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A functionalized Hf(IV)–organic framework introducing an efficient, recyclable, and size-selective heterogeneous catalyst for MPV reduction.
- Source :
- New Journal of Chemistry; 3/21/2023, Vol. 47 Issue 11, p5347-5355, 9p
- Publication Year :
- 2023
-
Abstract
- UiO-66 (UiO = University of Oslo) metal–organic frameworks (MOFs) exhibit high thermal and chemical stability, large surface area, and defined pore shape and size. On the other hand, Meerwein–Ponndorf–Verley (MPV) reduction is a selective hydrogenation reaction of carbonyl group through hydrogen transfer between ketones (aldehydes) and alcohols. Herein, in this work, a Hf(IV)-based UiO-66 MOF called CSMCRI-KNC (CSMCRI-KNC = Central Salt and Marine Chemicals Research Institute-Krishnath College) was synthesized using a 2-((2-hydroxy-4-methoxy-benzyl)amino) terephthalic acid linker via the solvothermal procedure. The guest-free form of CSMCRI-KNC (called CSMCRI-KNC′) was successfully employed as a reusable heterogeneous catalyst for the hydrogen-transfer reaction between carbonyl compounds and alcohol (isopropanol). The catalyst showed a high yield, high conversion, broad substrate scope, and high stability on the MPV reduction reaction. Interestingly, the catalyst was size-selective too. The catalytic performance of CSMCRI-KNC′ was compared with its Zr analog, UiO-66-NH<subscript>2</subscript>(Hf), UiO-66-NH<subscript>2</subscript>(Zr), UiO-66(Hf), and UiO-66(Zr). Interestingly, our developed catalyst showed much better activity compared to the others. The systematized research discovered that the excellent performance of CSMCRI-KNC′ predominantly originated from the more positively charged Hf(IV) species of [Hf<subscript>6</subscript>(OH)<subscript>4</subscript>(O)<subscript>4</subscript>]<superscript>12+</superscript>, which could boost the activation of the carbonyl group and instantaneously endorse the hydrogen-transfer process assisted by the available basic sites on CSMCRI-KNC′. The incorporation of the functional group also contributed to the excellent catalytic performance of CSMCRI-KNC′. Notably, the preparation of CSMCRI-KNC′ avoided the utilization of an expensive organic linker, and the prepared CSMCRI-KNC′ showed superior or similar catalytic activity than most reported Zr/Hf-containing catalysts, meaningfully empowering it to be a more practical option in the field of catalysis, and hydrogen transfer reactions. [ABSTRACT FROM AUTHOR]
Details
- Language :
- English
- ISSN :
- 11440546
- Volume :
- 47
- Issue :
- 11
- Database :
- Complementary Index
- Journal :
- New Journal of Chemistry
- Publication Type :
- Academic Journal
- Accession number :
- 162379474
- Full Text :
- https://doi.org/10.1039/d2nj06066c