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Production of 1,6-Hexanediol and 1,5-Pentanediol from Biomass-Derived Feedstocks over Heterogeneous Catalysts
Başlık:
Production of 1,6-Hexanediol and 1,5-Pentanediol from Biomass-Derived Feedstocks over Heterogeneous Catalysts
Yazar:
Burt, Samuel P., author.
ISBN:
9780438038448
Yazar Ek Girişi:
Fiziksel Tanımlama:
1 electronic resource (173 pages)
Genel Not:
Source: Dissertation Abstracts International, Volume: 79-10(E), Section: B.
Advisors: Ive Hermans; Manos Mavrikakis Committee members: James A. Dumesic; Ive Hermans; George W. Huber; Clark R. Landis; Manos Mavrikakis.
Özet:
Fossil fuels have driven our economy for decades, but we have come to a point where this is no longer ideal for a number of reasons. Most notably, processing of fossil fuels often leads to the production of environmentally harmful chemicals, such as greenhouse gases (e.g. CO 2, CH4) and gases leading to smog and acid rain (e.g. NO x). In this thesis, I present an alternative to fossil fuels to produce high-value alpha,o-diols, which are monomers for everyday products, such as polyesters, polyurethanes, polycarbonates, and nylons. Specifically, I will focus on the final steps of an integrated route to 1,6-hexanediol (1,6-HDO) and 1,5-pentanediol (1,5-PDO) from biomass over heterogeneous catalysts.
I will start with study of the hydrogenation/hydrogenolysis of furfuryl alcohol (FA) to 1,5-PDO. FA hydrogenation/hydrogenolysis is carried out over a Co/TiO2 catalyst which is stabilized by a TiO2 overcoat formed during high-temperature treatments. This overcoat is shown by Raman spectroscopy and Scanning Transmission Electron Microscopy (STEM). Later, hydrogenation of furfural---produced directly from hemicellulose and sugars---to THFA will be discussed. This is carried out over a Ni/TiO2 catalyst, with >95% combined selectivity to FA and THFA, both of which can be further converted to 1,5-PDO.
With regards to the six-carbon (C6) route, Rh-ReOx/C is known to be active for tetrahydropyran-2-methanol (THP2M) hydrogenolysis to 1,6-HDO in one-step. Here, I discuss a three-step route from THP2M to 1,6-HDO. This route benefits from orders-of-magnitude cheaper catalysts and lower hydrogen pressures, relative to the one-step route. This route consists of THP2M dehydration to 2,3,4,5-tetrahydrooxepine (THO) over a SiAl-based catalyst, rehydration of THO to 2-oxepanol in the absence of a catalyst, and hydrogenation of 2-oxepanol to 1,6-HDO over Ni/TiO2.
It was later discovered that tetrahydrofuran-dimethanol (THFDM)---a further upstream product of biomass processing compared to THP2M---could also be converted to 1,6-HDO in one step over a Pt-WO2/TiO 2 catalyst. In this thesis, Pt-WO2/TiO2 is thoroughly characterized by Raman spectroscopy, Fourier Transform Infrared (FTIR) spectroscopy, X-ray Photoelectron spectroscopy (XPS), and adsorption/desorption experiments to explain surprising trends in activity. Reaction and reduction conditions are then tailored for this catalyst, and replacements for Pt are tested.
Notlar:
School code: 0262
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Yer Numarası | Demirbaş Numarası | Shelf Location | Lokasyon / Statüsü / İade Tarihi |
---|---|---|---|
XX(681179.1) | 681179-1001 | Proquest E-Tez Koleksiyonu | Arıyor... |
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