Templating metastable Pd 2 carboxylate aggregates

Wang, Chen-Hao; Gao, Wen-Yang; Ma, Qing; Powers, David C.

doi:10.1039/C8SC04940H

Title: Templating metastable Pd ₂ carboxylate aggregates

Journal Article · Wed Feb 06 00:00:00 EST 2019 · Chemical Science

DOI:https://doi.org/10.1039/C8SC04940H· OSTI ID:1485518

^[1];

^[1]; Ma, Qing ^[2];

^[1]

Texas A&M University, Department of Chemistry, College Station, USA
DND-CAT, Northwestern Synchrotron Research Centre at the Advanced Photon Source, Argonne, USA

Evaluation of the potential for metal–metal (M–M) cooperation to enable catalysis requires access to specific polynuclear aggregates that display appropriate geometry and size. In many cases, exerting synthetic control over the aggregation of simple metal salts is a challenge. For example, Pd(II) acetate self assembles as a trimer (i.e. Pd₃(OAc)₆) both in the solid state and in solution and does not feature close Pd–Pd interactions. Related carboxylate-supported Pd2 aggregates (i.e. Pd₂(OAc)₄), which would feature close Pd–Pd interactions, are thermodynamically metastable in solution phase and thus largely unavailable. Here we demonstrate ion metathesis within pre-formed metal–organic frameworks (MOFs) to prepare metastable Pd₂ tetracarboxylates sites. The newly synthesized materials are characterized by elemental analysis, PXRD, SCXRD, EXAFS, XANES, and gas adsorption analysis. In addition, the critical role of network solvation on the kinetics of ion metathesis was revealed by coupled TGA-MS and ICP-MS experiments. The demonstration of templated ion metathesis to generate specific metastable coordination sites that are inaccessible in solution phase chemistry represents a new opportunity to interrogate the chemistry of specific polynuclear metal aggregates.

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Research Organization:: Argonne National Lab. (ANL), Argonne, IL (United States). Advanced Photon Source (APS)

Sponsoring Organization:: USDOE Office of Science (SC); National Science Foundation (NSF); Welch Foundation

Grant/Contract Number:: SC0018977; AC02-06CH11357; CHE-1346572; A-1907

OSTI ID:: 1485518

Alternate ID(s):: OSTI ID: 1497104

Journal Information:: Chemical Science, Journal Name: Chemical Science Vol. 10 Journal Issue: 6; ISSN 2041-6520

Publisher:: Royal Society of Chemistry (RSC)Copyright Statement

Country of Publication:: United Kingdom

Language:: English

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Cited by: 10 works

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1,3,5,7-Tetrakis(tetrazol-5-yl)-adamantane: the smallest tetrahedral tetrazole-functionalized ligand and its complexes formed by reaction with anhydrous M( ii )Cl ₂ (M = Mn, Cu, Zn, Cd) Boldog, Ishtvan; Domasevitch, Konstantin V.; Sanchiz, Joaquín Dalton Trans., Vol. 43, Issue 33 https://doi.org/10.1039/C4DT01022A	journal	January 2014

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