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Kinetic Methodology. Blackmond has pioneered the development of Reaction Progress Kinetic Analysis (RPKA), a methodology combining highly accurate in-situ data collection with a rigorous mathematical analysis that permits rapid determination of concentration dependences of reactants. In contrast to the classical role of kinetics, in which measurements of concentration dependences most often are asked simply to corroborate a previously proposed mechanism, the Blackmond group’s approach is to employ kinetic studies at the outset of an investigation of ill-defined reaction network to suggest reaction mechanisms. This “kinetic-assisted mechanistic analysis” aids in the design of further supporting experiments including conventional mechanistic tools such as studies of isotope effects and spectroscopic studies for structural and compositional information. One of the most powerful aspects of the methodology is its ability to deconvolute rate processes occurring on the catalytic cycle from those occurring off the cycle. Prominent examples of the application of this methodology to quantitative understanding of complex organic reactions and reaction networks include asymmetric hydrogenation, asymmetric organocatalytic reactions, Pd-catalyzed C-C and C-N bond forming reactions, and transition-metal catalyzed competitive reactions including kinetic resolutions. Reaction Progress Kinetic Analysis finds important application in the pharmaceutical industry, where streamlining process R&D based on Blackmond’s kinetic analysis is becoming an industry-wide standard.
Kinetic Methodology. Blackmond has pioneered the development of Reaction Progress Kinetic Analysis (RPKA), a methodology combining highly accurate in-situ data collection with a rigorous mathematical analysis that permits rapid determination of concentration dependences of reactants. In contrast to the classical role of kinetics, in which measurements of concentration dependences most often are asked simply to corroborate a previously proposed mechanism, the Blackmond group’s approach is to employ kinetic studies at the outset of an investigation of ill-defined reaction network to suggest reaction mechanisms. This “kinetic-assisted mechanistic analysis” aids in the design of further supporting experiments including conventional mechanistic tools such as studies of isotope effects and spectroscopic studies for structural and compositional information. One of the most powerful aspects of the methodology is its ability to deconvolute rate processes occurring on the catalytic cycle from those occurring off the cycle. Prominent examples of the application of this methodology to quantitative understanding of complex organic reactions and reaction networks include asymmetric hydrogenation, asymmetric organocatalytic reactions, Pd-catalyzed C-C and C-N bond forming reactions, and transition-metal catalyzed competitive reactions including kinetic resolutions. Reaction Progress Kinetic Analysis finds important application in the pharmaceutical industry, where streamlining process R&D based on Blackmond’s kinetic analysis is becoming an industry-wide standard.
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PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICAno. 7 (2024): e2315447121-e2315447121
Donna G. Blackmond, Marion Emmert, Donna M. Huryn, Michael L. Neidig, Thomas Schaub, Joseph J. Topczewski, Karla Bravo-Altamirano, Zachary Buchan, Pablo J. Cabrera
ORGANIC LETTERSno. 14 (2024): 2682-2685
ACS CATALYSISno. 5 (2023): 2904-2915
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