274 research outputs found

    In-situ EPR Studies of Reaction Pathways in Titania Photocatalyst-Promoted Alkylation of Alkenes

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    Acknowledgments This work was supported by Engineering and Physical Sciences Research Council (EPSRC) Grant EP/I00372X/1. The EPR spectrometer was purchased under EPSRC Grant EP/F032560/1. We thank Andrew Mills for use of the spectroradiometric measurement system.Peer reviewedPublisher PD

    Room temperature methoxylation in zeolite H-ZSM-5 : an operando DRIFTS/mass spectrometric study

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    The UK Catalysis Hub is thanked for resources and support provided via our membership of the UK Catalysis Hub Consortium and funded by EPSRC (grants EP/I038748/1, EP/I019693/1, EP/ K014706/1, EP/K014668/1, EP/K014854/1, EP/K014714/1 and EP/ M013219/1). Via our membership of the UK’s HEC Materials Chemistry Consortium, which is funded by EPSRC (EP/L000202), this work used the ARCHER UK National Supercomputing Service (www.archer.ac.uk). Johnson Matthey plc is thanked for the provision of the ZSM5. Dr A. J. O’Malley and Dr S. F. Parker are thanked for fruitful discussion.Peer reviewedPublisher PD

    Studies of propene conversion over H-ZSM-5 demonstrate the importance of propene as an intermediate in methanol-to-hydrocarbons chemistry

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    Funding Information: Johnson Matthey plc. is thanked for supplying the ZSM-5 zeolite and for financial support through the provision of industrial CASE studentships in partnership with the EPSRC (APH (EP/P510506/1), AZ (EP/N509176/1)). Experiments at the ISIS Neutron and Muon Source were made possible by a beam time allocation from the Science and Technologies Facilities Council. 53 The resources and support provided by the UK Catalysis Hubviamembership of the UK Catalysis Hub consortium and funded by EPSRC grants EP/R026815/1 and EP/R026939/1 are gratefully acknowledged. This research has been performed with the use of facilities and equipment at the Research Complex at Harwell; the authors are grateful to the Research Complex for this access and support.Peer reviewedPublisher PD

    Ultrafast 2D-IR spectroscopy of intensely optically scattering pelleted solid catalysts

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    ACKNOWLEDGMENTS This work was supported by a UKRI Future Leaders Fellowship grant (Grant No. MR/S015574/1), STFC-UKRI program access to CLF-ULTRA (Grant No. LSF1828), direct access to CLF-ULTRA (Grant Nos. Apps 17330043 and 19130012), and a group residency in the Research Complex at Harwell (RCaH). The authors are grateful to Kathryn Welsby, Ivalina Minova, and Santhosh Matam for support early in the project with samples and the Linkam cell. Mr. John Still of the School of Geosciences, University of Aberdeen is thanked for the SEM images, and Kieran Farrell/Martin Zanni is thanked for the discussion about the polarizations of the beams creating the thermal transientsPeer reviewedPublisher PD

    Cofactor NAD(P)H regeneration:how selective are the reactions?

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    The regeneration of NAD(P)H can be achieved via catalysis, but the unequivocal determination of the species involved has not yet been fully realized. The current analytical methods of reactant/product analysis based on UV-vis spectroscopy, enzymatic assays, NMR spectroscopy, and HPLC are critically examined here with suggestions for future development

    Onset of propene oligomerization reactivity in ZSM-5 studied by inelastic neutron scattering spectroscopy

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    The techniques of quasi-elastic and inelastic neutron scattering (QENS and INS) are applied to investigate the oligomerization of propene over a ZSM-5 zeolite. Investigations are performed at low temperatures, allowing identification of the onset of the oligomerization reaction and observation of the low-energy spectral changes due to intermediate formation that are difficult to observe by optical methods. Oligomerization proceeds via formation of a hydrogen-bonded precursor by an interaction of the propene with an internal acid site followed by protonation and chain growth with protonation being the rate-limiting step. The use of quasi-elastic neutron scattering to observe changes in system mobility with temperature via the elastic window scan technique allows identification of the active temperature range where catalyst activity commences and permits targeting of the more time-consuming INS investigations to conditions of interest. From examination of the product’s spectrum, the structure of the resulting oligomer is deduced to be primarily linear

    Investigation of the dynamics of 1-octene adsorption at 293 K in a ZSM-5 catalyst by inelastic and quasielastic neutron scattering

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    The properties of 1-octene adsorbed in zeolite ZSM-5 at 293 K are studied by means of inelastic and quasielastic neutron scattering (INS and QENS) in order to investigate interactions relevant to the zeolite solid acid catalysis of fluidised catalytic cracking reactions. The INS spectrum is compared to that recorded for the solid alkene and reveals significant changes of bonding on adsorption at ambient temperatures; the changes are attributed to the oligomerization of the adsorbed 1-octene to form a medium chain n-alkane or n-alkane cation. QENS analysis shows that these oligomers are immobilised within the zeolite pore structure but a temperature-dependant fraction is able to rotate around their long axis within the pore channels

    Reactions of Dimethylether in Single Crystals of the Silicoaluminophosphate STA-7 Studied via Operando Synchrotron Infrared Microspectroscopy

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    Open access via the Springer Compact Agreement. We thank the Diamond Light Source for provision of beam time and support facilities at the MIRIAM beamline B22 (Experiments SM11766-1 and SM13725-1). Financial support from the EPSRC Catalysis Hub (Suwardiyanto) and an Industrial CASE Award (EPSRC/BP Chemicals) (Price) are also acknowledged.Peer reviewedPublisher PD

    Improving photocatalytic energy conversion via NAD(P)H

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    NAD(P)H behaves as an energy/chemical “currency,” carrying hydrogen in a biologically convertible form and donates electrons in numerous biotransformations and artificial photosynthesis. Its high cost necessitates its regeneration for reuse where photocatalysis using light energy is attractive. However, high NAD(P)H yield is only achievable via organic mediators to transfer electrons. Here, we analyze the current issues in catalytic NAD(P)H regeneration and show that a continuous-flow reactor system can realize selective NAD(P)H regeneration with 100% yield using Pt/C3N4 as a photocatalyst
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