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In Situ X‐ray Absorption Spectroscopy to Study the Dehydrogenation and Decomposition Mechanisms of an Iridium Pincer Catalyst Exposed to Gaseous Isopropanol

Eriksson, Axl LU ; Subramaniyan, Vasudevan LU ; Kawde, Anurag LU ; Nordlander, Jonas Elmroth LU ; Just, Justus LU orcid ; Blomberg, Sara LU ; Wendt, Ola F. LU and Uhlig, Jens LU (2025) In ChemCatChem
Abstract
On-site hydrogen gas production from hydrogen-rich liquids offers a clean alternative to fossil fuels for combustion that is readily implemented in existing energy infrastructure. A heterogenized (POCOP)-Ir pincer catalyst can be operated at higher temperatures for higher turnover frequency, but the reaction pathway of the reported complex has not been well understood. Here, we report intermediary states and propose a reaction mechanism for the catalyzed dehydrogenation of isopropanol by in situ X-ray absorption spectroscopy at elevated temperatures. We identify that the catalytic resting states have the same oxidation state (+1), an insignificance of catalyst poisoning by CO contaminants, and the heat-induced deactivation pathway... (More)
On-site hydrogen gas production from hydrogen-rich liquids offers a clean alternative to fossil fuels for combustion that is readily implemented in existing energy infrastructure. A heterogenized (POCOP)-Ir pincer catalyst can be operated at higher temperatures for higher turnover frequency, but the reaction pathway of the reported complex has not been well understood. Here, we report intermediary states and propose a reaction mechanism for the catalyzed dehydrogenation of isopropanol by in situ X-ray absorption spectroscopy at elevated temperatures. We identify that the catalytic resting states have the same oxidation state (+1), an insignificance of catalyst poisoning by CO contaminants, and the heat-induced deactivation pathway resulting in Ir nanoparticles leached from the complex. (Less)
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author
; ; ; ; ; ; and
organization
publishing date
type
Contribution to journal
publication status
epub
subject
in
ChemCatChem
publisher
Wiley-VCH Verlag
external identifiers
  • scopus:105004213820
ISSN
1867-3880
DOI
10.1002/cctc.202500284
language
English
LU publication?
yes
id
c4af4ed5-8ff7-4dbc-a4d2-4092b012d6aa
date added to LUP
2025-05-15 12:43:04
date last changed
2025-05-21 09:34:55
@article{c4af4ed5-8ff7-4dbc-a4d2-4092b012d6aa,
  abstract     = {{On-site hydrogen gas production from hydrogen-rich liquids offers a clean alternative to fossil fuels for combustion that is readily implemented in existing energy infrastructure. A heterogenized (POCOP)-Ir pincer catalyst can be operated at higher temperatures for higher turnover frequency, but the reaction pathway of the reported complex has not been well understood. Here, we report intermediary states and propose a reaction mechanism for the catalyzed dehydrogenation of isopropanol by in situ X-ray absorption spectroscopy at elevated temperatures. We identify that the catalytic resting states have the same oxidation state (+1), an insignificance of catalyst poisoning by CO contaminants, and the heat-induced deactivation pathway resulting in Ir nanoparticles leached from the complex.}},
  author       = {{Eriksson, Axl and Subramaniyan, Vasudevan and Kawde, Anurag and Nordlander, Jonas Elmroth and Just, Justus and Blomberg, Sara and Wendt, Ola F. and Uhlig, Jens}},
  issn         = {{1867-3880}},
  language     = {{eng}},
  publisher    = {{Wiley-VCH Verlag}},
  series       = {{ChemCatChem}},
  title        = {{In Situ X‐ray Absorption Spectroscopy to Study the Dehydrogenation and Decomposition Mechanisms of an Iridium Pincer Catalyst Exposed to Gaseous Isopropanol}},
  url          = {{http://dx.doi.org/10.1002/cctc.202500284}},
  doi          = {{10.1002/cctc.202500284}},
  year         = {{2025}},
}