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Title: Sinter-Resistant Platinum Catalyst Supported by Metal-Organic Framework

Installed on the zirconia nodes of a metal-organic framework (MOF) NU-1000 via targeted vapor-phase synthesis. The catalytic Pt clusters, site-isolated by organic linkers, are shown to exhibit high catalytic activity for ethylene hydrogenation while exhibiting resistance to sintering up to 200 degrees C. In situ IR spectroscopy reveals the presence of both single atoms and few-atom clusters that depend upon synthesis conditions. Operando X-ray absorption spectroscopy and Xray pair distribution analyses reveal unique changes in chemical bonding environment and cluster size stability while on stream. Density functional theory calculations elucidate a favorable reaction pathway for ethylene hydrogenation with the novel catalyst. Lastly, these results provide evidence that atomic layer deposition (ALD) in MOFs is a versatile approach to the rational synthesis of size-selected clusters, including noble metals, on a high surface area support.
Authors:
 [1] ;  [2] ;  [3] ;  [4] ; ORCiD logo [5] ;  [6] ;  [7] ;  [3] ;  [4] ;  [5] ;  [2] ;  [5] ;  [6] ;  [5] ;  [4] ;  [3] ;  [3] ;  [3] ;  [2] ;  [8] more »; ORCiD logo [1] « less
  1. Argonne National Lab. (ANL), Argonne, IL (United States). Materials Science Division
  2. Northwestern Univ., Evanston, IL (United States). Dept. of Chemistry
  3. Pacific Northwest National Lab. (PNNL), Richland, WA (United States). Inst. for Integrated Catalysis
  4. Argonne National Lab. (ANL), Argonne, IL (United States). X-ray Science Division
  5. Univ. of Minnesota, Minneapolis, MN (United States). Dept. of Chemistry
  6. Clemson Univ., SC (United States). Chemical and Biomolecular Engineering
  7. Argonne National Lab. (ANL), Argonne, IL (United States). Chemical Sciences and Engineering Division
  8. Argonne National Lab. (ANL), Argonne, IL (United States). Materials Science Division; Northwestern Univ., Evanston, IL (United States). Dept. of Chemistry
Publication Date:
Grant/Contract Number:
AC02-06CH11357; SC0012702
Type:
Accepted Manuscript
Journal Name:
Angewandte Chemie (International Edition)
Additional Journal Information:
Journal Name: Angewandte Chemie (International Edition); Journal Volume: 57; Journal Issue: 4; Journal ID: ISSN 1433-7851
Publisher:
Wiley
Research Org:
Argonne National Lab. (ANL), Argonne, IL (United States); Energy Frontier Research Centers (EFRC) (United States). Energy Frontier Research Center for Inorganometallic Catalyst Design (ICDC)
Sponsoring Org:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; atomic layer deposition (ALD); heterogeneous catalysis; metal-organic framworks (MOFs); platinum; sinter-resistance
OSTI Identifier:
1433888
Alternate Identifier(s):
OSTI ID: 1415321

Kim, In Soo, Li, Zhanyong, Zheng, Jian, Platero-Prats, Ana E., Mavrandonakis, Andreas, Pellizzeri, Steven, Ferrandon, Magali, Vjunov, Aleksei, Gallington, Leighanne C., Webber, Thomas E., Vermeulen, Nicolaas A., Penn, R. Lee, Getman, Rachel B., Cramer, Christopher J., Chapman, Karena W., Camaioni, Donald M., Fulton, John L., Lercher, Johannes A., Farha, Omar K., Hupp, Joseph T., and Martinson, Alex B. F.. Sinter-Resistant Platinum Catalyst Supported by Metal-Organic Framework. United States: N. p., Web. doi:10.1002/anie.201708092.
Kim, In Soo, Li, Zhanyong, Zheng, Jian, Platero-Prats, Ana E., Mavrandonakis, Andreas, Pellizzeri, Steven, Ferrandon, Magali, Vjunov, Aleksei, Gallington, Leighanne C., Webber, Thomas E., Vermeulen, Nicolaas A., Penn, R. Lee, Getman, Rachel B., Cramer, Christopher J., Chapman, Karena W., Camaioni, Donald M., Fulton, John L., Lercher, Johannes A., Farha, Omar K., Hupp, Joseph T., & Martinson, Alex B. F.. Sinter-Resistant Platinum Catalyst Supported by Metal-Organic Framework. United States. doi:10.1002/anie.201708092.
Kim, In Soo, Li, Zhanyong, Zheng, Jian, Platero-Prats, Ana E., Mavrandonakis, Andreas, Pellizzeri, Steven, Ferrandon, Magali, Vjunov, Aleksei, Gallington, Leighanne C., Webber, Thomas E., Vermeulen, Nicolaas A., Penn, R. Lee, Getman, Rachel B., Cramer, Christopher J., Chapman, Karena W., Camaioni, Donald M., Fulton, John L., Lercher, Johannes A., Farha, Omar K., Hupp, Joseph T., and Martinson, Alex B. F.. 2018. "Sinter-Resistant Platinum Catalyst Supported by Metal-Organic Framework". United States. doi:10.1002/anie.201708092.
@article{osti_1433888,
title = {Sinter-Resistant Platinum Catalyst Supported by Metal-Organic Framework},
author = {Kim, In Soo and Li, Zhanyong and Zheng, Jian and Platero-Prats, Ana E. and Mavrandonakis, Andreas and Pellizzeri, Steven and Ferrandon, Magali and Vjunov, Aleksei and Gallington, Leighanne C. and Webber, Thomas E. and Vermeulen, Nicolaas A. and Penn, R. Lee and Getman, Rachel B. and Cramer, Christopher J. and Chapman, Karena W. and Camaioni, Donald M. and Fulton, John L. and Lercher, Johannes A. and Farha, Omar K. and Hupp, Joseph T. and Martinson, Alex B. F.},
abstractNote = {Installed on the zirconia nodes of a metal-organic framework (MOF) NU-1000 via targeted vapor-phase synthesis. The catalytic Pt clusters, site-isolated by organic linkers, are shown to exhibit high catalytic activity for ethylene hydrogenation while exhibiting resistance to sintering up to 200 degrees C. In situ IR spectroscopy reveals the presence of both single atoms and few-atom clusters that depend upon synthesis conditions. Operando X-ray absorption spectroscopy and Xray pair distribution analyses reveal unique changes in chemical bonding environment and cluster size stability while on stream. Density functional theory calculations elucidate a favorable reaction pathway for ethylene hydrogenation with the novel catalyst. Lastly, these results provide evidence that atomic layer deposition (ALD) in MOFs is a versatile approach to the rational synthesis of size-selected clusters, including noble metals, on a high surface area support.},
doi = {10.1002/anie.201708092},
journal = {Angewandte Chemie (International Edition)},
number = 4,
volume = 57,
place = {United States},
year = {2018},
month = {1}
}

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