Developing and understanding Leaching-Resistant cobalt nanoparticles via N/P incorporation for liquid phase hydroformylation

Galdeano-Ruano, Carmen, Gutiérrez-Tarriño, Silvia, Lopes, Christian W., Mazarío, Jaime, Chinchilla, Lidia E., Agostini, Giovanni, Calvino, Jose J., Holgado, Juan P., Rodríguez-Castellón, Enrique, Roldan, Alberto ORCID: https://orcid.org/0000-0003-0353-9004 and Oña-Burgos, Pascual 2024. Developing and understanding Leaching-Resistant cobalt nanoparticles via N/P incorporation for liquid phase hydroformylation. Journal of Catalysis 431 , 115374. 10.1016/j.jcat.2024.115374

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Abstract

The ultimate target in heterogeneous catalysis is the achievement of robust, resilient and highly efficient materials capable of resisting industrial reaction conditions. Pursuing that goal in liquid-phase hydroformylation poses a unique challenge due to carbon monoxide-induced metal carbonyl species formation, which is directly related to the formation of active homogeneous catalysts by metal leaching. Herein, supported heteroatom-incorporated (P and N) Co nanoparticles were developed to enhance the resistance compared with bare Co nanoparticles. The samples underwent characterization using operando XPS, XAS and HR electron microscopy. Overall, P- and N-doped catalysts increased reusability and suppressed leaching. Among the studied catalysts, the one with N as a dopant, CoNx@NC, presents excellent catalytic results for a Co-based catalyst, with a 94% conversion and a selectivity to aldehydes of 80% in only 7.5 h. Even under milder conditions, this catalyst outperformed existing benchmarks in Turnover Numbers (TON) and productivity. In addition, computational simulations provided atomistic insights, shedding light on the remarkable resistance of small Co clusters interacting with N-doped carbon patches.

Item Type:	Article
Date Type:	Publication
Status:	Published
Schools:	Chemistry Cardiff Catalysis Institute (CCI)
Publisher:	Elsevier
ISSN:	0021-9517
Date of First Compliant Deposit:	15 March 2024
Date of Acceptance:	15 February 2024
Last Modified:	19 Mar 2024 15:00
URI:	https://orca.cardiff.ac.uk/id/eprint/167292

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