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Title: Transition state and product diffusion control by polymer–nanocrystal hybrid catalysts

Abstract

Effective catalysts stabilize specific transition states and control the transport of species to and from catalytically active sites. Enzymes show these traits thanks to their diverse amino acid functional groups encapsulating metal centres, but are limited in the reaction conditions in which they can operate. Realizing a catalyst with this kinetic and transport control that can be used under demanding industrial conditions is challenging. Here, we show a modular approach for the systematic synthesis of polymer–nanocrystal hybrids, where palladium nanocrystals are encapsulated within tunable microporous polymer layers. The polymer chemistry and morphology control the catalytic performance of the metal sites, affecting the transition state for CO oxidation and controlling the transport of CO 2 away from the active site. In conclusion, this approach can be applied to other polymer–nanocrystal compositions and catalytic applications, and is therefore expected to have an impact in many areas of catalysis.

Authors:
ORCiD logo [1];  [1];  [2]; ORCiD logo [3];  [1];  [3];  [1]; ORCiD logo [3]; ORCiD logo [1]
  1. Stanford Univ., Stanford, CA (United States)
  2. National Inst. of Standards and Technology (NIST), Gaithersburg, MD (United States)
  3. SLAC National Accelerator Lab., Menlo Park, CA (United States)
Publication Date:
Research Org.:
SLAC National Accelerator Lab., Menlo Park, CA (United States)
Sponsoring Org.:
USDOE
OSTI Identifier:
1576519
Grant/Contract Number:  
AC02-76SF00515
Resource Type:
Accepted Manuscript
Journal Name:
Nature Catalysis
Additional Journal Information:
Journal Volume: 2; Journal Issue: 10; Journal ID: ISSN 2520-1158
Publisher:
Springer Nature
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats

Riscoe, Andrew R., Wrasman, Cody J., Herzing, Andrew A., Hoffman, Adam S., Menon, Aditya, Boubnov, Alexey, Vargas, Maria, Bare, Simon R., and Cargnello, Matteo. Transition state and product diffusion control by polymer–nanocrystal hybrid catalysts. United States: N. p., 2019. Web. doi:10.1038/s41929-019-0322-7.
Riscoe, Andrew R., Wrasman, Cody J., Herzing, Andrew A., Hoffman, Adam S., Menon, Aditya, Boubnov, Alexey, Vargas, Maria, Bare, Simon R., & Cargnello, Matteo. Transition state and product diffusion control by polymer–nanocrystal hybrid catalysts. United States. doi:10.1038/s41929-019-0322-7.
Riscoe, Andrew R., Wrasman, Cody J., Herzing, Andrew A., Hoffman, Adam S., Menon, Aditya, Boubnov, Alexey, Vargas, Maria, Bare, Simon R., and Cargnello, Matteo. Mon . "Transition state and product diffusion control by polymer–nanocrystal hybrid catalysts". United States. doi:10.1038/s41929-019-0322-7.
@article{osti_1576519,
title = {Transition state and product diffusion control by polymer–nanocrystal hybrid catalysts},
author = {Riscoe, Andrew R. and Wrasman, Cody J. and Herzing, Andrew A. and Hoffman, Adam S. and Menon, Aditya and Boubnov, Alexey and Vargas, Maria and Bare, Simon R. and Cargnello, Matteo},
abstractNote = {Effective catalysts stabilize specific transition states and control the transport of species to and from catalytically active sites. Enzymes show these traits thanks to their diverse amino acid functional groups encapsulating metal centres, but are limited in the reaction conditions in which they can operate. Realizing a catalyst with this kinetic and transport control that can be used under demanding industrial conditions is challenging. Here, we show a modular approach for the systematic synthesis of polymer–nanocrystal hybrids, where palladium nanocrystals are encapsulated within tunable microporous polymer layers. The polymer chemistry and morphology control the catalytic performance of the metal sites, affecting the transition state for CO oxidation and controlling the transport of CO2 away from the active site. In conclusion, this approach can be applied to other polymer–nanocrystal compositions and catalytic applications, and is therefore expected to have an impact in many areas of catalysis.},
doi = {10.1038/s41929-019-0322-7},
journal = {Nature Catalysis},
number = 10,
volume = 2,
place = {United States},
year = {2019},
month = {8}
}

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