3 research outputs found
Aromatic aldehydes as tuneable and ppm level potent promoters for zeolite catalysed methanol dehydration to DME
- Author
- Publication venue
- Publication date
- 24/01/2023
- Field of study
Dimethyl ether (DME) is a valuable chemical intermediate and renewable fuel that can be made, via methanol, from many sources of carbon, including carbon dioxide and biomass. Benzaldehyde and its derivatives have been found to be promoters for zeolite catalysed methanol dehydration to DME at low temperature (110 to 150 oC). For the 3-dimensional medium pore zeolite H-ZSM-5 (MFI) the promotion is readily reversible and the potency of the promoter can be tuned by varying the substituent on the aromatic ring of the aldehyde. The most potent promoters are active at concentrations as low as 1 ppm relative to methanol. High throughput experimentation (HTE) is used to screen and rank potential promoters and catalysts and to collect high quality kinetic data for the most promising candidates discovered. The catalytic data and in-situ FT-IR-MS experiments combined with molecular modelling studies indicate a mechanism involving competitive adsorption of the aldehyde promoter on a Brønsted acid (BA) site, followed by reaction with methanol to give a hemi-acetal intermediate. Loss of water from the hemi-acetal intermediate generates a transient and highly reactive methyl oxonium species, [ArC(H)(=O-Me)]+, which then directly reacts with methanol via a SN2 mechanism to give DME and regenerate the aldehyde promoter and BA site. The methyl oxonium species is stabilized by electron-donating groups on the aromatic ring and the solvent like effect of the zeolite pore walls. Molecular descriptors were calculated by molecular modelling for the 22 aromatic aldehyde promoters tested. Multivariate linear regression analysis was used to build an interpretable model for aldehyde promotional activity in H-ZSM-5 and in another 3-dimensional medium pore zeolite, H-ZSM-11 (MEL)
Quellenverzeichnis
- Author
- Abulafia David
- Adloff Mau
- Ahmad Salahuddin
- Akerman James R
- Albion
- Albion
- Alexander Caroline
- Allan David
- Allen Robert C
- Allen Robert C
- Allen Robert C
- Alston William P
- Amery Garvin
- Anderson Benedict
- Anderson Bern
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- Appleby Joyce
- Arendt Hannah
- Armitage David
- Arneil Barbara
- Asdaile Charles
- Attman A.
- Austin K.
- Bachmann-Medick Doris
- Bagchi
- Bagrow Leo
- Baker
- Baker John H
- Baker John H
- Banks R. E. R.
- Banner Stuart
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- Barber Lynn
- Barker Alan H
- Barker Dennis
- Barley Nigel
- Barlow Cleve
- Barnett Correlli
- Barrow Ian J
- Barrow Terence
- Barth Osterhammel
- Bartlett
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- Bastian Adolf
- Bastin
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- Beaglehole John C
- Beastall T. W.
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- Beyrau Hochgeschwender
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- Abulafia David
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- Hoppen
- Hore Peter
- Horsfield John
- Hudson K.
- Hugelmann Frank
- Hugill Peter J
- Humble
- Humble Richard
- Hume David
- Hume David
- Hume David
- Hume David
- Hyam
- Iliffe Robert
- Iliffe Robert
- Iliopoulou Despina
- Inden Ronald
- Ingleton Geoffrey C
- Ingram Edward
- Ivison Duncan
- Jacob M. C.
- James Lawrence
- James Raj
- Jardine Lisa
- Jasanoff Maya
- Jenkins T. A.
- Joel Craig R
- Johnson Franklyn Arthur
- Johnston Anna
- Jon Tetsuro Sumida
- Jones
- Jones C. G.
- Judd Denis
- Kain Roger J. P.
- Kain Roger J. P.
- Kambartel Friedrich
- Kapur Kim
- Kaufmann Stefan
- Keay John
- Keay John
- Keller
- Kemp P. K.
- Kemp Peter
- Kemp Peter
- Kempe Michael
- Kennedy Paul
- Kennedy Paul
- Kennedy Paul
- Kennedy Paul
- Kern Stephen
- Kerridge Eric
- Kießling Friedrich
- Kießling Friedrich
- Killingray David
- Kinahan Jill
- King Kendall
- King Robert D
- Kirkby Diane
- Kjosavik Darley
- Knight R. J. B.
- Koerner Linnaeus
- Kohl
- Kolonien
- Kopf David
- Kopsidis Agrarentwicklung
- Koselleck R.
- Koselleck Reinhart
- Koselleck Reinhart
- Koselleck Reinhart
- Kosselleck Reinhart
- Kraus
- Krause Müller
- Kretschmann Carsten
- Kroll Ashcraft
- Krüger Peter
- Krüger Schroeder
- Kundrus Birthe
- Kuper Adam
- Kwasny Kurt
- Köhn Jens
- Köstering Susanne
- Kühne Ziemann
- Laidlaw Zoë
- Lambert Andrew
- Lambert Andrew
- Lambert Andrew
- Lambert Andrew D
- Landwehr Achim
- Langewiesche Dieter
- Langewiesche Dieter
- Langewiesche Dieter
- Langford P.
- Langford Paul
- Langford Paul
- Lapassade Georges
- Laukötter Anja
- Lavery Brian
- Lavery Brian
- Lavery Brian
- Layton Simon
- Lea David R
- Lefebvre Henri
- Lefèbvre Henri
- Leibfried Zürn
- Lemmon Kenneth
- Lenzen Manuela
- Leonhard Jörn
- Lewis Michael A
- Leyland John
- Lincoln Margarette
- Lincoln Margarette
- Linke Ute
- Lloyd
- Lloyd Christopher
- Lloyd Christopher
- Lloyd Mr
- Locke John
- Locke John
- Locke John
- Locke John
- Loth Osterhammel
- Louis Wm
- Louis Wm
- Louis Wm.
- Lubbock Basil
- Lummis Trevor
- Lupton Kenneth
- Lynn Martin
- Lyte Charles
- Löw Martina
- Mabberley D. J.
- MacArthur D.
- MacCalman
- MacDonagh O.
- Macfarlane Alan
- MacGregor Arthur
- Mack James D
- Mackaness G.
- Mackay David
- Mackay Ruddock F
- MacKenzie John M
- MacKenzie John M
- MacKinder
- Macpherson
- Mahan
- Mahan
- Maier Charles S
- Maier Charles S
- Maier Hans
- Maier Stolleis
- Malinwoski Bronislaw
- Mandler P.
- Mandler P.
- Manning Patrick
- Marcus
- Marder Arthur J
- Marder Arthur J
- Marder Arthur J
- Marder Arthur J
- Mares Detlev
- Markham
- Markham Clements R
- Markham Clements R
- Marshall Peter J
- Marshall Peter J
- Marshall Peter J
- Marx Jennifer
- Masefield
- Massie Robert K
- McClellan James E
- McClellan James E
- McCormick E. H.
- McKee Christopher
- McLaren John
- McLaren P.
- McLean David
- McLynn Frank
- Medlicott W. N.
- Mehta
- Mehta
- Meinecke Friedrich
- Meisel Joseph S
- Meißner Joachim
- Melson P. J.
- Mergel Thomas
- Merkens Hans
- Merwick Donna
- Metcalf Thomas R
- Metzler Gabriele
- Mike Hawkins
- Mill
- Miller Benjamin
- Miller David
- Mingay G. E.
- Mitchell A.
- Mitchell Leslie
- Mitchell T. C.
- Moebius Papilloud
- Morgan Kenneth
- Morris Roger
- Morriss Roger
- Mountbatten Milford Haven
- Muir Rory
- Mukherjee Nilmani
- Musgrave Gardener
- Müller
- Müller
- Münch Richard
- Nadler S.
- Nagl Dominik
- Neeson J. M.
- Neeson J. M.
- Neilson Kennedy
- Neitzel Sönke
- No Vol
- Nolte Paul
- Nußberger Angelika
- Nye Joseph S
- Nye Joseph S
- Nye Joseph S
- O'Brian H.M.S.
- O'Brian Patrick
- O'Brien Patrick K
- O'Byrne William R
- Oexle Otto Gerhard
- Offer Avner
- Oldroyd David R
- Oliver Douglas
- Omerod Henry
- Osterhammel Jürgen
- Osterhammel Jürgen
- Osterhammel Jürgen
- Osterhammel Jürgen
- Osterhammel Jürgen
- Osterhammel Jürgen
- Osterhammel Jürgen
- Osterhammel Jürgen
- Osterhammel Jürgen
- Osterhammel Jürgen
- Osterhammel Jürgen
- Osterhammel Jürgen
- Osterhammel Jürgen
- Osterhammel Jürgen
- Osterhammel Jürgen
- Osterhammel Petersson
- Overton Campbell
- Overton Mark
- Oxford Dictionary of National Biography.
- Pack A. J.
- Padfield Peter
- Padfield Peter
- Pagden Anthony
- Pagden Anthony
- Parkinson C. Northcote
- Parris Henry
- Parry Benita
- Parry John H
- Parry John H
- Paulmann Johannes
- Penny H.
- Penny H.
- Perkin
- Petermann Werner
- Petersson Niels P
- Philips C. H.
- Phillipson David
- Pietschmann Horst
- Pinkney D.
- Pittock
- Pitts Jenniffer
- Pocock Tom
- Pollock Maitland
- Ponting Clive
- Pool Ian
- Porter Andrew
- Porter Andrew
- Porter Andrew
- Porter Andrew N
- Porter Bernard
- Porter Enlightenment
- Porter Roy
- Porter Roy
- Porter Teich
- Powell David
- Pratt Michael
- Prest John M
- Preston Antony
- Preston Antony
- Priest Stephen
- Pugh Martin
- Ramsden John
- Ransome-Wallis Cosnett
- Raphael Lutz
- Raphael Lutz
- Raphael Lutz
- Rappaport Rhoda
- Rasor Eugene L
- Rasor Eugene L
- Rasor Eugene L
- Raymond Joad
- Rediker Marcus
- Reilly Michael
- Reinhard Wolfgang
- Rice Anthony L
- Richardson Bogart
- Richmond H. W.
- Rigby Nigel
- Rippon Peter M
- Ritchie G. S.
- Ritchie Robert C
- Robbins Keith
- Robinson Gallagher
- Robinson Howard
- Robinson Jane
- Rodger
- Rodger
- Rodger
- Rodger
- Rodger
- Rodger
- Rodger N. A. M.
- Rohe Karl
- Romani Roberto
- Roscoe
- Roskill Stephen
- Rotberg Robert
- Rubin Alfred P
- Rudwick
- Ruggles Richard J
- Ruoff Michael
- Russell C.
- Rüger Jan
- Sack
- Sack
- Said Edward W
- Said Edward W
- Sainsbury Antony B
- Sainty J. C.
- Salewski Michael
- Sarazin Philipp
- Sartori Andrew
- Savours Ann
- Schirrmacher Arne
- Schluchter Wolfgang
- Schlögel Karl
- Schmidt Gustav
- Schmidt Gustav
- Schneer Cecil J
- Schneider Ute
- Schofield R.
- Schonhardt-Bailey Cheryl
- Schorn-Schütte Luise
- Schröder Höhler
- Schwartz Stuart
- Schwerhoff Gerd
- Schöllgen Gregor
- Schöllgen Gregor
- Scott Ernest
- Scott James C
- Scott James C
- Seeley
- Seeley
- Semmel Bernard
- Semmel Bernard
- Semmel Bernard
- Shaw-Taylor L.
- Sheets-Pyenson Susan
- Sheppard Eric
- Sheridan R. B.
- Sherwood Marika
- Shiel Robert S
- Shrubb R. E. A.
- Shulman
- Siegrist Sugarman
- Simpson Donald
- Skelton
- Spenser Wilkinson
- Syrett DiNardo
- van Laak
- Vgl
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- 'Vandenhoeck & Ruprecht GmbH & Co, KG'
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