The full-text may be used and/or reproduced, and given to third parties in any format or medium, without prior permission or charge, for personal research or study, educational, or not-for-prot purposes provided that:• a full bibliographic reference is made to the original source • a link is made to the metadata record in DRO • the full-text is not changed in any way The full-text must not be sold in any format or medium without the formal permission of the copyright holders.Please consult the full DRO policy for further details.
Hydrogenation of aromatic molecules
in fossil- and bio-derived
fuels is essential for decreasing emissions of harmful combustion
products and addressing growing concerns around urban air pollution.
In this work, we used atomic layer deposition to significantly enhance
the hydrogenation performance of a conventional supported Pd catalyst
by applying an ultrathin coating of TiO2 in a scalable
powder coating process. The TiO2-coated catalyst showed
substantial gains in the conversion of multiple aromatic molecules,
including a 5-fold improvement in turnover frequency versus the uncoated
catalyst in the hydrogenation of naphthalene. This activity enhancement
was maintained upon scaling the coating synthesis process from 3 to
100 g. Based on the results from X-ray photoelectron spectroscopy,
X-ray absorption spectroscopy, and computational modeling, the activity
enhancement was attributed to ensemble effects resulting from partial
TiO2 coverage of the Pd surface rather than fundamental
changes to the Pd electronic structure. Additional durability testing
confirmed that the TiO2 coating improved the thermal and
hydrothermal stability of the catalyst as well as tolerance toward
sulfur impurities in the reactant stream. Using an economic model
of an industrial deep hydrogenation process, we found that an increase
in catalyst activity or lifetime of 2× would justify even a relatively
high estimate for the cost of TiO2 atomic layer deposition
coatings at scale.
Citation for published item:ist¡ evezD v ur nd uxworthD vuke F nd otiropoulosD te nEw r nd hyerD hilip F hyer nd wiqueuD u rinne @PHIRA 9gom ined hp nd experiment l studies of g!g nd g! elimin tion re tions promoted y hel ting phosphine! lkene lig nd X the key role of pent E oordin te dssF9D h lton tr ns tionsFD RQ @PWAF ppF IIITSEIIIUWF Further information on publisher's website:httpXGGdxFdoiForgGIHFIHQWG RdtHHQRH Publisher's copyright statement:
Use policyThe full-text may be used and/or reproduced, and given to third parties in any format or medium, without prior permission or charge, for personal research or study, educational, or not-for-pro t purposes provided that:• a full bibliographic reference is made to the original source • a link is made to the metadata record in DRO • the full-text is not changed in any way The full-text must not be sold in any format or medium without the formal permission of the copyright holders.Please consult the full DRO policy for further details.
scite is a Brooklyn-based organization that helps researchers better discover and understand research articles through Smart Citations–citations that display the context of the citation and describe whether the article provides supporting or contrasting evidence. scite is used by students and researchers from around the world and is funded in part by the National Science Foundation and the National Institute on Drug Abuse of the National Institutes of Health.