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  5. Continuous production of hydrogen from formic acid decomposition over heterogeneous nanoparticle catalysts: from batch to continuous flow
 
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Continuous production of hydrogen from formic acid decomposition over heterogeneous nanoparticle catalysts: from batch to continuous flow
File(s)
HCOOH.pdf (4.52 MB)
Accepted version
Author(s)
Caiti, Massimiliano
Padovan, Daniele
Hammond, Ceri
Type
Journal Article
Abstract
We investigate the continuous generation of hydrogen via the low temperature (<110 °C), additive-free dehydrogenation of formic acid over heterogeneous Pd/C. Through a combination of kinetic (batch and continuous), spectroscopic, and mechanistic studies, we develop structure–activity–lifetime relationships for this process and in doing so reveal that a combination of pore fouling and poisoning by formate ions results in deactivation of the catalyst during continuous operation. Although these factors result in extensive deactivation in Plug Flow mode, promising results can be obtained by minimizing the steady state concentration of formic acid by operating in a continuous stirred tank reactor. In doing so, continuous operation of the system without a loss of activity for over 2500 turnovers is achieved, under mild conditions and in the absence of stoichiometric additives.
Date Issued
2019-10-01
Date Acceptance
2019-08-01
Citation
ACS Catalysis, 2019, 9 (10), pp.9188-9198
URI
http://hdl.handle.net/10044/1/76633
URL
https://pubs.acs.org/doi/10.1021/acscatal.9b01977
DOI
https://www.dx.doi.org/10.1021/acscatal.9b01977
ISSN
2155-5435
Publisher
American Chemical Society
Start Page
9188
End Page
9198
Journal / Book Title
ACS Catalysis
Volume
9
Issue
10
Copyright Statement
© 2019 American Chemical Society. This is the author’s version of the work. It is posted here by permission of the AAAS for personal use, not for redistribution. The definitive version was published in ACS Catalysis on Volume no. 9, 05 August 2019, DOI: https://doi.org/10.1021/acscatal.9b01977
Identifier
http://gateway.webofknowledge.com/gateway/Gateway.cgi?GWVersion=2&SrcApp=PARTNER_APP&SrcAuth=LinksAMR&KeyUT=WOS:000489204000038&DestLinkType=FullRecord&DestApp=ALL_WOS&UsrCustomerID=1ba7043ffcc86c417c072aa74d649202
Subjects
Science & Technology
Physical Sciences
Chemistry, Physical
Chemistry
hydrogen production
continuous flow
Pd nanoparticles
catalyst deactivation
hydrogen storage
METAL-ORGANIC FRAMEWORK
GENERATION
STORAGE
DEHYDROGENATION
FUEL
FEEDSTOCKS
OXIDATION
CO2
Publication Status
Published
Date Publish Online
2019-08-05
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