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Reactions at Surfaces: from Atoms to Complexity (Nobel Lecture)** Gerhard Ertl*

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Reactions at Surfaces: from Atoms to Complexity (Nobel Lecture)** Gerhard Ertl* Reviews G. Ertl Angewandte Chemie 3524 www.angewandte.org 2008 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim Angew. Chem. Int. Ed. 2008, 47, 3524 – 3535 Angewandte Heterogeneous Catalysis Chemie DOI: 10.1002/anie.200800480 Heterogeneous Catalysis Reactions at Surfaces: From Atoms to Complexity (Nobel Lecture)** Gerhard Ertl* Keywords: ammonia synthesis · carbon monoxide · Nobel lecture · oscillating reactions · surface chemistry From the Contents 1. Introduction 3525 2. The Surface Science Approach to Heterogeneous Catalysis: Ammonia Synthesis 3527 3. Self-Organisation and Complexity: Oxidation of Carbon Monoxide 3529 4. Conclusions 3534 1. Introduction The secretary of the Royal Swedish Academy of Sciences, the famous chemist Jöns Jacob Berzelius, published since 1820 annual review articles on the most significant new develop- ments in his field. Since the early 19th century there were observations from several laboratories that certain substances influenced the progress of a chemical reaction without being consumed and hence apparently not being affected by this Figure 1. Energy diagram illustrating the progress of a chemical reaction. For example, Johann Wolfgang Döbereiner, profes- reaction with and without a catalyst. sor of chemistry at the University of Jena, reported in July 1823 to his minister, Johann Wolfgang von Goethe, “that finely divided platinum powder causes hydrogen gas to react with k being Boltzmanns constant and T the temperature, with oxygen gas by mere contact to water whereby the platinum and accordingly not all molecular encounters will be success- itself is not altered”.[1][***] In his report published in 1835, ful, but only a fraction eÀE*/kT. An increase of the reaction Berzelius defined this phenomenon as “catalysis”, rather in probability (= rate) can be achieved by either increasing the order to introduce a classification than to offer a possible explanation.[2] Throughout the rest of this century, the term catalysis remained heavily debated[3] until around 1900 [*] Prof. Dr. G. Ertl Fritz-Haber-Institut der Max-Planck-Gesellschaft Wilhelm Ostwald proposed its valid definition in terms of 14195 Berlin (Germany) the concepts of chemical kinetics: “A catalyst is a substance Fax : (+ 49)30-8413-5106 which affects the rate of a chemical reaction without being part E-mail: [email protected] [4][ ] of its end products”. **** In 1909, Ostwald was awarded the [**] Copyright The Nobel Foundation 2007. We thank the Nobel Nobel Prize in Chemistry for his contributions to catalysis. Foundation, Stockholm, for permission to print this lecture. A chemical reaction involves breaking of bonds between Supporting information for this article is available on the WWW atoms and the formation of new ones. This process is under http://www.angewandte.org or from the author. [***] “daß das rein metallische staubfeine Platin die höchst merkwürdige associated with transformation of energy, and the energy Eigenschaft hat, das Wasserstoffgas durch bloße Berührung zu bestim- diagram illustrating the progress of a reaction A + B!Cis men, daß es sich mit Sauerstoffgas zu Wasser verbindet” depicted schematically in Figure 1. The activation energy E* [****] “Ein Katalysator ist jeder Stoff, der, ohne im Endprodukt einer to be surmounted is usually provided by thermal energy kT, chemischen Reaktion zu erscheinen, ihre Geschwindigkeit verändert.” Angew. Chem. Int. Ed. 2008, 47, 3524 – 3535 2008 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim 3525 Reviews G. Ertl temperature or by lowering the activation energy E*. The molecules eventually leave the surface (= desorption). If latter is provided by the catalyst, which through the formation operated in a flow reactor, the catalyst can in this way of intermediate compounds with the molecules involved in continuously operate without being consumed. the reaction provides an alternate reaction path as sketched One of the first and still most important technical by the dashed line in Figure 1 which is associated with smaller applications of this principle was realized about 100 years activation barriers and hence a higher overall reaction rate. In ago: Owing to the continuous increase of the world popula- the last step, the product molecules are released from the tion and exhaustion of the natural supply of nitrogen catalyst, which is now available for the next reaction cycle. If fertilizers, the world was facing a global threat of starvation. the reacting molecules and the catalyst are in the same As Sir William Crookes, president of the British Association (gaseous or liquid) phase, the effect is called homogeneous for the Advancement of Science, formulated it:[5] “... all catalysis. In living systems, macromolecules (= enzymes) play civilized nations stand in deadly peril of not having enough to the role of catalysts. In technical reactions, mostly the eat … the fixation of atmospheric nitrogen is one of the great interaction of molecules with the surface of a solid is decisive. discoveries awaiting the ingenuity of chemists”. The principle of this heterogeneous catalysis is depicted Nitrogen fixation means transformation of the abundant schematically in Figure 2. N2 molecule (which constitutes about 80% of our air) from its state of very strong bond between the two N atoms into a more reactive form according to the reaction N2 + 3H2 ! 2NH3. This reaction of ammonia formation could be realized in 1909 by Fritz Haber (Nobel Prize 1919) in the laboratory by the use of an osmium catalyst in a high-pressure flow apparatus.[6] Carl Bosch (Nobel Prize 1931) from the BASF company started immediately to develop this method into a technical process, and the first industrial plant started operation in 1913, only a few years later. Figure 3 shows the growth of the world population together with the ammonia production over the last century,[7] and it is quite obvious that our present life would be quite different without the develop- ment of the Haber–Bosch process. Figure 2. The principle of heterogeneous catalysis. The atoms in the surface layer of a solid have fewer neighbors than those in the bulk and are hence chemically unsaturated and may form new bonds (= chemisorption) with suitable molecules impinging from the adjacent gas or liquid phase. By this step, existing bonds will be modified or may even be broken (= dissociative chemisorption). The surface species formed may jump from one site to neighboring ones, then may react with others, and the formed produced Gerhard Ertl was born in 1936. He studied physics at the University of Stuttgart and Figure 3. Variation of the world population (in 109) and the ammonia received his PhD in physical chemistry in production (in 106 metric tons of nitrogen) during the 20th century.[7] 1965 from the Technical University of Munich under the supervision of Heinz Gerischer in the field of electrochemistry. In However, large-scale technical production would not have 1968 he became professor of physical been possible without the availability of large quantities of a chemistry at the Technical University of cheap catalyst. (The complete world supply of the precious Hanover, in 1973 he moved to the Ludwig metal osmium was only 80kg in those days.) This task could Maximilians University of Munich, and in be solved successfully by Alwin Mittasch[8] who in thousands 1986 he became the successor of his PhD of tests found that a material derived from a Swedish iron ore advisor as director of the Fritz Haber Insti- tute. At the same time he became honorary exhibited satisfactory activity. This type of doubly promoted professor at the Technical University of Berlin and the Free University of iron catalyst is in fact still in use today in almost all industrial Berlin; in 1992 the Humboldt University of Berlin also awarded him this plants. title. Among his many other awards are the Wolf Prize in Chemistry Remarkably, despite the enormous technical significance (1998), the Japan Prize of the Science and Technology Foundation of of the Haber–Bosch reaction and despite of numerous Japan (1992), and the Karl Ziegler Prize of the German Chemical Society laboratory studies, its actual mechanism remained unclear (Gesellschaft Deutscher Chemiker, GDCh, 1998). over many years. P. H. Emmett, one of the pioneers of 3526 www.angewandte.org 2008 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim Angew. Chem. Int. Ed. 2008, 47, 3524 – 3535 Angewandte Heterogeneous Catalysis Chemie catalysis research, was honored in 1974 by a symposium at The “surface science” approach that Langmuir had in which he concluded:[9] “The experimental work of the past mind was experimentally not yet accessible in his days, but 50 years leads to the conclusion that the rate-limiting step in began to become only available during the 1960s with the ammonia synthesis over iron catalysts is the chemisorption of advent of ultrahigh vacuum (UHV) and surface sensitive nitrogen. The question as to whether the nitrogen species physical methods.[12] Nowadays a whole arsenal of such involved is molecular or atomic is still not conclusively techniques is available to study the structural, electronic, or resolved …”. dynamic properties of such well-defined single-crystal surfa- ces. Bond-breaking upon chemisorption is perhaps the most 2. The Surface Science Approach to Heterogeneous important role of a catalyst. Figure 5 shows schematically the Catalysis: Ammonia Synthesis The problem involved in the study of the surface chemistry of “real” catalysts becomes evident if we look on an electron micrograph of the Mittasch catalyst as reproduced in Figure 4:[10] A catalyst with high activity has to exhibit a Figure 4. Surface topography and chemical composition of an indus- trial ammonia synthesis catalyst.[10] 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 rather high specific surface area, which in this case is about the distance x of the molecule from the surface and the separation y 2 1 20m gÀ as reflected by nanometer-sized active particles.
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