); otherlinks(hwnd, 'fig018', size); imagelink(hwnd, = i[size]); gcaption_fig018(hwnd); caption_fig018(hwnd); doctail(hwnd); = hwnd.document.close(); hwnd.focus(); } =0A= function caption_fig019(hwnd) { hwnd.document.write('Figure 19. Theoretical description of the oscillatory kinetics of CO oxidation on = a Pt(110) surface.[42] T=3D540 K; pO2=3D6.7=D710-5 mbar; pCO=3D3=D710-5 mbar.
    '); } = =0A= function gcaption_fig019(hwnd) { hwnd.document.write('WILEY-VCH

    '); } =0A= function display_fig019(size) { var i =3D new Array(); i[0] =3D = 'nfig019'; i[1] =3D 'mfig019'; var hwnd =3D newfigwin(); dochead(hwnd, = ''); copyright(hwnd); otherlinks(hwnd, 'fig019', size); imagelink(hwnd, = i[size]); gcaption_fig019(hwnd); caption_fig019(hwnd); doctail(hwnd); = hwnd.document.close(); hwnd.focus(); } =0A= function caption_fig020(hwnd) { hwnd.document.write('Figure 20. Spatio-temporal self-organization in open systems far from = equilibrium.
    '); } =0A= function gcaption_fig020(hwnd) { hwnd.document.write('WILEY-VCH

    '); } =0A= function display_fig020(size) { var i =3D new Array(); i[0] =3D = 'nfig020'; i[1] =3D 'mfig020'; var hwnd =3D newfigwin(); dochead(hwnd, = ''); copyright(hwnd); otherlinks(hwnd, 'fig020', size); imagelink(hwnd, = i[size]); gcaption_fig020(hwnd); caption_fig020(hwnd); doctail(hwnd); = hwnd.document.close(); hwnd.focus(); } =0A= function caption_fig021(hwnd) { hwnd.document.write('Figure 21. Target patterns in catalytic oxidation of CO on a Pt(110) surface as = imaged by PEEM.[47] A real-time movie showing the pattern changes is presented in = the Supporting Information.
    '); } =0A= function gcaption_fig021(hwnd) { hwnd.document.write('WILEY-VCH

    '); } =0A= function display_fig021(size) { var i =3D new Array(); i[0] =3D = 'nfig021'; i[1] =3D 'mfig021'; var hwnd =3D newfigwin(); dochead(hwnd, = ''); copyright(hwnd); otherlinks(hwnd, 'fig021', size); imagelink(hwnd, = i[size]); gcaption_fig021(hwnd); caption_fig021(hwnd); doctail(hwnd); = hwnd.document.close(); hwnd.focus(); } =0A= function caption_fig022(hwnd) { hwnd.document.write('Figure 22. PEEM image of the formation of spiral waves in catalytic CO oxidation = on a Pt(110) surface.[48] T=3D448 K; pO2=3D4=D710-4 mbar; pCO=3D4.3=D710-5 mbar. The diameter of the = picture is 500 m. A real-time movie showing the pattern changes is = presented in the Supporting Information.
    '); } =0A= function gcaption_fig022(hwnd) { hwnd.document.write('WILEY-VCH

    '); } =0A= function display_fig022(size) { var i =3D new Array(); i[0] =3D = 'nfig022'; i[1] =3D 'mfig022'; var hwnd =3D newfigwin(); dochead(hwnd, = ''); copyright(hwnd); otherlinks(hwnd, 'fig022', size); imagelink(hwnd, = i[size]); gcaption_fig022(hwnd); caption_fig022(hwnd); doctail(hwnd); = hwnd.document.close(); hwnd.focus(); } =0A= function caption_fig023(hwnd) { hwnd.document.write('Figure 23. Computer simulation of the evolution of spiral waves in catalytic CO = oxidation.[49]
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    '); } =0A= function display_fig023(size) { var i =3D new Array(); i[0] =3D = 'nfig023'; i[1] =3D 'mfig023'; var hwnd =3D newfigwin(); dochead(hwnd, = ''); copyright(hwnd); otherlinks(hwnd, 'fig023', size); imagelink(hwnd, = i[size]); gcaption_fig023(hwnd); caption_fig023(hwnd); doctail(hwnd); = hwnd.document.close(); hwnd.focus(); } =0A= function caption_fig024(hwnd) { hwnd.document.write('Figure 24. Computer simulation of the break up of spiral waves to chemical = turbulence.
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    '); } =0A= function display_fig024(size) { var i =3D new Array(); i[0] =3D = 'nfig024'; i[1] =3D 'mfig024'; var hwnd =3D newfigwin(); dochead(hwnd, = ''); copyright(hwnd); otherlinks(hwnd, 'fig024', size); imagelink(hwnd, = i[size]); gcaption_fig024(hwnd); caption_fig024(hwnd); doctail(hwnd); = hwnd.document.close(); hwnd.focus(); } =0A= function caption_fig025(hwnd) { hwnd.document.write('Figure 25. PEEM image from a Pt(110) surface in the state of chemical turbulence. = T=3D548 K; pO2=3D4=D710-4 mbar; pCO=3D1.2=D710-4 mbar. The image size is = 360=D7360 m. A real-time movie showing the pattern changes is = presented in the Supporting Information.
    '); } =0A= function gcaption_fig025(hwnd) { hwnd.document.write('WILEY-VCH

    '); } =0A= function display_fig025(size) { var i =3D new Array(); i[0] =3D = 'nfig025'; i[1] =3D 'mfig025'; var hwnd =3D newfigwin(); dochead(hwnd, = ''); copyright(hwnd); otherlinks(hwnd, 'fig025', size); imagelink(hwnd, = i[size]); gcaption_fig025(hwnd); caption_fig025(hwnd); doctail(hwnd); = hwnd.document.close(); hwnd.focus(); } =0A= function caption_fig026(hwnd) { hwnd.document.write('Figure 26. Transformation of a state of spiral turbulence into other different = patterns by a feedback mechanism with different strength and delay of = the feedback.[51]
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    3D""=20

    Angewandte Chemie International = Edition

    What=20 is RSS?

    Volume 47, Issue 19, Pages 3524-3535

    Published Online: 20 Mar 2008

    Copyright =A9 2008 WILEY-VCH Verlag GmbH & Co. KGaA,=20 Weinheim

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     Review
    Reactions at Surfaces: From Atoms = to=20 Complexity (Nobel Lecture)
    Gerhard Ertl, Prof. Dr.=20 *
    Fritz-Haber-Institut der Max-Planck-Gesellschaft, 14195 = Berlin,=20 Germany, Fax: (+49) 30-8413-5106
    email: Gerhard Ertl (ertl@fhi-berlin.mpg.de)

    *Correspondence to Gerhard = Ertl,=20 Fritz-Haber-Institut der Max-Planck-Gesellschaft, 14195 Berlin, = Germany,=20 Fax: (+49) 30-8413-5106

    Copyright=A9 The Nobel Foundation 2007. We thank = the Nobel=20 Foundation, Stockholm, for permission to print this lecture. = Supporting=20 information for this article is available on the WWW under=20 http://www.angewandte.org or from the author.

    Keywords
    ammonia synthesis =95 carbon monoxide =95 Nobel lecture = =95=20 oscillating reactions =95 surface = chemistry

    Abstract
    3DAbstract=20
    No Abstract

    Received: 30 January 2008

    Digital Object = Identifier=20 = (DOI)

    10.1002/anie.200800480  = About=20 DOI

    Additional=20 Material

    Supporting = information for this=20 article is available on the WWW under http://www.wiley-vch.de/contents/jc_2002/2008/a800480_s.htm= l=20 or from the author.

    Article=20 Text

    1. Introduction
    3D1. Introduction=20

    The secretary of the Royal Swedish Academy of Sciences, the = famous=20 chemist J=F6ns Jacob Berzelius, published since 1820 annual review = articles=20 on the most significant new developments in his field. Since the = early=20 19th century there were observations from several laboratories = that=20 certain substances influenced the progress of a chemical reaction = without=20 being consumed and hence apparently not being affected by this = reaction.=20 For example, Johann Wolfgang D=F6bereiner, professor of chemistry = at the=20 University of Jena, reported in July 1823 to his minister, Johann = Wolfgang=20 von Goethe, that finely divided platinum powder causes hydrogen = gas to=20 react with oxygen gas by mere contact to water whereby the = platinum itself=20 is not altered.[1][Note=20 ]=20 In his report published in 1835, Berzelius defined this phenomenon = as catalysis, rather in order to introduce a classification than to = offer a=20 possible explanation.[2]=20 Throughout the rest of this century, the term catalysis remained = heavily=20 debated[3]=20 until around 1900 Wilhelm Ostwald proposed its valid definition in = terms=20 of the concepts of chemical kinetics: A catalyst is a substance which affects the rate of = a chemical=20 reaction without being part of its end products.[4][Note=20 ]=20 In 1909, Ostwald was awarded the Nobel Prize in Chemistry for his=20 contributions to catalysis.[da=DF das rein metallische staubfeine Platin die = h=F6chst=20 merkw=FCrdige Eigenschaft hat, das Wasserstoffgas durch blo=DFe = Ber=FChrung zu=20 bestimmen, da=DF es sich mit Sauerstoffgas zu Wasser = verbindet][Ein Katalysator ist jeder Stoff, der, ohne im = Endprodukt einer=20 chemischen Reaktion zu erscheinen, ihre Geschwindigkeit = ver=E4ndert.]

    A chemical reaction involves breaking of bonds between atoms = and the=20 formation of new ones. This process is associated with = transformation of=20 energy, and the energy diagram illustrating the progress of a = reaction=20 A+BC is depicted schematically in Figure 1.=20 The activation energy E* to be surmounted is usually = provided by=20 thermal energy kT, with k being Boltzmann's constant = and=20 T the temperature, and accordingly not all molecular = encounters=20 will be successful, but only a fraction = e-E*/kT.=20 An increase of the reaction probability (=3Drate) can be achieved = by either=20 increasing the temperature or by lowering the activation energy = E*.=20 The latter is provided by the catalyst, which through the = formation of=20 intermediate compounds with the molecules involved in the reaction = provides an alternate reaction path as sketched by the dashed line = in=20 Figure 1=20 which is associated with smaller activation barriers and hence a = higher=20 overall reaction rate. In the last step, the product molecules are = released from the catalyst, which is now available for the next = reaction=20 cycle. If the reacting molecules and the catalyst are in the same = (gaseous=20 or liquid) phase, the effect is called homogeneous catalysis. In = living=20 systems, macromolecules (=3Denzymes) play the role of catalysts. = In=20 technical reactions, mostly the interaction of molecules with the = surface=20 of a solid is decisive. The principle of this heterogeneous = catalysis is=20 depicted schematically in Figure 2.=20

    Figure 1. Energy = diagram=20 illustrating the progress of a chemical reaction with and = without a=20 catalyst.
    [Normal View=20 5K | Magnified = View=20 10K]

    Figure 2. The = principle of=20 heterogeneous catalysis.
    [Normal View 13K | = Magnified View=20 31K]

    The atoms in the surface layer of a solid have fewer neighbors = than=20 those in the bulk and are hence chemically unsaturated and may = form new=20 bonds (=3Dchemisorption) with suitable molecules impinging from = the adjacent=20 gas or liquid phase. By this step, existing bonds will be modified = or may=20 even be broken (=3Ddissociative chemisorption). The surface = species formed=20 may jump from one site to neighboring ones, then may react with = others,=20 and the formed produced molecules eventually leave the surface=20 (=3Ddesorption). If operated in a flow reactor, the catalyst can = in this way=20 continuously operate without being consumed.

    One of the first and still most important technical = applications of=20 this principle was realized about 100 years ago: Owing to the = continuous increase of the world population and exhaustion of the = natural=20 supply of nitrogen fertilizers, the world was facing a global = threat of=20 starvation. As Sir William Crookes, president of the British = Association=20 for the Advancement of Science, formulated it:[5]=20 ... all civilized nations stand in deadly peril of = not having=20 enough to eat =20 the fixation of atmospheric nitrogen is one of the great = discoveries=20 awaiting the ingenuity of chemists.

    Nitrogen fixation means transformation of the abundant = N2=20 molecule (which constitutes about 80 % of our air) from its = state of=20 very strong bond between the two N atoms into a more reactive form = according to the reaction N2+3 H22 NH3. This reaction of ammonia = formation could=20 be realized in 1909 by Fritz Haber (Nobel Prize 1919) in the = laboratory by=20 the use of an osmium catalyst in a high-pressure flow = apparatus.[6]=20 Carl Bosch (Nobel Prize 1931) from the BASF company started = immediately to=20 develop this method into a technical process, and the first = industrial=20 plant started operation in 1913, only a few years later. = Figure 3=20 shows the growth of the world population together with the ammonia = production over the last century,[7]=20 and it is quite obvious that our present life would be quite = different=20 without the development of the Haber-Bosch process.=20

    Figure 3. Variation of = the world=20 population (in 109) and the ammonia production = (in=20 106 metric tons of nitrogen) during the 20th = century.[7]
    [Normal View 9K | = Magnified View=20 17K]

    However, large-scale technical production would not have been = possible=20 without the availability of large quantities of a cheap catalyst. = (The=20 complete world supply of the precious metal osmium was only = 80 kg in=20 those days.) This task could be solved successfully by Alwin = Mittasch[8]=20 who in thousands of tests found that a material derived from a = Swedish=20 iron ore exhibited satisfactory activity. This type of doubly = promoted=20 iron catalyst is in fact still in use today in almost all = industrial=20 plants.

    Remarkably, despite the enormous technical significance of the=20 Haber-Bosch reaction and despite of numerous laboratory studies, = its=20 actual mechanism remained unclear over many years. P. H. = Emmett, one=20 of the pioneers of catalysis research, was honored in 1974 by a = symposium=20 at which he concluded:[9]=20 The experimental work of the past 50 years = leads to the=20 conclusion that the rate-limiting step in ammonia synthesis over = iron=20 catalysts is the chemisorption of nitrogen. The question as to = whether the=20 nitrogen species involved is molecular or atomic is still not = conclusively=20 resolved .

    2. The Surface = Science=20 Approach to Heterogeneous Catalysis: Ammonia Synthesis

    The problem involved in the study of the surface chemistry of = real=20 catalysts becomes evident if we look on an electron micrograph of = the=20 Mittasch catalyst as reproduced in Figure 4:[10]=20 A catalyst with high activity has to exhibit a rather high = specific=20 surface area, which in this case is about=20 20 m2 g-1 as reflected by = nanometer-sized=20 active particles. (In fact, catalysis has been a nanotechnology = long=20 before this term was introduced.) Under reaction conditions, these = particles are reduced into metallic iron covered by a submonolayer = of=20 K(+O), which acts as an electronic=20 promoter. The configuration of active particles is stabilized = against=20 sintering by a framework of Al2O3 (and CaO); = these=20 compounds act as structural=20 promoters. The active component itself will expose different = crystal=20 planes apart from various defects, and all these various = structural=20 parameters are expected to exhibit varying reactivity. Moreover, = the=20 question arises: how can the two-dimensional chemistry taking = place in the=20 chemisorbed overlayer be investigated on the atomic scale?=20

    Figure 4. Surface = topography and=20 chemical composition of an industrial ammonia synthesis = catalyst.[10]
    [Normal View 34K | = Magnified View=20 76K]

    A possible strategy to overcome this problem had been suggested = by=20 Irving Langmuir (Nobel Prize 1932) already many years ago:[11]=20 Most finely divided catalysts must have structures = of great=20 complexity. In order to simplify our theoretical consideration of=20 reactions at surfaces, let us confine our attention to reactions = on plane=20 surfaces. If the principles in this case are well understood, it = should=20 then be possible to extend the theory to the case of porous = bodies. In=20 general, we should look upon the surface as consisting of a = checkerboard=20

    The surface science=20 approach that Langmuir had in mind was experimentally not yet = accessible=20 in his days, but began to become only available during the 1960s = with the=20 advent of ultrahigh vacuum (UHV) and surface sensitive physical=20 methods.[12]=20 Nowadays a whole arsenal of such techniques is available to study = the=20 structural, electronic, or dynamic properties of such well-defined = single-crystal surfaces.

    Bond-breaking upon chemisorption is perhaps the most important = role of=20 a catalyst. Figure 5=20 shows schematically the energetic transformations in such a = process if a=20 diatomic molecule interacts with a perfect surface. Upon = approaching the=20 surface, the molecule may initiate the formation of new bonds to = the=20 surface atoms whereby the bond between the two atoms is weakened. = A=20 corresponding one-dimensional energy diagram as proposed by=20 Lennard-Jones[13]=20 is depicted in Figure 5 b:=20 If the molecule A2 forms a bond with the surface, a = shallow=20 minimum (A2,ad) is reached. If instead the free = A2=20 molecule dissociates, the dissociation energy = Ediss is=20 needed. Chemisorption of two A atoms would be associated with = strong bond=20 formation (2Aad), and the crossing point between the = two curves=20 marks the activation energy for dissociative chemisorption, = namely, the=20 reaction A22Aad. Even more instructive is a = two-dimensional=20 diagram (Figure 5 c),=20 in which lines of equal energy are plotted as a function of the = distance=20 x between the molecule and the surface and the separation = y=20 between the two atoms. (A full multidimensional description would = require=20 knowledge of the energy also as function of the point of impact = within the=20 unit cell of the surface as well as of the orientation of the = molecular=20 axis, and theory is nowadays able to provide this information as = well as=20 on the dynamics of energy transfer between the different degrees = of=20 freedom.[14])=20

    Figure 5. = a) Illustration=20 of the process of dissociative chemisorption of a diatomic = molecule;=20 b) one-dimensional Lennard-Jones diagram;=20 c) two-dimensional representation of equipotential = lines as=20 function of the distance x of the molecule from the = surface=20 and the separation y between the two atoms.
    [Normal View 19K | = Magnified View=20 40K]

    Figure 6=20 shows a scanning tunneling microscope (STM) picture from a Pt(111) = surface=20 with atomic resolution after exposure to a small amount of = O2=20 molecules at 165 K.[15]=20 Apart from the Pt atoms from the topmost layer, additional = features,=20 namely pairs of bright dots surrounded by dark rings, are visible. = The=20 dots mark the positions of O atoms resulting from dissociative=20 chemisorption. Whereas at 120 K chemisorbed O2 = molecules=20 are discernible, at 165 K the thermal energy suffices to = overcome the=20 activation barrier for dissociation. The dark rings around the = bright=20 spots reflect the modification of the local electronic structure = near the=20 chemisorbed species. As a consequence, neighboring particles = interact with=20 each other through the electronic system of the substrate, whereby = these=20 interactions may be repulsive as well as attractive.[16]=20 At the low temperature of 165 K, on the other hand, the = chemisorbed O=20 atoms are immobile and rest at those sites at which transfer of = the=20 chemisorption energy to the solid has been completed. This process = requires a certain relaxation time during which the two separating = O atoms=20 move apart from each other, which is why two O atoms are never on=20 neighboring sites, but are typically separated by 0.5-0.8 nm = from=20 each other. Taking into account the chemisorption energy released = leads to=20 an estimate of about 3=D710-13 s for the lifetime = of these=20 hot=20 adatoms.=20

    Figure 6. STM image = from a=20 Pt(111) surface (5.3=D75.5 mm) after exposure to a = small=20 concentration of O2 molecules at 165 K.[15]
    [Normal View 44K | = Magnified View=20 103K]

    More detailed insight into the dynamics of energy exchange = between the=20 solid and chemisorbed species can be obtained by application of = ultrafast=20 (femtosecond) laser techniques, and it can be generally concluded = that=20 with metal surfaces complete thermal equilibrium between all = degrees of=20 freedom is typically reached after about = 10-12 s.[17]

    The mean residence time of a chemisorbed particle on its = momentary=20 adsorption site is given by =3D0 e/kT, whereby is the activation energy for surface = diffusion=20 to a neighboring site. ( is always much smaller than the = adsorption=20 energy, so that the adparticle makes many jumps before it = eventually=20 desorbs into the gas phase.) Figure 7 a=20 shows a snapshot taken with a fast STM from a Ru(0001) surface at=20 300 K covered by a small concentration of O atoms. The latter = jump=20 around like with two-dimensional Brownian motion with a mean = of about 6=D710-2 s. However, = varies with the mutual separation between two = neighboring=20 O atoms because of the operation of the above mentioned = interactions=20 and reaches about 0.22 s if the two O atoms are = separated from=20 each other by 2 lattice constants.[19]=20 As a consequence of the operation of these weak attractive = interactions,=20 at higher surface concentrations the adsorbed particles are no = longer=20 uniformly and randomly distributed across the surface, but = segregate into=20 two phases as shown in Figure 7 b:=20 A two-dimensional quasi-crystalline phase is in equilibrium with a = quasi-gas phase, where continuous nucleation, condensation, and=20 sublimation occur like in analogous solid-gas equilibria. Such=20 observations also reveal that the definition of a surface = diffusion=20 coefficient for adsorbates is meaningful only at low surface=20 concentrations as long as the adsorbed particles can be considered = to be=20 independent from each other.[20]=20

    Figure 7. STM = snapshots from=20 O atoms adsorbed on a Ru(001) surface at 300 K:[18]=20 a) at very small coverage; b) at higher coverage. = A short=20 movie showing the motion of the O atoms in real time is = presented in the Supporting Information.
    [Normal View 61K | = Magnified View=20 149K]

    The formation of ordered adsorbate phases with long-range = periodicity=20 such as in Figure 7 b=20 is quite common and permits determination of the actual structural = parameters by a diffraction technique, preferably low-energy = electron=20 diffraction (LEED).[12]=20 If we now return to the original problem of ammonia synthesis,=20 dissociative chemisorption of nitrogen on various Fe = single-crystal=20 surfaces causes indeed also the formation of such structures = derived from=20 chemisorbed N atoms, such as reproduced in Figure 8=20 for the c2=D72-N phase on the Fe(100) surface.[21]=20 The probability for this process (=3Dsticking coefficient) is very = low,=20 typically of the order 10-6, which reflects the fact = that this=20 step is indeed rate-limiting in the overall reaction of ammonia = synthesis.=20 Figure 9=20 shows the variation of the surface concentration y (in = relative=20 units) of N atoms chemisorbed on various Fe single-crystal = surfaces=20 with exposure (i.e. number of molecules impinging per = cm2 and=20 s) to N2 gas at 693 K.[22]=20 There is a pronounced influence of the surface structure: The most = densely=20 packed (110) surface is least active, whereas the open (111) plane = exhibits the highest sticking coefficient and is indeed also = responsible=20 for the overall activity of the industrial catalyst.[23]=20 This activity is further enhanced by the presence of the = electronic=20 promoter potassium, which stabilizes the intermediate = N2,ad=20 complex and hence increases its dissociation probability.[24]=20 The same sequence in reactivity as found for the sticking = coefficient for=20 dissociative nitrogen adsorption under low-pressure conditions was = also=20 found for the yield of ammonia production at a pressure of = 20 bar.[25]=20 Thus, it is also demonstrated that in this case there exists no = pressure gap.=20

    Figure 8. The = structure of=20 N atoms chemisorbed on a Fe(100) surface:[21]=20 a) top view; b) side view. The distances are given = in =C5=20 (1 =C5=3D10 nm).
    [Normal View 17K | = Magnified View=20 34K]

    Figure 9. The = variation of the=20 relative coverage N atoms (y) chemisorbed at = 693 K=20 at various Fe single-crystal surfaces with exposure to = gaseous=20 N2[22]=20 (1 L=3D1.33=D710-6 mbar s is about = the=20 exposure that would suffice to form a complete monolayer if = each=20 incident molecule is adsorbed).
    [Normal View 15K | = Magnified View=20 31K]

    All further steps involved in the ammonia synthesis reaction = could be=20 identified and analyzed similarly, so that the overall mechanism = and=20 energy diagram reproduced in Figure 10=20 could be derived.[26]=20 This diagram exhibits the general features of the schematic = diagram of=20 Figure 1:=20 Instead of overcoming the prohibitively high energy barrier for=20 dissociation of the reacting molecules, the catalyst offers an = alternate=20 reaction path through formation of intermediate chemisorption = complexes=20 whose energy differences can be readily surmounted by the = available=20 thermal energy.=20

    Figure 10. Mechanism = and=20 potential energy diagram of ammonia synthesis on iron.[26]=20 The energies are given in kJ mol-1.
    [Normal View 14K | = Magnified View=20 27K]

    The kinetic parameters associated with the individual reaction = steps=20 can be put together to calculate the steady-state yield of ammonia = formation for given external parameters. Figure 11=20 shows a plot of the ammonia yield derived on the basis of this = kinetic=20 model as a function of the experimental yields in industrial = plants.[27]=20 The data points barely deviate from the straight line marking = complete=20 agreement between theory and experiment. This result could be = confirmed=20 also by others[28]=20 and demonstrates that in this case the surface science=20 approach is indeed able to lead even to a quantitative description = of an=20 industrial reaction of great relevance.=20

    Figure 11. = Microkinetics of=20 catalytic ammonia synthesis: Comparison of the yield = calculated on=20 the basis of the mechanism presented in Figure 10=20 (y axis) with experimental data from industrial = plants=20 (x axis).[27]
    [Normal View 5K | = Magnified View=20 9K]

    3. Self-Organisation and=20 Complexity: Oxidation of Carbon Monoxide

    One of the major applications of heterogeneous catalysis in our = days=20 concerns protection of the environment through removal of toxic = substances=20 from car exhausts. Oxidation of carbon monoxide to carbon dioxide=20 (2 CO+O22 CO2) is the simplest of these = reactions and is=20 depicted schematically in Figure 12.=20 The exhaust gas flows through the catalytic converter, where the = molecules=20 interact with the surfaces of finely divided metal particles from = the=20 platinum group. Thereby the O2 molecules are = dissociatively=20 chemisorbed, and the formed Oad species interact with=20 chemisorbed CO molecules to form CO2, which is = immediately=20 released into the gas phase.=20

    Figure 12. Cartoon = illustrating=20 a car exhaust catalyst and the mechanism of CO = oxidation.
    [Normal View 48K | = Magnified View=20 106K]

    The structures formed by chemisorbed O and CO on a Rh(111) = surface are=20 shown as an example in Figure 13:[29]=20 The CO molecules are in this case bonded through the C atom = in on top=20 positions. They exhibit always the tendency to form densely packed = layers,=20 eventually even with occupancy of different adsorption sites[30]=20 (Figure 13 a).=20 The O atoms, on the other hand, occupy threefold-coordinated = sites=20 and form a rather open mesh of a 2=D72 structure = (Figure 13 b).=20 Since an O2 molecule in order to become dissociated = requires an=20 ensemble of neighboring empty surface atoms, this process will be=20 inhibited as soon as the CO coverage exceeds a certain critical = value. The=20 open structure of the O adlayer, on the other hand, still = permits=20 adsorption of CO, leading to a mixed phase, as reproduced in=20 Figure 13 c,=20 where the two reactants are in close contact and can readily react = to form=20 CO2. Under steady-state flow conditions in a mixture of = O2+CO, the surface of the catalyst will soon be fully = covered=20 by adsorbed CO, which prevents oxygen adsorption and hence = suppresses the=20 reaction. This problem can only be overcome if the temperature is = high=20 enough (450 K) to enable continuous desorption of part of = the=20 adsorbed CO so that gaseous O2 may compete for these = free=20 adsorption sites. (This is the reason why the catalyst of your car = does=20 not work in the cold but needs a certain minimum temperature.) The = sequence of reaction steps and the energy diagram for this = reaction are=20 depicted in Figure 14:=20 After chemisorption of the reactants, = Oad+COad may=20 react according to the Langmuir-Hinshelwood mechanism[31]=20 by overcoming an activation barrier of = 100 kJ mol-1=20 (which is only about half as high at higher coverages[31]) - a=20 result that could also be confirmed theoretically on the basis of = DFT=20 calculations.[32]=20

    Figure 13. Structures = of CO (a),=20 O (b), and O+CO (c) chemisorbed on a Rh(111) surface.[29]=20 Distances are given in =C5.
    [Normal View 36K | = Magnified View=20 83K]

    Figure 14. Mechanism = and energy=20 diagram for the catalytic oxidation of CO on Pt.
    [Normal View 12K | = Magnified View=20 25K]

    Under steady-state flow conditions, the rate of product = formation will=20 usually be constant and a function of the external parameters = temperature=20 and partial pressure of O2 and CO - however, = there=20 are exceptions under rare conditions: Already around 1970 it was = found in=20 Wicke's laboratory[33]=20 that, for supported Pt catalysts, the rate sometimes exhibits = temporal=20 oscillations. Such a situation can also be found with a = well-defined=20 Pt(110) surface as shown in Figure 15:[34]=20 At the time marked by an arrow, the O2 pressure was = raised=20 stepwise from 2.0 to 2.7=D710-4 mbar. As a = consequence the=20 rate slowly increased and then developed periodic variations with=20 eventually constant high amplitudes.=20

    Figure 15. Onset of = temporal=20 oscillations of the rate of CO2 formation on a = Pt(110)=20 surface.[34]=20 T=3D470 K;=20 = pCO=3D3=D710-5 mbar.
    [Normal View 17K | = Magnified View=20 37K]

    Characteristic for the present system is that it is far away = from=20 equilibrium and may develop so-called dissipative structures, as = explored=20 in detail by Prigogine (Nobel Prize 1977)[35]=20 and by Haken[36]=20 in the framework of synergetics. A particularly spectacular = example for=20 such behavior from population dynamics is reproduced in = Figure 16,[37]=20 which shows the variation with time of the number of furs from = hares and=20 lynxes delivered to Hudson's Bay Company. The oscillating = populations of=20 both species are coupled to each other, with a certain phase = shift. The=20 reason seems to be quite obvious: If the lynxes find enough food = (=3Dhares)=20 their population grows, while that of the hares decays as soon as = their=20 birth rate cannot compensate their loss any more. When the supply = of hares=20 drops, the lynxes begin to starve and their population also decays = so that=20 that of the hares can recover. The variations of the populations = of the=20 two species x and y can be approximately modeled in = the=20 language of chemical kinetics in terms of two coupled, nonlinear=20 (ordinary) differential equations (Lotka-Volterra model) as shown = in=20 Figure 17=20 together with their solution for properly chosen parameters = and . This solution exhibits just the = qualitative=20 behavior of the data of Figure 16.=20

    Figure 16. Variation = of the=20 number of furs n (in thousands) from hares and lynxes = delivered to Hudson's Bay Company with time.[37]
    [Normal View 43K | = Magnified View=20 96K]

    Figure 17. The = Lotka-Volterra=20 model describing the observation in Figure 16.
    [Normal View 27K | = Magnified View=20 58K]

    Mathematical description in terms of nonlinear differential = equations=20 is essential for these effects, and therefore this field is also = denoted=20 as nonlinear dynamics.

    With the oscillatory kinetics in the CO oxidation on Pt(110), = the=20 situation is still somewhat more complicated. In this case, the = reason for=20 this effect has to be primarily sought in the structure of the = Pt(110)=20 surface and its transformation under the influence of adsorbates. = As=20 already recognized by Langmuir:[38]=20 The atoms in the surface of a crystal must tend to = arrange=20 themselves so that the total energy will be a minimum. In general, = this=20 will involve a shifting of the positions of the atoms with respect = to each=20 other.

    Such a reconstruction is exhibited by the clean Pt(110) = surface.[39]=20 Instead of the termination by the corresponding bulk crystal plane = (Figure 18 b:=20 1=D71 structure), every second row along the [10] direction is missing, giving = rise to a=20 1=D72 structure (Figure 18 a).=20 In this way, small facets with (111) orientation are exposed, = leading=20 to a lower energy than with the 1=D71 phase. The two phases = differ also=20 with respect to their adsorption properties: Chemisorption of CO = is=20 accompanied by a higher adsorption energy on the 1=D71 phase = than on=20 the 1=D72 structure, so that local 1=D721=D71 transformation takes place as soon as the CO = coverage exceeds=20 a value of 0.2 monolayers (ML).[40]=20 On the other hand, the sticking coefficient for dissociative = oxygen=20 coverage on the 1=D71 phase exceeds that on the = 1=D72 phase by about=20 50 %.[41]=20 The occurrence of temporal oscillations in the rate of = CO2 can=20 now be rationalized as follows: If a clean Pt(110) surface (1=D72) = is=20 exposed to a proper mixture of CO+O2, adsorption of CO = will=20 suffice to cause local 1=D721=D71 transformation. On the newly created = 1=D71 patches, the=20 oxygen sticking coefficient will be higher, so that a higher=20 O coverage will be built up, giving rise to an enhanced = production of=20 CO2. By this latter process, the excess CO will be = consumed so=20 that the surface structure transforms back from 1=D71 to 1=D72, = and one cycle=20 is completed. Mathematical modeling requires in this case three = variables,=20 the coverages of O and CO, and the fraction of the surface present = as the=20 1=D71 phase. Solution of the resulting three coupled = nonlinear=20 differential equations for properly chosen parameters is shown in=20 Figure 19=20 and reproduces the experimental findings.[42]=20

    Figure 18. Structures = of the=20 Pt(110) surface:[39]=20 a) the 1=D72 structure of the clean surface; = b) the=20 1=D71 structure representing termination of the bulk=20 structure.
    [Normal View=20 11K | Magnified = View=20 25K]

    Figure 19. Theoretical = description of the oscillatory kinetics of CO oxidation on a = Pt(110)=20 surface.[42]=20 T=3D540 K;=20 = pO2=3D6.7=D710-5 mbar;=20 = pCO=3D3=D710-5 mbar.
    [Normal View 15K | = Magnified View=20 28K]

    However, so far the story is still incomplete: If the elements = of an=20 extended system exhibit temporal oscillations as a whole, some = kind of=20 lateral coupling between these elements is required in order to = achieve=20 synchronization. As a consequence of these considerations, the = state=20 variables (i.e. the surface concentrations of the adsorbates=20 xi) are in general not only dependent on time = t=20 but also on the spatial coordinates ri. As = summarized in=20 Figure 20,=20 coupling between different regions on the surface is achieved by = transport=20 processes. If the heat capacity of the catalyst is low enough, = spots with=20 surface concentrations favoring higher reaction rates will also = attain=20 higher local temperature as a result of the exothermicity of the = overall=20 reaction, and then heat conduction across the catalyst surface = will=20 provide coupling between different parts. Such a situation will = usually be=20 found with oscillatory kinetics on supported catalysts under = high-pressure=20 conditions,[43]=20 but has also been studied in detail with a very thin=20 (ca. 200 nm) Pt(110) single-crystal foil, where periodic = variation of the reaction rate caused corresponding changes of the = temperature. The latter effect initiated varying thermal expansion = and=20 hence deformation, which was denoted as heartbeats of a catalyst.[44]=20

    Figure 20. = Spatio-temporal=20 self-organization in open systems far from = equilibrium.
    [Normal View 10K | = Magnified View=20 19K]

    Under isothermal conditions at low pressures, local differences = of the=20 surface concentrations cause surface diffusion of the adsorbates, = and a=20 mathematical description can now be obtained in terms of=20 reaction-diffusion equations, that is, a set of coupled nonlinear = partial=20 differential equations combining the kinetics with the diffusion = of the=20 adsorbed species (Figure 20).=20 The length scale of the resulting spatio-temporal concentration = patterns=20 is no longer governed by atomic dimensions but by the so-called = diffusion=20 length, which in our case is of the order of some tens of = micrometers.[45]=20 These patterns were imaged by the technique of photoemission = electron=20 microscopy (PEEM):[46]=20 Adsorbed O and CO species are accompanied by different electric = dipole=20 moments and hence different work function changes, which in turn = give rise=20 to varying intensities of photoemitted electrons. Dark areas in = the images=20 are essentially O-covered while brighter patches are CO-covered. = As an=20 example, Figure 21=20 shows so-called target patterns, concentric elliptic features = propagating=20 preferentially along the [10] direction of the Pt(110) = surface (where=20 CO diffusion is faster than along the [001] direction) on a=20 background changing periodically between bright (=3DCO-covered) = and dark=20 (=3DO-covered), while the external parameters of temperature and = partial=20 pressures are kept constant as indicated.[47]=20

    Figure 21. Target = patterns in=20 catalytic oxidation of CO on a Pt(110) surface as imaged by = PEEM.[47]=20 A real-time movie showing the pattern changes is presented = in the Supporting Information.
    [Normal View 38K | = Magnified View=20 88K]

    Under other external parameters, typical spiral waves as shown = in=20 Figure 22=20 develop and propagate with front speeds of a few m s-1. The core of a = spiral is=20 often formed by a region on the surface with enhanced defect = density, and=20 this effect is also responsible for the fact that the wavelengths = of the=20 spiral waves vary to some extent.[48]=20

    Figure 22. PEEM image = of the=20 formation of spiral waves in catalytic CO oxidation on a = Pt(110)=20 surface.[48]=20 T=3D448 K;=20 = pO2=3D4=D710-4 mbar;=20 pCO=3D4.3=D710-5 mbar. The = diameter of=20 the picture is 500 m. A real-time movie showing = the pattern=20 changes is presented in the Supporting Information.
    [Normal View 34K | = Magnified View=20 79K]

    Since the mechanism of this reaction and all its parameters are = well=20 established experimentally, these data may also be used to = simulate the=20 resulting patterns by numerical solution of the underlying = differential=20 equations. This is shown in Figure 23=20 for the case of spiral wave development.[49]=20 If the parameters are changed slightly, the solution no longer = exhibits=20 regular spirals, but they break up to form spiral turbulence or=20 spatio-temporal chaos (Figure 24).=20 Experimental verification of such a situation is demonstrated by=20 Figure 25.=20

    Figure 23. Computer = simulation=20 of the evolution of spiral waves in catalytic CO = oxidation.[49]
    [Normal View 79K | = Magnified View=20 192K]

    Figure 24. Computer = simulation=20 of the break up of spiral waves to chemical = turbulence.
    [Normal View 114K | = Magnified View=20 273K]

    Figure 25. PEEM image = from a=20 Pt(110) surface in the state of chemical turbulence.=20 T=3D548 K;=20 = pO2=3D4=D710-4 mbar;=20 pCO=3D1.2=D710-4 mbar. The = image size=20 is 360=D7360 m. A real-time movie showing = the pattern=20 changes is presented in the Supporting Information.
    [Normal View 39K | = Magnified View=20 86K]

    We have now reached a state in which a system that in principle = is very=20 simple - a chemical reaction between two diatomic = molecules on a=20 well-defined single-crystal surface with fixed external parameters = and for=20 which all individual reaction steps are = known - nevertheless=20 exhibits rather complex behavior. Such effects are generally = expected for=20 open systems far from equilibrium and are hence believed to govern = also=20 processes in nature. Our system can be considered to be a rather = simple=20 model for studying these types of phenomena. One might for example = be=20 interested to modify pattern formation from outside by affecting = one of=20 the control parameters. This can be done either locally be heating = a small=20 spot on the surface by laser light[50]=20 or globally by a feedback mechanism in which the actual reaction = rate (or=20 integral coverage of one of the surface species) is used to = regulate the=20 flow of one of the reacting gases.[51]=20 A series of patterns created in this way from a turbulent initial = state by=20 different strength and delay of the feedback is reproduced in=20 Figure 26.=20 These patterns are reminiscent of similar phenomena found in = nature=20 (Figure 27),=20 but also of Vincent van Gogh's vision of our world in his = painting=20 The Starry Night (Figure 28).=20

    Figure 26. = Transformation of a=20 state of spiral turbulence into other different patterns by = a=20 feedback mechanism with different strength and delay of the=20 feedback.[51]
    [Normal View 69K | = Magnified View=20 135K]

    Figure 27. Phenomena = of pattern=20 formation found in nature: the structure of the retina and = leopard=20 fur.
    [Normal = View 39K=20 | Magnified View=20 96K]

    Figure 28. Vincent=20 van Gogh's painting The Starry Night.
    [Normal View 70K | = Magnified View=20 157K]

    4. Conclusions
    3D4. Conclusions=20

    This is no review article but more a brief account for a = broader=20 audience of some of the work that had been considered to be the = basis for=20 the awarding of the Nobel Prize. Numerous co-workers were involved = in our=20 continuing attempt to understand how chemical reactions on solid = surfaces=20 take place. Without their efforts, the results presented herein = could not=20 have been achieved, and therefore I am heartily grateful to all of = them.=20 Their names as well as a complete bibliography up to 2004 can be = found in=20 a recent special issue of the Journal of Physical Chemistry = B.[52]

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    52 Special issue: J. Phys. Chem. B=20 2004, 108, 14 183-14 788. ------=_NextPart_000_0043_01C915B5.F66DBAA0 Content-Type: text/html; charset="Windows-1252" Content-Transfer-Encoding: quoted-printable Content-Location: http://www3.interscience.wiley.com/blank.html UNTITLED_PAGE= ------=_NextPart_000_0043_01C915B5.F66DBAA0--