One-Pot Intercalation Strategy for the Encapsulation of a CO-Releasing Organometallic Molecule in a Layered Double Hydroxide

authors	Calhau, IB; Gomes, AC; Bruno, SM; Coelho, AC; Magalhaes, CIR; Romao, CC; Valente, AA; Goncalves, IS; Pillinger, M
nationality	International
journal	EUROPEAN JOURNAL OF INORGANIC CHEMISTRY
author keywords	Molybdenum; Carbon monoxide; Isocyanide ligands; Drug delivery; Layered compounds
keywords	CARBON-MONOXIDE; NANOPARTICLES; DELIVERY; COMPLEX; OXIDE; EXCHANGE; CARRIERS; DESIGN
abstract	The photoactivatable CO-releasing molecule (photoCORM) [Mo(CO)(3)(CNCH2COOH)(3)] (ALF795) has been incorporated into a Zn,Al layered double hydroxide (LDH) host by a coprecipitation synthesis strategy. Powder X-ray diffraction (PXRD) of the resultant material Zn,Al-ALF795 showed that the ALF795 guest molecules assembled into a monolayer to give a basal spacing of 16.0 angstrom. FTIR and(13)C{H-1} CP MAS NMR spectroscopy confirmed that the molecular structure of the tricarbonyl complex was retained upon intercalation. Scanning electron microscopy (SEM), energy-dispersive X-ray spectroscopy (EDS) and elemental analyses confirmed the phase-purity of Zn,Al-ALF795. The myoglobin assay was used to demonstrate that intercalated ALF795 retains the photoactive behavior of the free CORM, with a substantial fraction (42 %) of the high CO payload (2.46 mmol g(-1)) being released after exposure to UV light for 3 h under simulated physiological conditions. In addition, gas chromatography was used to track sequential light- and H2O2-triggered decarbonylation of free and intercalated ALF795. In biological buffer solution (HEPES), less than 2 % Mo leaching from Zn,Al-ALF795 took place after 5 h, showing the strong capacity of the LDH host to retain the unaltered complex and decarbonylation fragments.
publisher	WILEY-V C H VERLAG GMBH
issn	1434-1948
isbn	1099-0682
year published	2020
volume	2020
issue	28
beginning page	2726
ending page	2736
digital object identifier (doi)	10.1002/ejic.202000202
web of science category	Chemistry, Inorganic & Nuclear
subject category	Chemistry
unique article identifier	WOS:000548603500001