Author
Claire A Murray
Bio: Claire A Murray is an academic researcher from Diamond Light Source (United Kingdom). The author has contributed to research in topics: Carboxylation & Butene. The author has an hindex of 1, co-authored 1 publications receiving 7 citations.
Topics: Carboxylation, Butene, Decarboxylation
Papers
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TL;DR: In this paper, a catalytic process of decarboxylating gamma-valerolactone, GVL (the biomass derived lactone as an example) over Zn/ZSM-5 to butene, followed by aromatization at high yield with co-feed water.
Abstract: Here, we report a catalytic process of decarboxylating gamma-valerolactone, GVL (the biomass derived lactone as an example) over Zn/ZSM-5 to butene, followed by aromatization at high yield with co-feed water. Evaluation of catalytic performance at prolonged time shows that water molecule is essential in maintaining the decarboxylation/ aromatization activity without rapid deactivation. Synchrotron X-ray diffraction and Rietveld refinement are then used to elucidate the adsorbed structures of GVL and immobilized Zn-species with the support of EXAFS and NMR. A new route of cooperative hydrolysis of GVL by framework Zn-OH and Bronsted acid sites to butene and then to aromatics is for the first time demonstrated. The structures and fundamental pathways for nucleophilic attack of terminal Zn-OH site are comparable to that of reported Zn-containing enzymes in biological systems.
8 citations
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TL;DR: In this paper, an investigation on the efficient production of GVL from biomass-based carbonyl compounds such as furfural, levulinic acid, and its esters using 2-propanol as H-donor and solvent over stable Zr-incorporated mesoporous silica (KIT-5) catalysts was presented.
43 citations
TL;DR: A review of the use of synchrotron X-ray powder diffraction as the primary tool for the study of fundamental interactions with organic molecules with active sites in powder zeolites, as well as some perspectives based on this experimental capability is provided in this paper.
38 citations
TL;DR: In this paper, a series of delaminated MWW-type Zr-Al-SCM-1 zeolites with large external surface area have been synthesized through a post-synthesized method by partial dealumination of SCM 1 and Zr incorporation, and used in the conversion of furfural and xylose to γ-valerolactone (GVL).
27 citations
TL;DR: The first selective oxidation of methane to methanol is reported herein for zinc-exchanged MOR (Zn/MOR) and lays the foundation for developing structure-function correlations for methane conversion over zinc- exchanged zeolites.
Abstract: The first selective oxidation of methane to methanol is reported herein for zinc‐exchanged MOR (Zn/MOR). Under identical conditions, Zn/FER and Zn/ZSM‐5 both form zinc formate and methanol. Selective methane activation to form [Zn‐CH 3 ] + species was confirmed by 13 C MAS NMR spectroscopy for all three frameworks. The percentage of active zinc sites, measured through quantitative NMR spectroscopy studies, varied with the zeolite framework and was found to be ZSM‐5 (5.7%), MOR (1.2%) and FER (0.8%). For Zn/MOR, two signals were observed in the 13 C MAS NMR spectrum, resulting from two distinct [Zn‐CH 3 ] + species present in the 12 MR and 8 MR side pockets, as supported by additional NMR experiments. The observed products of oxidation of the [Zn‐CH 3 ] + species is shown to depend on the zeolite framework type and the oxidative conditions used. These results lay the foundation for developing structure‐function correlations for methane conversion over zinc‐exchanged zeolites
10 citations
TL;DR: By tailoring the acidity of Brønsted acid sites in an aluminophosphate molecular sieve through incorporation of Zn2+ into the framework, a new selective and effective catalyst is accessed for GVL conversion to PA.
Abstract: γ-Valerolactone (GVL) is regarded as a key platform molecule in the production of fine chemicals such as pentenoic acid (PA) from biomass. Although PA is believed to be the key intermediate in solid-acid-catalyzed reactions of GVL, due to subsequent facile decarboxylation reactions further alkene products are formed. Here, by tailoring the acidity of Bronsted acid sites in an aluminophosphate (AlPO) molecular sieve through incorporation of Zn2+ into the framework, we access a new selective and effective catalyst for GVL conversion to PA.
7 citations