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Investigation of the Deactivation and Reactivation Mechanism of a Heterogeneous Palladium(II) Catalyst in the Cycloisomerization of Acetylenic Acids by In Situ XAS

Yuan, Ning and Gudmundsson, Arnar and Gustafson, Karl P. J. and Oschmann, Michael and Tai, Cheuk-Wai and Persson, Ingmar and Zou, Xiaodong and Verho, Oscar and Bajnóczi, Eva and Backvall, Jan-E (2021). Investigation of the Deactivation and Reactivation Mechanism of a Heterogeneous Palladium(II) Catalyst in the Cycloisomerization of Acetylenic Acids by In Situ XAS. ACS Catalysis. 11 , 2999-3008
[Research article]

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Abstract

A well-studied heterogeneous palladium(II) catalyst used for the cycloisomerization of acetylenic acids is known to be susceptible to deactivation through reduction. To gain a deeper understanding of this deactivation process and to enable the design of a reactivation strategy, in situ X-ray absorption spectroscopy (XAS) was used. With this technique, changes in the palladium oxidation state and coordination environment could be studied in close detail, which provided experimental evidence that the deactivation was primarily caused by triethylamine-promoted reduction of palladium(II) to metallic palladium nanoparticles. Furthermore, it was observed that the choice of the acetylenic acid substrate influenced the distribution between palladium(II) and palladium(0) species in the heterogeneous catalyst after the reaction. From the mechanistic insight gained through XAS, an improved catalytic protocol was developed that did not suffer from deactivation and allowed for more efficient recycling of the catalyst.

Authors/Creators:Yuan, Ning and Gudmundsson, Arnar and Gustafson, Karl P. J. and Oschmann, Michael and Tai, Cheuk-Wai and Persson, Ingmar and Zou, Xiaodong and Verho, Oscar and Bajnóczi, Eva and Backvall, Jan-E
Title:Investigation of the Deactivation and Reactivation Mechanism of a Heterogeneous Palladium(II) Catalyst in the Cycloisomerization of Acetylenic Acids by In Situ XAS
Series Name/Journal:ACS Catalysis
Year of publishing :2021
Volume:11
Page range:2999-3008
Number of Pages:10
Publisher:AMER CHEMICAL SOC
Language:English
Publication Type:Research article
Article category:Scientific peer reviewed
Version:Published version
Copyright:Creative Commons: Attribution 4.0
Full Text Status:Public
Subjects:(A) Swedish standard research categories 2011 > 1 Natural sciences > 104 Chemical Sciences > Physical Chemistry
Keywords:X-ray absorption spectroscopy, cycloisomerization, deactivation/reactivation, heterogeneous, palladium catalysis
URN:NBN:urn:nbn:se:slu:epsilon-p-111516
Permanent URL:
http://urn.kb.se/resolve?urn=urn:nbn:se:slu:epsilon-p-111516
Additional ID:
Type of IDID
DOI10.1021/acscatal.0c04374
Web of Science (WoS)000626844200049
ID Code:23299
Faculty:NJ - Fakulteten för naturresurser och jordbruksvetenskap
Department:(NL, NJ) > Department of Molecular Sciences
Deposited By: SLUpub Connector
Deposited On:19 Apr 2021 14:04
Metadata Last Modified:19 Apr 2021 14:11

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