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US 6,440,711B1 34 hyde and from formaldehyde to methanol. Thus, the present invention is also directed to each of such steps and sub combinations of steps, Which are assisted by retaining the enZymes in a microporous matrix. Accordingly, the present invention is also directed to a novel method comprising reduction of formaldehyde to methanol by alcohol dehydrogenase catalysis, to a novel methodcomprisingreductionofformatetoformaldehydeby formaldehyde dehydrogenase catalysis, to a novel method comprisingreductionofcarbondioxidetoformatebyfor 10 matedehydrogenasecatalysis,toanovelmethodcomprising reduction of carbon dioxide to formaldehyde by a combi nation of formate dehydrogenase catalysis and formalde hyde dehydrogenase catalysis, and to a method comprising reduction of formate to methanol by a combination of 15 formaldehyde dehydrogenase catalysis and alcohol dehy drogenasecatalysis. Among the several advantages found to be achieved by the present invention, therefore, may be noted the provision of a method for synthesis of methanol from carbon dioxide at loW temperature; the provision of such method that is energy efficient; the provision of such method that yields high conversion rates; the provision of such method that avoids the need for special equipment adapted to high temperatureorhighlycorrosiveenvironments;andthepro 25 vision of related methods associated With the intermediary steps of such synthesis. In addition, it also has been found that the reduced form of the cofactor can be regenerated, recycled and re-used repeatedly. In other Words, after the reduced form of the cofactor is oxidiZed by donating an electron to the dehy drogenase catalyZed reduction scheme of carbon dioxide to methanol, the reduced form of the cofactor may be regen erated from the form resulting from the oxidation, thereby alloWing repeated re-use of a single dose of the cofactor. In fact, it has been found that the reduced cofactor serving as theelectrondonorcanberegeneratedandreusednotjusta feW times, but at least many thousands of times. As a result, the method of this invention provides a surprisingly practical, loW-cost, loW energy consumption and efficient mechanism for converting carbon dioxide to methanol. Inshort,accordingtotheprocessofthepresentinvention, a matrix containing a certain combination of dehydrogenase enZymes may be contacted With carbon dioxide to induce an ordered series of reduction reactions catalyZed by those enZymes ultimately to produce methanol. In practice, atmo spheric carbon dioxide from any source, even atmosph may simplybebubbledthroughWatercontainingaporousmatrix that contains the enZymes entrapped in its pores. The Water or matrix may contain several other components as Well. Among the potential additional components may be noted severalthatareparticularlydesirable;namely,aterminal electron donor, Which donates electrons to the reduction reactions, and a mechanism for regeneration of the electron donor for further electron donation. Each reduction step in the reaction scheme from carbon dioxide to methanol also consumes tWo hydrogen ions (protons) and so requires a source for such ions. In the embodiment of this invention that incorporates regeneration of the electron donor, the aqueous system may also include a mechanism for such regeneration. TheMatrix The matrix Within the enZymes are entrapped is, as noted above, a microporous, even nano-porous, structure capable of retaining the enZymes Within the pores or interstices, but such that the enZymes also may be exposed to carbon dioxide transported (such as by bubbling) to or through the matrix. The matrix may be in the form of small particles or a poWder (perhaps as the result of grinding) and suspended in the medium (e.g., Water) in Which the series of reduction reactions takes place. As Will be explained beloW in the sectiondiscussingregenerationoftheterminalelectron BRIEF DESCRIPTION OF THE DRAWINGS FIG. 1 is a schematic illustration of the series of reduction reactions of this invention; and FIG. 2 is a schematic illustration of the the reduction of this invention from carbon dioxide to methanol, With regen eration and recycling of NADH. DETAILED DESCRIPTION OF THE PREFERRED EMBODIMENTS 35 In accordance With the present invention, it has been discovered that by contacting a combination of dehydroge nase enZymes With carbon dioxide, a loW temperature, high-yield reduction of the carbon dioxide to methanol may be carried out Without special equipment designed for high temperatures or corrosive environments. Moreover, it has been found that this process is highly selective, resulting in highyieldofmethanolandlitleifanyformationofunde 45 sirableby-products.Thisdiscoveryisparticularlysurprising donor,aparticularlyadvantageoustechniqueforsuchregen in vieW of the fact that the presence of the dehydrogenase enZymes employed in the subject reduction are knoWn under conventional conditions to induce the opposite reaction, from methanol to carbon dioxide. HoWever, itnoW has been found that by entrapping the enZymes Within a matrix of micropores(i.e.,verysmallpores)—especially,nano-pores on the order of billionths of meters in diameter—and par ticularly When driven by the presence of an abundance of donative electrons, for instance from an excess of the 55 reduced form of a cofactor of the enZymes (such as nicoti namide adenine dinucleotide relative to the unre duced form (such as nicotinamide adenine dinucleotide (AND’')), the equilibrium of the reaction can be shifted so that the tendency toWard oxidation can be reversed, causing the reaction to proceed as a reduction of carbon dioxide to methanol. Although the inventor does not Wish to be bound to any particular theory, he believes that the physical con straints of the small volume pores results in localiZed areas ofrelativereactantconcentrationsthatadjustthestoichiom 65 etry at the reaction sites such that the equilibrium of the reaction favor reduction rather than oxidation. eration involves photo-regeneration. Therefore, because photo-regeneration relies on transmission of light through thematrix(orsuspensionofmatrixparticles),itisdesirable in such case that the matrix be transparent. The matrix may be made up of an inorganic solid such as an oxide, Zeolite, meso-porous silicates, extended netWorks or layered materials. HoWever, ithas been found that sol-gel glasses are especially Well suited to the subject process and so are particularly desirable matrix materials. The sol-gel process is a Well-known technique involving the transition of a solution system from a liquid “sol” into a solid “gel” phase. Sols usually are prepared from a precursor such as an inorganic metal salt, a metal alkoxide or another metal organiccompound.Preferably,thesol-gelglassusefulinthe subject invention is based on a silica precursor, such as those of the type (OR)4Si, RSi(OR)3, RSi(OR)2, or (OR)3Si spacer-Si(OR)3,WhereinR isanalkyl,alkenyl,alkynyl,or aryl group, and the spacer unit comprises an organic unit, an inorganicunit,oracombinationthereof.Althoughalkoxides or silicon are preferred, other metal oxides, such as those prepared by adding methanol, ethanol, isopropanol or otherPDF Image | DEHYDROGENASE ENZYMATIC SYNTHESIS OF METHANOL
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