Catalytic Process Development for Renewable Materials

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Much less explored is the valorization of sulfur- and phosphorus-containing biomass components, although they find some high market value applications. Catalysis plays a central role to enable the conversion of biomass into value-added products with high activity and selectivity. Further developments made by chemical engineers and process technologists will be required to make those processes economically feasible and competitive with current synthetic schemes from fossil resources.

This perspective highlights the most recent advances and the upcoming challenges in the development of renewable and sustainable routes toward heteroatom-containing chemicals. More by Max J. More by Huiying Yang. More by Ning Yan. Article Views Altmetric -. Citations Cited By. This article is cited by 17 publications. ACS Omega , 4 11 , DOI: ACS Omega , 4 5 , Organic Letters , 21 9 , Journal of the American Chemical Society , 9 , Production of 1,2-Cyclohexanedicarboxylates from Diacetone Alcohol and Fumarates.

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Organic Letters , 20 19 , Dina Maniar, Katharina F. Although biomimetic catalysts were catalytic under mild conditions for hydroxylation of certain alkanes, their potential commercial use is limited. None has been robust enough to merit continued research, and rates per volume of catalyst in the most optimistic extrapolation of possibilities are still orders of magnitude below commercial requirements. Stable, heterogeneous, mixed-metal oxide analogs might provide the same advantages as biomimetic catalysts without their limitations.

Additional novel nonbiomimetic-catalytic approaches to primary oxidation of alkanes to alcohols should be investigated by academia.

The recent increase in the production of fine chemicals has been driven by the increasing number of new pharmaceuticals, many of which are being synthesized as single enantiomers. The fine chemical industry is actively pursuing the use of catalysis in chiral syntheses. Given the high value and strict purity control necessary for manufacturing fine chemicals, product yield and selectivity are important criteria in the design of catalytic processes. The functional complexity of the reaction substrates and products present significant challenges to chemoselectivity, regioselectivity, and stereoselectivity.

In addition to metallic and organometallic catalysts, enzymes and microorganisms both biocatalysts are rapidly becoming attractive for chiral synthesis, especially for specific reaction steps that are difficult to achieve by other chemical methods. Biocatalysis or biotransformation is also proving to be valuable in the chemical modification of naturally synthesized compounds e.

The identification and exploitation of new catalysts in the synthesis of fine chemicals will require continuing development of enabling technologies. Rapid preparation and screening of candidates by high-speed automation and analytical detection systems will greatly accelerate the identification of novel catalysts, as well as provide efficient optimization within catalyst families. The rational design of metal ligands the basis for many stereoselective catalysts will be assisted by advances in computational chemistry towards predicting optimal transition-state behaviors.

For heterogeneous catalysts, computational chemistry and the analysis of surface-bound intermediates will improve our understanding of catalytic mechanisms and lead to improved catalysts. And finally, the use of in-situ analytical probes to uncover catalytic reaction mechanisms will lead to better optimization of their yield and selectivity.

Catalytic processes could enable the use of simpler, cheaper substrates while minimizing prefunctionalization or the need for protecting groups. Thus, synthetic versatility would be enhanced without requiring more complex substrates. The development of selective catalytic oxidations using simple oxidants, and catalytic activation of carbon-hydrogen bonds and schemes to generate carbon-carbon bonds would all be of great benefit to the fine-chemical industry. The Office of Industrial Technologies should support the development of catalysts with substantially improved synthetic versatility and atom economy.

Catalytic selectivity is essential to the synthesis of fine chemicals, where yields of products from high-value substrates are paramount and the minimization of difficult-to-remove impurities can determine the choice of synthetic options. In particular, the asymmetric hydrogenation of carbon-carbon, carbon-oxygen, and carbonnitrogen bonds by organometallic complexes, which is used extensively in fine-chemical processing, could be improved by the development of novel chiral ligands. Selectivity in heterogeneously catalyzed, fine-chemical reactions is also important, and the development by the commercial pharmaceutical industry of novel catalysts, chiral surface modifiers, and fundamental knowledge of reaction mechanisms will lead to improvements in selectivities.

Successful processing of a catalytic reaction step often involves optimizing of reaction conditions to increase yield and selectivity, as well as careful control of catalyst deactivation and recovery to allow for the recycling and reuse of expensive catalysts. The efficient development of a biocatalyst for the synthesis of both fine chemicals and bulk chemicals will require the parallel development of three enabling technologies.

Screening, miniaturization, and automation will also be required to evaluate available and potential biocatalysts. Second, the development of microchip technology for the rapid study of enzyme kinetics under a variety of chemical and physical conditions is very important for rapid process scale-up. Microchips can also enable molecular biologists to identify genes responsible for specific biocatalysts of interest. Finally, data management systems must be developed to ensure that the enormous amount of data being generated from enzyme screening and characterization can be easily retrieved and reviewed in a way that leads to a better understanding of trends in biocatalyst performance.

Catalytic process development for renewable materials : Green Processing and Synthesis

A number of separate steps should be investigated in the biocatalyst enzymatic process. The first step, and the most critical, is to design enzymes with specific characteristics e. The second step is to stabilize this enzyme long enough to produce the desired product. The third step is to maintain the enzymatic activity in a nonaqueous environment because the organic synthetic product is often nonaqueous.

The fourth step is to maintain the level of reactivity of the enzyme throughout the production period, which can be done by a cofactor generation process. Enzymes are well known catalysts that accept not only their specific native substrates but also closely related ones.

Characterization

However, to increase their yield or conversion rate, the fine-chemical industry must learn how to alter their substrate specificity e. Fundamental studies of enzyme structures coupled with molecular biology studies will be important for achieving this goal. The committee believes that designing enzymes with specific characteristics e. The Office of Industrial Technologies should support the development of enzymes with substrate specificity and stereoselectivity for chiral synthesis in fine chemicals.

Continued research in this area will have a high probability of improving enzyme stability. A fundamental knowledge base will be necessary to achieve stability at the molecular level when a biocatalyst is exposed to various environments. In addition to chemical and physical studies, methods of improving intrinsic enzyme stability through molecular biological approaches, such as directed evolution, should be investigated. Many chemical intermediates that become enzyme substrates are insoluble in aqueous solutions, requiring that the enzyme system function in a nonaqueous environment.

Frequently, this causes a considerable decrease in enzyme activity.

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Additional studies should be conducted to achieve equal performance in both aqueous and organic solvents, but also to enhance performance in the organic solvents. A number of specific chemical reactions e. In the opinion of the committee, enzyme stability in nonaqueous environments is an important subject for further industry and university research.


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To ensure that certain important enzymes remain active throughout the reaction, the presence of another component, called a cofactor, is necessary. As the enzymatic reaction takes place, the cofactor component is reduced and must be regenerated to maintain the same level of enzymatic activity throughout the reaction. Although in-situ regeneration with isolated NADH-dependent nicotinamide adenine dinucleotide based enzymes has been used, alternatives should be investigated by industry or academia, including molecular biology to modify or eliminate the need for a cofactor.

Currently, crude petroleum is the primary source of petrochemicals. As domestic reserves of crude petroleum are reduced, U.

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Foreign oil-producing regions are trying to attract higher value products and higher value manufacturing jobs for their own populations, and the production of petrochemicals in proximity to the sources of crude petroleum gives them a significant cost advantage. In addition, although there is no shortage of crude petroleum today, long-term availability is a concern. In the near term, the U. In the longer term, however, the U. The United States still has plentiful reserves of coal and natural gas. Indeed, natural gas, which is plentiful worldwide, is increasingly being used.

Increasing the use of these domestic resources would somewhat negate the logistical advantages of other oil-producing regions. The large capacity of the U.


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In the terms of this discussion, alternative resources refers to noncrude-oil-based resources. Renewable resources refers to carbon resources available from biological, especially agricultural, sources. Catalysis will be crucial to using both alternative and renewable resources. Natural gas and, to a much lesser extent, coal are already being used to make synthesis gas used by the chemical industry: 1 to generate methanol and, in further reactions, with carbon monoxide to generate downstream products e.

Chemical Catalysis for Bioenergy Consortium (ChemCatBio)

Synthesis gas has several additional, smaller scale uses in the functionalization of various chemicals. However, this potential has not been completely realized. A large number of other potential products e. In many cases, the biggest hurdle to the commercialization of these chemicals is the high capital cost of generating and separating synthesis gas components. Therefore, the highest priority for the chemical industry is to increase the availability and reduce the cost of synthesis gas. A large number of processes for the generation of chemicals based on synthesis gas are competitive or nearly competitive with existing technology.

Examples include, but are not limited to, the production of ethylene glycol, ethanol, ethyl acetate, acetaldehyde, isobutanol, linear alcohols, and vinyl acetate. The high capital expenditures related to the generation and separation of synthesis gas components are the limiting factor in the implementation of these technologies. Therefore, the development of lower cost processes for generating, separating, and.

The Office of Industrial Technologies should support a study of alternative, lower cost means of producing synthesis gas from alternative resources. The chemical industry would greatly benefit from new technologies for the conversion of synthesis gas to chemicals. Most research is currently focused on the generation of oxygenates. The committee has strong reservations about using carbon dioxide as a carbon source in the chemical industry because a substantial amount of energy will probably be required to reduce it to an oxidation state useful for organic synthesis.

Therefore, it is not likely that carbon dioxide will be a cost-effective source of carbon, except as a means of increasing the carbon content of synthesis gas through the shift reaction or as a reaction solvent. The transportation-fuel industry may provide a strong impetus for shifting toward alternative resources. The transportation industry is now anticipating a need to reformulate transportation fuels to reduce their environmental impact, which could require fuels with a significant oxygen content. It is widely believed that the most likely source of the oxygenated component will be a synthesis gas-derived material.