Literature DB >> 24153305

Thermal maps of gases in heterogeneous reactions.

Nanette N Jarenwattananon1, Stefan Glöggler, Trenton Otto, Arek Melkonian, William Morris, Scott R Burt, Omar M Yaghi, Louis-S Bouchard.   

Abstract

More than 85 per cent of all chemical industry products are made using catalysts, the overwhelming majority of which are heterogeneous catalysts that function at the gas-solid interface. Consequently, much effort is invested in optimizing the design of catalytic reactors, usually by modelling the coupling between heat transfer, fluid dynamics and surface reaction kinetics. The complexity involved requires a calibration of model approximations against experimental observations, with temperature maps being particularly valuable because temperature control is often essential for optimal operation and because temperature gradients contain information about the energetics of a reaction. However, it is challenging to probe the behaviour of a gas inside a reactor without disturbing its flow, particularly when trying also to map the physical parameters and gradients that dictate heat and mass flow and catalytic efficiency. Although optical techniques and sensors have been used for that purpose, the former perform poorly in opaque media and the latter perturb the flow. NMR thermometry can measure temperature non-invasively, but traditional approaches applied to gases produce signals that depend only weakly on temperature are rapidly attenuated by diffusion or require contrast agents that may interfere with reactions. Here we present a new NMR thermometry technique that circumvents these problems by exploiting the inverse relationship between NMR linewidths and temperature caused by motional averaging in a weak magnetic field gradient. We demonstrate the concept by non-invasively mapping gas temperatures during the hydrogenation of propylene in reactors packed with metal nanoparticles and metal-organic framework catalysts, with measurement errors of less than four per cent of the absolute temperature. These results establish our technique as a non-invasive tool for locating hot and cold spots in catalyst-packed gas-solid reactors, with unprecedented capabilities for testing the approximations used in reactor modelling.

Entities:  

Year:  2013        PMID: 24153305     DOI: 10.1038/nature12568

Source DB:  PubMed          Journal:  Nature        ISSN: 0028-0836            Impact factor:   49.962


  13 in total

1.  A thermometer for nonspinning solid-state NMR spectroscopy

Authors: 
Journal:  J Magn Reson       Date:  2000-10       Impact factor: 2.229

2.  Catalytic activity in individual cracking catalyst particles imaged throughout different life stages by selective staining.

Authors:  Inge L C Buurmans; Javier Ruiz-Martínez; William V Knowles; David van der Beek; Jaap A Bergwerff; Eelco T C Vogt; Bert M Weckhuysen
Journal:  Nat Chem       Date:  2011-09-18       Impact factor: 24.427

3.  Magnetic resonance imaging methods for in situ studies in heterogeneous catalysis.

Authors:  Anna A Lysova; Igor V Koptyug
Journal:  Chem Soc Rev       Date:  2010-10-11       Impact factor: 54.564

4.  NMR imaging of catalytic hydrogenation in microreactors with the use of para-hydrogen.

Authors:  Louis-S Bouchard; Scott R Burt; M Sabieh Anwar; Kirill V Kovtunov; Igor V Koptyug; Alexander Pines
Journal:  Science       Date:  2008-01-25       Impact factor: 47.728

5.  Observation of parahydrogen-induced polarization in heterogeneous hydrogenation on supported metal catalysts.

Authors:  Kirill V Kovtunov; Irene E Beck; Valery I Bukhtiyarov; Igor V Koptyug
Journal:  Angew Chem Int Ed Engl       Date:  2008       Impact factor: 15.336

6.  Thermographic selection of effective catalysts from an encoded polymer-bound library

Authors: 
Journal:  Science       Date:  1998-04-10       Impact factor: 47.728

7.  Accurate temperature imaging based on intermolecular coherences in magnetic resonance.

Authors:  Gigi Galiana; Rosa T Branca; Elizabeth R Jenista; Warren S Warren
Journal:  Science       Date:  2008-10-17       Impact factor: 47.728

8.  Isoreticular metalation of metal-organic frameworks.

Authors:  Christian J Doonan; William Morris; Hiroyasu Furukawa; Omar M Yaghi
Journal:  J Am Chem Soc       Date:  2009-07-15       Impact factor: 15.419

9.  Reversible interactions with para-hydrogen enhance NMR sensitivity by polarization transfer.

Authors:  Ralph W Adams; Juan A Aguilar; Kevin D Atkinson; Michael J Cowley; Paul I P Elliott; Simon B Duckett; Gary G R Green; Iman G Khazal; Joaquín López-Serrano; David C Williamson
Journal:  Science       Date:  2009-03-27       Impact factor: 47.728

10.  Strongly hyperpolarized gas from parahydrogen by rational design of ligand-capped nanoparticles.

Authors:  Ramesh Sharma; Louis-S Bouchard
Journal:  Sci Rep       Date:  2012-02-20       Impact factor: 4.379

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