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      A generalized kinetic model for compartmentalization of organometallic catalysis†

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      Chemical Science
      The Royal Society of Chemistry

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          Abstract

          Compartmentalization is an attractive approach to enhance catalytic activity by retaining reactive intermediates and mitigating deactivating pathways. Such a concept has been well explored in biochemical and more recently, organometallic catalysis to ensure high reaction turnovers with minimal side reactions. However, the scarcity of theoretical frameworks towards confined organometallic chemistry impedes broader utility for the implementation of compartmentalization. Herein, we report a general kinetic model and offer design guidance for a compartmentalized organometallic catalytic cycle. In comparison to a non-compartmentalized catalysis, compartmentalization is quantitatively shown to prevent the unwanted intermediate deactivation, boost the corresponding reaction efficiency ( γ), and subsequently increase catalytic turnover frequency (TOF). The key parameter in the model is the volumetric diffusive conductance ( F V) that describes catalysts' diffusion propensity across a compartment's boundary. Optimal values of F V for a specific organometallic chemistry are needed to achieve maximal values of γ and TOF. As illustrated in specific reaction examples, our model suggests that a tailored compartment design, including the use of nanomaterials, is needed to suit a specific organometallic catalytic cycle. This work provides justification and design principles for further exploration into compartmentalizing organometallics to enhance catalytic performance. The conclusions from this work are generally applicable to other catalytic systems that need proper design guidance in confinement and compartmentalization.

          Abstract

          Compartmentalization is an attractive approach to enhance catalytic activity by retaining reactive intermediates and mitigating deactivating pathways.

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          Most cited references4

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          Random Walks in Biology

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            Organometallic Chemistry and Catalysis

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              Transport and diffusion across cell membranes

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                Author and article information

                Journal
                Chem Sci
                Chem Sci
                SC
                CSHCBM
                Chemical Science
                The Royal Society of Chemistry
                2041-6520
                2041-6539
                5 January 2022
                26 January 2022
                5 January 2022
                : 13
                : 4
                : 1101-1110
                Affiliations
                [a] Department of Chemistry and Biochemistry, University of California Los Angeles California 90095 USA pld@ 123456chem.ucla.edu chongliu@ 123456chem.ucla.edu
                [b] California NanoSystems Institute (CNSI), University of California Los Angeles CA 90095 USA
                Author information
                https://orcid.org/0000-0003-4991-5212
                https://orcid.org/0000-0002-7678-8653
                https://orcid.org/0000-0003-0764-0126
                https://orcid.org/0000-0003-2732-4155
                https://orcid.org/0000-0001-5546-3852
                Article
                d1sc04983f
                10.1039/d1sc04983f
                8790775
                35211276
                a5b8bde6-9848-457e-b7ab-c868e439350f
                This journal is © The Royal Society of Chemistry
                History
                : 9 September 2021
                : 21 December 2021
                Page count
                Pages: 10
                Funding
                Funded by: Division of Chemistry, doi 10.13039/100000165;
                Award ID: CHE-2023955
                Funded by: University of California, doi 10.13039/100005595;
                Award ID: Unassigned
                Categories
                Chemistry
                Custom metadata
                Paginated Article

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