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Selective Catalysis in Nanoparticle ...

Stephenson, Casey Justin.

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Selective Catalysis in Nanoparticle Metal-Organic Framework Composites.

Record Type:	Electronic resources : Monograph/item
Title/Author:	Selective Catalysis in Nanoparticle Metal-Organic Framework Composites./
Author:	Stephenson, Casey Justin.
Description:	100 p.
Notes:	Source: Dissertation Abstracts International, Volume: 77-10(E), Section: B.
Contained By:	Dissertation Abstracts International77-10B(E).
Subject:	Inorganic chemistry. -
Online resource:	http://pqdd.sinica.edu.tw/twdaoapp/servlet/advanced?query=10117293
ISBN:	9781339786957

Selective Catalysis in Nanoparticle Metal-Organic Framework Composites.
Stephenson, Casey Justin.

Selective Catalysis in Nanoparticle Metal-Organic Framework Composites. - 100 p.

Source: Dissertation Abstracts International, Volume: 77-10(E), Section: B.

Thesis (Ph.D.)--Northwestern University, 2016.

The design of highly selective catalysts are becoming increasingly important, especially as chemical and pharmaceutical industries seek to improve atom economy and minimize energy intensive separations that are often required to separate side products from the desired product. Enzymes are among the most selective of all catalysts, generally operating through molecular recognition whereby an active site analogous to a lock and the substrate is analogous to a key. The assembly of a porous, crystalline material around a catalytically active metal particle could serve as an artificial enzyme.

ISBN: 9781339786957Subjects--Topical Terms:

3173556
Inorganic chemistry.

Selective Catalysis in Nanoparticle Metal-Organic Framework Composites.
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020 $a 9781339786957
035 $a (MiAaPQ)AAI10117293
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100 1 $a Stephenson, Casey Justin. $3 3194681
245 1 0 $a Selective Catalysis in Nanoparticle Metal-Organic Framework Composites.
300 $a 100 p.
500 $a Source: Dissertation Abstracts International, Volume: 77-10(E), Section: B.
500 $a Adviser: Joseph T. Hupp.
502 $a Thesis (Ph.D.)--Northwestern University, 2016.
520 $a The design of highly selective catalysts are becoming increasingly important, especially as chemical and pharmaceutical industries seek to improve atom economy and minimize energy intensive separations that are often required to separate side products from the desired product. Enzymes are among the most selective of all catalysts, generally operating through molecular recognition whereby an active site analogous to a lock and the substrate is analogous to a key. The assembly of a porous, crystalline material around a catalytically active metal particle could serve as an artificial enzyme.
520 $a In this vein, we first synthesized the polyvinylpyrrolidone (PVP) coated nanoparticles of interest and then encapsulated them within zeolitic imidazolate framework 8 or ZIF-8. 2.8 nm Pt-PVP nanoparticles, which were encapsulated within ZIF-8 to form Pt ZIF-8 composite. Pt ZIF-8 was inactive for the hydrogenation of cyclic olefins such as cis-cyclooctene and cis-cyclohexene while the composite proved to be a highly selective catalyst for the hydrogenation of terminal olefins, hydrogenating trans-1,3-hexadiene to 3-hexene in 95% selectivity after 24 hours under 1 bar H2.
520 $a We extended our encapsulation method to sub-2 nm Au nanoparticles to form Au ZIF-8. Au ZIF-8 served as a highly chemoselective catalyst for the hydrogenation of crotonaldehyde an alpha,beta-unsaturated aldehyde, to crotyl alcohol an alpha,beta-unsaturated alcohol, in 90-95% selectivity. In order to investigate nanoparticle size effects on selectivity, 6-10 nm Au nanoparticles were encapsulated within ZIF-8 to form Au6 ZIF-8. Control catalysts with nanoparticles supported on the surface of ZIF-8 were synthesized as well, Au/ZIF-8 and Au6/ZIF-8. Au6 ZIF-8 hydrogenated crotonaldehyde in 85% selectivity towards the unsaturated alcohol. Catalysts with nanoparticles supported on the exterior of ZIF-8 were far less selective towards the unsaturated alcohol. Post-catalysis transmission electron microscopy analysis of Au ZIF-8 and Au/ZIF-8 shows that the nanoparticles of Au ZIF-8 remain within experimental uncertainty and unchanged, whereas Au nanoparticles of Au/ZIF suffered from server sintering.
520 $a We performed solvent assisted linker exchange, a single-crystal to single-crystal transformation, on Pt ZIF-8 to exchange the 2-methylimidazole linkers with imidazole to form Pt SALEM-2. Since Pt SALEM-2 should have larger apertures than Pt ZIF-8, we investigated Pt ZIF-8 and Pt SALEM-2 as catalysts for the hydrogenation of substrates with increasingly larger kinetic diameter: 1-octene, cis-cyclohexene, and beta-pinene. Both catalysts were active for the hydrogenation of 1-octene, while only Pt SALEM-2 was active for cis-cyclohexene hydrogenation. Neither catalyst was active for the hydrogenation of beta-pinene, indicating that the Pt nanoparticles remained well encapsulated throughout the SALE process.
590 $a School code: 0163.
650 4 $a Inorganic chemistry. $3 3173556
650 4 $a Nanoscience. $3 587832
690 $a 0488
690 $a 0565
710 2 $a Northwestern University. $b Chemistry. $3 1030729
773 0 $t Dissertation Abstracts International $g 77-10B(E).
790 $a 0163
791 $a Ph.D.
792 $a 2016
793 $a English
856 4 0 $u http://pqdd.sinica.edu.tw/twdaoapp/servlet/advanced?query=10117293