Editorial pubs.acs.org/accounts
Faster, Catalyst! React! React! Exploiting Computational Chemistry for Catalyst Development and Design Guest Editorial for the Accounts of Chemical Research special issue on “Computational Catalysis for Organic Synthesis”.
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Schoenebeck, Sunoj, Tantillo, and Wheeler). In most cases, examples are discussed in which theory and experiment were used together to tackle complex mechanistic problems. Many contributions also describe tested or testable predictions made on the basis of results from computations. The scope of reactions and catalyst families covered in these Accounts is a clear indication that modern computational methods are applicable to many systems of synthetic interest and that applied theoretical chemists are not afraid to charge into these areas in pursuit of both understanding of minute mechanistic details and the development of general models of reactivity and selectivity that can be applied by synthetic chemists, even in the absence of high-level computations.
ow does one obtain a catalyst that accelerates a desired organic reaction or controls its selectivity such that one of many possible products is produced in high yield? There are many answers to this question: first, one might screen existing catalysts and hope for the best; second, one could systematically, randomly, or rationally make changes to known catalysts and test the activity of the modified molecules; third, one could try to design rationally a new catalyst from scratch. Computational chemistry can help with all of these approaches. It is possible to screen existing catalysts for activity and selectivity computationally. In addition, computational prediction of structure−activity relationships (SARs) for catalyst families can be carried out. And, one can obtain detailed information about transition state structures that can be used in the design of new catalysts that will bind transition state structures for desired reactions selectively. Why are such computational approaches not commonplace? Two reasons jump to mind: (1) Specialized skills are required to carry out the necessary calculations correctlyan argument for more skilled applied theoretical organic chemists. (2) Sufficiently accurate calculations are not always affordable; that is, meaningful results may not be obtainable quickly enough to be usefulan argument for continued development of both software and hardware for use by chemists. Nonetheless, the field of computational chemistry has progressed to the point where the mechanisms and selectivity of many catalyzed organic reactions can be interrogated at atomic resolution without the use of model catalysts and substrates, often in an acceptable amount of time. While challenges and pitfalls remain, for example, appropriate treatment of solvent effects, entropy contributions, and conformational mobility, meaningful predictions of reactivity can be made, allowing for full engagement in an explain → predict → design→ test process. This is true in the fields of homogeneous, heterogeneous, and enzymatic catalysis, but this special issue of Accounts of Chemical Research is focused on the first, highlighting recent contributions from computational/ theoretical chemists studying organocatalysts and organometallic catalysts for reactions of interest to those embroiled in the synthesis of both simple and terribly complex organic molecules. Contributors to this issue describe successes and limits in modeling selectivity (Aviyente, Cheong, Eisenstein, Goodman, Himo, Houk, Jørgensen, Paton, Sigman, Sunoj, Tantillo, Wheeler, Wiest, and Wu), nonstandard methods for obtaining and characterizing structures and dynamical properties of catalyst−transition state assemblies (Morokuma, Ujaque, and Wiest), and the unique features of both metal-based catalysts (Baik, Chen, Eisenstein, Himo, Houk, Morokuma, Paton, Schoenebeck, Tantillo, Ujaque, Wiest, Wu, and Yoshizawa) and organocatalysts (Aviyente, Cheong, Houk, Jørgensen, Paton, © 2016 American Chemical Society
Dean J. Tantillo, Guest Editor
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University of CaliforniaDavis
AUTHOR INFORMATION
Notes
Views expressed in this editorial are those of the author and not necessarily the views of the ACS.
Published: June 21, 2016 1079
DOI: 10.1021/acs.accounts.6b00249 Acc. Chem. Res. 2016, 49, 1079−1079
