Catalytically Active Site Mapping Realized through Energy Transfer Modeling

Thompson, William J.; Maldeni Kankanamalage, Buddhima K. P.; Thaggard, Grace C.; Park, Kyoung Chul; Martin, Corey R.; Niu, Jia; Byers, Jeffery A.; Shustova, Natalia B.

doi:10.1002/anie.202416695

Title: Catalytically Active Site Mapping Realized through Energy Transfer Modeling

Journal Article · 08 November 2024 · Angewandte Chemie (International Edition)

DOI: https://doi.org/10.1002/anie.202416695 · OSTI ID:2504617

Thompson, William J. ^[1]; Maldeni Kankanamalage, Buddhima K. P. ^[2]; Thaggard, Grace C. ^[2]; Park, Kyoung Chul ^[2]; Martin, Corey R. ^[3]; Niu, Jia ^[1]; Byers, Jeffery A. ^[1];

^[2]

Department of Chemistry Boston College 02467 Chestnut Hill MA USA
Department of Chemistry and Biochemistry University of South Carolina 29208 Columbia SC USA
Savannah River National Laboratory 29808 Aiken SC USA

Abstract The demands of a sustainable chemical industry are a driving force for the development of heterogeneous catalytic platforms exhibiting facile catalyst recovery, recycling, and resilience to diverse reaction conditions. Homogeneous‐to‐heterogeneous catalyst transitions can be realized through the integration of efficient homogeneous catalysts within porous matrices. Herein, we offer a versatile approach to understanding how guest distribution and evolution impact the catalytic performance of heterogeneous host–guest catalytic platforms by implementing the resonance energy transfer (RET) concept using fluorescent model systems mimicking the steric constraints of targeted catalysts. Using the RET‐based methodology, we mapped condition‐dependent guest (re)distribution within a porous support on the example of modular matrices such as metal–organic frameworks (MOFs). Furthermore, we correlate RET results performed on the model systems with the catalytic performance of two MOF‐encapsulated catalysts used to promote CO ₂ hydrogenation and ring‐closing metathesis. Guests are incorporated using aperture‐opening encapsulation, and catalyst redistribution is not observed under practical reaction conditions, showcasing a pathway to advance catalyst recyclability in the case of host–guest platforms. These studies represent the first generalizable approach for mapping the guest distribution in heterogeneous host–guest catalytic systems, providing a foundation for predicting and tailoring the performance of catalysts integrated into various porous supports.

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Sponsoring Organization:: USDOE

Grant/Contract Number:: NONE; SC0019055; SC0023182

OSTI ID:: 2504617

Journal Information:: Angewandte Chemie (International Edition), Journal Name: Angewandte Chemie (International Edition) Journal Issue: 4 Vol. 64; ISSN 1433-7851

Publisher:: Wiley Blackwell (John Wiley & Sons)Copyright Statement

Country of Publication:: Germany

Language:: English

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Diffusion as a function of guest molecule length and functionalization in flexible metal–organic frameworks Zheng, B.; Wang, L. L.; Du, L. Materials Horizons, Vol. 3, Issue 4 https://doi.org/10.1039/C6MH00047A	journal	January 2016
Uniform distribution of post-synthetic linker exchange in metal–organic frameworks revealed by Rutherford backscattering spectrometry Fluch, Ulrike; Paneta, Valentina; Primetzhofer, Daniel Chemical Communications, Vol. 53, Issue 48 https://doi.org/10.1039/C7CC02631E	journal	January 2017
Confinement-guided photophysics in MOFs, COFs, and cages Leith, Gabrielle A.; Martin, Corey R.; Mayers, Jacob M. Chemical Society Reviews, Vol. 50, Issue 7 https://doi.org/10.1039/D0CS01519A	journal	January 2021
Transition metal-based bimetallic MOFs and MOF-derived catalysts for electrochemical oxygen evolution reaction Li, Songsong; Gao, Yangqin; Li, Ning Energy & Environmental Science, Vol. 14, Issue 4 https://doi.org/10.1039/D0EE03697H	journal	January 2021
MOF-enabled confinement and related effects for chemical catalyst presentation and utilization Liu, Jian; Goetjen, Timothy A.; Wang, Qining Chemical Society Reviews, Vol. 51, Issue 3 https://doi.org/10.1039/D1CS00968K	journal	January 2022
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Self-healing mixed matrix membranes containing metal–organic frameworks Mondal, Prantik; Cohen, Seth M. Chemical Science, Vol. 13, Issue 41 https://doi.org/10.1039/D2SC04345A	journal	January 2022
Rapid, high-capacity adsorption of iodine from aqueous environments with amide functionalized covalent organic frameworks Arora, Niyati; Debnath, Tanay; Senarathna, Milinda C. Chemical Science, Vol. 15, Issue 10 https://doi.org/10.1039/D3SC06004G	journal	January 2024
Homogeneous and heterogeneous catalysis in industry de Vries, Johannes G.; Jackson, S. David Catalysis Science & Technology, Vol. 2, Issue 10 https://doi.org/10.1039/c2cy90039d	journal	January 2012
Switching in harmony: Tailoring the properties of functional materials with orthogonal stimuli Thaggard, Grace C.; Maldeni Kankanamalage, Buddhima K. P.; Park, Kyoung Chul Chemical Physics Reviews, Vol. 5, Issue 1 https://doi.org/10.1063/5.0189069	journal	February 2024
Host–guest chemistry of mesoporous silicas: precise design of location, density and orientation of molecular guests in mesopores Sohmiya, Minoru; Saito, Kanji; Ogawa, Makoto Science and Technology of Advanced Materials, Vol. 16, Issue 5 https://doi.org/10.1088/1468-6996/16/5/054201	journal	October 2015
Hierarchically porous metal–organic frameworks: synthetic strategies and applications Feng, Liang; Wang, Kun-Yu; Lv, Xiu-Liang National Science Review, Vol. 7, Issue 11 https://doi.org/10.1093/nsr/nwz170	journal	November 2019
Direct evaluation of self-quenching behavior of fluorophores at high concentrations using an evanescent field Bae, Wooli; Yoon, Tae-Young; Jeong, Cherlhyun PLOS ONE, Vol. 16, Issue 2 https://doi.org/10.1371/journal.pone.0247326	journal	February 2021
Encapsulation of Dyes in Luminescent Metal-Organic Frameworks for White Light Emitting Diodes Sun, Zhihong; Khurshid, Aaqib; Sohail, Muhammad Nanomaterials, Vol. 11, Issue 10 https://doi.org/10.3390/nano11102761	journal	October 2021

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