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Biochemical Evolution. I. Polymerization on Internal, Organophilic Silica Surfaces of Dealuminated Zeolites and Feldspars (Biological Evolution͞volcanic Emissions)

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Biochemical Evolution. I. Polymerization on Internal, Organophilic Silica Surfaces of Dealuminated Zeolites and Feldspars (Biological Evolution͞volcanic Emissions) Proc. Natl. Acad. Sci. USA Vol. 95, pp. 3370–3375, March 1998 Geology Biochemical evolution. I. Polymerization on internal, organophilic silica surfaces of dealuminated zeolites and feldspars (biological evolutionyvolcanic emissions) JOSEPH V. SMITH* Department of Geophysical Sciences and Center for Advanced Radiation Sources, 5734 S. Ellis Avenue, University of Chicago, Chicago, IL 60637 and UOP Research Center, Des Plaines, IL 60017-5016 Contributed by Joseph V. Smith, December 29, 1997 ABSTRACT Catalysis at mineral surfaces might generate specimens. Bernal (1) preferred ‘‘life’’ to begin by catalytic replicating biopolymers from simple chemicals supplied by assembly on a mineral surface, but all attempts to assemble an meteorites, volcanic gases, and photochemical gas reactions. integrated scheme of physicochemical processes have signifi- Many ideas are implausible in detail because the proposed cant weaknesses. Concepts of catalysis that use organic com- mineral surfaces strongly prefer water and other ionic species pounds dispersed in aqueous ‘‘soups’’ require a mechanism for to organic ones. The molecular sieve silicalite (Union Carbide; concentrating the organic species next to each other on a 5 Al-free Mobil ZSM-5 zeolite) has a three-dimensional, catalytic substrate. After catalysis, the biochemically signifi- 10-ring channel system whose electrically neutral Si-O sur- cant polymers such as polypeptides and RNAs must be pro- face strongly adsorbs organic species over water. Three -O-Si tected from photochemical destruction by solar radiation and tetrahedral bonds lie in the surface, and the fourth Si-O points must not be heated too much. Only then could the energy- inwards. In contrast, the outward Si-OH of simple quartz and consuming replication/mutation of polymers yield the first feldspar crystals generates their ionic organophobicity. The primitive organisms. I am not concerned here with the sub- ZSM-5-type zeolite mutinaite occurs in Antarctica with sequent irreversible forward march to increasing diversity of boggsite and tschernichite (Al-analog of Mobil Beta). Archean species immune to Earth’s slings and arrows, although mineral mutinaite might have become de-aluminated toward silicalite surfaces are important for lichens and bacteria. during hot/cold/wet/dry cycles. Catalytic activity of silicalite The new concept is that certain materials have internal increases linearly with Al-OH substitution for Si, and Al surfaces that are both organophilic and catalytic, allowing atoms tend to avoid each other. Adjacent organophilic and efficient capture of organic species for catalytic assembly into catalytic Al-OH regions in nanometer channels might have polymers in a protective environment. These physicochemical scavenged organic species for catalytic assembly into specific features are related to the state-of-the art for zeolite catalysts polymers protected from prompt photochemical destruction. in the chemical industry, the observed properties of naturally Polymer migration along weathered silicic surfaces of mi- occurring zeolite and feldspar minerals, and a plausible frame- crometer-wide channels of feldspars might have led to assem- work for the accretion and early history of the Earth’s crust and bly of replicating catalytic biomolecules and perhaps primitive atmosphere. The accompanying paper in this issue of Proceed- cellular organisms. Silica-rich volcanic glasses should have ings (12) on weathered feldspars contains relevant concepts been abundant on the early Earth, ready for crystallization and observations. into zeolites and feldspars, as in present continental basins. The present proposal does not provide a detailed recipe for Abundant chert from weakly metamorphosed Archaean rocks catalytic formation of a replicating polymer. However, it may might retain microscopic clues to the proposed mineral ad- provide a conceptual framework from which plausible recipes sorbent/catalysts. Other framework silicas are possible, in- will ensue from laboratory experiments and crystal-chemical cluding ones with laevo/dextro one-dimensional channels. modeling. Although all biochemical ‘‘life’’ might have devel- Organic molecules, transition-metal ions, and P occur inside oped from a single left-handed chance event that has essen- modern feldspars. tially zero ‘‘probability’’ in terms of conventional ideas for chemical syntheses, multiple events of high probability are Although extended Darwinian natural selection coupled with preferred, of which one event may have been the actual trigger. Mendel–Watson–Crick genetic inheritance/mutation provides It would be wonderful, of course, if polypeptide chains, or even a plausible framework for integrating the patchy paleontolog- better RNA replicator/catalysts, turned up in actual experi- ical record with the increasingly complex biochemical zoo of ments on the proposed organophilic materials. It would be the present Earth, the actual chemical beginning of ‘‘life’’ still even more thrilling if a fragment of the abundant chert or other poses major challenges (1–11). How could the first replicating sediments in surviving Archaean terranes had survived meta- and energy-supplying molecules have been assembled from morphism to preserve some convincing evidence of primary simpler materials that were undoubtedly available on the early biocatalysis. Unless such encouraging evidence turns up, cau- proto-continents? Most cosmoscientists abhor spontaneous tion is warranted in proposing that ‘‘life’’ began merely as a generation—or the wave of a magic wand from ‘‘God’’ or trivial scientific event on a mineral catalyst. (From a philo- inheritance of ‘‘living’’ organisms from outer space. They sophic viewpoint, this is only a very restricted scientific aspect search for a plausible integrated geological/biochemical frame- of ‘‘life,’’ namely the assumed common ancestry and subse- work that allows Oparin–Watson–Crick–Darwin biological quent linkage of all biochemicals found in organisms. The evolution to begin on Earth using scientific features testable in complex debates on the cultural, societal, religious, and hu- a chemical laboratory and perhaps even observable in geologic manistic aspects of ‘‘life’’ are linked to the biochemistry but only at a simple level.) The publication costs of this article were defrayed in part by page charge First, the evidence from synthetic molecular sieves: general payment. This article must therefore be hereby marked ‘‘advertisement’’ in review (12). Silicalite, a molecular sieve invented by chemists accordance with 18 U.S.C. §1734 solely to indicate this fact. © 1998 by The National Academy of Sciences 0027-8424y98y953370-6$2.00y0 *To whom reprint requests should be addressed. e-mail: smith@geo1. PNAS is available online at http:yywww.pnas.org. uchicago-edu. 3370 Downloaded by guest on October 1, 2021 Geology: Smith Proc. Natl. Acad. Sci. USA 95 (1998) 3371 at Union Carbide Corporation (13), can be as close to pure molecules into the ZSM-5–silicalite and catalytic activity, the silica as the quality of the materials used for synthesis. Its following representative papers are selected: linear decrease of three-dimensional channel system is bounded by 10-rings from hydrophobicity with Al substitution (42); methanol adsorption a four-connected tetrahedral framework (14). All Si atoms are on acidic ZSM-5 and conversion to gasoline, xylene, etc. (43); surrounded by four oxygen atoms, and the stereogeometry is water adsorption and evidence for insignificant interaction such that the channels are lined by a three-connected net with with a dehydroxylated silica surface (44, 45); dependence of the fourth Si-O bond pointing into the silica. Hence, there are relaxation time of CH2 and CH3 groups on chain length and no silanol (Si-OH) species projecting into the channels. Sili- degree of adsorption of amines and conversion to diamines calite can adsorb molecules up to 6 Å across, including upon heating (46); structural positions, diffuse-reflectance benzene. Figure 5 of Flanigen et al. (13) demonstrates that spectroscopy, and two-patch heterogeneous model for adsorp- silicalite has a remarkable organophilic/hydrophobic nature, tion of benzene (47–51); structural perturbation of framework thus: ‘‘Traces of methanol, propanol, butanol, phenol, 1,4- geometry of H-ZSM-5 by sorbed p-xylene and naphthalene dioxane, pentane and hexane have been removed from water’’ (51–53); adsorption of CO on H-ZSM-5 and a hydrothermal and ‘‘Silicalite possesses a remarkable stability for a 33% product (54); and nature of silanol groups, defects, and porous crystal. It is stable in air to over 1,100°C, and only slowly structural heterogeneities in relation to water and benzene converts to an amorphous glass at 1,300°C. It is stable to most adsorption (55–58). mineral acids but reacts with HF similarly to quartz.’’ Based on this overall concept of a van der Waals silica-rich The reason for the organophilic/hydrophobic nature is quite surface, Pandora’s box of '4,000 minerals was examined for simple. Oil and water do not mix because the water molecules potential candidates as biochemical adsorbent/catalysts. In prefers ionic bonding and the organic molecules of the oil general, most ionic minerals, including clay minerals, are prefer van der Waals bonding. Hence, for a truly neutral unpromising. The obvious candidates come from three mineral surface, water molecules remain bonded to each other in an families: zeolites, feldspars, and silicas. ionic environment, allowing the organic molecules
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