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Title: Sintering-Resistant Single-Site Nickel Catalyst Supported by Metal–Organic Framework

Abstract

Developing supported single-site catalysts is an important goal in heterogeneous catalysis since the welldefined active sites afford opportunities for detailed mechanistic studies, thereby facilitating the design of improved catalysts. We present in this paper a method for installing Ni ions uniformly and precisely on the node of a Zr-based metal–organic framework (MOF), NU-1000, in high density and large quantity (denoted as Ni-AIM) using atomic layer deposition (ALD) in a MOF (AIM). Ni-AIM is demonstrated to be an efficient gas-phase hydrogenation catalyst upon activation. The structure of the active sites in Ni-AIM is proposed, revealing its single-site nature. More importantly, due to the organic linker used to construct the MOF support, the Ni ions stay isolated throughout the hydrogenation catalysis, in accord with its long-term stability. A quantum chemical characterization of the catalyst and the catalytic process complements the experimental results. With validation of computational modeling protocols, we further targeted ethylene oligomerization catalysis by Ni-AIM guided by theoretical prediction. Given the generality of the AIM methodology, this emerging class of materials should prove ripe for the discovery of new catalysts for the transformation of volatile substrates.

Authors:
 [1];  [1];  [2];  [2];  [1];  [3];  [1];  [4];  [5];  [5];  [6];  [2];  [2];  [1];  [7]
  1. Northwestern Univ., Evanston, IL (United States)
  2. Univ. of Minnesota, Minneapolis, MN (United States)
  3. Argonne National Lab. (ANL), Argonne, IL (United States). Advanced Photon Source (APS)
  4. Argonne National Lab. (ANL), Argonne, IL (United States). Advanced Photon Source (APS); Purdue Univ., West Lafayette, IN (United States)
  5. Pacific Northwest National Lab. (PNNL), Richland, WA (United States). Inst. for Integrated Catalysis
  6. Pacific Northwest National Lab. (PNNL), Richland, WA (United States). Inst. for Integrated Catalysis; Technische Univ. Munchen, Garching (Germany)
  7. Northwestern Univ., Evanston, IL (United States); King Abdulaziz Univ., Jeddah (Saudi Arabia)
Publication Date:
Research Org.:
Energy Frontier Research Centers (EFRC) (United States). Energy Frontier Research Center for Inorganometallic Catalyst Design (ICDC); Argonne National Lab. (ANL), Argonne, IL (United States). Advanced Photon Source (APS)
Sponsoring Org.:
USDOD; USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division; National Science Foundation (NSF); International Institute for Nanotechnology (IIN); State of Illinois; National Institutes of Health (NIH)
OSTI Identifier:
1387404
Grant/Contract Number:  
SC0012702; AC02-06CH11357
Resource Type:
Accepted Manuscript
Journal Name:
Journal of the American Chemical Society
Additional Journal Information:
Journal Volume: 138; Journal Issue: 6; Related Information: ICDC partners with University of Minnesota(lead); Argonne National Laboratory; Clemson University; Dow Chemical Company; Northwestern University; Pacific Northwest National Laboratory; University of California Davis; University of Washington; Journal ID: ISSN 0002-7863
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; catalysis (heterogeneous); materials and chemistry by design; synthesis (novel materials); hydrocarbons; metals; metal organic frameworks; catalysts; catalytic reactions

Citation Formats

Li, Zhanyong, Schweitzer, Neil M., League, Aaron B., Bernales, Varinia, Peters, Aaron W., Getsoian, Andrew “Bean”, Wang, Timothy C., Miller, Jeffrey T., Vjunov, Aleksei, Fulton, John L., Lercher, Johannes A., Cramer, Christopher J., Gagliardi, Laura, Hupp, Joseph T., and Farha, Omar K.. Sintering-Resistant Single-Site Nickel Catalyst Supported by Metal–Organic Framework. United States: N. p., 2016. Web. https://doi.org/10.1021/jacs.5b12515.
Li, Zhanyong, Schweitzer, Neil M., League, Aaron B., Bernales, Varinia, Peters, Aaron W., Getsoian, Andrew “Bean”, Wang, Timothy C., Miller, Jeffrey T., Vjunov, Aleksei, Fulton, John L., Lercher, Johannes A., Cramer, Christopher J., Gagliardi, Laura, Hupp, Joseph T., & Farha, Omar K.. Sintering-Resistant Single-Site Nickel Catalyst Supported by Metal–Organic Framework. United States. https://doi.org/10.1021/jacs.5b12515
Li, Zhanyong, Schweitzer, Neil M., League, Aaron B., Bernales, Varinia, Peters, Aaron W., Getsoian, Andrew “Bean”, Wang, Timothy C., Miller, Jeffrey T., Vjunov, Aleksei, Fulton, John L., Lercher, Johannes A., Cramer, Christopher J., Gagliardi, Laura, Hupp, Joseph T., and Farha, Omar K.. Tue . "Sintering-Resistant Single-Site Nickel Catalyst Supported by Metal–Organic Framework". United States. https://doi.org/10.1021/jacs.5b12515. https://www.osti.gov/servlets/purl/1387404.
@article{osti_1387404,
title = {Sintering-Resistant Single-Site Nickel Catalyst Supported by Metal–Organic Framework},
author = {Li, Zhanyong and Schweitzer, Neil M. and League, Aaron B. and Bernales, Varinia and Peters, Aaron W. and Getsoian, Andrew “Bean” and Wang, Timothy C. and Miller, Jeffrey T. and Vjunov, Aleksei and Fulton, John L. and Lercher, Johannes A. and Cramer, Christopher J. and Gagliardi, Laura and Hupp, Joseph T. and Farha, Omar K.},
abstractNote = {Developing supported single-site catalysts is an important goal in heterogeneous catalysis since the welldefined active sites afford opportunities for detailed mechanistic studies, thereby facilitating the design of improved catalysts. We present in this paper a method for installing Ni ions uniformly and precisely on the node of a Zr-based metal–organic framework (MOF), NU-1000, in high density and large quantity (denoted as Ni-AIM) using atomic layer deposition (ALD) in a MOF (AIM). Ni-AIM is demonstrated to be an efficient gas-phase hydrogenation catalyst upon activation. The structure of the active sites in Ni-AIM is proposed, revealing its single-site nature. More importantly, due to the organic linker used to construct the MOF support, the Ni ions stay isolated throughout the hydrogenation catalysis, in accord with its long-term stability. A quantum chemical characterization of the catalyst and the catalytic process complements the experimental results. With validation of computational modeling protocols, we further targeted ethylene oligomerization catalysis by Ni-AIM guided by theoretical prediction. Given the generality of the AIM methodology, this emerging class of materials should prove ripe for the discovery of new catalysts for the transformation of volatile substrates.},
doi = {10.1021/jacs.5b12515},
journal = {Journal of the American Chemical Society},
number = 6,
volume = 138,
place = {United States},
year = {2016},
month = {2}
}

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