Universität zu Köln

Koikolainen, Olga, Sondermann, Linda, Roitsch, Stefan, Simon, Ilka ORCID: 0000-0002-1143-4205, Dietrich, Dennis, Gvilava, Vasily, Barthel, Juri, Thomas, Joerg, Janiak, Christoph and Boldog, Ishtvan (2022). Pd(/Fe3O4)-on-ZIFs: nanoparticle deposition on (nano-)MOFs from ionic liquids. J. Mater. Chem. A, 10 (22). S. 11955 - 11971. CAMBRIDGE: ROYAL SOC CHEMISTRY. ISSN 2050-7496

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Abstract

Well-defined spherical Pd-NPs (similar to 6-12 nm size, 4-17% wt content) were efficiently deposited on nano- or micro- (similar to 100-2500 nm) crystals of zeolite imidazolate frameworks (ZIFs) from different ionic liquids (ILs, typically 1-butyl-3-methylimidazolium bistriflimidate, [BMIm]NTf2) at 180-230 degrees C under microwave (MW) heating for 1-10 min. The firm, nearly exclusive on-surface deposition, proven by systematic analysis of TEM micrographs, is achieved via size-exclusion of the IL-solvated PdCl2 precursor. The one-pot high-quality NP deposition from partially stabilizing IL media leads to particularly well-defined metal nanoparticles-on-metal-organic frameworks, MNP-on-MOF(NP)s. They are contraposed to MNP@MOFs or non-specified MNP/MOFs, and are viewed as an extension of MNPs from ionic liquids, securing MNP-agglomeration protection after removal of the IL and reversible redispersion, and offering the functionality of the porous support. Pd-on-ZIF-8-NP (R = Me substituent of the azole ligand) demonstrated the highest stability and morphological quality, while the ZIF-90 analogues with the same sod topology (R = COOH, CHO, CH2CH2NH2) or the triazolate MAF-66 (R = NH2) with dia topology showed lesser stability (particularly for R = COOH and CHO). Ferromagnetic Pd/Fe3O4- and Fe3O4/Pd-on-ZIF-8-NP, ZIF-90-NH2(-NP), and MAF-66 composites with nanoparticulated Fe3O4 (5-13 nm size, 5-22%(wt) content) demonstrate the feasibility of sequential NP deposition of varied nature. The Pd-on-ZIF composites demonstrated high catalytic activity in the reduction of 4-nitrophenol to 4-aminophenol by NaBH4 in water (TOF 0.38-4.10 vs. 0.088 s(-1) for 10%(wt) Pd/C; amino-functionalization and the presence of Fe3O4 are a major and a minor factor, respectively). The reduction of the same substrate with H-2 in apolar media was much slower for the composite catalysts compared to Pd/C (10%(wt)) due to possible poisoning by the residual IL.

Item Type:	Journal Article
Creators:	Creators Email ORCID ORCID Put Code Koikolainen, Olga UNSPECIFIED UNSPECIFIED UNSPECIFIED Sondermann, Linda UNSPECIFIED UNSPECIFIED UNSPECIFIED Roitsch, Stefan UNSPECIFIED UNSPECIFIED UNSPECIFIED Simon, Ilka UNSPECIFIED orcid.org/0000-0002-1143-4205 UNSPECIFIED Dietrich, Dennis UNSPECIFIED UNSPECIFIED UNSPECIFIED Gvilava, Vasily UNSPECIFIED UNSPECIFIED UNSPECIFIED Barthel, Juri UNSPECIFIED UNSPECIFIED UNSPECIFIED Thomas, Joerg UNSPECIFIED UNSPECIFIED UNSPECIFIED Janiak, Christoph UNSPECIFIED UNSPECIFIED UNSPECIFIED Boldog, Ishtvan UNSPECIFIED UNSPECIFIED UNSPECIFIED
URN:	urn:nbn:de:hbz:38-674813
DOI:	10.1039/d2ta00883a
Journal or Publication Title:	J. Mater. Chem. A
Volume:	10
Number:	22
Page Range:	S. 11955 - 11971
Date:	2022
Publisher:	ROYAL SOC CHEMISTRY
Place of Publication:	CAMBRIDGE
ISSN:	2050-7496
Language:	English
Faculty:	Unspecified
Divisions:	Unspecified
Subjects:	no entry
Uncontrolled Keywords:	Keywords Language METAL-ORGANIC FRAMEWORK; SELECTIVE HYDROGENATION; PD NANOPARTICLES; PALLADIUM NANOPARTICLES; PD-AT-ZIF-8 CATALYSTS; SYNERGISTIC CATALYSIS; ENERGY-STORAGE; ZIF-8; EFFICIENT; PT-AT-ZIF-8 Multiple languages Chemistry, Physical; Energy & Fuels; Materials Science, Multidisciplinary Multiple languages
URI:	http://kups.ub.uni-koeln.de/id/eprint/67481