Title: Isomerization and Selective Hydrogenation of Propyne: Screening of Metal–Organic Frameworks Modified by Atomic Layer Deposition

Abstract

Various metal oxide clusters upward of 8 atoms (Cu, Cd, Co, Fe, Ga, Mn, Mo, Ni, Sn, W, Zn, In, and Al) were incorporated into the pores of the metal–organic framework (MOF) NU-1000 via atomic layer deposition (ALD) and tested via high-throughput screening for catalytic isomerization and selective hydrogenation of propyne. Cu and Co were found to be the most active for propyne hydrogenation to propylene, and synergistic bimetallic combinations of Co and Zn, along with standalone Zn and Cd, were established as the most active for conversion to the isomerized product, propadiene. The combination of Co and Zn in NU-1000 diminished the propensity for full hydrogenation to propane as well as coking compared to its individual components. Finally, this study highlights the potential for high-throughput screening to survey monometallic and bimetallic cluster combinations that best affect the efficient transformation of small molecules, while discerning mechanistic differences in isomerization and hydrogenation by different metals.

Authors:

Hackler, Ryan A.  ^[1];

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• Search DOE PAGES for ORCID "0000-0003-4698-6074"

Pandharkar, Riddhish ^[2]; Ferrandon, Magali S. ^[1]; Kim, In Soo ^[3]; Vermeulen, Nicolaas A. ^[4]; Gallington, Leighanne C.  ^[1];

• Search DOE PAGES for author "Gallington, Leighanne C."
• Search DOE PAGES for ORCID "0000-0002-0383-7522"

Chapman, Karena W.  ^[5];

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• Search DOE PAGES for ORCID "0000-0002-8725-5633"

Farha, Omar K.  ^[4];

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• Search DOE PAGES for ORCID "0000-0002-9904-9845"

Cramer, Christopher J.  ^[2];

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• Search DOE PAGES for ORCID "0000-0001-5048-1859"

Sauer, Joachim  ^[6];

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• Search DOE PAGES for ORCID "0000-0001-6798-6212"

Gagliardi, Laura  ^[2];

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• Search DOE PAGES for ORCID "0000-0001-5227-1396"

Martinson, Alex F.  ^[1];

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• Search DOE PAGES for ORCID "0000-0003-3916-1672"

Delferro, Massimiliano  ^[1]

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• Search DOE PAGES for ORCID "0000-0002-4443-165X"

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+ Show Author Affiliations

1. Argonne National Lab. (ANL), Argonne, IL (United States)
2. Univ. of Minnesota-Twin Cities, Minneapolis, MN (United States)
3. Korea Inst. of Science and Technology (KIST), Seoul (Korea)
4. Northwestern Univ., Evanston, IL (United States)
5. Stony Brook Univ., NY (United States)
6. Humboldt-Univ. zu Berlin (Germany)

Publication Date:

Tue Nov 17 00:00:00 EST 2020

Research Org.:

Argonne National Laboratory (ANL), Argonne, IL (United States); Univ. of Minnesota, Minneapolis, MN (United States)

Sponsoring Org.:

USDOE Office of Science (SC), Basic Energy Sciences (BES)

OSTI Identifier:

1776840

Alternate Identifier(s):

OSTI ID: 1721711

Grant/Contract Number:  

AC02-06CH11357; SC0012702

Resource Type:

Accepted Manuscript

Journal Name:

Journal of the American Chemical Society

Additional Journal Information:

Journal Volume: 142; Journal Issue: 48; 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; metals; metal organic frameworks; catalysts; isomerization; hydrogenation