dc.contributor.author |
Liseev, Timofey |
dc.contributor.author |
Howe, Andrew |
dc.contributor.author |
Hoque, Asmaul |
dc.contributor.author |
Gimbert-Suriñach, Carolina |
dc.contributor.author |
Llobet, Antoni |
dc.contributor.author |
Ott, Sascha |
dc.date.accessioned |
2020-10-20T10:45:17Z |
dc.date.available |
2020-10-20T10:45:17Z |
dc.date.issued |
2020-09-25 |
dc.identifier.uri |
http://hdl.handle.net/2072/377628 |
dc.format.extent |
13753 p. |
dc.language.iso |
eng |
dc.rights |
L'accés als continguts d'aquest document queda condicionat a l'acceptació de les condicions d'ús establertes per la següent llicència Creative Commons:http://creativecommons.org/licenses/by-nc-nd/4.0/ |
dc.source |
RECERCAT (Dipòsit de la Recerca de Catalunya) |
dc.subject.other |
54 |
dc.title |
Synthetic strategies to incorporate Ru-terpyridyl water oxidation catalysts into MOFs: direct synthesis vs. post-synthetic approach |
dc.type |
info:eu-repo/semantics/article |
dc.type |
info:eu-repo/semantics/acceptedVersion |
dc.embargo.terms |
cap |
dc.relation.projectID |
ERC-CoG2015-681895_MOFcat |
dc.relation.projectID |
(Grant agreement ID: 765376) |
dc.identifier.doi |
10.1039/D0DT01890B |
dc.rights.accessLevel |
info:eu-repo/semantics/openAccess |
dc.description.abstract |
Incorporating molecular catalysts into metal–organic frameworks (MOFs) is a promising strategy for
improving their catalytic longevity and recyclability. In this article, we investigate and compare synthetic
routes for the incorporation of the potent water oxidation catalyst Ru(tda)(pyCO2H)2 (tda = 2,2’:6’,2’’-terpyridine-
6,6’’-dicarboxylic acid, pyCO2H = iso-nicotinic acid) as a structural linker into a Zr-based UiOtype
MOF. The task is challenging with this particular metallo-linker because of the equatorial dangling
carboxylates that can potentially compete for Zr-coordination, as well as free rotation of the pyCO2H
groups around the HO2Cpy⋯Ru⋯pyCO2H axis. As a consequence, all attempts to synthesize a MOF with
the metallo-linker directly under solvothermal conditions led to amorphous materials with the Ru(tda)
(pyCO2H)2 linker coordinating to the Zr nodes in ill-defined ways, resulting in multiple waves in the cyclic
voltammograms of the solvothermally obtained materials. On the other hand, an indirect post-synthetic
approach in which the Ru(tda)(pyCO2H)2 linker is introduced into a preformed edba-MOF (edba = ethyne
dibenzoic acid) of UiO topology results in the formation of the desired material. Interestingly, two distinctly
different morphologies of the parent edba-MOF have been discovered, and the impact that the
morphological difference has on linker incorporation is investigated |